page source_page_order layout_page_order layout_order ref label role_guess included_in_body excluded_risk_level body_decision_reason parser_body_decision_reason production_usage visual_asset_type visual_asset_label visual_asset_caption_preview truncation_marker inside_body_region body_region_id zone column column_index column_count region_id background_rgb background_class is_gray_background has_frame_evidence bbox text_preview cleaned_text_preview text cleaned_text 1 1 1 0 #/texts/0 page_header page_header False low document_ui document_ui True p1:body_region:0 top_margin column_1_of_2 1 2 p1:top_margin:column_1_of_2:white [255, 255, 255] white False True [50.81, 28.94, 126.19, 12.11] RESEARCH ARTICLE RESEARCH ARTICLE RESEARCH ARTICLE RESEARCH ARTICLE 1 2 2 1 #/texts/1 text page_margin_header False low document_web_address document_web_address True p1:body_region:1 top_margin column_2_of_2 2 2 p1:top_margin:column_2_of_2:white [255, 255, 255] white False False [472.46, 49.98, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 1 3 3 2 #/texts/2 section_header title_candidate False low first_page_front_matter_heading first_page_front_matter_heading True p1:body_region:0 front_matter column_1_of_2 1 2 p1:front_matter:column_1_of_2:white [255, 255, 255] white False False [50.81, 77.5, 441.13, 63.65] Local Electronic Structure Modulation Enables Fast-Charging Capability for Li-Rich Mn-Based Oxides Cathodes With Reversible Anionic Redox Activity Local Electronic Structure Modulation Enables Fast-Charging Capability for Li-Rich Mn-Based Oxides Cathodes With Reversible Anionic Redox Activity Local Electronic Structure Modulation Enables Fast-Charging Capability for Li-Rich Mn-Based Oxides Cathodes With Reversible Anionic Redox Activity Local Electronic Structure Modulation Enables Fast-Charging Capability for Li-Rich Mn-Based Oxides Cathodes With Reversible Anionic Redox Activity 1 4 4 3 #/texts/3 text affiliation False low first_page_author_or_affiliation first_page_author_or_affiliation True p1:body_region:0 front_matter column_1_of_2 1 2 p1:front_matter:column_1_of_2:white [255, 255, 255] white False False [50.81, 160.21, 487.97, 30.54] Xianggang Gao, Haiyan Zhang, Shihao Li, Shuai Zhang, Chaohong Guan, Xiaoping Hu, Juanlang Guo, Yanqing Lai,* and Zhian Zhang* Xianggang Gao, Haiyan Zhang, Shihao Li, Shuai Zhang, Chaohong Guan, Xiaoping Hu, Juanlang Guo, Yanqing Lai,* and Zhian Zhang* Xianggang Gao, Haiyan Zhang, Shihao Li, Shuai Zhang, Chaohong Guan, Xiaoping Hu, Juanlang Guo, Yanqing Lai,* and Zhian Zhang* Xianggang Gao, Haiyan Zhang, Shihao Li, Shuai Zhang, Chaohong Guan, Xiaoping Hu, Juanlang Guo, Yanqing Lai,* and Zhian Zhang* 1 7 7 6 #/texts/6 text affiliation False low affiliation_block affiliation_block True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 513.78, 127.19, 7.2] School of Metallurgy and Environment School of Metallurgy and Environment School of Metallurgy and Environment School of Metallurgy and Environment 1 8 8 7 #/texts/7 text affiliation False low affiliation_block affiliation_block True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 522.75, 234.43, 25.14] Hunan Province Key Laboratory of Nonferrous Value-Added Metallurgy Engineering Research Center of the Ministry of Education for Advanced Battery Materials Hunan Province Key Laboratory of Nonferrous Value-Added Metallurgy Engineering Research Center of the Ministry of Education for Advanced Battery Materials Hunan Province Key Laboratory of Nonferrous Value-Added Metallurgy Engineering Research Center of the Ministry of Education for Advanced Battery Materials Hunan Province Key Laboratory of Nonferrous Value-Added Metallurgy Engineering Research Center of the Ministry of Education for Advanced Battery Materials 1 9 9 8 #/texts/8 text affiliation False low affiliation_block affiliation_block True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 549.65, 80.2, 7.2] Central South University Central South University Central South University Central South University 1 11 11 10 #/texts/10 text metadata False low first_page_metadata first_page_metadata True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 567.58, 191.32, 7.2] E-mail: laiyanqingcsu@163.com; zhangzhian@csu.edu.cn E-mail: laiyanqingcsu@163.com; zhangzhian@csu.edu.cn E-mail: laiyanqingcsu@163.com; zhangzhian@csu.edu.cn E-mail: laiyanqingcsu@163.com; zhangzhian@csu.edu.cn 1 12 12 11 #/texts/11 text metadata False low document_web_address document_web_address True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False True [50.81, 578.54, 30.54, 7.2] H.Zhang H.Zhang H.Zhang H.Zhang 1 14 14 13 #/texts/13 text affiliation False low contextual_affiliation_fragment contextual_affiliation_fragment True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 596.47, 121.28, 7.2] Changsha,Hunan410205,P.R.China Changsha,Hunan410205,P.R.China Changsha,Hunan410205,P.R.China Changsha,Hunan410205,P.R.China 1 15 15 14 #/texts/14 text affiliation False low contextual_affiliation_fragment contextual_affiliation_fragment True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 607.44, 26.12, 7.2] C. Guan C. Guan C. Guan C. Guan 1 16 16 15 #/texts/15 text affiliation False low affiliation_block affiliation_block True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 616.4, 216.68, 7.2] University of Michigan-Shanghai Jiao Tong University Joint Institute University of Michigan-Shanghai Jiao Tong University Joint Institute University of Michigan-Shanghai Jiao Tong University Joint Institute University of Michigan-Shanghai Jiao Tong University Joint Institute 1 18 18 17 #/texts/17 text affiliation False low contextual_affiliation_fragment contextual_affiliation_fragment True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 634.33, 166.08, 7.2] 800DongchuanRoad,Shanghai200240,P.R.China 800DongchuanRoad,Shanghai200240,P.R.China 800DongchuanRoad,Shanghai200240,P.R.China 800DongchuanRoad,Shanghai200240,P.R.China 1 19 19 18 #/texts/18 text affiliation False low contextual_affiliation_fragment contextual_affiliation_fragment True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 645.29, 18.22, 7.2] X. Hu X. Hu X. Hu X. Hu 1 21 21 20 #/texts/20 text affiliation False low affiliation_block affiliation_block True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 663.23, 78.63, 7.2] Central South University Central South University Central South University Central South University 1 22 22 21 #/texts/21 text affiliation False low contextual_affiliation_fragment contextual_affiliation_fragment True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 672.19, 121.28, 7.2] Changsha,Hunan410083,P.R.China Changsha,Hunan410083,P.R.China Changsha,Hunan410083,P.R.China Changsha,Hunan410083,P.R.China 1 23 23 22 #/texts/22 text metadata False low first_page_metadata first_page_metadata True p1:body_region:0 body_zone column_1_of_2 1 2 p1:body_zone:column_1_of_2:white [255, 255, 255] white False False [68.79, 690.25, 222.97, 16.17] The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.202304065 The ORCID identification number(s) for the author(s) of this article can be found under The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.202304065 The ORCID identification number(s) for the author(s) of this article can be found under 1 24 24 23 #/texts/23 text page_margin_footer False low first_page_metadata first_page_metadata True p1:body_region:0 bottom_margin column_1_of_2 1 2 p1:bottom_margin:column_1_of_2:white [255, 255, 255] white False True [50.81, 712.5, 114.86, 8.02] DOI: 10.1002/adfm.202304065 DOI: 10.1002/adfm.202304065 DOI: 10.1002/adfm.202304065 DOI: 10.1002/adfm.202304065 1 25 25 24 #/texts/24 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_page_footer True p1:body_region:0 bottom_margin column_1_of_2 1 2 p1:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 1 26 26 25 #/texts/25 section_header body_heading False low body_heading body_heading True p1:body_region:1 body_zone column_2_of_2 2 2 p1:body_zone:column_2_of_2:white [255, 255, 255] white False False [384.63, 219.54, 70.41, 10.25] 1. Introduction 1. Introduction 1. Introduction 1. Introduction 1 30 30 29 #/texts/29 page_footer page_footer False low docling_page_footer docling_page_footer True p1:body_region:0 bottom_margin column_2_of_2 2 2 p1:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [266.69, 744.38, 64.3, 8.02] 2304065 (1 of 11) 2304065 (1 of 11) 2304065 (1 of 11) 2304065 (1 of 11) 1 31 31 30 #/texts/30 page_footer page_footer False low first_page_metadata first_page_metadata True p1:body_region:1 bottom_margin column_2_of_2 2 2 p1:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [469.66, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 2 1 1 31 #/texts/28#prov1 text page_margin_header False low page_margin_header page_margin_header False None top_margin column_1_of_2 1 2 p2:top_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 2 5 2 32 #/texts/32 caption caption False low outside_body_flow_caption outside_body_flow_caption False None page_body column_1_of_2 1 2 p2:page_body:column_1_of_2:white [255, 255, 255] white False False [47.98, 388.13, 405.37, 7.2] Figure 1. Schematic of surface defect engineering and the transformation of surface crystal structures for LRMO materials. Figure 1. Schematic of surface defect engineering and the transformation of surface crystal structures for LRMO materials. Figure 1. Schematic of surface defect engineering and the transformation of surface crystal structures for LRMO materials. Figure 1. Schematic of surface defect engineering and the transformation of surface crystal structures for LRMO materials. 2 6 4 34 #/texts/33 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_page_footer False None bottom_margin column_1_of_2 1 2 p2:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 2 4 5 35 #/texts/31 page_header page_header False low docling_page_header docling_page_header False None top_margin column_2_of_2 2 2 p2:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 2 2 6 36 #/texts/28#prov2 text page_margin_header False low page_margin_header page_margin_header True p2:body_region:0 top_margin column_2_of_2 2 2 p2:top_margin:column_2_of_2:white [255, 255, 255] white False False [469.62, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 2 9 9 39 #/texts/36 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_2_of_2 2 2 p2:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [263.85, 744.38, 64.3, 8.02] 2304065 (2 of 11) 2304065 (2 of 11) 2304065 (2 of 11) 2304065 (2 of 11) 2 10 10 40 #/texts/37 page_footer page_footer False low docling_page_footer docling_page_footer True p2:body_region:0 bottom_margin column_2_of_2 2 2 p2:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [466.82, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 3 2 1 41 #/texts/38 page_header page_header False low docling_page_header docling_page_header False None top_margin column_1_of_2 1 2 p3:top_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 3 3 2 42 #/texts/39 page_header page_header False low docling_page_header docling_page_header False None top_margin column_2_of_2 2 2 p3:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 3 5 3 43 #/texts/41 section_header metadata False low outside_body_flow_metadata_line outside_body_flow_metadata_line True p3:body_region:0 top_margin column_2_of_2 2 2 p3:top_margin:column_2_of_2:white [255, 255, 255] white False False [472.46, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 3 4 4 44 #/texts/40 caption caption False low outside_body_flow_caption outside_body_flow_caption False None front_matter column_1_of_2 1 2 p3:front_matter:column_1_of_2:white [255, 255, 255] white False False [50.81, 575.36, 496.07, 26.13] Figure 2. a) The XRD patterns of P0 and NHCO-5 samples with the enlarged images of (003), (101), and (104) peaks, respectively. Refined XRD data of b) P0 and c) NHCO-5. Raman spectra of d) P0 and e) NHCO-5. The TEM and … Figure 2. a) The XRD patterns of P0 and NHCO-5 samples with the enlarged images of (003), (101), and (104) peaks, respectively. Refined XRD data of b) P0 and c) NHCO-5. Raman spectra of d) P0 and e) NHCO-5. The TEM and … Figure 2. a) The XRD patterns of P0 and NHCO-5 samples with the enlarged images of (003), (101), and (104) peaks, respectively. Refined XRD data of b) P0 and c) NHCO-5. Raman spectra of d) P0 and e) NHCO-5. The TEM and HRTEM images of f,g) P0 and h,i) NHCO-5. j) STEM-EDS mapping of Ni, Co, Mn, and O elements of NHCO-5 samples. Figure 2. a) The XRD patterns of P0 and NHCO-5 samples with the enlarged images of (003), (101), and (104) peaks, respectively. Refined XRD data of b) P0 and c) NHCO-5. Raman spectra of d) P0 and e) NHCO-5. The TEM and HRTEM images of f,g) P0 and h,i) NHCO-5. j) STEM-EDS mapping of Ni, Co, Mn, and O elements of NHCO-5 samples. 3 6 6 46 #/texts/42 section_header body_heading False low body_heading body_heading False None body_zone column_1_of_2 1 2 p3:body_zone:column_1_of_2:white [255, 255, 255] white False False [50.81, 681.93, 122.45, 10.25] 2. Results and Discussion 2. Results and Discussion 2. Results and Discussion 2. Results and Discussion 3 9 8 48 #/texts/44 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_1_of_2 1 2 p3:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 3 10 10 50 #/texts/45 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_2_of_2 2 2 p3:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [266.69, 744.38, 64.3, 8.02] 2304065 (3 of 11) 2304065 (3 of 11) 2304065 (3 of 11) 2304065 (3 of 11) 3 11 11 51 #/texts/46 page_footer page_footer False low docling_page_footer docling_page_footer True p3:body_region:0 bottom_margin column_2_of_2 2 2 p3:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [469.66, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 4 1 1 52 #/texts/43#prov2 text page_margin_header False low page_margin_header page_margin_header True p4:body_region:0 top_margin column_1_of_2 1 2 p4:top_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 4 4 4 55 #/texts/48 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_page_footer True p4:body_region:0 bottom_margin column_1_of_2 1 2 p4:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 4 9 5 56 #/texts/53#prov0 text reference False low empty_after_cleaning empty_after_cleaning False None top_margin column_2_of_2 2 2 p4:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 4 5 6 57 #/texts/49 text page_margin_header False low page_margin_header page_margin_header True p4:body_region:1 top_margin column_2_of_2 2 2 p4:top_margin:column_2_of_2:white [255, 255, 255] white False False [469.62, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 4 10 10 61 #/texts/54 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_2_of_2 2 2 p4:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [263.85, 744.38, 64.3, 8.02] 2304065 (4 of 11) 2304065 (4 of 11) 2304065 (4 of 11) 2304065 (4 of 11) 4 11 11 62 #/texts/55 page_footer page_footer False low docling_page_footer docling_page_footer True p4:body_region:1 bottom_margin column_2_of_2 2 2 p4:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [466.82, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 5 1 1 63 #/texts/53#prov1 text page_margin_header False low page_margin_header page_margin_header True p5:body_region:0 top_margin column_1_of_2 1 2 p5:top_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 5 2 2 64 #/texts/56 page_header page_header False low docling_page_header docling_page_header False None top_margin column_2_of_2 2 2 p5:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 5 4 3 65 #/texts/58 text page_margin_header False low page_margin_header page_margin_header True p5:body_region:1 top_margin column_2_of_2 2 2 p5:top_margin:column_2_of_2:white [255, 255, 255] white False False [472.46, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 5 3 4 66 #/texts/57 caption caption False low outside_body_flow_caption outside_body_flow_caption False None page_body column_1_of_2 1 2 p5:page_body:column_1_of_2:white [255, 255, 255] white False False [50.81, 486.36, 496.05, 16.66] Figure 3. High-resolution XPS spectra of O 1s for a) P0 and b) NHCO-5. c) EPR spectra of P0 and NHCO-5. d) Normalized O K-edge sXAS spectra of P0 and NHCO-5. The XPS spectra of Mn 2p for e) P0 and f) NHCO-5. g) The XPS … Figure 3. High-resolution XPS spectra of O 1s for a) P0 and b) NHCO-5. c) EPR spectra of P0 and NHCO-5. d) Normalized O K-edge sXAS spectra of P0 and NHCO-5. The XPS spectra of Mn 2p for e) P0 and f) NHCO-5. g) The XPS … Figure 3. High-resolution XPS spectra of O 1s for a) P0 and b) NHCO-5. c) EPR spectra of P0 and NHCO-5. d) Normalized O K-edge sXAS spectra of P0 and NHCO-5. The XPS spectra of Mn 2p for e) P0 and f) NHCO-5. g) The XPS spectra of Mn 3s for P0, NHCO-3, NHCO-5, and NHCO-8. Figure 3. High-resolution XPS spectra of O 1s for a) P0 and b) NHCO-5. c) EPR spectra of P0 and NHCO-5. d) Normalized O K-edge sXAS spectra of P0 and NHCO-5. The XPS spectra of Mn 2p for e) P0 and f) NHCO-5. g) The XPS spectra of Mn 3s for P0, NHCO-3, NHCO-5, and NHCO-8. 5 8 6 68 #/texts/61 page_footer page_footer False low docling_page_footer docling_page_footer True p5:body_region:0 bottom_margin column_1_of_2 1 2 p5:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 5 9 9 71 #/texts/62 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_2_of_2 2 2 p5:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [266.69, 744.38, 64.3, 8.02] 2304065 (5 of 11) 2304065 (5 of 11) 2304065 (5 of 11) 2304065 (5 of 11) 5 10 10 72 #/texts/63 page_footer page_footer False low docling_page_footer docling_page_footer True p5:body_region:1 bottom_margin column_2_of_2 2 2 p5:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [469.66, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 6 3 1 73 #/texts/64 page_header page_header False low docling_page_header docling_page_header True p6:body_region:0 top_margin column_1_of_2 1 2 p6:top_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 6 4 2 74 #/texts/65 page_header page_header False low docling_page_header docling_page_header False None top_margin column_2_of_2 2 2 p6:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 6 6 3 75 #/texts/67 section_header metadata False low outside_body_flow_metadata_line outside_body_flow_metadata_line True p6:body_region:1 top_margin column_2_of_2 2 2 p6:top_margin:column_2_of_2:white [255, 255, 255] white False False [469.62, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 6 5 4 76 #/texts/66 caption caption False low outside_body_flow_caption outside_body_flow_caption False None page_body column_1_of_2 1 2 p6:page_body:column_1_of_2:white [255, 255, 255] white False False [47.98, 482.35, 496.08, 35.6] Figure 4. The electrochemical performance of P0 and NHCO-5 electrodes: charge-discharge curves of a) P0 electrode and b) NHCO-5 electrode. c) The rate performance. d) Cycling performance. The initial charge and discharg… Figure 4. The electrochemical performance of P0 and NHCO-5 electrodes: charge-discharge curves of a) P0 electrode and b) NHCO-5 electrode. c) The rate performance. d) Cycling performance. The initial charge and discharg… Figure 4. The electrochemical performance of P0 and NHCO-5 electrodes: charge-discharge curves of a) P0 electrode and b) NHCO-5 electrode. c) The rate performance. d) Cycling performance. The initial charge and discharge curves at e) 3 C and f) 5 C fast charging rate after three cycle activation. g) Constant current and voltage of charging capacity obtained from the 1st, 50th, and 100th at 5 C charging rate. h) Charging SOC versus time curves at 3 C and 5 C. i) Cycling performance at 5 C charging rate and 1 C discharge rate. Figure 4. The electrochemical performance of P0 and NHCO-5 electrodes: charge-discharge curves of a) P0 electrode and b) NHCO-5 electrode. c) The rate performance. d) Cycling performance. The initial charge and discharge curves at e) 3 C and f) 5 C fast charging rate after three cycle activation. g) Constant current and voltage of charging capacity obtained from the 1st, 50th, and 100th at 5 C charging rate. h) Charging SOC versus time curves at 3 C and 5 C. i) Cycling performance at 5 C charging rate and 1 C discharge rate. 6 1 5 77 #/texts/60#prov1 text back_matter_heading False low back_matter_heading back_matter_heading stop_trigger True p6:body_region:0 bottom_margin column_1_of_2 1 2 p6:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 536.6, 240.96, 183.79] Supporting Information, shows the first and last charge and discharge curves at 3 and 5 C charging rate, respectively. There is no obvious difference as charged at 3 C for the two electrodes. However, P0 electrode shows… Supporting Information, shows the first and last charge and discharge curves at 3 and 5 C charging rate, respectively. There is no obvious difference as charged at 3 C for the two electrodes. However, P0 electrode shows… Supporting Information, shows the first and last charge and discharge curves at 3 and 5 C charging rate, respectively. There is no obvious difference as charged at 3 C for the two electrodes. However, P0 electrode shows larger voltage polarization as charged at 5 C in comparison with NHCO-5 electrode, indicating surface defect and spinel phase can reduce voltage polarization. The capacity of P0 and NHCO-5 electrodes obtained from constant current charging (CC-Capacity) and constant voltage charging (CV-Capacity) section at 3 and 5 C rate are shown in Figure S5e, Supporting Information; Figure 4 g, respectively. To charge more capacity during the constant current charging state can shorten the total charging time. The charging capacity of P0 and NHCO-5 electrodes driving from CC-Capacity and CV-Capacity show less difference as charged at 3 C. However, higher capacity of NHCO5 electrode can be obtained from the CC-Capacity section than P0 electrode at 5 C fast-charging rate. Consequently, the time to charge 80% SOC capacity of NHCO-5 can be shortened to 9.4 min Supporting Information, shows the first and last charge and discharge curves at 3 and 5 C charging rate, respectively. There is no obvious difference as charged at 3 C for the two electrodes. However, P0 electrode shows larger voltage polarization as charged at 5 C in comparison with NHCO-5 electrode, indicating surface defect and spinel phase can reduce voltage polarization. The capacity of P0 and NHCO-5 electrodes obtained from constant current charging (CC-Capacity) and constant voltage charging (CV-Capacity) section at 3 and 5 C rate are shown in Figure S5e, Supporting Information; Figure 4 g, respectively. To charge more capacity during the constant current charging state can shorten the total charging time. The charging capacity of P0 and NHCO-5 electrodes driving from CC-Capacity and CV-Capacity show less difference as charged at 3 C. However, higher capacity of NHCO5 electrode can be obtained from the CC-Capacity section than P0 electrode at 5 C fast-charging rate. Consequently, the time to charge 80% SOC capacity of NHCO-5 can be shortened to 9.4 min 6 7 6 78 #/texts/68 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p6:body_region:0 bottom_margin column_1_of_2 1 2 p6:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 6 2 7 79 #/texts/60#prov2 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p6:body_region:1 bottom_margin column_2_of_2 2 2 p6:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [303.09, 536.61, 240.96, 183.78] and less than P0 ( ≈ 11 min), as seen in the Figure 4h. Figure S5f, Supporting Information; Figure 5 i show the comparison of the cycling performance of P0 and NHCO-5 electrodes at 3 and 5 C fast-charging rate. P0 and N… and less than P0 ( ≈ 11 min), as seen in the Figure 4h. Figure S5f, Supporting Information; Figure 5 i show the comparison of the cycling performance of P0 and NHCO-5 electrodes at 3 and 5 C fast-charging rate. P0 and N… and less than P0 ( ≈ 11 min), as seen in the Figure 4h. Figure S5f, Supporting Information; Figure 5 i show the comparison of the cycling performance of P0 and NHCO-5 electrodes at 3 and 5 C fast-charging rate. P0 and NHCO-5 electrodes have similar initial charging capacity and show little difference on capacity loss as cycled at 3 C fast-charging rate after 100 cycles. Nevertheless, NHCO-5 electrode still can deliver high reversible initial discharged capacity of ≈ 250 mAh · g -1 and obtain a reversible capacity of 189.4 mAh · g -1 as cycled at 5 C after 150 cycles. These results have clearly demonstrated that the 5 C fast charging capability of LRMOis enhanced after ammonium oxalate treatment. The surface spinel phase provides a 3D lithium-ion channel with fast Li + diffusion, and oxygen vacancies can synergistically improve the electronic and ionic conductivity of LRMO. [9b,17c] Therefore, the increasing fast-charging capability is ascribed to the enhanced diffusion kinetic and fast charge transfer after the local electronic structure modulation via surface defect engineering. [ 24] and less than P0 ( ≈ 11 min), as seen in the Figure 4h. Figure S5f, Supporting Information; Figure 5 i show the comparison of the cycling performance of P0 and NHCO-5 electrodes at 3 and 5 C fast-charging rate. P0 and NHCO-5 electrodes have similar initial charging capacity and show little difference on capacity loss as cycled at 3 C fast-charging rate after 100 cycles. Nevertheless, NHCO-5 electrode still can deliver high reversible initial discharged capacity of ≈ 250 mAh · g -1 and obtain a reversible capacity of 189.4 mAh · g -1 as cycled at 5 C after 150 cycles. These results have clearly demonstrated that the 5 C fast charging capability of LRMOis enhanced after ammonium oxalate treatment. The surface spinel phase provides a 3D lithium-ion channel with fast Li + diffusion, and oxygen vacancies can synergistically improve the electronic and ionic conductivity of LRMO. [9b,17c] Therefore, the increasing fast-charging capability is ascribed to the enhanced diffusion kinetic and fast charge transfer after the local electronic structure modulation via surface defect engineering. [ 24] 6 8 8 80 #/texts/69 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop False None bottom_margin column_2_of_2 2 2 p6:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [263.85, 744.38, 64.3, 8.02] 2304065 (6 of 11) 2304065 (6 of 11) 2304065 (6 of 11) 2304065 (6 of 11) 6 9 9 81 #/texts/70 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p6:body_region:1 bottom_margin column_2_of_2 2 2 p6:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [466.82, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 7 2 1 82 #/texts/72 text page_margin_header False low after_back_matter_stop after_back_matter_stop after_stop True p7:body_region:0 top_margin column_1_of_2 1 2 p7:top_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 7 1 2 83 #/texts/71 page_header page_header False low after_back_matter_stop after_back_matter_stop after_stop False None top_margin column_2_of_2 2 2 p7:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 7 4 3 84 #/texts/74 section_header metadata False low after_back_matter_stop after_back_matter_stop after_stop True p7:body_region:1 top_margin column_2_of_2 2 2 p7:top_margin:column_2_of_2:white [255, 255, 255] white False False [472.46, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 7 3 4 85 #/texts/73 caption caption False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_1_of_2 1 2 p7:page_body:column_1_of_2:white [255, 255, 255] white False False [50.81, 561.36, 496.06, 35.6] Figure 5. The O 1s XPS spectra at different charging/discharging states of a) P0 electrode and b) NHCO-5 electrode. The normalized O pre K-edge and Mn pre L-edge XAS spectra for c,e) P0 electrode and d,f) NHCO-5 electro… Figure 5. The O 1s XPS spectra at different charging/discharging states of a) P0 electrode and b) NHCO-5 electrode. The normalized O pre K-edge and Mn pre L-edge XAS spectra for c,e) P0 electrode and d,f) NHCO-5 electro… Figure 5. The O 1s XPS spectra at different charging/discharging states of a) P0 electrode and b) NHCO-5 electrode. The normalized O pre K-edge and Mn pre L-edge XAS spectra for c,e) P0 electrode and d,f) NHCO-5 electrode. Ex situ XRD patterns of g) P0 electrode and h) NHCO-5 electrode in the initial cyclic process. Density of states of the i) P0 and j) NHCO-5 sample. Maps of ELF for the k) P0 and l) NHCO-5; circles show there are more delocalized electrons around the transition metal. Figure 5. The O 1s XPS spectra at different charging/discharging states of a) P0 electrode and b) NHCO-5 electrode. The normalized O pre K-edge and Mn pre L-edge XAS spectra for c,e) P0 electrode and d,f) NHCO-5 electrode. Ex situ XRD patterns of g) P0 electrode and h) NHCO-5 electrode in the initial cyclic process. Density of states of the i) P0 and j) NHCO-5 sample. Maps of ELF for the k) P0 and l) NHCO-5; circles show there are more delocalized electrons around the transition metal. 7 5 5 86 #/texts/75#prov0 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p7:body_region:0 bottom_margin column_1_of_2 1 2 p7:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 624.27, 240.97, 96.11] As far as mechanisms of the improved rate performance and fast-charging capability are concerned, previous reports have demonstrated that oxygen redox chemistry results in sluggish kinetics with low Li + diffusion rate … As far as mechanisms of the improved rate performance and fast-charging capability are concerned, previous reports have demonstrated that oxygen redox chemistry results in sluggish kinetics with low Li + diffusion rate … As far as mechanisms of the improved rate performance and fast-charging capability are concerned, previous reports have demonstrated that oxygen redox chemistry results in sluggish kinetics with low Li + diffusion rate and high charge-transfer resistance. [ 5c,25] Therefore, tuning anionic redox chemistry plays a vital role in raising the electrochemical performance with excellent fast-charging capability. EIS and the GITT were employed to measure the kinetic variation before and after the electronic structure modulation. Figure S6a, Supporting Information As far as mechanisms of the improved rate performance and fast-charging capability are concerned, previous reports have demonstrated that oxygen redox chemistry results in sluggish kinetics with low Li + diffusion rate and high charge-transfer resistance. [ 5c,25] Therefore, tuning anionic redox chemistry plays a vital role in raising the electrochemical performance with excellent fast-charging capability. EIS and the GITT were employed to measure the kinetic variation before and after the electronic structure modulation. Figure S6a, Supporting Information 7 7 6 87 #/texts/76 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p7:body_region:0 bottom_margin column_1_of_2 1 2 p7:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 7 6 7 88 #/texts/75#prov1 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p7:body_region:1 bottom_margin column_2_of_2 2 2 p7:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [305.92, 624.27, 240.96, 96.11] shows the EIS Nyquist plots of P0 and NHCO-5 electrodes before electrochemical cycles. All the curves include three regions. Asmall interrupt in the high frequency represents the Ohmic resistance ( R s ) of the cell. On… shows the EIS Nyquist plots of P0 and NHCO-5 electrodes before electrochemical cycles. All the curves include three regions. Asmall interrupt in the high frequency represents the Ohmic resistance ( R s ) of the cell. On… shows the EIS Nyquist plots of P0 and NHCO-5 electrodes before electrochemical cycles. All the curves include three regions. Asmall interrupt in the high frequency represents the Ohmic resistance ( R s ) of the cell. One semicircle in the middle-high frequency represents the charge transfer resistance ( R ct ). A sloping line in the low-frequency regions represents the Warburg impedance ( W ). [ 10] The related fitting parameters are listed in Table S2, Supporting Information. The R ct of NHCO-5 is 7.525 Ω smaller than P0 (9.660 Ω ), demonstrating a low charge transfer shows the EIS Nyquist plots of P0 and NHCO-5 electrodes before electrochemical cycles. All the curves include three regions. Asmall interrupt in the high frequency represents the Ohmic resistance ( R s ) of the cell. One semicircle in the middle-high frequency represents the charge transfer resistance ( R ct ). A sloping line in the low-frequency regions represents the Warburg impedance ( W ). [ 10] The related fitting parameters are listed in Table S2, Supporting Information. The R ct of NHCO-5 is 7.525 Ω smaller than P0 (9.660 Ω ), demonstrating a low charge transfer 7 8 8 89 #/texts/77 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop False None bottom_margin column_2_of_2 2 2 p7:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [266.69, 744.38, 64.3, 8.02] 2304065 (7 of 11) 2304065 (7 of 11) 2304065 (7 of 11) 2304065 (7 of 11) 7 9 9 90 #/texts/78 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p7:body_region:1 bottom_margin column_2_of_2 2 2 p7:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [469.66, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 8 1 1 91 #/texts/79 section_header metadata False low after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:0 top_margin column_1_of_2 1 2 p8:top_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 8 2 2 92 #/texts/80 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:0 page_body column_1_of_2 1 2 p8:page_body:column_1_of_2:white [255, 255, 255] white False False [47.97, 76.43, 240.96, 172.83] impedance of NHCO-5 with surface defect construction. [17c] The GITT measurement is also conducted to compare the kinetic performance of P0 and NHCO-5 electrodes after five cycles at 0.04 C (Figure S6b, Supporting Infor… impedance of NHCO-5 with surface defect construction. [17c] The GITT measurement is also conducted to compare the kinetic performance of P0 and NHCO-5 electrodes after five cycles at 0.04 C (Figure S6b, Supporting Infor… impedance of NHCO-5 with surface defect construction. [17c] The GITT measurement is also conducted to compare the kinetic performance of P0 and NHCO-5 electrodes after five cycles at 0.04 C (Figure S6b, Supporting Information). Figure S6c,d, Supporting Information, show the calculated D Li + of the charging and discharging process according to the Equation (S2), Supporting Information. The D Li + of the NHCO-5 electrode in 'sluggish kinetic region' ( < 3.5 V and > 4.0 V) is increased in comparison with P0. The average D Li + of NHCO-5 electrode in 'sluggish kinetic region' is 8.70 × 10 -10 cm 2 s -1 and 6.40 × 10 -10 cm 2 s -1 during charging process and discharging process respectively, which is larger than the values of 5.97 × 10 -10 cm 2 s -1 and4.56 × 10 -10 cm 2 s -1 for P0 electrode. The improved lithium diffusion rate and fast charge transfer, ascribing to the local electronic structure modulation, result in boosting the rate performance and fast-charging capability of LRMO. impedance of NHCO-5 with surface defect construction. [17c] The GITT measurement is also conducted to compare the kinetic performance of P0 and NHCO-5 electrodes after five cycles at 0.04 C (Figure S6b, Supporting Information). Figure S6c,d, Supporting Information, show the calculated D Li + of the charging and discharging process according to the Equation (S2), Supporting Information. The D Li + of the NHCO-5 electrode in 'sluggish kinetic region' ( < 3.5 V and > 4.0 V) is increased in comparison with P0. The average D Li + of NHCO-5 electrode in 'sluggish kinetic region' is 8.70 × 10 -10 cm 2 s -1 and 6.40 × 10 -10 cm 2 s -1 during charging process and discharging process respectively, which is larger than the values of 5.97 × 10 -10 cm 2 s -1 and4.56 × 10 -10 cm 2 s -1 for P0 electrode. The improved lithium diffusion rate and fast charge transfer, ascribing to the local electronic structure modulation, result in boosting the rate performance and fast-charging capability of LRMO. 8 3 3 93 #/texts/81 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:0 bottom_margin column_1_of_2 1 2 p8:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.97, 251.77, 240.97, 468.71] The O 1s XPS spectra of P0 and NHCO-5 electrodes at charging and discharging state in the first cycle are conducted for exploring the mechanisms of oxygen redox (Figure 5a,b). Three obvious peaks appearing at ≈ 529.5, ≈… The O 1s XPS spectra of P0 and NHCO-5 electrodes at charging and discharging state in the first cycle are conducted for exploring the mechanisms of oxygen redox (Figure 5a,b). Three obvious peaks appearing at ≈ 529.5, ≈… The O 1s XPS spectra of P0 and NHCO-5 electrodes at charging and discharging state in the first cycle are conducted for exploring the mechanisms of oxygen redox (Figure 5a,b). Three obvious peaks appearing at ≈ 529.5, ≈ 531.9, and ≈ 533.2 eV contributing to the lattice oxygen, oxygenated deposited species, and weak electrolyte oxidation, respectively, whether in the charging state of 4.8 V or discharging state 2.0 V, can be found. [ 26] However, an additional peak at ≈ 530.5 eV appears in both the XPS spectra of P0 and NHCO-5 electrodes at the charging state of 4.8 V, contributing to the preoxo-like O 2 n -( n < 2) with a lower electronic density in comparison with lattice oxygen (O 2 -). [ 9a] Nevertheless, compared with P0 electrode, the larger area ratio of O 2 n -peak in NHCO-5 electrode indicates more reversible anionic redox participation in charge compensation. It is worth noting that the increasing content of electrolyte oxides at 4.8 V for both P0 and NHCO-5 electrodes can be ascribed to the side reaction and decomposition of electrolyte at high voltage. [ 27] The disappearance of the preoxo-like O 2 n -peak after discharging to 2.0 V indicates the O 2 n -can convert back to O 2 -. [ 28] These results perfectly demonstrate that the existence of oxygen vacancies in the NHCO5 electrode can greatly stimulate the reversible anionic redox activity. In addition, soft X-ray absorption spectroscopy (sXAS) can prove the reversible oxygen redox and irreversible oxygen release. The total d electronic holes in the hybridized O 2p-TM 3d can be reflected in the pre-edge peaks of O K-edge spectra at ≈ 530 eV. The pre-edge peak of P0 electrode largely reduces during charging process, which may be ascribed to the Mn reduction resulting from oxygen loss (Figure 5c). Previous works have proved that the oxidation of lattice oxygen can trigger the charge transfer from oxygen to TM with release of oxygen. [ 29] The decreasing density of electronic holes in O 2p-Mn 3d due to the reduction of Mn can weaken the O k-edge pre-edge peaks. However, the intensity of pre-edge peaks for charged NHCO-5 electrode shows no obvious changes in comparison with the initial state, indicating the inhibition of oxygen release (Figure 5d). Besides, a new peak located at around 530.5 eV in NHCO-5 electrode is speculated to be the characteristic peak of reversible anionic redox (O 2 -to O 2 n -), conforming to the results of XPS. [5b] Figure 5e,f shows the Mn L-edge XAS spectra at different states for P0 and NHCO-5electrodes. Compared with NHCO-5 electrode, the peak at around 646.5 eV contributes to Mn 4 + for P0 electrode shifts more to low energy, indicating the reduction of Mn due to the irreversible oxygen release. [ 19] Therefore, both the XPS and XAS The O 1s XPS spectra of P0 and NHCO-5 electrodes at charging and discharging state in the first cycle are conducted for exploring the mechanisms of oxygen redox (Figure 5a,b). Three obvious peaks appearing at ≈ 529.5, ≈ 531.9, and ≈ 533.2 eV contributing to the lattice oxygen, oxygenated deposited species, and weak electrolyte oxidation, respectively, whether in the charging state of 4.8 V or discharging state 2.0 V, can be found. [ 26] However, an additional peak at ≈ 530.5 eV appears in both the XPS spectra of P0 and NHCO-5 electrodes at the charging state of 4.8 V, contributing to the preoxo-like O 2 n -( n < 2) with a lower electronic density in comparison with lattice oxygen (O 2 -). [ 9a] Nevertheless, compared with P0 electrode, the larger area ratio of O 2 n -peak in NHCO-5 electrode indicates more reversible anionic redox participation in charge compensation. It is worth noting that the increasing content of electrolyte oxides at 4.8 V for both P0 and NHCO-5 electrodes can be ascribed to the side reaction and decomposition of electrolyte at high voltage. [ 27] The disappearance of the preoxo-like O 2 n -peak after discharging to 2.0 V indicates the O 2 n -can convert back to O 2 -. [ 28] These results perfectly demonstrate that the existence of oxygen vacancies in the NHCO5 electrode can greatly stimulate the reversible anionic redox activity. In addition, soft X-ray absorption spectroscopy (sXAS) can prove the reversible oxygen redox and irreversible oxygen release. The total d electronic holes in the hybridized O 2p-TM 3d can be reflected in the pre-edge peaks of O K-edge spectra at ≈ 530 eV. The pre-edge peak of P0 electrode largely reduces during charging process, which may be ascribed to the Mn reduction resulting from oxygen loss (Figure 5c). Previous works have proved that the oxidation of lattice oxygen can trigger the charge transfer from oxygen to TM with release of oxygen. [ 29] The decreasing density of electronic holes in O 2p-Mn 3d due to the reduction of Mn can weaken the O k-edge pre-edge peaks. However, the intensity of pre-edge peaks for charged NHCO-5 electrode shows no obvious changes in comparison with the initial state, indicating the inhibition of oxygen release (Figure 5d). Besides, a new peak located at around 530.5 eV in NHCO-5 electrode is speculated to be the characteristic peak of reversible anionic redox (O 2 -to O 2 n -), conforming to the results of XPS. [5b] Figure 5e,f shows the Mn L-edge XAS spectra at different states for P0 and NHCO-5electrodes. Compared with NHCO-5 electrode, the peak at around 646.5 eV contributes to Mn 4 + for P0 electrode shifts more to low energy, indicating the reduction of Mn due to the irreversible oxygen release. [ 19] Therefore, both the XPS and XAS 8 4 4 94 #/texts/82 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:0 bottom_margin column_1_of_2 1 2 p8:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 8 9 5 95 #/texts/87#prov0 text reference False low after_back_matter_stop after_back_matter_stop after_stop False None top_margin column_2_of_2 2 2 p8:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 8 5 6 96 #/texts/83 text page_margin_header False low after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:1 top_margin column_2_of_2 2 2 p8:top_margin:column_2_of_2:white [255, 255, 255] white False False [469.62, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 8 6 7 97 #/texts/84 text body_heading False low after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:1 page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [303.09, 76.42, 240.93, 30.37] results successfully demonstrate the surface oxygen vacancies, and spinel phase can enhance the reversible anionic redox and suppress irreversible oxygen release. results successfully demonstrate the surface oxygen vacancies, and spinel phase can enhance the reversible anionic redox and suppress irreversible oxygen release. results successfully demonstrate the surface oxygen vacancies, and spinel phase can enhance the reversible anionic redox and suppress irreversible oxygen release. results successfully demonstrate the surface oxygen vacancies, and spinel phase can enhance the reversible anionic redox and suppress irreversible oxygen release. 8 7 8 98 #/texts/85 text back_matter_text False low after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:1 page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [303.09, 109.3, 240.96, 293.38] Ex situ XRD is applied to figure out the influence of the surface treatment on the crystal structural evolution of LRMO. The associated results are displayed in Figure 5g,h. The shift of (003) peak can directly reflect … Ex situ XRD is applied to figure out the influence of the surface treatment on the crystal structural evolution of LRMO. The associated results are displayed in Figure 5g,h. The shift of (003) peak can directly reflect … Ex situ XRD is applied to figure out the influence of the surface treatment on the crystal structural evolution of LRMO. The associated results are displayed in Figure 5g,h. The shift of (003) peak can directly reflect the changes of lattice parameter c value. Both P0 and NHCO-5 electrodes show similar shift direction during the charging and discharging process. Before the voltage is charged to 4.5 V, the peak of (003) shifts to a low angle, indicating the increasing crystal plane spacing due to the increasing electrostatic repulsion and the expansion of the c -axis after the removal of Li + from the LiTMO 2 phase. [3a] After the voltage reaches to 4.8 V, the peak of (003) shifts to a high angle, which derives from the activation of Li 2 MnO3 phase. The lattice oxygen release of Li 2 MnO3 phase causes the decrease of electrostatic repulsion, inducing the TM to migrate into the Li layer. [ 30] During the discharging process, the peak shifts to left due to the expansion of the crystal plane spacing after the intercalation of Li + . According to the above analysis, the shift angle of the (003) peak for NHCO-5electrode is always smaller than that of P0 electrode during both the charging and discharging process, indicating better structural stability and less oxygen release. In addition, the (003) peak of NHCO-5 electrode at full discharging state is closer to the initial position in comparison with P0 electrode, demonstrating that less irreversible phase transformation occurs in the NHCO-5 electrode. Therefore, these results successfully prove that oxygen vacancies can enhance the structural stability and suppress lattice oxygen loss, which is the foundation for achieving fast-charging properties with reversible oxygen redox. Ex situ XRD is applied to figure out the influence of the surface treatment on the crystal structural evolution of LRMO. The associated results are displayed in Figure 5g,h. The shift of (003) peak can directly reflect the changes of lattice parameter c value. Both P0 and NHCO-5 electrodes show similar shift direction during the charging and discharging process. Before the voltage is charged to 4.5 V, the peak of (003) shifts to a low angle, indicating the increasing crystal plane spacing due to the increasing electrostatic repulsion and the expansion of the c -axis after the removal of Li + from the LiTMO 2 phase. [3a] After the voltage reaches to 4.8 V, the peak of (003) shifts to a high angle, which derives from the activation of Li 2 MnO3 phase. The lattice oxygen release of Li 2 MnO3 phase causes the decrease of electrostatic repulsion, inducing the TM to migrate into the Li layer. [ 30] During the discharging process, the peak shifts to left due to the expansion of the crystal plane spacing after the intercalation of Li + . According to the above analysis, the shift angle of the (003) peak for NHCO-5electrode is always smaller than that of P0 electrode during both the charging and discharging process, indicating better structural stability and less oxygen release. In addition, the (003) peak of NHCO-5 electrode at full discharging state is closer to the initial position in comparison with P0 electrode, demonstrating that less irreversible phase transformation occurs in the NHCO-5 electrode. Therefore, these results successfully prove that oxygen vacancies can enhance the structural stability and suppress lattice oxygen loss, which is the foundation for achieving fast-charging properties with reversible oxygen redox. 8 8 9 99 #/texts/86 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:1 bottom_margin column_2_of_2 2 2 p8:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [303.09, 405.2, 240.96, 315.29] To further demonstrate and understand the influencing mechanisms of surface defect structure on the electrochemical performance, first principles calculations are conducted for studying the electronic structure of P0 an… To further demonstrate and understand the influencing mechanisms of surface defect structure on the electrochemical performance, first principles calculations are conducted for studying the electronic structure of P0 an… To further demonstrate and understand the influencing mechanisms of surface defect structure on the electrochemical performance, first principles calculations are conducted for studying the electronic structure of P0 and NHCO-5 according to the density functional theory method (DFT). Figure S7a,b, Supporting Information, shows the computational model, and one oxygen vacancy is chosen in the model of NHCO-5. According to this model, the density of states of O 2p and TM 3d band for P0 and NHCO-5 are first computed. Figure 5i,j shows the corresponding computational results. The obvious electron density of TM 3d and O 2p close to the Femi energy indicate that both the P0 and NHCO-5 possess good electrical conductivity. [10] Nevertheless, a careful comparison shows that the density of O 2p band of NHCO-5 decreases in comparison with P0. The decrease of O 2p density can promote lattice oxygen to participate in the charge compensation stably and preclude the oxygen loss, contributing to the enhanced reversible anionic redox. [ 31] Figure 5k,l displays the isosurface images of electron localization function (ELF), which can clearly depict the cationic charge compensation. The red and light blue regions represent the lattice electrons and active covalent electrons, respectively. The P0 show more localized electrons around the oxygen and transition metal (Figure 5k). In contrast, more delocalized electrons appear around Mn in the NHCO-5, as shown by the red dashed coil in Figure 5l. The change of the local electronic structure around the Mn ion can improve the Mn octahedral distortion reversibility and promote the reduced Mn to participate in the charge compensation. [28,32] Therefore, the surface oxygen defect can modulate the electronic structure around oxygen and Mn, resulting in not only To further demonstrate and understand the influencing mechanisms of surface defect structure on the electrochemical performance, first principles calculations are conducted for studying the electronic structure of P0 and NHCO-5 according to the density functional theory method (DFT). Figure S7a,b, Supporting Information, shows the computational model, and one oxygen vacancy is chosen in the model of NHCO-5. According to this model, the density of states of O 2p and TM 3d band for P0 and NHCO-5 are first computed. Figure 5i,j shows the corresponding computational results. The obvious electron density of TM 3d and O 2p close to the Femi energy indicate that both the P0 and NHCO-5 possess good electrical conductivity. [10] Nevertheless, a careful comparison shows that the density of O 2p band of NHCO-5 decreases in comparison with P0. The decrease of O 2p density can promote lattice oxygen to participate in the charge compensation stably and preclude the oxygen loss, contributing to the enhanced reversible anionic redox. [ 31] Figure 5k,l displays the isosurface images of electron localization function (ELF), which can clearly depict the cationic charge compensation. The red and light blue regions represent the lattice electrons and active covalent electrons, respectively. The P0 show more localized electrons around the oxygen and transition metal (Figure 5k). In contrast, more delocalized electrons appear around Mn in the NHCO-5, as shown by the red dashed coil in Figure 5l. The change of the local electronic structure around the Mn ion can improve the Mn octahedral distortion reversibility and promote the reduced Mn to participate in the charge compensation. [28,32] Therefore, the surface oxygen defect can modulate the electronic structure around oxygen and Mn, resulting in not only 8 10 10 100 #/texts/88 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop False None bottom_margin column_2_of_2 2 2 p8:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [263.85, 744.38, 64.3, 8.02] 2304065 (8 of 11) 2304065 (8 of 11) 2304065 (8 of 11) 2304065 (8 of 11) 8 11 11 101 #/texts/89 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p8:body_region:1 bottom_margin column_2_of_2 2 2 p8:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [466.82, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 9 1 1 102 #/texts/87#prov1 text page_margin_header False low after_back_matter_stop after_back_matter_stop after_stop True p9:body_region:0 top_margin column_1_of_2 1 2 p9:top_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 9 4 2 103 #/texts/90 page_header page_header False low after_back_matter_stop after_back_matter_stop after_stop False None top_margin column_2_of_2 2 2 p9:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 9 2 3 104 #/texts/87#prov2 text page_margin_header False low after_back_matter_stop after_back_matter_stop after_stop True p9:body_region:1 top_margin column_2_of_2 2 2 p9:top_margin:column_2_of_2:white [255, 255, 255] white False False [472.46, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 9 5 4 105 #/texts/91 caption caption False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_1_of_2 1 2 p9:page_body:column_1_of_2:white [255, 255, 255] white False False [50.81, 473.35, 496.06, 16.67] Figure 6. The analysis of P0 and NHCO-5 electrodes after 200 cycles: a) The comparison of XRD pattern. b) Raman spectra. The SEM images of c) P0 and e) NHCO-5. HRTEM images of d) P0 and f) NHCO-5. g) The schematic of th… Figure 6. The analysis of P0 and NHCO-5 electrodes after 200 cycles: a) The comparison of XRD pattern. b) Raman spectra. The SEM images of c) P0 and e) NHCO-5. HRTEM images of d) P0 and f) NHCO-5. g) The schematic of th… Figure 6. The analysis of P0 and NHCO-5 electrodes after 200 cycles: a) The comparison of XRD pattern. b) Raman spectra. The SEM images of c) P0 and e) NHCO-5. HRTEM images of d) P0 and f) NHCO-5. g) The schematic of the crystal structure deterioration for P0 electrode. Figure 6. The analysis of P0 and NHCO-5 electrodes after 200 cycles: a) The comparison of XRD pattern. b) Raman spectra. The SEM images of c) P0 and e) NHCO-5. HRTEM images of d) P0 and f) NHCO-5. g) The schematic of the crystal structure deterioration for P0 electrode. 9 3 5 106 #/texts/87#prov3 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p9:body_region:0 page_body column_1_of_2 1 2 p9:page_body:column_1_of_2:white [255, 255, 255] white False False [50.81, 514.68, 240.95, 41.32] increasing electrical conductivity, facilitating lithium ion diffusion and fast charge transfer, but also suppressing oxygen release and promoting the charge compensation of both cationic and anionic redox. increasing electrical conductivity, facilitating lithium ion diffusion and fast charge transfer, but also suppressing oxygen release and promoting the charge compensation of both cationic and anionic redox. increasing electrical conductivity, facilitating lithium ion diffusion and fast charge transfer, but also suppressing oxygen release and promoting the charge compensation of both cationic and anionic redox. increasing electrical conductivity, facilitating lithium ion diffusion and fast charge transfer, but also suppressing oxygen release and promoting the charge compensation of both cationic and anionic redox. 9 6 6 107 #/texts/92 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p9:body_region:0 bottom_margin column_1_of_2 1 2 p9:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 558.52, 240.96, 161.87] To explore the structural evolution of P0 and NHCO-5 electrodes after 200 cycles, relevant characterizations were employed to study the changes of crystal structure and morphology. Figure 6 a shows the comparison of XRD… To explore the structural evolution of P0 and NHCO-5 electrodes after 200 cycles, relevant characterizations were employed to study the changes of crystal structure and morphology. Figure 6 a shows the comparison of XRD… To explore the structural evolution of P0 and NHCO-5 electrodes after 200 cycles, relevant characterizations were employed to study the changes of crystal structure and morphology. Figure 6 a shows the comparison of XRD results for P0 and NHCO-5 electrodes after cycling. The value of I (003) / I (104) for P0 is smaller than NHCO-5, indicating the higher degree of cation mixing due to the irreversible migration of transition metal ions. [17a] In addition, Raman spectroscopy was also used to detect the surface structural evolution after cycling and the corresponding results are displayed in Figure 6b. Two obvious peaks located at around 480 and 605 cm -1 contribute to the vibrations of the layered structure with R-3m spacing group. [ 33] Aweakpeak at about 430 cm -1 is assigned to the Li 2 MnO3 phase. The peak II at around 650 cm -1 of both samples is the evidence of the spinel/rock-salt structure due to the shortening of M-O To explore the structural evolution of P0 and NHCO-5 electrodes after 200 cycles, relevant characterizations were employed to study the changes of crystal structure and morphology. Figure 6 a shows the comparison of XRD results for P0 and NHCO-5 electrodes after cycling. The value of I (003) / I (104) for P0 is smaller than NHCO-5, indicating the higher degree of cation mixing due to the irreversible migration of transition metal ions. [17a] In addition, Raman spectroscopy was also used to detect the surface structural evolution after cycling and the corresponding results are displayed in Figure 6b. Two obvious peaks located at around 480 and 605 cm -1 contribute to the vibrations of the layered structure with R-3m spacing group. [ 33] Aweakpeak at about 430 cm -1 is assigned to the Li 2 MnO3 phase. The peak II at around 650 cm -1 of both samples is the evidence of the spinel/rock-salt structure due to the shortening of M-O 9 8 7 108 #/texts/94 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p9:body_region:0 bottom_margin column_1_of_2 1 2 p9:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [50.81, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 9 7 8 109 #/texts/93#prov0 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p9:body_region:1 bottom_margin column_2_of_2 2 2 p9:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [305.92, 513.64, 240.97, 206.75] bonds. [5b] The smaller area ratio of spinel-like component for NHCO-5 suggests that minor structural transformation occurs from layer to spinel/rock-salt phase. It is mainly ascribed to be the fact that surface defect … bonds. [5b] The smaller area ratio of spinel-like component for NHCO-5 suggests that minor structural transformation occurs from layer to spinel/rock-salt phase. It is mainly ascribed to be the fact that surface defect … bonds. [5b] The smaller area ratio of spinel-like component for NHCO-5 suggests that minor structural transformation occurs from layer to spinel/rock-salt phase. It is mainly ascribed to be the fact that surface defect and spinel-like phase can stabilize the crystal structure via suppressing oxygen release. What is more, the impedance changes of P0 and NHCO-5 electrodes after cycling are also detected, as shown in Figure S8a, Supporting Information. Compared with the EIS spectra of P0 and NHCO-5 electrodes before cycling, additional semicircle belonging to the impedance R f of cathode-electrolyte interphase (CEI) appears in the middle-high frequency after cycling. According to the equivalent circuit, the corresponding fitting parameters are listed in Table S2, Supporting Information. The impedance of CEI film and the charge transfer for NHCO-5 electrode are 8.81 and 36.28 Ω after cycling, respectively, lower than P0 electrode (10.01 and 40.09 Ω ), demonstrating better CEI film with low impedance and fast charge transfer for NHCO-5. The contents of Mn and Co elements deposited on the anode after cycling are quantitated by the ICP-MS. The corresponding results are shown in Figure bonds. [5b] The smaller area ratio of spinel-like component for NHCO-5 suggests that minor structural transformation occurs from layer to spinel/rock-salt phase. It is mainly ascribed to be the fact that surface defect and spinel-like phase can stabilize the crystal structure via suppressing oxygen release. What is more, the impedance changes of P0 and NHCO-5 electrodes after cycling are also detected, as shown in Figure S8a, Supporting Information. Compared with the EIS spectra of P0 and NHCO-5 electrodes before cycling, additional semicircle belonging to the impedance R f of cathode-electrolyte interphase (CEI) appears in the middle-high frequency after cycling. According to the equivalent circuit, the corresponding fitting parameters are listed in Table S2, Supporting Information. The impedance of CEI film and the charge transfer for NHCO-5 electrode are 8.81 and 36.28 Ω after cycling, respectively, lower than P0 electrode (10.01 and 40.09 Ω ), demonstrating better CEI film with low impedance and fast charge transfer for NHCO-5. The contents of Mn and Co elements deposited on the anode after cycling are quantitated by the ICP-MS. The corresponding results are shown in Figure 9 9 9 110 #/texts/95 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop False None bottom_margin column_2_of_2 2 2 p9:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [266.69, 744.38, 64.3, 8.02] 2304065 (9 of 11) 2304065 (9 of 11) 2304065 (9 of 11) 2304065 (9 of 11) 9 10 10 111 #/texts/96 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p9:body_region:1 bottom_margin column_2_of_2 2 2 p9:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [469.66, 745.82, 77.21, 6.3] ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH ©2023 Wiley-VCH GmbH 10 1 1 112 #/texts/93#prov1 text page_margin_header False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:0 top_margin column_1_of_2 1 2 p10:top_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 50.12, 120.78, 8.02] www.advancedsciencenews.com www.advancedsciencenews.com 10 2 2 113 #/texts/93#prov2 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:0 front_matter column_1_of_2 1 2 p10:front_matter:column_1_of_2:white [255, 255, 255] white False False [47.97, 76.43, 240.96, 337.21] S8b, Supporting Information. Both P0 and NHCO-5 show the high content of Mn in comparison with Co, which demonstrates that Mn dissolves in the electrolyte more easily. In addition, the dissolution content of Mn and Co f… S8b, Supporting Information. Both P0 and NHCO-5 show the high content of Mn in comparison with Co, which demonstrates that Mn dissolves in the electrolyte more easily. In addition, the dissolution content of Mn and Co f… S8b, Supporting Information. Both P0 and NHCO-5 show the high content of Mn in comparison with Co, which demonstrates that Mn dissolves in the electrolyte more easily. In addition, the dissolution content of Mn and Co for the NHCO-5 electrode shows to be less than P0 electrode, indicating oxygen vacancies and integrated spinel-like phase can reduce the side reaction and dissolution of transition metals. SEM images of the cycled P0 and NHCO-5 electrodes are shown in Figures 6c,e, respectively. An obvious crack can be observed on the surface of P0 electrode, which is the result of continuing oxygen release, the formation of microscopic defects, and electrolyte corrosion. [ 34] In contrast, the NCHO-5 electrode still shows intact morphology. Enlarged TEM images of the P0 and NHCO-5 electrodes are shown in Figures 6d,f, respectively. The surface of P0 shows a mixed phase of layered phase (red box) and disorder rock-salt phase (Yellow box), which can be proved by the FFT images. The appearance of disordered rock-salt structure demonstrates the irreversible structural deterioration: first, the layered structure ( R-3m ) transforms to spinel-like phase ( Fd-3m ) and last, to inactive rock-salt phase ( Fm-3m ). This structural transformation occurs from the surface to bulk as shown in Figure 6g. Previous studies have proved that the irreversible lattice oxygen release and migration of transition metal ions mainly cause the structure deterioration and degradation of electrochemical performance. [35] In contrast, the clear lattice fringe of NHCO-5 electrode, corresponding to the (003) facet of R3m space structure, directly demonstrates the relatively intact layered structure after cycling. These results indicate the surface defect can suppress irreversible oxygen release, migration, and dissolution of transition metals and alleviate the side reaction for stabilizing the structure of LRMO. S8b, Supporting Information. Both P0 and NHCO-5 show the high content of Mn in comparison with Co, which demonstrates that Mn dissolves in the electrolyte more easily. In addition, the dissolution content of Mn and Co for the NHCO-5 electrode shows to be less than P0 electrode, indicating oxygen vacancies and integrated spinel-like phase can reduce the side reaction and dissolution of transition metals. SEM images of the cycled P0 and NHCO-5 electrodes are shown in Figures 6c,e, respectively. An obvious crack can be observed on the surface of P0 electrode, which is the result of continuing oxygen release, the formation of microscopic defects, and electrolyte corrosion. [ 34] In contrast, the NCHO-5 electrode still shows intact morphology. Enlarged TEM images of the P0 and NHCO-5 electrodes are shown in Figures 6d,f, respectively. The surface of P0 shows a mixed phase of layered phase (red box) and disorder rock-salt phase (Yellow box), which can be proved by the FFT images. The appearance of disordered rock-salt structure demonstrates the irreversible structural deterioration: first, the layered structure ( R-3m ) transforms to spinel-like phase ( Fd-3m ) and last, to inactive rock-salt phase ( Fm-3m ). This structural transformation occurs from the surface to bulk as shown in Figure 6g. Previous studies have proved that the irreversible lattice oxygen release and migration of transition metal ions mainly cause the structure deterioration and degradation of electrochemical performance. [35] In contrast, the clear lattice fringe of NHCO-5 electrode, corresponding to the (003) facet of R3m space structure, directly demonstrates the relatively intact layered structure after cycling. These results indicate the surface defect can suppress irreversible oxygen release, migration, and dissolution of transition metals and alleviate the side reaction for stabilizing the structure of LRMO. 10 4 3 114 #/texts/98 section_header body_heading False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:0 body_zone column_1_of_2 1 2 p10:body_zone:column_1_of_2:white [255, 255, 255] white False False [47.98, 440.84, 64.45, 10.25] 3. Conclusion 3. Conclusion 3. Conclusion 3. Conclusion 10 5 4 115 #/texts/99 text body_candidate_excluded False medium after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:0 bottom_margin column_1_of_2 1 2 p10:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 460.19, 240.95, 260.51] In summary, a facile surface defect construction strategy is proved to address the issues of irreversible oxygen release and sluggish kinetic for Li-rich Mn-based oxides cathodes, resulting in the excellent rate perform… In summary, a facile surface defect construction strategy is proved to address the issues of irreversible oxygen release and sluggish kinetic for Li-rich Mn-based oxides cathodes, resulting in the excellent rate perform… In summary, a facile surface defect construction strategy is proved to address the issues of irreversible oxygen release and sluggish kinetic for Li-rich Mn-based oxides cathodes, resulting in the excellent rate performance and fast-charging capability with enhanced reversible anionic redox. The modified material NHCO-5 with appropriate oxygen vacancies and integrated spinel-like phase significantly exhibits outstanding electrochemical performance, including a high reversible specific capacity of 297.0 mAh · g -1 with 86.98% capacity retention after 100 cycles, high capacity of 180.7 mAh · g -1 at 5 C, and excellent fastcharging capability. Systematical characterization and theoretical calculation confirm that the surface defect can modulate the local electronic structure around Mn and O for suppressing oxygen release, irreversible migration of transition metals, and phase transformation. Moreover, the electrochemical activity of Li 2 MnO3 phase is largely stimulated with the synergistic function of reduced Mn and oxygen vacancies, resulting in both reversible anionic and cationic redox during cycling. The improved electrical conductivity, fast charge transfer, and existence of spinellike phase with 3D Li + diffusion channels accelerates the kinetics of LRMO, contributing to the enhanced fast-charging capability. Therefore, we believe this work can provide new insight into enhancing fast-charging capability with reversible anionic redox for LRMO via the strategy of modulating local electronic structure. In summary, a facile surface defect construction strategy is proved to address the issues of irreversible oxygen release and sluggish kinetic for Li-rich Mn-based oxides cathodes, resulting in the excellent rate performance and fast-charging capability with enhanced reversible anionic redox. The modified material NHCO-5 with appropriate oxygen vacancies and integrated spinel-like phase significantly exhibits outstanding electrochemical performance, including a high reversible specific capacity of 297.0 mAh · g -1 with 86.98% capacity retention after 100 cycles, high capacity of 180.7 mAh · g -1 at 5 C, and excellent fastcharging capability. Systematical characterization and theoretical calculation confirm that the surface defect can modulate the local electronic structure around Mn and O for suppressing oxygen release, irreversible migration of transition metals, and phase transformation. Moreover, the electrochemical activity of Li 2 MnO3 phase is largely stimulated with the synergistic function of reduced Mn and oxygen vacancies, resulting in both reversible anionic and cationic redox during cycling. The improved electrical conductivity, fast charge transfer, and existence of spinellike phase with 3D Li + diffusion channels accelerates the kinetics of LRMO, contributing to the enhanced fast-charging capability. Therefore, we believe this work can provide new insight into enhancing fast-charging capability with reversible anionic redox for LRMO via the strategy of modulating local electronic structure. 10 6 5 116 #/texts/100 page_footer page_footer False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:0 bottom_margin column_1_of_2 1 2 p10:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [47.98, 745.71, 105.61, 6.3] Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 Adv. Funct. Mater. 2023 , 33 , 2304065 10 3 6 117 #/texts/97 page_header page_header False low after_back_matter_stop after_back_matter_stop after_stop False None top_margin column_2_of_2 2 2 p10:top_margin:column_2_of_2:off_white [246, 246, 246] off_white False False [579.16, 15.65, 4.41, 751.61] 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wile… 16163028, 2023, 43, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/adfm.202304065 by Jilin University, Wiley Online Library on [12/07/2026]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License 10 24 7 118 #/texts/118 text page_margin_header False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 top_margin column_2_of_2 2 2 p10:top_margin:column_2_of_2:white [255, 255, 255] white False False [469.62, 50.12, 74.39, 8.02] www.afm-journal.de www.afm-journal.de 10 7 8 119 #/texts/101 section_header back_matter_heading False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 76.58, 112.02, 10.25] Supporting Information Supporting Information Supporting Information Supporting Information 10 8 9 120 #/texts/102 text back_matter_heading False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 95.35, 240.96, 16.67] Supporting Information is available from the Wiley Online Library or from the author. Supporting Information is available from the Wiley Online Library or from the author. Supporting Information is available from the Wiley Online Library or from the author. Supporting Information is available from the Wiley Online Library or from the author. 10 9 10 121 #/texts/103 section_header back_matter_heading False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 136.03, 92.58, 10.25] Acknowledgements Acknowledgements Acknowledgements Acknowledgements 10 10 11 122 #/texts/104 text back_matter_text False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 154.8, 240.95, 35.6] The authors acknowledge the financial support of the National Natural Science Foundation of China (52274309). This work also was supported by the Beamlines MCD-A and MCD-B (Soochow Beamline for Energy Materials) at NSRL. The authors acknowledge the financial support of the National Natural Science Foundation of China (52274309). This work also was supported by the Beamlines MCD-A and MCD-B (Soochow Beamline for Energy Materials) at NSRL. The authors acknowledge the financial support of the National Natural Science Foundation of China (52274309). This work also was supported by the Beamlines MCD-A and MCD-B (Soochow Beamline for Energy Materials) at NSRL. The authors acknowledge the financial support of the National Natural Science Foundation of China (52274309). This work also was supported by the Beamlines MCD-A and MCD-B (Soochow Beamline for Energy Materials) at NSRL. 10 11 12 123 #/texts/105 section_header back_matter_heading False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 214.4, 87.65, 10.25] Conflict of Interest Conflict of Interest Conflict of Interest Conflict of Interest 10 12 13 124 #/texts/106 text back_matter_text False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 233.17, 139.61, 7.2] The authors declare no conflict of interest. The authors declare no conflict of interest. The authors declare no conflict of interest. The authors declare no conflict of interest. 10 13 14 125 #/texts/107 section_header back_matter_heading False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 264.37, 128.2, 10.25] Data Availability Statement Data Availability Statement Data Availability Statement Data Availability Statement 10 14 15 126 #/texts/108 text metadata False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 283.15, 240.92, 16.67] The data that support the findings of this study are available from the corresponding author upon reasonable request. The data that support the findings of this study are available from the corresponding author upon reasonable request. The data that support the findings of this study are available from the corresponding author upon reasonable request. The data that support the findings of this study are available from the corresponding author upon reasonable request. 10 15 16 127 #/texts/109 section_header front_matter_heading False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 323.81, 45.87, 10.25] Keywords Keywords Keywords Keywords 10 16 17 128 #/texts/110 text unknown_text False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [303.09, 342.59, 240.96, 16.67] anionic redox, electronic structure modulation, fast-charging, Li-rich Mnbased oxides cathodes, oxygen vacancy anionic redox, electronic structure modulation, fast-charging, Li-rich Mnbased oxides cathodes, oxygen vacancy anionic redox, electronic structure modulation, fast-charging, Li-rich Mnbased oxides cathodes, oxygen vacancy anionic redox, electronic structure modulation, fast-charging, Li-rich Mnbased oxides cathodes, oxygen vacancy 10 17 18 129 #/texts/111 text metadata False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [465.28, 373.47, 78.77, 16.67] Received: April 12, 2023 Revised: May 22, 2023 Received: April 12, 2023 Revised: May 22, 2023 Received: April 12, 2023 Revised: May 22, 2023 Received: April 12, 2023 Revised: May 22, 2023 10 18 19 130 #/texts/112 text metadata False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [440.13, 392.41, 103.92, 7.2] Published online: June 21, 2023 Published online: June 21, 2023 Published online: June 21, 2023 Published online: June 21, 2023 10 19 20 131 #/texts/113 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop True p10:body_region:1 front_matter column_2_of_2 2 2 p10:front_matter:column_2_of_2:white [255, 255, 255] white False False [307.08, 434.21, 236.97, 37.09] a) S. 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