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{"ref": "#/texts/9", "page": 1, "label": "text", "order": 9000, "source_page_order": 11, "layout_order": 8, "layout_page_order": 9, "bbox": [60.49, 291.3, 316.21, 130.86], "page_size": {"width": 625.44, "height": 818.36}, "text": "ABSTRACT: Though Li2MnO3 was originally considered to be electrochemically inert, its observed activation has spawned a new class of Li-rich layered compounds that deliver capacities beyond the traditional transition-metal redox limit. Despite progress in our understanding of oxygen redox in Li-rich compounds, the underlying origin of the initial charge capacity of Li2MnO3 remains hotly contested. To resolve this issue, we review all possible charge compensation mechanisms including bulk oxygen redox, oxidation of Mn 4+ , and surface degradation for Li2MnO3 cathodes displaying capacities exceeding 350 mAh g -1 . Using elemental and orbital selective X-ray spectroscopy techniques, we rule out oxidation of Mn 4+ and bulk oxygen redox during activation of Li2MnO3. Quantitative gas-evolution and titration studies reveal that O2 and CO2 release accounted for a large fraction of the observed capacity", "text_preview": "ABSTRACT: Though Li2MnO3 was originally considered to be electrochemically inert, its observed activation has spawned a new class of Li-rich layered compounds that deliver capacities beyond the traditional transition-me…", "word_count": 132, "cleaned_text": "ABSTRACT: Though Li2MnO3 was originally considered to be electrochemically inert, its observed activation has spawned a new class of Li-rich layered compounds that deliver capacities beyond the traditional transition-metal redox limit. Despite progress in our understanding of oxygen redox in Li-rich compounds, the underlying origin of the initial charge capacity of Li2MnO3 remains hotly contested. To resolve this issue, we review all possible charge compensation mechanisms including bulk oxygen redox, oxidation of Mn 4+ , and surface degradation for Li2MnO3 cathodes displaying capacities exceeding 350 mAh g -1 . Using elemental and orbital selective X-ray spectroscopy techniques, we rule out oxidation of Mn 4+ and bulk oxygen redox during activation of Li2MnO3. Quantitative gas-evolution and titration studies reveal that O2 and CO2 release accounted for a large fraction of the observed capacity", "cleaned_text_preview": "ABSTRACT: Though Li2MnO3 was originally considered to be electrochemically inert, its observed activation has spawned a new class of Li-rich layered compounds that deliver capacities beyond the traditional transition-me…", "included_in_body": false, "body_decision_reason": "inline_abstract", "parser_body_decision_reason": "inline_abstract", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p1:body_region:0", "role_guess": "abstract_candidate", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [244, 244, 245], "page_background_rgb": [255, 255, 255], "background_delta": 11, "background_class": "gray", "is_gray_background": true, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.096, "bottom": 0.032, "left": 0.0, "right": 0.077}, "excluded_risk_level": "medium", "region_id": "p1:page_body:column_1_of_2:gray", "truncation_marker": ""}
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{"ref": "#/texts/14", "page": 1, "label": "text", "order": 14000, "source_page_order": 16, "layout_order": 15, "layout_page_order": 16, "bbox": [60.49, 423.34, 504.01, 30.63], "page_size": {"width": 625.44, "height": 818.36}, "text": "during activation with minor contributions from reduced Mn species on the surface. These studies reveal that, although Li2 MnO3 is considered critical for promoting bulk anionic redox in Li-rich layered oxides, Li2MnO3 by itself does not exhibit bulk oxygen redox or manganese oxidation beyond its initial Mn 4+ valence.", "text_preview": "during activation with minor contributions from reduced Mn species on the surface. These studies reveal that, although Li2 MnO3 is considered critical for promoting bulk anionic redox in Li-rich layered oxides, Li2MnO3 …", "word_count": 49, "cleaned_text": "during activation with minor contributions from reduced Mn species on the surface. These studies reveal that, although Li2 MnO3 is considered critical for promoting bulk anionic redox in Li-rich layered oxides, Li2MnO3 by itself does not exhibit bulk oxygen redox or manganese oxidation beyond its initial Mn 4+ valence.", "cleaned_text_preview": "during activation with minor contributions from reduced Mn species on the surface. These studies reveal that, although Li2 MnO3 is considered critical for promoting bulk anionic redox in Li-rich layered oxides, Li2MnO3 …", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p1:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [244, 244, 245], "page_background_rgb": [255, 255, 255], "background_delta": 11, "background_class": "gray", "is_gray_background": true, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.057, "bottom": 0.01, "left": 0.125, "right": 0.062}, "excluded_risk_level": "high", "region_id": "p1:page_body:column_1_of_2:gray", "truncation_marker": ""}
{"ref": "#/texts/15", "page": 1, "label": "text", "order": 15000, "source_page_order": 17, "layout_order": 16, "layout_page_order": 17, "bbox": [60.49, 477.74, 240.01, 279.62], "page_size": {"width": 625.44, "height": 818.36}, "text": "O riginally considered electrochemically inactive, 1 Li2MnO3 can deliver substantial capacity during charge, as demonstrated by Kalyani et al. 2 Later, Robertson and Bruce 3 revealed how Li2MnO3 could be activated through the use of nanosized particles. Indeed, capacities exceeding 300 mAh g -1 have been reported during the fi rst charge activation of Li2MnO3. 3 -10 The large irreversible capacity observed during the fi rst charge is primarily attributed to irreversible oxygen release, 11 -16 which presumably activates lattice oxygen redox along with other degradation mechanisms, ultimately leading to severe capacity fade upon cycling. 3,4,6,7,17 Li-rich layered oxides (LR-NMC), derived from Li2MnO3 are often regarded as nanocomposites of Li2MnO3 and LiMO2 (M = Ni, Mn, Co) components and exhibit a similar fi rst charge activation plateau at 4.5 V vs Li/ Li + . 11,18 -21 In fact, a direct correlation observed between the 4.5 V plateau capacity and Li2MnO3 content of LR-NMC 22 has been used to quantify the extent of bulk oxygen redox in LRNMCs. 23 Unlike Li2MnO3, LR-NMCs maintain stable cycling performance with high reversible capacities. 24,25 Meanwhile, lattice oxygen redox in LR-NMCs has been supported by numerous O K-edge resonant inelastic X-ray scattering (RIXS) studies, 26 -28 with the recent beam exposure studies con fi rming that the RIXS feature is intrinsic to oxidized lattice oxygen. 29", "text_preview": "O riginally considered electrochemically inactive, 1 Li2MnO3 can deliver substantial capacity during charge, as demonstrated by Kalyani et al. 2 Later, Robertson and Bruce 3 revealed how Li2MnO3 could be activated throu…", "word_count": 222, "cleaned_text": "O riginally considered electrochemically inactive, 1 Li2MnO3 can deliver substantial capacity during charge, as demonstrated by Kalyani et al. 2 Later, Robertson and Bruce 3 revealed how Li2MnO3 could be activated through the use of nanosized particles. Indeed, capacities exceeding 300 mAh g -1 have been reported during the fi rst charge activation of Li2MnO3. 3 -10 The large irreversible capacity observed during the fi rst charge is primarily attributed to irreversible oxygen release, 11 -16 which presumably activates lattice oxygen redox along with other degradation mechanisms, ultimately leading to severe capacity fade upon cycling. 3,4,6,7,17 Li-rich layered oxides (LR-NMC), derived from Li2MnO3 are often regarded as nanocomposites of Li2MnO3 and LiMO2 (M = Ni, Mn, Co) components and exhibit a similar fi rst charge activation plateau at 4.5 V vs Li/ Li + . 11,18 -21 In fact, a direct correlation observed between the 4.5 V plateau capacity and Li2MnO3 content of LR-NMC 22 has been used to quantify the extent of bulk oxygen redox in LRNMCs. 23 Unlike Li2MnO3, LR-NMCs maintain stable cycling performance with high reversible capacities. 24,25 Meanwhile, lattice oxygen redox in LR-NMCs has been supported by numerous O K-edge resonant inelastic X-ray scattering (RIXS) studies, 26 -28 with the recent beam exposure studies con fi rming that the RIXS feature is intrinsic to oxidized lattice oxygen. 29", "cleaned_text_preview": "O riginally considered electrochemically inactive, 1 Li2MnO3 can deliver substantial capacity during charge, as demonstrated by Kalyani et al. 2 Later, Robertson and Bruce 3 revealed how Li2MnO3 could be activated throu…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p1:body_region:0", "role_guess": "body_candidate_excluded", "zone": "bottom_margin", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.0, "bottom": 0.005, "left": 0.0, "right": 0.0}, "excluded_risk_level": "high", "region_id": "p1:bottom_margin:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/16", "page": 1, "label": "text", "order": 16000, "source_page_order": 18, "layout_order": 17, "layout_page_order": 18, "bbox": [324.45, 479.72, 240.07, 208.53], "page_size": {"width": 625.44, "height": 818.36}, "text": "While Li2MnO3 is regarded as a model compound for describing bulk oxygen redox activity in LR-NMCs, recent RIXS studies did not detect similar spectroscopic signatures of oxidized lattice oxygen in Li2MnO3. 30 Additionally, an alternative scenario explaining the origin of anomalous capacity in LR-NMCs has been proposed by Radin et al. 23 According to this new perspective based on fi rst-principle calculations, the reversible formation of molecular oxygen or peroxide ions in combination with Mn 4+ /Mn 7+ redox could explain the characteristic electrochemical behavior of LR-NMCs. Meanwhile, the appearance of O K-edge RIXS feature for numerous conventional Mn-free layered oxides questions the role of Li2MnO3 in activating lattice oxygen redox in LR-NMCs. 31,32 Understanding the underlying charge compensation mechanism in Li 2 MnO3 is critical for progressing the development of LR-NMCs. This requires answering two fundamental questions: (1) should Li2MnO3 be regarded as a model compound describing anionic redox activity and (2) are there any", "text_preview": "While Li2MnO3 is regarded as a model compound for describing bulk oxygen redox activity in LR-NMCs, recent RIXS studies did not detect similar spectroscopic signatures of oxidized lattice oxygen in Li2MnO3. 30 Additiona…", "word_count": 156, "cleaned_text": "While Li2MnO3 is regarded as a model compound for describing bulk oxygen redox activity in LR-NMCs, recent RIXS studies did not detect similar spectroscopic signatures of oxidized lattice oxygen in Li2MnO3. 30 Additionally, an alternative scenario explaining the origin of anomalous capacity in LR-NMCs has been proposed by Radin et al. 23 According to this new perspective based on fi rst-principle calculations, the reversible formation of molecular oxygen or peroxide ions in combination with Mn 4+ /Mn 7+ redox could explain the characteristic electrochemical behavior of LR-NMCs. Meanwhile, the appearance of O K-edge RIXS feature for numerous conventional Mn-free layered oxides questions the role of Li2MnO3 in activating lattice oxygen redox in LR-NMCs. 31,32 Understanding the underlying charge compensation mechanism in Li 2 MnO3 is critical for progressing the development of LR-NMCs. This requires answering two fundamental questions: (1) should Li2MnO3 be regarded as a model compound describing anionic redox activity and (2) are there any", "cleaned_text_preview": "While Li2MnO3 is regarded as a model compound for describing bulk oxygen redox activity in LR-NMCs, recent RIXS studies did not detect similar spectroscopic signatures of oxidized lattice oxygen in Li2MnO3. 30 Additiona…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p1:body_region:1", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.035, "bottom": 0.015, "left": 0.154, "right": 0.09}, "excluded_risk_level": "high", "region_id": "p1:page_body:column_2_of_2:white", "truncation_marker": ""}
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{"ref": "#/texts/29", "page": 2, "label": "caption", "order": 29000, "source_page_order": 4, "layout_order": 30, "layout_page_order": 4, "bbox": [60.49, 412.0, 503.99, 17.75], "page_size": {"width": 625.44, "height": 818.36}, "text": "Figure 1. Structure and electrochemistry of Li2MnO3. (a) XRD pattern and (b) SEM image showing particles morphology of Li2MnO3 synthesized at 600 ◦ C. The fi rst cycle voltage pro fi les and subsequent cycling performance are shown in (c) and (d), respectively.", "text_preview": "Figure 1. Structure and electrochemistry of Li2MnO3. (a) XRD pattern and (b) SEM image showing particles morphology of Li2MnO3 synthesized at 600 ◦ C. The fi rst cycle voltage pro fi les and subsequent cycling performan…", "word_count": 43, "cleaned_text": "Figure 1. Structure and electrochemistry of Li2MnO3. (a) XRD pattern and (b) SEM image showing particles morphology of Li2MnO3 synthesized at 600 ◦ C. The fi rst cycle voltage pro fi les and subsequent cycling performance are shown in (c) and (d), respectively.", "cleaned_text_preview": "Figure 1. Structure and electrochemistry of Li2MnO3. (a) XRD pattern and (b) SEM image showing particles morphology of Li2MnO3 synthesized at 600 ◦ C. The fi rst cycle voltage pro fi les and subsequent cycling performan…", "included_in_body": false, "body_decision_reason": "outside_body_flow_caption", "parser_body_decision_reason": "outside_body_flow_caption", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": false, "body_region_id": null, "role_guess": "caption", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.122, "bottom": 0.022, "left": 0.115, "right": 0.064}, "excluded_risk_level": "low", "region_id": "p2:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/30", "page": 2, "label": "text", "order": 30000, "source_page_order": 5, "layout_order": 31, "layout_page_order": 5, "bbox": [60.49, 442.75, 239.96, 19.97], "page_size": {"width": 625.44, "height": 818.36}, "text": "alternative charge compensation mechanisms that could explain the electrochemical activity of Li2MnO3?", "text_preview": "alternative charge compensation mechanisms that could explain the electrochemical activity of Li2MnO3?", "word_count": 12, "cleaned_text": "alternative charge compensation mechanisms that could explain the electrochemical activity of Li2MnO3?", "cleaned_text_preview": "alternative charge compensation mechanisms that could explain the electrochemical activity of Li2MnO3?", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p2:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.02, "bottom": 0.007, "left": 0.089, "right": 0.111}, "excluded_risk_level": "high", "region_id": "p2:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/31", "page": 2, "label": "text", "order": 31000, "source_page_order": 6, "layout_order": 32, "layout_page_order": 6, "bbox": [60.49, 464.98, 240.0, 220.33], "page_size": {"width": 625.44, "height": 818.36}, "text": "To resolve these issues, we considered all possible charge compensation mechanisms including bulk oxygen redox, Mn 4+ /Mn 7+ redox, and surface degradation. Our investigation employed a combination of techniques sensitive to oxygen oxidation (O K-edge RIXS) Mn oxidation (operando Mn Kedge X-ray absorption spectroscopy (XAS)) and gas evolution (di ff erential electrochemical mass spectroscopy (DEMS)). No signi fi cant evidence of Mn 7+ and/or oxidized lattice oxygen were observed by X-ray spectroscopy. Quantitative analysis of the measured gas evolution almost entirely accounted for the observed capacity during the fi rst charge activation, with minor contributions from lattice oxygen redox, carbonate decomposition, and oxidation of reduced Mn species on the surface. Despite being considered critical for understanding bulk oxygen redox activity in LR-NMCs, the parent Li 2 MnO3 itself does not exhibit this exotic charge compensation mechanism. Instead, irreversible oxygen release during activation likely paves the way for other degradation mechanisms, e.g., Mn migration, which will be addressed separately in our future study.", "text_preview": "To resolve these issues, we considered all possible charge compensation mechanisms including bulk oxygen redox, Mn 4+ /Mn 7+ redox, and surface degradation. Our investigation employed a combination of techniques sensiti…", "word_count": 163, "cleaned_text": "To resolve these issues, we considered all possible charge compensation mechanisms including bulk oxygen redox, Mn 4+ /Mn 7+ redox, and surface degradation. Our investigation employed a combination of techniques sensitive to oxygen oxidation (O K-edge RIXS) Mn oxidation (operando Mn Kedge X-ray absorption spectroscopy (XAS)) and gas evolution (di ff erential electrochemical mass spectroscopy (DEMS)). No signi fi cant evidence of Mn 7+ and/or oxidized lattice oxygen were observed by X-ray spectroscopy. Quantitative analysis of the measured gas evolution almost entirely accounted for the observed capacity during the fi rst charge activation, with minor contributions from lattice oxygen redox, carbonate decomposition, and oxidation of reduced Mn species on the surface. Despite being considered critical for understanding bulk oxygen redox activity in LR-NMCs, the parent Li 2 MnO3 itself does not exhibit this exotic charge compensation mechanism. Instead, irreversible oxygen release during activation likely paves the way for other degradation mechanisms, e.g., Mn migration, which will be addressed separately in our future study.", "cleaned_text_preview": "To resolve these issues, we considered all possible charge compensation mechanisms including bulk oxygen redox, Mn 4+ /Mn 7+ redox, and surface degradation. Our investigation employed a combination of techniques sensiti…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p2:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.024, "bottom": 0.0, "left": 0.09, "right": 0.103}, "excluded_risk_level": "high", "region_id": "p2:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/32", "page": 2, "label": "text", "order": 32000, "source_page_order": 7, "layout_order": 33, "layout_page_order": 7, "bbox": [60.49, 687.55, 240.01, 75.64], "page_size": {"width": 625.44, "height": 818.36}, "text": "Figure 1a shows the XRD pattern of the as-synthesized material, where all re fl ections can be indexed in the monoclinic system with the space group C 2/ m . 33 In the layered structure of Li 2 MnO3, the interslab octahedral sites are occupied by Li + only, while the octahedral sites within the [Li1/3Mn2/3]O2 slabs are ordered with Li + and Mn 4+ in a ratio of 1:2, which is indicated by the superlattice re fl ections in the 2 θ range from", "text_preview": "Figure 1a shows the XRD pattern of the as-synthesized material, where all re fl ections can be indexed in the monoclinic system with the space group C 2/ m . 33 In the layered structure of Li 2 MnO3, the interslab octah…", "word_count": 85, "cleaned_text": "Figure 1a shows the XRD pattern of the as-synthesized material, where all re fl ections can be indexed in the monoclinic system with the space group C 2/ m . 33 In the layered structure of Li 2 MnO3, the interslab octahedral sites are occupied by Li + only, while the octahedral sites within the [Li1/3Mn2/3]O2 slabs are ordered with Li + and Mn 4+ in a ratio of 1:2, which is indicated by the superlattice re fl ections in the 2 θ range from", "cleaned_text_preview": "Figure 1a shows the XRD pattern of the as-synthesized material, where all re fl ections can be indexed in the monoclinic system with the space group C 2/ m . 33 In the layered structure of Li 2 MnO3, the interslab octah…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p2:body_region:0", "role_guess": "body_candidate_excluded", "zone": "bottom_margin", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.049, "bottom": 0.016, "left": 0.051, "right": 0.115}, "excluded_risk_level": "high", "region_id": "p2:bottom_margin:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/33", "page": 2, "label": "text", "order": 33000, "source_page_order": 8, "layout_order": 34, "layout_page_order": 8, "bbox": [324.45, 439.45, 240.05, 301.52], "page_size": {"width": 625.44, "height": 818.36}, "text": "20 to 34 ° . However, these superlattice re fl ections appear convoluted into a broad asymmetric peak as shown in Figure 1a. Previously, the intensity and asymmetry of these superlattice re fl ections are correlated with the degree of disorder in the stacking sequence of [Li1/3Mn2/3]O2 slabs along the c -direction of the monoclinic lattice. 34 Moreover, the SEM micrograph of the as-synthesized material in Figure 1b reveals the agglomerated primary particles of less than 100 nm in size. Thus, the observed asymmetric superlattice re fl ection in the XRD pattern con fi rms an increased degree of stacking faults in the nanocrystalline Li 2 MnO3 synthesized in the present study. Figure 1c demonstrates the voltage pro fi le of Li2MnO3 in the fi rst cycle at a rate of C/50 (1 C = 230 mA g -1 assumed), while subsequent cycling was performed at C/10. The large irreversible capacity observed during activation, which results in poor Coulombic e ffi ciency of the fi rst cycle, is a characteristic electrochemical feature of Li2MnO3. Although cycling performance of Li2MnO3 shown in Figure 1d reveals improved Coulombic e ffi ciency for the subsequent cycles, continued degradation leads to signi fi cant loss of capacity upon cycling. In other words, the fi rst cycle activation processes likely persist in subsequent cycles but to a much lesser extent. The general consensus in literature is that the fi rst cycle irreversibility in Li2MnO3 is due to an irreversible oxygen release. 11 -15 Our cycling data indicate that Li2MnO3 continues to degas during subsequent cycles, but to a much lesser extent than in the fi rst cycle.", "text_preview": "20 to 34 ° . However, these superlattice re fl ections appear convoluted into a broad asymmetric peak as shown in Figure 1a. Previously, the intensity and asymmetry of these superlattice re fl ections are correlated wit…", "word_count": 272, "cleaned_text": "20 to 34 ° . However, these superlattice re fl ections appear convoluted into a broad asymmetric peak as shown in Figure 1a. Previously, the intensity and asymmetry of these superlattice re fl ections are correlated with the degree of disorder in the stacking sequence of [Li1/3Mn2/3]O2 slabs along the c -direction of the monoclinic lattice. 34 Moreover, the SEM micrograph of the as-synthesized material in Figure 1b reveals the agglomerated primary particles of less than 100 nm in size. Thus, the observed asymmetric superlattice re fl ection in the XRD pattern con fi rms an increased degree of stacking faults in the nanocrystalline Li 2 MnO3 synthesized in the present study. Figure 1c demonstrates the voltage pro fi le of Li2MnO3 in the fi rst cycle at a rate of C/50 (1 C = 230 mA g -1 assumed), while subsequent cycling was performed at C/10. The large irreversible capacity observed during activation, which results in poor Coulombic e ffi ciency of the fi rst cycle, is a characteristic electrochemical feature of Li2MnO3. Although cycling performance of Li2MnO3 shown in Figure 1d reveals improved Coulombic e ffi ciency for the subsequent cycles, continued degradation leads to signi fi cant loss of capacity upon cycling. In other words, the fi rst cycle activation processes likely persist in subsequent cycles but to a much lesser extent. The general consensus in literature is that the fi rst cycle irreversibility in Li2MnO3 is due to an irreversible oxygen release. 11 -15 Our cycling data indicate that Li2MnO3 continues to degas during subsequent cycles, but to a much lesser extent than in the fi rst cycle.", "cleaned_text_preview": "20 to 34 ° . However, these superlattice re fl ections appear convoluted into a broad asymmetric peak as shown in Figure 1a. Previously, the intensity and asymmetry of these superlattice re fl ections are correlated wit…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p2:body_region:1", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.0, "bottom": 0.004, "left": 0.103, "right": 0.038}, "excluded_risk_level": "high", "region_id": "p2:page_body:column_2_of_2:white", "truncation_marker": ""}
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{"ref": "#/texts/39", "page": 3, "label": "page_header", "order": 39000, "source_page_order": 4, "layout_order": 39, "layout_page_order": 2, "bbox": [537.79, 49.99, 19.7, 7.35], "page_size": {"width": 625.44, "height": 818.36}, "text": "Letter", "text_preview": "Letter", "word_count": 1, "cleaned_text": "Letter", "cleaned_text_preview": "Letter", "included_in_body": false, "body_decision_reason": "docling_page_header", "parser_body_decision_reason": "docling_page_header", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p3:body_region:1", "role_guess": "page_header", "zone": "top_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [159, 182, 177], "page_background_rgb": [255, 255, 255], "background_delta": 96, "background_class": "colored", "is_gray_background": false, "has_frame_evidence": true, "edge_dark_ratios": {"top": 0.989, "bottom": 0.925, "left": 0.864, "right": 0.879}, "excluded_risk_level": "low", "region_id": "p3:top_margin:column_2_of_2:colored", "truncation_marker": ""}
{"ref": "#/texts/38", "page": 3, "label": "page_header", "order": 38000, "source_page_order": 3, "layout_order": 40, "layout_page_order": 3, "bbox": [278.65, 50.28, 118.38, 6.98], "page_size": {"width": 625.44, "height": 818.36}, "text": "http://pubs.acs.org/journal/aelccp", "text_preview": "http://pubs.acs.org/journal/aelccp", "word_count": 1, "cleaned_text": "", "cleaned_text_preview": "", "included_in_body": false, "body_decision_reason": "docling_page_header", "parser_body_decision_reason": "docling_page_header", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p3:body_region:1", "role_guess": "page_header", "zone": "top_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": true, "metadata_line": true, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.034, "bottom": 0.375, "left": 0.183, "right": 0.167}, "excluded_risk_level": "low", "region_id": "p3:top_margin:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/40", "page": 3, "label": "caption", "order": 40000, "source_page_order": 5, "layout_order": 41, "layout_page_order": 4, "bbox": [60.49, 357.75, 503.97, 17.75], "page_size": {"width": 625.44, "height": 818.36}, "text": "Figure 2. Bulk O and Mn redox activity in Li2MnO3. O K-edge TFY XAS data (a), and RIXS maps of Li2MnO3 electrodes charged to 4.8 V (b) and 5.0 V (c). Operando Mn K-edge XANES (d) and EXAFS (e) data for charged and discharged states during the fi rst cycle.", "text_preview": "Figure 2. Bulk O and Mn redox activity in Li2MnO3. O K-edge TFY XAS data (a), and RIXS maps of Li2MnO3 electrodes charged to 4.8 V (b) and 5.0 V (c). Operando Mn K-edge XANES (d) and EXAFS (e) data for charged and disch…", "word_count": 50, "cleaned_text": "Figure 2. Bulk O and Mn redox activity in Li2MnO3. O K-edge TFY XAS data (a), and RIXS maps of Li2MnO3 electrodes charged to 4.8 V (b) and 5.0 V (c). Operando Mn K-edge XANES (d) and EXAFS (e) data for charged and discharged states during the fi rst cycle.", "cleaned_text_preview": "Figure 2. Bulk O and Mn redox activity in Li2MnO3. O K-edge TFY XAS data (a), and RIXS maps of Li2MnO3 electrodes charged to 4.8 V (b) and 5.0 V (c). Operando Mn K-edge XANES (d) and EXAFS (e) data for charged and disch…", "included_in_body": false, "body_decision_reason": "outside_body_flow_caption", "parser_body_decision_reason": "outside_body_flow_caption", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": false, "body_region_id": null, "role_guess": "caption", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.088, "bottom": 0.033, "left": 0.095, "right": 0.024}, "excluded_risk_level": "low", "region_id": "p3:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/34#prov1", "page": 3, "label": "text", "order": 34001, "source_page_order": 1, "layout_order": 42, "layout_page_order": 5, "bbox": [60.49, 386.73, 240.0, 233.52], "page_size": {"width": 625.44, "height": 818.36}, "text": "charge compensation mechanisms, such as oxidation of Mn 4+ and/or lattice oxygen redox need to be considered to fully account for the observed total capacity. 23 We fi rst employed O K-edge XAS and RIXS studies to probe bulk redox activity of oxygen anions in Li2MnO3. Figure 2a shows the O K-edge spectra in the bulk sensitive total fl uorescence yield (TFY) mode for the pristine Li2MnO3 and charged electrodes. Corresponding RIXS maps for the charged electrodes are shown in Figure 2b,c. The pre-edge peaks at 529.6 and 531.9 eV are attributed to the hybridization of Mn 3d -O 2p orbitals into t 2g and eg states. 35 At these excitation energies, RIXS maps show two broad density of state (DOS)-like features that are associated with the hybridized Mn -O states. The emergence of RIXS loss feature at 523.5 eVdue to X-ray absorption at 531 eV is regarded as a spectroscopic signature of bulk oxygen redox activity. 27,28,31,36 Our RIXS maps show no evidence of this RIXS feature for the charged electrodes, matching a recent Li2MnO3 study, 30 which rules out bulk oxygen redox activity in Li2MnO3. The increased weight observed at 531 eV in the O K-edge XAS correlates with broadening of the hybridized t 2g and eg states in the corresponding RIXS maps (Figure 2b,c).", "text_preview": "charge compensation mechanisms, such as oxidation of Mn 4+ and/or lattice oxygen redox need to be considered to fully account for the observed total capacity. 23 We fi rst employed O K-edge XAS and RIXS studies to probe…", "word_count": 217, "cleaned_text": "charge compensation mechanisms, such as oxidation of Mn 4+ and/or lattice oxygen redox need to be considered to fully account for the observed total capacity. 23 We fi rst employed O K-edge XAS and RIXS studies to probe bulk redox activity of oxygen anions in Li2MnO3. Figure 2a shows the O K-edge spectra in the bulk sensitive total fl uorescence yield (TFY) mode for the pristine Li2MnO3 and charged electrodes. Corresponding RIXS maps for the charged electrodes are shown in Figure 2b,c. The pre-edge peaks at 529.6 and 531.9 eV are attributed to the hybridization of Mn 3d -O 2p orbitals into t 2g and eg states. 35 At these excitation energies, RIXS maps show two broad density of state (DOS)-like features that are associated with the hybridized Mn -O states. The emergence of RIXS loss feature at 523.5 eVdue to X-ray absorption at 531 eV is regarded as a spectroscopic signature of bulk oxygen redox activity. 27,28,31,36 Our RIXS maps show no evidence of this RIXS feature for the charged electrodes, matching a recent Li2MnO3 study, 30 which rules out bulk oxygen redox activity in Li2MnO3. The increased weight observed at 531 eV in the O K-edge XAS correlates with broadening of the hybridized t 2g and eg states in the corresponding RIXS maps (Figure 2b,c).", "cleaned_text_preview": "charge compensation mechanisms, such as oxidation of Mn 4+ and/or lattice oxygen redox need to be considered to fully account for the observed total capacity. 23 We fi rst employed O K-edge XAS and RIXS studies to probe…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p3:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.007, "bottom": 0.037, "left": 0.077, "right": 0.09}, "excluded_risk_level": "high", "region_id": "p3:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/41#prov0", "page": 3, "label": "text", "order": 41000, "source_page_order": 6, "layout_order": 43, "layout_page_order": 6, "bbox": [60.49, 621.34, 240.0, 141.86], "page_size": {"width": 625.44, "height": 818.36}, "text": "These results are further complemented by a quantitative measure of oxide oxidation using an acid titration of extracted Li2MnO3 cathodes. Previous studies on NMC cathode materials have found that O 2 evolves from partially delithiated cathodes when exposed to water if oxygen redox participated in charge compensation. The oxygen evolved from these electrodes is closely related to the well established titrations of lithium peroxide, 37 following the reaction: Li2O2 + H2O → 2LiOH + 1 /2 O2. Therefore, to quantify oxidized oxygen in a state similar to that in Li 2O2, titrations were used with electrodes extracted at various states of charge (Table S1). An indication of the degree of ' reversible ' oxygen redox was estimated by comparing electrodes extracted at the top of the", "text_preview": "These results are further complemented by a quantitative measure of oxide oxidation using an acid titration of extracted Li2MnO3 cathodes. Previous studies on NMC cathode materials have found that O 2 evolves from parti…", "word_count": 126, "cleaned_text": "These results are further complemented by a quantitative measure of oxide oxidation using an acid titration of extracted Li2MnO3 cathodes. Previous studies on NMC cathode materials have found that O 2 evolves from partially delithiated cathodes when exposed to water if oxygen redox participated in charge compensation. The oxygen evolved from these electrodes is closely related to the well established titrations of lithium peroxide, 37 following the reaction: Li2O2 + H2O → 2LiOH + 1 /2 O2. Therefore, to quantify oxidized oxygen in a state similar to that in Li 2O2, titrations were used with electrodes extracted at various states of charge (Table S1). An indication of the degree of ' reversible ' oxygen redox was estimated by comparing electrodes extracted at the top of the", "cleaned_text_preview": "These results are further complemented by a quantitative measure of oxide oxidation using an acid titration of extracted Li2MnO3 cathodes. Previous studies on NMC cathode materials have found that O 2 evolves from parti…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p3:body_region:0", "role_guess": "body_candidate_excluded", "zone": "bottom_margin", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.048, "bottom": 0.009, "left": 0.064, "right": 0.115}, "excluded_risk_level": "high", "region_id": "p3:bottom_margin:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/41#prov1", "page": 3, "label": "text", "order": 41001, "source_page_order": 7, "layout_order": 44, "layout_page_order": 7, "bbox": [324.45, 387.94, 240.04, 53.76], "page_size": {"width": 625.44, "height": 818.36}, "text": "fi rst charge and the bottom of the fi rst discharge. Here we have found that these titrations demonstrate minimal contributions from bulk oxygen redox (only 10 mAh g -1 ), which is in agreement with the lack of spectroscopic feature corresponding to oxidized oxygen in our RIXS measurements (Figure 2b,c).", "text_preview": "fi rst charge and the bottom of the fi rst discharge. Here we have found that these titrations demonstrate minimal contributions from bulk oxygen redox (only 10 mAh g -1 ), which is in agreement with the lack of spectro…", "word_count": 51, "cleaned_text": "fi rst charge and the bottom of the fi rst discharge. Here we have found that these titrations demonstrate minimal contributions from bulk oxygen redox (only 10 mAh g -1 ), which is in agreement with the lack of spectroscopic feature corresponding to oxidized oxygen in our RIXS measurements (Figure 2b,c).", "cleaned_text_preview": "fi rst charge and the bottom of the fi rst discharge. Here we have found that these titrations demonstrate minimal contributions from bulk oxygen redox (only 10 mAh g -1 ), which is in agreement with the lack of spectro…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p3:body_region:1", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.039, "bottom": 0.028, "left": 0.119, "right": 0.143}, "excluded_risk_level": "high", "region_id": "p3:page_body:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/42", "page": 3, "label": "text", "order": 42000, "source_page_order": 8, "layout_order": 45, "layout_page_order": 8, "bbox": [324.45, 443.95, 240.05, 197.31], "page_size": {"width": 625.44, "height": 818.36}, "text": "We then turn to operando Mn K-edge XAS to probe bulk Mn redox activity in Li2MnO3 involving Mn 4+ /Mn 7+ redox as proposed by Radin et al. 23 However, the experimental veri fi cation of the proposed Mn 4+ /Mn 7+ redox is considered to be extremely challenging due to fragility of Mn 7+ under Xray irradiation. 23 We collected synchrotron XAS data of KMnO4 to inspect the susceptibility of Mn 7+ -containing oxides to beam damage. Indeed, experimental data could successfully reproduce all major spectral features predicted by calculations from Materials Project 38 (Figure S1). Furthermore, our Mn Kedge XAS data of KMnO4 (Figure S1) are consistent with those reported by others. 5,39,40 These indicate that Mn 7+ , if present, would be experimentally detected in operando XAS experiments. Notwithstanding this and as an added safeguard, we cycled the pouch cell o ff -line and exposed to X-rays for data collection only at the predetermined states of charge/ discharge, instead of continuously acquiring data by irradiating the cell throughout the entire charge/discharge cycle.", "text_preview": "We then turn to operando Mn K-edge XAS to probe bulk Mn redox activity in Li2MnO3 involving Mn 4+ /Mn 7+ redox as proposed by Radin et al. 23 However, the experimental veri fi cation of the proposed Mn 4+ /Mn 7+ redox i…", "word_count": 175, "cleaned_text": "We then turn to operando Mn K-edge XAS to probe bulk Mn redox activity in Li2MnO3 involving Mn 4+ /Mn 7+ redox as proposed by Radin et al. 23 However, the experimental veri fi cation of the proposed Mn 4+ /Mn 7+ redox is considered to be extremely challenging due to fragility of Mn 7+ under Xray irradiation. 23 We collected synchrotron XAS data of KMnO4 to inspect the susceptibility of Mn 7+ -containing oxides to beam damage. Indeed, experimental data could successfully reproduce all major spectral features predicted by calculations from Materials Project 38 (Figure S1). Furthermore, our Mn Kedge XAS data of KMnO4 (Figure S1) are consistent with those reported by others. 5,39,40 These indicate that Mn 7+ , if present, would be experimentally detected in operando XAS experiments. Notwithstanding this and as an added safeguard, we cycled the pouch cell o ff -line and exposed to X-rays for data collection only at the predetermined states of charge/ discharge, instead of continuously acquiring data by irradiating the cell throughout the entire charge/discharge cycle.", "cleaned_text_preview": "We then turn to operando Mn K-edge XAS to probe bulk Mn redox activity in Li2MnO3 involving Mn 4+ /Mn 7+ redox as proposed by Radin et al. 23 However, the experimental veri fi cation of the proposed Mn 4+ /Mn 7+ redox i…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p3:body_region:1", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.078, "bottom": 0.019, "left": 0.09, "right": 0.103}, "excluded_risk_level": "high", "region_id": "p3:page_body:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/43#prov0", "page": 3, "label": "text", "order": 43000, "source_page_order": 9, "layout_order": 46, "layout_page_order": 9, "bbox": [324.45, 643.51, 240.05, 119.7], "page_size": {"width": 625.44, "height": 818.36}, "text": "Parts d and e of Figure 2 show operando Mn K-edge X-ray absorption near-edge structure (XANES) and extended X-ray absorption fi ne structure (EXAFS) data of Li2MnO3. At 5.0 V, no clear shift of the main edge beyond that of the pristine state is observed, which rules out the oxidation of Mn 4+ . The splitting of Mn 3d orbitals into t 2g and eg levels by an octahedral fi eld of the surrounding oxygen can be seen in the pre-edge region, which becomes more intense upon charging to 5.0 V. Meanwhile, reduction in the amplitude of the EXAFS signal observed upon charging to 5.0 V corresponds to increased disorder in the system. 5,10 Indeed, the observed", "text_preview": "Parts d and e of Figure 2 show operando Mn K-edge X-ray absorption near-edge structure (XANES) and extended X-ray absorption fi ne structure (EXAFS) data of Li2MnO3. At 5.0 V, no clear shift of the main edge beyond that…", "word_count": 117, "cleaned_text": "Parts d and e of Figure 2 show operando Mn K-edge X-ray absorption near-edge structure (XANES) and extended X-ray absorption fi ne structure (EXAFS) data of Li2MnO3. At 5.0 V, no clear shift of the main edge beyond that of the pristine state is observed, which rules out the oxidation of Mn 4+ . The splitting of Mn 3d orbitals into t 2g and eg levels by an octahedral fi eld of the surrounding oxygen can be seen in the pre-edge region, which becomes more intense upon charging to 5.0 V. Meanwhile, reduction in the amplitude of the EXAFS signal observed upon charging to 5.0 V corresponds to increased disorder in the system. 5,10 Indeed, the observed", "cleaned_text_preview": "Parts d and e of Figure 2 show operando Mn K-edge X-ray absorption near-edge structure (XANES) and extended X-ray absorption fi ne structure (EXAFS) data of Li2MnO3. At 5.0 V, no clear shift of the main edge beyond that…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p3:body_region:1", "role_guess": "body_candidate_excluded", "zone": "bottom_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.041, "bottom": 0.004, "left": 0.139, "right": 0.139}, "excluded_risk_level": "high", "region_id": "p3:bottom_margin:column_2_of_2:white", "truncation_marker": ""}
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{"ref": "#/texts/50", "page": 4, "label": "caption", "order": 50000, "source_page_order": 5, "layout_order": 53, "layout_page_order": 4, "bbox": [60.49, 481.34, 503.96, 17.81], "page_size": {"width": 625.44, "height": 818.36}, "text": "Figure 3. Gas evolution and surface studies of Li2MnO3. (a) DEMS for the fi rst charge and (b) XPS/HAXPES data and (c) Mn L3-edge TEY data for the pristine and electrolyte-soaked material.", "text_preview": "Figure 3. Gas evolution and surface studies of Li2MnO3. (a) DEMS for the fi rst charge and (b) XPS/HAXPES data and (c) Mn L3-edge TEY data for the pristine and electrolyte-soaked material.", "word_count": 32, "cleaned_text": "Figure 3. Gas evolution and surface studies of Li2MnO3. (a) DEMS for the fi rst charge and (b) XPS/HAXPES data and (c) Mn L3-edge TEY data for the pristine and electrolyte-soaked material.", "cleaned_text_preview": "Figure 3. Gas evolution and surface studies of Li2MnO3. (a) DEMS for the fi rst charge and (b) XPS/HAXPES data and (c) Mn L3-edge TEY data for the pristine and electrolyte-soaked material.", "included_in_body": false, "body_decision_reason": "outside_body_flow_caption", "parser_body_decision_reason": "outside_body_flow_caption", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": false, "body_region_id": null, "role_guess": "caption", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.145, "bottom": 0.004, "left": 0.103, "right": 0.051}, "excluded_risk_level": "low", "region_id": "p4:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/43#prov1", "page": 4, "label": "text", "order": 43001, "source_page_order": 1, "layout_order": 54, "layout_page_order": 5, "bbox": [60.49, 512.15, 240.0, 184.95], "page_size": {"width": 625.44, "height": 818.36}, "text": "increase in the intensity of the pre-edge region can now be correlated to major restructuring during activation. This restructuring also likely accounts for the observed broadening of the O K-edge spectral features in Figure 2a -c. 41,42 Upon discharge to 2.0 V, the main edge shifts slightly toward lower energy with respect to that of the charged state, which indicates reduction of Mn 4+ during lithium reinsertion. To further clarify these trends, we extended our investigation to the second cycle. Similar trends are observed for the charged/ discharged states of the second cycle (see Figure S2), except that the second discharge shows even more reduction of Mn 4+ than the fi rst discharge. These results are in direct agreement with those reported by Croy et al. 10 and con fi rm that Mn does not oxidize beyond the 4+ oxidation state during charge but undergoes reduction during discharge. These reduced Mn species would then be oxidized during Li extraction on subsequent charge.", "text_preview": "increase in the intensity of the pre-edge region can now be correlated to major restructuring during activation. This restructuring also likely accounts for the observed broadening of the O K-edge spectral features in F…", "word_count": 162, "cleaned_text": "increase in the intensity of the pre-edge region can now be correlated to major restructuring during activation. This restructuring also likely accounts for the observed broadening of the O K-edge spectral features in Figure 2a -c. 41,42 Upon discharge to 2.0 V, the main edge shifts slightly toward lower energy with respect to that of the charged state, which indicates reduction of Mn 4+ during lithium reinsertion. To further clarify these trends, we extended our investigation to the second cycle. Similar trends are observed for the charged/ discharged states of the second cycle (see Figure S2), except that the second discharge shows even more reduction of Mn 4+ than the fi rst discharge. These results are in direct agreement with those reported by Croy et al. 10 and con fi rm that Mn does not oxidize beyond the 4+ oxidation state during charge but undergoes reduction during discharge. These reduced Mn species would then be oxidized during Li extraction on subsequent charge.", "cleaned_text_preview": "increase in the intensity of the pre-edge region can now be correlated to major restructuring during activation. This restructuring also likely accounts for the observed broadening of the O K-edge spectral features in F…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p4:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.02, "bottom": 0.018, "left": 0.064, "right": 0.103}, "excluded_risk_level": "high", "region_id": "p4:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/51#prov0", "page": 4, "label": "text", "order": 51000, "source_page_order": 6, "layout_order": 55, "layout_page_order": 6, "bbox": [60.49, 697.52, 240.0, 66.84], "page_size": {"width": 625.44, "height": 818.36}, "text": "Without oxidation of Mn 4+ and/or reversible participation of lattice oxygen in charge-compensation processes, a remaining possibility is the irreversible oxidation of lattice oxygen to oxygen gas. We employed DEMS to monitor gas evolution from Li2MnO3 during the fi rst charge (Figure 3a). Upon application of current, CO 2 was immediately detected, which", "text_preview": "Without oxidation of Mn 4+ and/or reversible participation of lattice oxygen in charge-compensation processes, a remaining possibility is the irreversible oxidation of lattice oxygen to oxygen gas. We employed DEMS to m…", "word_count": 53, "cleaned_text": "Without oxidation of Mn 4+ and/or reversible participation of lattice oxygen in charge-compensation processes, a remaining possibility is the irreversible oxidation of lattice oxygen to oxygen gas. We employed DEMS to monitor gas evolution from Li2MnO3 during the fi rst charge (Figure 3a). Upon application of current, CO 2 was immediately detected, which", "cleaned_text_preview": "Without oxidation of Mn 4+ and/or reversible participation of lattice oxygen in charge-compensation processes, a remaining possibility is the irreversible oxidation of lattice oxygen to oxygen gas. We employed DEMS to m…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p4:body_region:0", "role_guess": "body_candidate_excluded", "zone": "bottom_margin", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.018, "bottom": 0.009, "left": 0.09, "right": 0.103}, "excluded_risk_level": "high", "region_id": "p4:bottom_margin:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/51#prov1", "page": 4, "label": "text", "order": 51001, "source_page_order": 7, "layout_order": 56, "layout_page_order": 7, "bbox": [324.45, 512.15, 240.05, 101.16], "page_size": {"width": 625.44, "height": 818.36}, "text": "quickly rose to a sharp peak in evolution rate. As the voltage plateau region was reached, oxygen gas became the dominant evolution product, though CO2 continued to evolve at a lower rate. Total gas evolved across the fi rst charge summed to be 38 mmol of CO2 per mol of active material and 113 mmol of O2 per mol of active material. Note that higher applied currents (20 mA g -1 ) during DEMS experiments due to instrument availability, as well as variation in the cell design led to the decreased fi rst charge capacity of 177 mAh g -1 .", "text_preview": "quickly rose to a sharp peak in evolution rate. As the voltage plateau region was reached, oxygen gas became the dominant evolution product, though CO2 continued to evolve at a lower rate. Total gas evolved across the f…", "word_count": 101, "cleaned_text": "quickly rose to a sharp peak in evolution rate. As the voltage plateau region was reached, oxygen gas became the dominant evolution product, though CO2 continued to evolve at a lower rate. Total gas evolved across the fi rst charge summed to be 38 mmol of CO2 per mol of active material and 113 mmol of O2 per mol of active material. Note that higher applied currents (20 mA g -1 ) during DEMS experiments due to instrument availability, as well as variation in the cell design led to the decreased fi rst charge capacity of 177 mAh g -1 .", "cleaned_text_preview": "quickly rose to a sharp peak in evolution rate. As the voltage plateau region was reached, oxygen gas became the dominant evolution product, though CO2 continued to evolve at a lower rate. Total gas evolved across the f…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p4:body_region:1", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.039, "bottom": 0.009, "left": 0.077, "right": 0.077}, "excluded_risk_level": "high", "region_id": "p4:page_body:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/52#prov0", "page": 4, "label": "text", "order": 52000, "source_page_order": 8, "layout_order": 57, "layout_page_order": 8, "bbox": [324.45, 615.78, 240.05, 147.42], "page_size": {"width": 625.44, "height": 818.36}, "text": "The source of oxygen gas is the formation of oxidized lattice oxygen species followed by gas evolution, 15 as no O2 evolution results from electrolyte degradation or carbonate oxidation. 37 O2 evolution from the oxide lattice is a 4e -process, such that the irreversible oxygen contribution to capacity can be calculated from the total oxygen evolved as 125 mAh g -1 , or 71% of the total fi rst charge capacity. This oxygen evolved on the fi rst charge accounts for 9.1% of the total oxygen present in the pristine active material. After an initial delay, oxygen evolution proceeds at a rate near that of 4 electrons per molecule oxygen gas released. A 4-electron process involving oxygen molecule would require an oxygen gas release rate of 363 μ mol min -1 mol -1 if oxygen gas accounted for the entire", "text_preview": "The source of oxygen gas is the formation of oxidized lattice oxygen species followed by gas evolution, 15 as no O2 evolution results from electrolyte degradation or carbonate oxidation. 37 O2 evolution from the oxide l…", "word_count": 140, "cleaned_text": "The source of oxygen gas is the formation of oxidized lattice oxygen species followed by gas evolution, 15 as no O2 evolution results from electrolyte degradation or carbonate oxidation. 37 O2 evolution from the oxide lattice is a 4e -process, such that the irreversible oxygen contribution to capacity can be calculated from the total oxygen evolved as 125 mAh g -1 , or 71% of the total fi rst charge capacity. This oxygen evolved on the fi rst charge accounts for 9.1% of the total oxygen present in the pristine active material. After an initial delay, oxygen evolution proceeds at a rate near that of 4 electrons per molecule oxygen gas released. A 4-electron process involving oxygen molecule would require an oxygen gas release rate of 363 μ mol min -1 mol -1 if oxygen gas accounted for the entire", "cleaned_text_preview": "The source of oxygen gas is the formation of oxidized lattice oxygen species followed by gas evolution, 15 as no O2 evolution results from electrolyte degradation or carbonate oxidation. 37 O2 evolution from the oxide l…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p4:body_region:1", "role_guess": "body_candidate_excluded", "zone": "bottom_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.057, "bottom": 0.013, "left": 0.192, "right": 0.192}, "excluded_risk_level": "high", "region_id": "p4:bottom_margin:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/53", "page": 4, "label": "page_footer", "order": 53000, "source_page_order": 9, "layout_order": 58, "layout_page_order": 9, "bbox": [306.43, 774.02, 12.06, 6.54], "page_size": {"width": 625.44, "height": 818.36}, "text": "637", "text_preview": "637", "word_count": 1, "cleaned_text": "637", "cleaned_text_preview": "637", "included_in_body": false, "body_decision_reason": "docling_page_footer", "parser_body_decision_reason": "docling_page_footer", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": false, "body_region_id": null, "role_guess": "page_footer", "zone": "bottom_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": true, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.231, "bottom": 0.102, "left": 0.25, "right": 0.167}, "excluded_risk_level": "low", "region_id": "p4:bottom_margin:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/54", "page": 4, "label": "page_footer", "order": 54000, "source_page_order": 10, "layout_order": 59, "layout_page_order": 10, "bbox": [439.88, 774.81, 124.6, 12.72], "page_size": {"width": 625.44, "height": 818.36}, "text": "https://dx.doi.org/10.1021/acsenergylett.9b02799 ACS Energy Lett. 2020, 5, 634 -641", "text_preview": "https://dx.doi.org/10.1021/acsenergylett.9b02799 ACS Energy Lett. 2020, 5, 634 -641", "word_count": 8, "cleaned_text": "ACS Energy Lett. 2020, 5, 634 -641", "cleaned_text_preview": "ACS Energy Lett. 2020, 5, 634 -641", "included_in_body": false, "body_decision_reason": "docling_page_footer", "parser_body_decision_reason": "docling_page_footer", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p4:body_region:1", "role_guess": "page_footer", "zone": "bottom_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": true, "metadata_line": true, "affiliation_block": false, "reference_item": true, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.074, "bottom": 0.009, "left": 0.061, "right": 0.123}, "excluded_risk_level": "low", "region_id": "p4:bottom_margin:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/55", "page": 5, "label": "page_header", "order": 55000, "source_page_order": 2, "layout_order": 60, "layout_page_order": 1, "bbox": [60.49, 48.93, 84.37, 8.72], "page_size": {"width": 625.44, "height": 818.36}, "text": "ACS Energy Letters", "text_preview": "ACS Energy Letters", "word_count": 3, "cleaned_text": "ACS Energy Letters", "cleaned_text_preview": "ACS Energy Letters", "included_in_body": false, "body_decision_reason": "docling_page_header", "parser_body_decision_reason": "docling_page_header", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:0", "role_guess": "page_header", "zone": "top_margin", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": true, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.059, "bottom": 0.446, "left": 0.09, "right": 0.179}, "excluded_risk_level": "low", "region_id": "p5:top_margin:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/52#prov1", "page": 5, "label": "text", "order": 52001, "source_page_order": 1, "layout_order": 61, "layout_page_order": 2, "bbox": [60.49, 68.75, 239.99, 20.65], "page_size": {"width": 625.44, "height": 818.36}, "text": "fi rst charge capacity. As this is not the case, we examined other capacity contributions.", "text_preview": "fi rst charge capacity. As this is not the case, we examined other capacity contributions.", "word_count": 15, "cleaned_text": "fi rst charge capacity. As this is not the case, we examined other capacity contributions.", "cleaned_text_preview": "fi rst charge capacity. As this is not the case, we examined other capacity contributions.", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.02, "bottom": 0.002, "left": 0.104, "right": 0.021}, "excluded_risk_level": "high", "region_id": "p5:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/58", "page": 5, "label": "text", "order": 58000, "source_page_order": 5, "layout_order": 62, "layout_page_order": 3, "bbox": [60.49, 91.71, 240.01, 435.42], "page_size": {"width": 625.44, "height": 818.36}, "text": "We note that the CO2 evolution is remarkably high for a transition metal oxide material. The large quantity of CO2 evolved (Figure 3c) could originate from a variety of mechanisms, including electrolyte reaction with generated singlet oxygen, 43 surface peroxo species at high voltages, or the oxidation of carbonate impurities in the as-prepared material. To understand the origin of CO 2 evolution, we performed acid titrations and X-ray photoemission spectroscopy (XPS)/hard X-ray photoemission spectroscopy (HAXPES) studies on the extracted electrodes. Acid titrations revealed the presence of 0.4 wt % (6.2 mmol mol -1 ) of carbonates in the pristine material used for the DEMS study, which is much lower than the total CO2 evolution observed during galvanostatic charge (38 mmol mol -1 ). This suggests that electrolyte degradation is the dominant contributor to CO2 evolution. Interestingly, a titration study on a separate batch of Li2MnO3 electrodes both in its pristine state and in the postelectrolyte soak revealed that carbonate content increased by 69% (Table S2) as a result of simply exposing the material to the electrolyte, indicating that the electrolyte largely decomposes and deposits a solid degradation product on the material surface. This is consistent with the XPS O 1s region of the pristine material (Figure 3b) showing a peak between 531.5 and 534 eV binding energy due to the formation of surface carbonates. 44 -48 Note the absence of a similar peak in the bulk sensitive HAXPES O 1s region of the pristine material. Meanwhile, Mn L3-edge TEY XAS data reveal the presence of reduced Mn species on the surface of pristine material (Figure 3c). The amount of surface carbonates and reduced Mn species greatly increased once the electrode is exposed to the electrolyte (Figure 3b,c), which can be attributed to higher surface reactivity of Li2MnO3. 49 It is this chemical process that may be the dominant electrolyte degradation mechanism throughout the fi rst charge, although future studies employing isotopic labeling and 1 O2 detection are needed to fully understand electrolyte degradation. Nevertheless, our results strongly suggest that the predominant origin for CO2 evolution is the continuous degradation of the electrolyte to solid surface species, which then oxidize at high voltages to evolve CO2.", "text_preview": "We note that the CO2 evolution is remarkably high for a transition metal oxide material. The large quantity of CO2 evolved (Figure 3c) could originate from a variety of mechanisms, including electrolyte reaction with ge…", "word_count": 365, "cleaned_text": "We note that the CO2 evolution is remarkably high for a transition metal oxide material. The large quantity of CO2 evolved (Figure 3c) could originate from a variety of mechanisms, including electrolyte reaction with generated singlet oxygen, 43 surface peroxo species at high voltages, or the oxidation of carbonate impurities in the as-prepared material. To understand the origin of CO 2 evolution, we performed acid titrations and X-ray photoemission spectroscopy (XPS)/hard X-ray photoemission spectroscopy (HAXPES) studies on the extracted electrodes. Acid titrations revealed the presence of 0.4 wt % (6.2 mmol mol -1 ) of carbonates in the pristine material used for the DEMS study, which is much lower than the total CO2 evolution observed during galvanostatic charge (38 mmol mol -1 ). This suggests that electrolyte degradation is the dominant contributor to CO2 evolution. Interestingly, a titration study on a separate batch of Li2MnO3 electrodes both in its pristine state and in the postelectrolyte soak revealed that carbonate content increased by 69% (Table S2) as a result of simply exposing the material to the electrolyte, indicating that the electrolyte largely decomposes and deposits a solid degradation product on the material surface. This is consistent with the XPS O 1s region of the pristine material (Figure 3b) showing a peak between 531.5 and 534 eV binding energy due to the formation of surface carbonates. 44 -48 Note the absence of a similar peak in the bulk sensitive HAXPES O 1s region of the pristine material. Meanwhile, Mn L3-edge TEY XAS data reveal the presence of reduced Mn species on the surface of pristine material (Figure 3c). The amount of surface carbonates and reduced Mn species greatly increased once the electrode is exposed to the electrolyte (Figure 3b,c), which can be attributed to higher surface reactivity of Li2MnO3. 49 It is this chemical process that may be the dominant electrolyte degradation mechanism throughout the fi rst charge, although future studies employing isotopic labeling and 1 O2 detection are needed to fully understand electrolyte degradation. Nevertheless, our results strongly suggest that the predominant origin for CO2 evolution is the continuous degradation of the electrolyte to solid surface species, which then oxidize at high voltages to evolve CO2.", "cleaned_text_preview": "We note that the CO2 evolution is remarkably high for a transition metal oxide material. The large quantity of CO2 evolved (Figure 3c) could originate from a variety of mechanisms, including electrolyte reaction with ge…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.027, "bottom": 0.007, "left": 0.051, "right": 0.09}, "excluded_risk_level": "high", "region_id": "p5:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/59", "page": 5, "label": "text", "order": 59000, "source_page_order": 6, "layout_order": 63, "layout_page_order": 4, "bbox": [60.49, 529.44, 240.0, 98.77], "page_size": {"width": 625.44, "height": 818.36}, "text": "The fi rst charge capacity for Li2MnO3 as observed during the DEMS measurement can now be analyzed in terms of the contributions from the processes examined in this study (Table 1). O2 evolution originating from oxygen oxidation accounts for roughly 70% of the total charge capacity. CO2 evolution originating from the decomposition of carbonates both present in the initial material as well as formed by electrolyte decomposition accounts for another 10% of the charge capacity. Titrations probing the ' reversible ' oxygen oxidation", "text_preview": "The fi rst charge capacity for Li2MnO3 as observed during the DEMS measurement can now be analyzed in terms of the contributions from the processes examined in this study (Table 1). O2 evolution originating from oxygen …", "word_count": 83, "cleaned_text": "The fi rst charge capacity for Li2MnO3 as observed during the DEMS measurement can now be analyzed in terms of the contributions from the processes examined in this study (Table 1). O2 evolution originating from oxygen oxidation accounts for roughly 70% of the total charge capacity. CO2 evolution originating from the decomposition of carbonates both present in the initial material as well as formed by electrolyte decomposition accounts for another 10% of the charge capacity. Titrations probing the ' reversible ' oxygen oxidation", "cleaned_text_preview": "The fi rst charge capacity for Li2MnO3 as observed during the DEMS measurement can now be analyzed in terms of the contributions from the processes examined in this study (Table 1). O2 evolution originating from oxygen …", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:0", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.04, "bottom": 0.016, "left": 0.038, "right": 0.038}, "excluded_risk_level": "high", "region_id": "p5:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/60", "page": 5, "label": "section_header", "order": 60000, "source_page_order": 7, "layout_order": 64, "layout_page_order": 5, "bbox": [60.49, 638.64, 189.99, 12.35], "page_size": {"width": 625.44, "height": 818.36}, "text": "Table 1. First Charge Capacity Contributions a", "text_preview": "Table 1. First Charge Capacity Contributions a", "word_count": 7, "cleaned_text": "Table 1. First Charge Capacity Contributions a", "cleaned_text_preview": "Table 1. First Charge Capacity Contributions a", "included_in_body": false, "body_decision_reason": "visual_caption_heading", "parser_body_decision_reason": "visual_caption_heading", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:0", "role_guess": "caption", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.0, "bottom": 0.016, "left": 0.028, "right": 0.065}, "excluded_risk_level": "low", "region_id": "p5:page_body:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/61", "page": 5, "label": "text", "order": 61000, "source_page_order": 8, "layout_order": 65, "layout_page_order": 6, "bbox": [60.49, 732.89, 239.98, 30.06], "page_size": {"width": 625.44, "height": 818.36}, "text": "a Capacity contributions as determined using gas evolution and titration techniques compared to the total fi rst charge capacity of the cell run on the DEMS system.", "text_preview": "a Capacity contributions as determined using gas evolution and titration techniques compared to the total fi rst charge capacity of the cell run on the DEMS system.", "word_count": 27, "cleaned_text": "a Capacity contributions as determined using gas evolution and titration techniques compared to the total fi rst charge capacity of the cell run on the DEMS system.", "cleaned_text_preview": "a Capacity contributions as determined using gas evolution and titration techniques compared to the total fi rst charge capacity of the cell run on the DEMS system.", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:0", "role_guess": "body_candidate_excluded", "zone": "bottom_margin", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.002, "bottom": 0.002, "left": 0.067, "right": 0.078}, "excluded_risk_level": "high", "region_id": "p5:bottom_margin:column_1_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/57", "page": 5, "label": "page_header", "order": 57000, "source_page_order": 4, "layout_order": 66, "layout_page_order": 7, "bbox": [537.79, 49.99, 19.7, 7.35], "page_size": {"width": 625.44, "height": 818.36}, "text": "Letter", "text_preview": "Letter", "word_count": 1, "cleaned_text": "Letter", "cleaned_text_preview": "Letter", "included_in_body": false, "body_decision_reason": "docling_page_header", "parser_body_decision_reason": "docling_page_header", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:1", "role_guess": "page_header", "zone": "top_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [159, 182, 177], "page_background_rgb": [255, 255, 255], "background_delta": 96, "background_class": "colored", "is_gray_background": false, "has_frame_evidence": true, "edge_dark_ratios": {"top": 0.989, "bottom": 0.925, "left": 0.864, "right": 0.879}, "excluded_risk_level": "low", "region_id": "p5:top_margin:column_2_of_2:colored", "truncation_marker": ""}
{"ref": "#/texts/56", "page": 5, "label": "page_header", "order": 56000, "source_page_order": 3, "layout_order": 67, "layout_page_order": 8, "bbox": [278.65, 50.28, 118.38, 6.98], "page_size": {"width": 625.44, "height": 818.36}, "text": "http://pubs.acs.org/journal/aelccp", "text_preview": "http://pubs.acs.org/journal/aelccp", "word_count": 1, "cleaned_text": "", "cleaned_text_preview": "", "included_in_body": false, "body_decision_reason": "docling_page_header", "parser_body_decision_reason": "docling_page_header", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:1", "role_guess": "page_header", "zone": "top_margin", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": true, "page_margin_noise": true, "metadata_line": true, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.034, "bottom": 0.375, "left": 0.183, "right": 0.167}, "excluded_risk_level": "low", "region_id": "p5:top_margin:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/62", "page": 5, "label": "text", "order": 62000, "source_page_order": 9, "layout_order": 68, "layout_page_order": 9, "bbox": [324.45, 65.25, 240.04, 156.7], "page_size": {"width": 625.44, "height": 818.36}, "text": "(O 2 -/O -) revealed about 6% contribution to the total charge capacity. We suspect the remaining 14% of the fi rst charge capacity (Table 1) results from a combination of processes including electrolyte decomposition given the high cuto ff voltage, as well as the oxidation of reduced Mn species in the near surface region (Figure 3c). Electrolyte decomposition was regarded as a likely source of protons for the previously proposed Li + /H + exchange in Li2MnO3. 3,5,50 However, like those previous studies, the X-ray techniques employed in the present study are not directly sensitive to structural protons. Meanwhile, a recent NMR study by Dogan et al. 7 found signi fi cant evidence for proton-containing species on the surface of the charged electrode due to side reactions but ruled out insertion of structural protons in Li2MnO3.", "text_preview": "(O 2 -/O -) revealed about 6% contribution to the total charge capacity. We suspect the remaining 14% of the fi rst charge capacity (Table 1) results from a combination of processes including electrolyte decomposition g…", "word_count": 137, "cleaned_text": "(O 2 -/O -) revealed about 6% contribution to the total charge capacity. We suspect the remaining 14% of the fi rst charge capacity (Table 1) results from a combination of processes including electrolyte decomposition given the high cuto ff voltage, as well as the oxidation of reduced Mn species in the near surface region (Figure 3c). Electrolyte decomposition was regarded as a likely source of protons for the previously proposed Li + /H + exchange in Li2MnO3. 3,5,50 However, like those previous studies, the X-ray techniques employed in the present study are not directly sensitive to structural protons. Meanwhile, a recent NMR study by Dogan et al. 7 found signi fi cant evidence for proton-containing species on the surface of the charged electrode due to side reactions but ruled out insertion of structural protons in Li2MnO3.", "cleaned_text_preview": "(O 2 -/O -) revealed about 6% contribution to the total charge capacity. We suspect the remaining 14% of the fi rst charge capacity (Table 1) results from a combination of processes including electrolyte decomposition g…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:1", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.0, "bottom": 0.009, "left": 0.09, "right": 0.077}, "excluded_risk_level": "high", "region_id": "p5:page_body:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/63", "page": 5, "label": "text", "order": 63000, "source_page_order": 10, "layout_order": 69, "layout_page_order": 10, "bbox": [324.45, 224.2, 240.05, 318.46], "page_size": {"width": 625.44, "height": 818.36}, "text": "In summary, using the combination of operando Mn K-edge XAS, O K-edge RIXS, XPS/HAXPES, and DEMS, we interpret and quantify the capacity contributions observed during electrochemical activation of Li2MnO3. Taken together, the fi rst charge capacity of Li2MnO3 originates primarily from oxygen release, with much smaller contributions from reversible lattice oxygen redox, decomposition of surface carbonates and oxidation of reduced Mn species on the surface. Furthermore, our results conclude that Li2MnO3 does not exhibit the recently proposed Mn 4+ /Mn 7+ redox. For Li2MnO3, the octahedrally coordinated Mn prefers not to oxidize beyond 4+ at high voltages consistent with the lack of Mn 7+ signatures in delithiated LR-NMCs reported thus far. Interestingly, Ceder and co-workers 16 attributed bulk oxygen redox to the labile oxygen states resulting from the Li -O -Li correlations as in Li2MnO3. However, the lack of RIXS feature in the charged samples clearly ruled out signi fi cant contribution from bulk oxygen redox in Li 2 MnO3. In contrast, the conventional layered oxides without Li -O -Li correlations demonstrated an RIXS feature indicating the onset of bulk oxygen redox at higher degrees of delithiation. 31,32,51 These reports suggest that increased covalency a ff orded by highly oxidized Ni and Co ions is an important precursor to promoting bulk oxygen redox. 16,52 -54 Simply put, the Li2MnO3 component in LR-NMC nanocomposites acts as a reservoir of excess Li ions, facilitating capacity beyond the conventional transition-metal (TM) redox by utilizing the inherent TM-O covalency-driven bulk oxygen redox at higher potentials.", "text_preview": "In summary, using the combination of operando Mn K-edge XAS, O K-edge RIXS, XPS/HAXPES, and DEMS, we interpret and quantify the capacity contributions observed during electrochemical activation of Li2MnO3. Taken togethe…", "word_count": 251, "cleaned_text": "In summary, using the combination of operando Mn K-edge XAS, O K-edge RIXS, XPS/HAXPES, and DEMS, we interpret and quantify the capacity contributions observed during electrochemical activation of Li2MnO3. Taken together, the fi rst charge capacity of Li2MnO3 originates primarily from oxygen release, with much smaller contributions from reversible lattice oxygen redox, decomposition of surface carbonates and oxidation of reduced Mn species on the surface. Furthermore, our results conclude that Li2MnO3 does not exhibit the recently proposed Mn 4+ /Mn 7+ redox. For Li2MnO3, the octahedrally coordinated Mn prefers not to oxidize beyond 4+ at high voltages consistent with the lack of Mn 7+ signatures in delithiated LR-NMCs reported thus far. Interestingly, Ceder and co-workers 16 attributed bulk oxygen redox to the labile oxygen states resulting from the Li -O -Li correlations as in Li2MnO3. However, the lack of RIXS feature in the charged samples clearly ruled out signi fi cant contribution from bulk oxygen redox in Li 2 MnO3. In contrast, the conventional layered oxides without Li -O -Li correlations demonstrated an RIXS feature indicating the onset of bulk oxygen redox at higher degrees of delithiation. 31,32,51 These reports suggest that increased covalency a ff orded by highly oxidized Ni and Co ions is an important precursor to promoting bulk oxygen redox. 16,52 -54 Simply put, the Li2MnO3 component in LR-NMC nanocomposites acts as a reservoir of excess Li ions, facilitating capacity beyond the conventional transition-metal (TM) redox by utilizing the inherent TM-O covalency-driven bulk oxygen redox at higher potentials.", "cleaned_text_preview": "In summary, using the combination of operando Mn K-edge XAS, O K-edge RIXS, XPS/HAXPES, and DEMS, we interpret and quantify the capacity contributions observed during electrochemical activation of Li2MnO3. Taken togethe…", "included_in_body": false, "body_decision_reason": "inside_front_matter", "parser_body_decision_reason": "inside_front_matter", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:1", "role_guess": "body_candidate_excluded", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": true, "body_candidate": true, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.035, "bottom": 0.002, "left": 0.09, "right": 0.064}, "excluded_risk_level": "high", "region_id": "p5:page_body:column_2_of_2:white", "truncation_marker": ""}
{"ref": "#/texts/64", "page": 5, "label": "section_header", "order": 64000, "source_page_order": 11, "layout_order": 70, "layout_page_order": 11, "bbox": [324.45, 547.02, 122.94, 23.97], "page_size": {"width": 625.44, "height": 818.36}, "text": "■ ASSOCIATED CONTENT", "text_preview": "■ ASSOCIATED CONTENT", "word_count": 3, "cleaned_text": "■ ASSOCIATED CONTENT", "cleaned_text_preview": "■ ASSOCIATED CONTENT", "included_in_body": false, "body_decision_reason": "non_body_heading", "parser_body_decision_reason": "non_body_heading", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p5:body_region:1", "role_guess": "body_heading", "zone": "page_body", "column": "column_2_of_2", "column_index": 2, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.0, "bottom": 0.0, "left": 0.056, "right": 0.042}, "excluded_risk_level": "low", "region_id": "p5:page_body:column_2_of_2:white", "truncation_marker": ""}
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{"ref": "#/texts/91", "page": 6, "label": "text", "order": 91000, "source_page_order": 19, "layout_order": 95, "layout_page_order": 17, "bbox": [60.49, 521.06, 157.05, 13.38], "page_size": {"width": 625.44, "height": 818.36}, "text": "¶ J.R. and J.K.P. had equal contributions.", "text_preview": "¶ J.R. and J.K.P. had equal contributions.", "word_count": 7, "cleaned_text": "¶ J.R. and J.K.P. had equal contributions.", "cleaned_text_preview": "¶ J.R. and J.K.P. had equal contributions.", "included_in_body": false, "body_decision_reason": "after_back_matter_stop", "parser_body_decision_reason": "after_back_matter_stop", "production_usage": "", "visual_asset_type": "", "visual_asset_label": "", "visual_asset_caption_preview": "", "visual_asset_anchor_ref": "", "inside_body_region": true, "body_region_id": "p6:body_region:0", "role_guess": "unknown_text", "zone": "page_body", "column": "column_1_of_2", "column_index": 1, "column_count": 2, "flags": {"docling_non_body_label": false, "page_margin_noise": false, "metadata_line": false, "affiliation_block": false, "reference_item": false, "body_sentence": false, "body_candidate": false, "body_heading": false, "heading_kind": null, "has_front_matter_zone": false, "visual_text": false, "publisher_landing_page": false, "caption_continuation_used_by_asset": false}, "background_rgb": [255, 255, 255], "page_background_rgb": [255, 255, 255], "background_delta": 0, "background_class": "white", "is_gray_background": false, "has_frame_evidence": false, "edge_dark_ratios": {"top": 0.109, "bottom": 0.017, "left": 0.05, "right": 0.025}, "excluded_risk_level": "low", "region_id": "p6:page_body:column_1_of_2:white", "truncation_marker": "after_stop"}
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