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 2 1 0 #/texts/1 section_header title_candidate False low non_body_heading non_body_heading True p1:body_region:0 page_body column_1_of_2 1 2 p1:page_body:column_1_of_2:white [255, 255, 255] white False False [51.82, 65.4, 418.82, 77.58] Formation of the Spinel Phase in the Layered Composite Cathode Used in Li-Ion Batteries Formation of the Spinel Phase in the Layered Composite Cathode Used in Li-Ion Batteries Formation of the Spinel Phase in the Layered Composite Cathode Used in Li-Ion Batteries Formation of the Spinel Phase in the Layered Composite Cathode Used in Li-Ion Batteries 1 15 2 1 #/texts/30 text page_margin_header False low document_ui document_ui False None top_margin column_2_of_2 2 2 p1:top_margin:column_2_of_2:colored [230, 168, 56] colored False True [536.95, 47.22, 28.39, 112.47] ARTICLE ARTICLE ARTICLE ARTICLE 1 3 3 2 #/texts/2 text body_candidate_excluded False medium before_body_started before_body_started True p1:body_region:0 page_body column_1_of_2 1 2 p1:page_body:column_1_of_2:white [255, 255, 255] white False False [51.82, 159.22, 416.72, 35.89] Meng Gu, † Ilias Belharouak, ‡ Jianming Zheng, # Huiming Wu, ‡ Jie Xiao, # Arda Genc, § Khalil Amine, ‡ Suntharampillai Thevuthasan, † Donald R. Baer, † Ji-Guang Zhang, # Nigel D. Browning, ^ Jun Liu, ^ and Chongmin Wan… Meng Gu, † Ilias Belharouak, ‡ Jianming Zheng, # Huiming Wu, ‡ Jie Xiao, # Arda Genc, § Khalil Amine, ‡ Suntharampillai Thevuthasan, † Donald R. Baer, † Ji-Guang Zhang, # Nigel D. Browning, ^ Jun Liu, ^ and Chongmin Wan… Meng Gu, † Ilias Belharouak, ‡ Jianming Zheng, # Huiming Wu, ‡ Jie Xiao, # Arda Genc, § Khalil Amine, ‡ Suntharampillai Thevuthasan, † Donald R. Baer, † Ji-Guang Zhang, # Nigel D. Browning, ^ Jun Liu, ^ and Chongmin Wang †, * Meng Gu, † Ilias Belharouak, ‡ Jianming Zheng, # Huiming Wu, ‡ Jie Xiao, # Arda Genc, § Khalil Amine, ‡ Suntharampillai Thevuthasan, † Donald R. Baer, † Ji-Guang Zhang, # Nigel D. Browning, ^ Jun Liu, ^ and Chongmin Wang †, * 1 1 5 4 #/texts/0 page_header page_header False low docling_page_header docling_page_header False None page_body column_1_of_2 1 2 p1:page_body:column_1_of_2:white [255, 255, 255] white False False [3.34, 277.91, 14.66, 284.86] Downloaded via JILIN UNIV on July 12, 206 at 12:068 (UTC). See https:/pubs.acs.org/sharinguidelines for options on how to legitimately share published articles. Downloaded via JILIN UNIV on July 12, 206 at 12:068 (UTC). See https:/pubs.acs.org/sharinguidelines for options on how to legitimately share published articles. Downloaded via JILIN UNIV on July 12, 206 at 12:068 (UTC). See https:/pubs.acs.org/sharinguidelines for options on how to legitimately share published articles. Downloaded via JILIN UNIV on July 12, 206 at 12:068 (UTC). See https:/pubs.acs.org/sharinguidelines for options on how to legitimately share published articles. 1 7 6 5 #/texts/6 text front_matter_heading False low front_matter_heading front_matter_heading True p1:body_region:0 page_body column_1_of_2 1 2 p1:page_body:column_1_of_2:white [255, 255, 255] white False False [51.82, 480.41, 322.14, 7.2] KEYWORDS: lithium ion battery . layered structure . spinel formation . phase transformation KEYWORDS: lithium ion battery . layered structure . spinel formation . phase transformation KEYWORDS: lithium ion battery . layered structure . spinel formation . phase transformation KEYWORDS: lithium ion battery . layered structure . spinel formation . phase transformation 1 6 7 6 #/texts/5 text abstract_candidate False medium implicit_abstract implicit_abstract True p1:body_region:0 page_body column_1_of_2 1 2 p1:page_body:column_1_of_2:colored [254, 246, 232] colored False False [58.79, 401.69, 452.29, 63.58] consequence of the lattice breakdown and vacancy condensation upon removal of lithium ions. The AlF 3 -coating can partially relieve the spinel formation in the layered structure during cycling, resulting in a slower ca… consequence of the lattice breakdown and vacancy condensation upon removal of lithium ions. The AlF 3 -coating can partially relieve the spinel formation in the layered structure during cycling, resulting in a slower ca… consequence of the lattice breakdown and vacancy condensation upon removal of lithium ions. The AlF 3 -coating can partially relieve the spinel formation in the layered structure during cycling, resulting in a slower capacity decay. However, the AlF 3 -coating on the layered structure cannot ultimately stop the spinel formation. The observation of structure transition characteristics discussed in this paper provides direct explanation for the observed gradual capacity loss and poor rate performance of the layered composite. It also provides clues about how to improve the materials structure in order to improve electrochemical performance. consequence of the lattice breakdown and vacancy condensation upon removal of lithium ions. The AlF 3 -coating can partially relieve the spinel formation in the layered structure during cycling, resulting in a slower capacity decay. However, the AlF 3 -coating on the layered structure cannot ultimately stop the spinel formation. The observation of structure transition characteristics discussed in this paper provides direct explanation for the observed gradual capacity loss and poor rate performance of the layered composite. It also provides clues about how to improve the materials structure in order to improve electrochemical performance. 1 5 8 7 #/texts/4 text abstract_candidate False medium implicit_abstract implicit_abstract True p1:body_region:0 page_body column_1_of_2 1 2 p1:page_body:column_1_of_2:colored [254, 246, 232] colored False False [58.79, 276.17, 295.08, 119.36] ABSTRACT Pristine Li-rich layered cathodes, such as Li 1.2 Ni 0.2 Mn0.6 O2 and Li 1.2 Ni 0.1 Mn0.525 -Co0.175 O2 , were identi fi ed to exist in two di ff erent structures: LiMO 2 R 3 m and Li2MO3 C 2/ m phases. Upon 30… ABSTRACT Pristine Li-rich layered cathodes, such as Li 1.2 Ni 0.2 Mn0.6 O2 and Li 1.2 Ni 0.1 Mn0.525 -Co0.175 O2 , were identi fi ed to exist in two di ff erent structures: LiMO 2 R 3 m and Li2MO3 C 2/ m phases. Upon 30… ABSTRACT Pristine Li-rich layered cathodes, such as Li 1.2 Ni 0.2 Mn0.6 O2 and Li 1.2 Ni 0.1 Mn0.525 -Co0.175 O2 , were identi fi ed to exist in two di ff erent structures: LiMO 2 R 3 m and Li2MO3 C 2/ m phases. Upon 300 cycles of charge/discharge, both phases gradually transform to the spinel structure. The transition from LiMO 2 R 3 m to spinel is accomplished through the migration of transition metal ions to the Li site without breaking down the lattice, leading to the formation of mosaic structured spinel grains within the parent particle. In contrast, transition from Li2MO3 C 2/ m to spinel involves removal of Li þ and O 2 -, which produces large lattice strain and leads to the breakdown of the parent lattice. The newly formed spinel grains show random orientation within the same particle. Cracks and pores were also noticed within some layered nanoparticles after cycling, which is believed to be the ABSTRACT Pristine Li-rich layered cathodes, such as Li 1.2 Ni 0.2 Mn0.6 O2 and Li 1.2 Ni 0.1 Mn0.525 -Co0.175 O2 , were identi fi ed to exist in two di ff erent structures: LiMO 2 R 3 m and Li2MO3 C 2/ m phases. Upon 300 cycles of charge/discharge, both phases gradually transform to the spinel structure. The transition from LiMO 2 R 3 m to spinel is accomplished through the migration of transition metal ions to the Li site without breaking down the lattice, leading to the formation of mosaic structured spinel grains within the parent particle. In contrast, transition from Li2MO3 C 2/ m to spinel involves removal of Li þ and O 2 -, which produces large lattice strain and leads to the breakdown of the parent lattice. The newly formed spinel grains show random orientation within the same particle. Cracks and pores were also noticed within some layered nanoparticles after cycling, which is believed to be the 1 8 9 8 #/texts/7 text body_candidate_excluded False high inside_front_matter inside_front_matter 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 [51.82, 504.93, 161.35, 234.93] L i-ion batteries have been widely used as an energy storage device for modern electric devices, grid application, and renewable energy. 1 7 Cathodes with a layered structure such as Li1.2Ni0.2Mn0.6O2 (LNMO) andLi1.2N… L i-ion batteries have been widely used as an energy storage device for modern electric devices, grid application, and renewable energy. 1 7 Cathodes with a layered structure such as Li1.2Ni0.2Mn0.6O2 (LNMO) andLi1.2N… L i-ion batteries have been widely used as an energy storage device for modern electric devices, grid application, and renewable energy. 1 7 Cathodes with a layered structure such as Li1.2Ni0.2Mn0.6O2 (LNMO) andLi1.2Ni0.1Mn0.525Co0.175O2(LNMCO) can provide much higher capacity than the traditional cathode materials such as LiCoO2 and LiMn2O4 spinel. 8 12 Therefore, these layered structures are one of the most promising candidates for future heavy duty applications such as hybrid and electric vehicles. However, the application of these materials faces three fundamental challenges: (1) voltage instability, (2) capacity fading, and (3) slow charge/discharge rate. Collective experimental observations indicate these challenges are closely related to the structural characteristics of these materials, suchasthecrystal structure, spatial distribution L i-ion batteries have been widely used as an energy storage device for modern electric devices, grid application, and renewable energy. 1 7 Cathodes with a layered structure such as Li1.2Ni0.2Mn0.6O2 (LNMO) andLi1.2Ni0.1Mn0.525Co0.175O2(LNMCO) can provide much higher capacity than the traditional cathode materials such as LiCoO2 and LiMn2O4 spinel. 8 12 Therefore, these layered structures are one of the most promising candidates for future heavy duty applications such as hybrid and electric vehicles. However, the application of these materials faces three fundamental challenges: (1) voltage instability, (2) capacity fading, and (3) slow charge/discharge rate. Collective experimental observations indicate these challenges are closely related to the structural characteristics of these materials, suchasthecrystal structure, spatial distribution 1 16 10 9 #/texts/31 page_footer page_footer False low docling_page_footer docling_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 [50.74, 756.25, 30.97, 7.28] GU ET AL GU ET AL GU ET AL GU ET AL 1 9 11 10 #/texts/9 text body_candidate_excluded False high inside_front_matter inside_front_matter 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 [228.08, 504.93, 161.38, 234.94] of cations, and phase stability upon lithium extraction and insertion. Structurally, these layered structures are often composed of the intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases. 7,13 Nevertheless, it is not c… of cations, and phase stability upon lithium extraction and insertion. Structurally, these layered structures are often composed of the intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases. 7,13 Nevertheless, it is not c… of cations, and phase stability upon lithium extraction and insertion. Structurally, these layered structures are often composed of the intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases. 7,13 Nevertheless, it is not clear how each individual phase a ff ects the performance of these materials. Further, the cations are not necessarily uniformly distributed at nanometer scale. Recently, Gu et al . 7 reported a nanoscale phase separation caused by the preferential segregation of Ni atoms on the particle surface and boundaries in the layered lithium nickel manganese oxide cathode materials. They further predicted that the formation of the Ni-rich surface layer would a ff ect the di ff usion of Li ions, and thus possibly have an impact on the rate performance of this cathode. 7 Accompanying the extraction of Li from the Li2MO3 phase at the 4.5 V voltage plateau is of cations, and phase stability upon lithium extraction and insertion. Structurally, these layered structures are often composed of the intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases. 7,13 Nevertheless, it is not clear how each individual phase a ff ects the performance of these materials. Further, the cations are not necessarily uniformly distributed at nanometer scale. Recently, Gu et al . 7 reported a nanoscale phase separation caused by the preferential segregation of Ni atoms on the particle surface and boundaries in the layered lithium nickel manganese oxide cathode materials. They further predicted that the formation of the Ni-rich surface layer would a ff ect the di ff usion of Li ions, and thus possibly have an impact on the rate performance of this cathode. 7 Accompanying the extraction of Li from the Li2MO3 phase at the 4.5 V voltage plateau is 1 10 12 11 #/texts/18 text metadata False low first_page_metadata first_page_metadata True p1:body_region:0 page_body column_2_of_2 2 2 p1:page_body:column_2_of_2:white [255, 255, 255] white False False [401.39, 647.44, 86.99, 15.04] * Address correspondence to Chongmin.Wang@pnnl.gov. * Address correspondence to Chongmin.Wang@pnnl.gov. * Address correspondence to Chongmin.Wang@pnnl.gov. * Address correspondence to Chongmin.Wang@pnnl.gov. 1 11 13 12 #/texts/19 text metadata False low first_page_metadata first_page_metadata True p1:body_region:0 page_body column_2_of_2 2 2 p1:page_body:column_2_of_2:white [255, 255, 255] white False False [401.39, 675.84, 112.95, 15.04] Received for review October 31, 2012 and accepted December 13, 2012. Received for review October 31, 2012 and accepted December 13, 2012. Received for review October 31, 2012 and accepted December 13, 2012. Received for review October 31, 2012 and accepted December 13, 2012. 1 12 14 13 #/texts/20 text unknown_text False medium abstract_boundary_dates abstract_boundary_dates True p1:body_region:0 page_body column_2_of_2 2 2 p1:page_body:column_2_of_2:white [255, 255, 255] white False False [401.39, 702.45, 111.48, 15.3] December 13, 2012 Published online 10.1021/nn305065u December 13, 2012 Published online 10.1021/nn305065u December 13, 2012 Published online 10.1021/nn305065u December 13, 2012 Published online 10.1021/nn305065u 1 13 15 14 #/texts/21 text page_margin_footer False low page_margin_footer page_margin_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 [400.99, 733.59, 62.39, 5.87] C 201 American Chemical Society C 201 American Chemical Society C 201 American Chemical Society C 201 American Chemical Society 1 17 16 15 #/texts/32 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 [322.15, 755.18, 95.47, 8.29] VOL. - VOL. - VOL. - VOL. - 1 18 17 16 #/texts/33 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_2_of_2 2 2 p1:bottom_margin:column_2_of_2:white [255, 255, 255] white False True [551.96, 756.94, 10.09, 8.0] 760 760 760 760 1 14 18 17 #/texts/29 text page_margin_footer False low document_web_address document_web_address False None bottom_margin column_2_of_2 2 2 p1:bottom_margin:column_2_of_2:white [254, 254, 254] white False False [473.22, 770.6, 29.67, 5.64] w.acsnano.org w.acsnano.org w.acsnano.org w.acsnano.org 2 2 1 18 #/texts/35 text body_candidate_excluded False high inside_front_matter inside_front_matter True p2:body_region:0 front_matter column_1_of_2 1 2 p2:front_matter:column_1_of_2:white [255, 255, 255] white False False [64.74, 64.62, 201.27, 252.54] the release of oxygen and Li þ (removal of the Li2O part). 2 However, the e ff ect of the removal of the Li2O part on the lattice stability has not been established. The layered-to-spinel transformation has long been po… the release of oxygen and Li þ (removal of the Li2O part). 2 However, the e ff ect of the removal of the Li2O part on the lattice stability has not been established. The layered-to-spinel transformation has long been po… the release of oxygen and Li þ (removal of the Li2O part). 2 However, the e ff ect of the removal of the Li2O part on the lattice stability has not been established. The layered-to-spinel transformation has long been postulated as an important factor to account for the capacity fading and poor rate performance of the layered structure materials. 2,9,10,13 17 However, it is not clear where the spinel phase nucleates and how the spinel phase grows on the consumption of the layered structured phase. The answers to these questions critically depends on the atomic level structural and chemical analysis of materials and their correlation with the cyclic performance of the battery. On the basis of atomic scale Z -contrast imaging, Xu et al . have found that the migration of transition metal (TM) cations into the Li layers can initiate the formation of spinel near the particle surface region. 15 Apparently, a far more detailed microscopic understanding of the phase transformation characteristics in these layered structures will lead to tailoring of the materials structure for better electrochemical performance. the release of oxygen and Li þ (removal of the Li2O part). 2 However, the e ff ect of the removal of the Li2O part on the lattice stability has not been established. The layered-to-spinel transformation has long been postulated as an important factor to account for the capacity fading and poor rate performance of the layered structure materials. 2,9,10,13 17 However, it is not clear where the spinel phase nucleates and how the spinel phase grows on the consumption of the layered structured phase. The answers to these questions critically depends on the atomic level structural and chemical analysis of materials and their correlation with the cyclic performance of the battery. On the basis of atomic scale Z -contrast imaging, Xu et al . have found that the migration of transition metal (TM) cations into the Li layers can initiate the formation of spinel near the particle surface region. 15 Apparently, a far more detailed microscopic understanding of the phase transformation characteristics in these layered structures will lead to tailoring of the materials structure for better electrochemical performance. 2 3 2 19 #/texts/36 text body_candidate_excluded False high inside_front_matter inside_front_matter True p2:body_region:0 front_matter column_1_of_2 1 2 p2:front_matter:column_1_of_2:white [255, 255, 255] white False False [64.74, 321.3, 201.26, 264.02] In this paper, we use aberration-corrected scanning/ transmission electron microscopy (S/TEM) imaging and energy dispersive X-ray spectroscopy (EDS) to probe the atomic structure of the layer structured cathode material… In this paper, we use aberration-corrected scanning/ transmission electron microscopy (S/TEM) imaging and energy dispersive X-ray spectroscopy (EDS) to probe the atomic structure of the layer structured cathode material… In this paper, we use aberration-corrected scanning/ transmission electron microscopy (S/TEM) imaging and energy dispersive X-ray spectroscopy (EDS) to probe the atomic structure of the layer structured cathode materials before and after high voltage cycling. 18 The STEM high angle annular dark fi eld (HAADF) detector collects all the incoherently scattered electrons. The image intensity of each atomic column re fl ects the average atomic number of each atomic column ( ∼ Z 1.5 to Z 1.8 ), 18 which is therefore termed as Z -contrast imaging and is chemical sensitive, allowing us to intuitively interpret the atomic structure changes directly. We found that both LNMO and LNMCO layer structured cathodes are a random mixing of LiMO2 R 3 m and Li2MO3 C 2/ m phases, with both phases able to coexist in a single nanoparticle. Extraction of Li from the lattice of the layer-structured material leads to lattice break down, crack and porosity formation, and nucleation and growth of spinel. Mechanistically, the formation of spinel from LiMO2 R 3 m is distinctively di ff erent from the transition of Li2MO3 C 2/ m to spinel. In this paper, we use aberration-corrected scanning/ transmission electron microscopy (S/TEM) imaging and energy dispersive X-ray spectroscopy (EDS) to probe the atomic structure of the layer structured cathode materials before and after high voltage cycling. 18 The STEM high angle annular dark fi eld (HAADF) detector collects all the incoherently scattered electrons. The image intensity of each atomic column re fl ects the average atomic number of each atomic column ( ∼ Z 1.5 to Z 1.8 ), 18 which is therefore termed as Z -contrast imaging and is chemical sensitive, allowing us to intuitively interpret the atomic structure changes directly. We found that both LNMO and LNMCO layer structured cathodes are a random mixing of LiMO2 R 3 m and Li2MO3 C 2/ m phases, with both phases able to coexist in a single nanoparticle. Extraction of Li from the lattice of the layer-structured material leads to lattice break down, crack and porosity formation, and nucleation and growth of spinel. Mechanistically, the formation of spinel from LiMO2 R 3 m is distinctively di ff erent from the transition of Li2MO3 C 2/ m to spinel. 2 4 3 20 #/texts/37 section_header body_heading False low body_heading body_heading True p2:body_region:0 body_zone column_1_of_2 1 2 p2:body_zone:column_1_of_2:white [255, 255, 255] white False True [64.74, 601.09, 120.27, 7.65] RESULTS AND DISCUSSIONS RESULTS AND DISCUSSIONS RESULTS AND DISCUSSIONS RESULTS AND DISCUSSIONS 2 9 5 22 #/texts/41 page_footer page_footer False low docling_page_footer docling_page_footer True p2:body_region:0 bottom_margin column_1_of_2 1 2 p2:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [64.29, 760.66, 34.51, 7.08] GU ET AL . GU ET AL . GU ET AL . GU ET AL . 2 1 6 23 #/texts/34 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:white [255, 255, 255] white False False [540.13, 47.17, 28.39, 112.47] ARTICLE ARTICLE ARTICLE ARTICLE 2 7 7 24 #/texts/39 caption caption False low outside_body_flow_caption outside_body_flow_caption True p2:body_region:1 front_matter column_2_of_2 2 2 p2:front_matter:column_2_of_2:white [255, 255, 255] white False False [283.92, 394.54, 201.28, 24.87] Figure 1. (a) Cycling performance of LNMO and AlF3-coated LNMCO and (b) charge/discharge pro fi les of the LNMO cathode material. Figure 1. (a) Cycling performance of LNMO and AlF3-coated LNMCO and (b) charge/discharge pro fi les of the LNMO cathode material. Figure 1. (a) Cycling performance of LNMO and AlF3-coated LNMCO and (b) charge/discharge pro fi les of the LNMO cathode material. Figure 1. (a) Cycling performance of LNMO and AlF3-coated LNMCO and (b) charge/discharge pro fi les of the LNMO cathode material. 2 11 9 26 #/texts/43 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 [551.96, 758.01, 14.85, 10.27] 761 761 761 761 2 10 10 27 #/texts/42 page_footer page_footer False low docling_page_footer docling_page_footer True p2:body_region:1 bottom_margin column_2_of_2 2 2 p2:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [323.72, 759.15, 141.77, 8.55] VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 2 8 11 28 #/texts/40 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_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 True [473.22, 779.07, 59.2, 1.67] www.acsnano.org www.acsnano.org 3 3 1 29 #/texts/45 caption caption False low outside_body_flow_caption outside_body_flow_caption True p3:body_region:0 page_body column_1_of_2 1 2 p3:page_body:column_1_of_2:white [255, 255, 255] white False False [64.74, 275.79, 201.35, 79.28] Figure 2. R 3 m phase (a) Overview Z -contrast image of the pristine LNMO cathode; (b) magni fi ed image of the region shown as the green square in panel a; (c) atomic resolution image showing the Li-channels are very d… Figure 2. R 3 m phase (a) Overview Z -contrast image of the pristine LNMO cathode; (b) magni fi ed image of the region shown as the green square in panel a; (c) atomic resolution image showing the Li-channels are very d… Figure 2. R 3 m phase (a) Overview Z -contrast image of the pristine LNMO cathode; (b) magni fi ed image of the region shown as the green square in panel a; (c) atomic resolution image showing the Li-channels are very dark due to very small atomic number of Li, while TM cation has the highest intensity and oxygen ions are visible; (d) structural model of the [010] projection of the R 3 m phase; (e) simulated Z -contrast image the R 3 m phase based on a 10% Ni/Li disorder. Figure 2. R 3 m phase (a) Overview Z -contrast image of the pristine LNMO cathode; (b) magni fi ed image of the region shown as the green square in panel a; (c) atomic resolution image showing the Li-channels are very dark due to very small atomic number of Li, while TM cation has the highest intensity and oxygen ions are visible; (d) structural model of the [010] projection of the R 3 m phase; (e) simulated Z -contrast image the R 3 m phase based on a 10% Ni/Li disorder. 3 9 4 32 #/texts/50 page_footer page_footer False low docling_page_footer docling_page_footer True p3:body_region:0 bottom_margin column_1_of_2 1 2 p3:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [64.29, 760.66, 34.51, 7.08] GU ET AL . GU ET AL . GU ET AL . GU ET AL . 3 2 5 33 #/texts/44 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:white [255, 255, 255] white False False [540.13, 47.17, 28.39, 112.47] ARTICLE ARTICLE ARTICLE ARTICLE 3 6 6 34 #/texts/47 caption caption False low outside_body_flow_caption outside_body_flow_caption True p3:body_region:1 page_body column_2_of_2 2 2 p3:page_body:column_2_of_2:white [255, 255, 255] white False False [283.92, 271.25, 201.34, 79.28] Figure 3. Li2MO3 C 2/ m phase and atomic model of (a) Li2MnO3;(b) Ni-containing Li2MO3; (c) experimental Z-contrast image of the C 2/ m phase; (d) [100], [110], [1 10] zone projection of the C 2/ m phase; These zone a… Figure 3. Li2MO3 C 2/ m phase and atomic model of (a) Li2MnO3;(b) Ni-containing Li2MO3; (c) experimental Z-contrast image of the C 2/ m phase; (d) [100], [110], [1 10] zone projection of the C 2/ m phase; These zone a… Figure 3. Li2MO3 C 2/ m phase and atomic model of (a) Li2MnO3;(b) Ni-containing Li2MO3; (c) experimental Z-contrast image of the C 2/ m phase; (d) [100], [110], [1 10] zone projection of the C 2/ m phase; These zone axis projection regions are labeled with di ff erent colors lines in the image in panel c; these di ff erent zone axis regions in panel c are labeled with colored squares corresponding to the atomic modelin panel d; the Li fast ; di ff usion channels are labeled with a red arrow in panel c. Figure 3. Li2MO3 C 2/ m phase and atomic model of (a) Li2MnO3;(b) Ni-containing Li2MO3; (c) experimental Z-contrast image of the C 2/ m phase; (d) [100], [110], [1 10] zone projection of the C 2/ m phase; These zone axis projection regions are labeled with di ff erent colors lines in the image in panel c; these di ff erent zone axis regions in panel c are labeled with colored squares corresponding to the atomic modelin panel d; the Li fast ; di ff usion channels are labeled with a red arrow in panel c. 3 11 9 37 #/texts/52 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 [551.96, 758.01, 14.85, 10.27] 762 762 762 762 3 10 10 38 #/texts/51 page_footer page_footer False low docling_page_footer docling_page_footer True p3:body_region:1 bottom_margin column_2_of_2 2 2 p3:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [323.72, 759.15, 141.77, 8.55] VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 3 8 11 39 #/texts/49 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_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 True [473.22, 779.07, 59.2, 1.67] www.acsnano.org www.acsnano.org 4 4 1 40 #/texts/56 caption caption False low outside_body_flow_caption outside_body_flow_caption True p4:body_region:0 page_body column_1_of_2 1 2 p4:page_body:column_1_of_2:white [255, 255, 255] white False False [64.74, 262.5, 201.33, 96.58] Figure 4. LNMO after 300 cycles (a) overview of the nanoparticle with spinel structure showing very well faceted steps in the surface; the inset shows the di ff raction pattern (b) HRTEM image showing that a single crys… Figure 4. LNMO after 300 cycles (a) overview of the nanoparticle with spinel structure showing very well faceted steps in the surface; the inset shows the di ff raction pattern (b) HRTEM image showing that a single crys… Figure 4. LNMO after 300 cycles (a) overview of the nanoparticle with spinel structure showing very well faceted steps in the surface; the inset shows the di ff raction pattern (b) HRTEM image showing that a single crystal spinel projected along [001] zone axis. The spinel steps are well faceted in the { 100 } facets. The red arrows indicate the facets of the surface. (c) TEM image collected from the bulk region also revealed a cubic lattice after 60 cycles and (d) corresponding FFT at [001] zone; (e) atomic model and simulated di ff raction pattern of the LiMn2O4 spinel [001] zone axis. Figure 4. LNMO after 300 cycles (a) overview of the nanoparticle with spinel structure showing very well faceted steps in the surface; the inset shows the di ff raction pattern (b) HRTEM image showing that a single crystal spinel projected along [001] zone axis. The spinel steps are well faceted in the { 100 } facets. The red arrows indicate the facets of the surface. (c) TEM image collected from the bulk region also revealed a cubic lattice after 60 cycles and (d) corresponding FFT at [001] zone; (e) atomic model and simulated di ff raction pattern of the LiMn2O4 spinel [001] zone axis. 4 8 4 43 #/texts/60 page_footer page_footer False low docling_page_footer docling_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 [64.29, 760.66, 34.51, 7.08] GU ET AL . GU ET AL . GU ET AL . GU ET AL . 4 1 5 44 #/texts/53 page_header page_header False low docling_page_header docling_page_header False None top_margin column_2_of_2 2 2 p4:top_margin:column_2_of_2:white [255, 255, 255] white False False [540.13, 47.17, 28.39, 112.47] ARTICLE ARTICLE ARTICLE ARTICLE 4 2 6 45 #/texts/54 caption caption False low outside_body_flow_caption outside_body_flow_caption True p4:body_region:1 page_body column_2_of_2 2 2 p4:page_body:column_2_of_2:white [255, 255, 255] white False False [283.92, 276.9, 201.32, 78.99] Figure 5. Cycled LNMO sample after 100 cycles: (a) overview Z contrast image of R 3 m phase region projected along [010] zone; higher magni fi cation Z -contrast image showing the (b) surface region as labeled by the gr… Figure 5. Cycled LNMO sample after 100 cycles: (a) overview Z contrast image of R 3 m phase region projected along [010] zone; higher magni fi cation Z -contrast image showing the (b) surface region as labeled by the gr… Figure 5. Cycled LNMO sample after 100 cycles: (a) overview Z contrast image of R 3 m phase region projected along [010] zone; higher magni fi cation Z -contrast image showing the (b) surface region as labeled by the green square and (c) bulk region as labeled by the red square; (d) intensity line pro fi le of the surface region as highlighted by the green line and bulk region as highlighted by the red line in image a, and pristine materials in Figure 2c. Note: the red arrows in the Z -contrast images show the Li fast di ff usion path. Figure 5. Cycled LNMO sample after 100 cycles: (a) overview Z contrast image of R 3 m phase region projected along [010] zone; higher magni fi cation Z -contrast image showing the (b) surface region as labeled by the green square and (c) bulk region as labeled by the red square; (d) intensity line pro fi le of the surface region as highlighted by the green line and bulk region as highlighted by the red line in image a, and pristine materials in Figure 2c. Note: the red arrows in the Z -contrast images show the Li fast di ff usion path. 4 11 8 47 #/texts/63 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 [551.96, 758.01, 14.85, 10.27] 763 763 763 763 4 9 9 48 #/texts/61 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 [323.72, 759.15, 117.92, 8.55] VOL. 7 ' NO. 1 ' 760 -767 ' VOL. 7 ' NO. 1 ' 760 -767 ' VOL. 7 ' NO. 1 ' 760 -767 ' VOL. 7 ' NO. 1 ' 760 -767 ' 4 10 10 49 #/texts/62 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 [447.76, 766.03, 17.73, 1.67] 2013 2013 2013 2013 4 5 11 50 #/texts/57 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_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 True [473.22, 779.07, 59.2, 1.67] www.acsnano.org www.acsnano.org 5 3 1 51 #/texts/65 caption caption False low outside_body_flow_caption outside_body_flow_caption True p5:body_region:0 page_body column_1_of_2 1 2 p5:page_body:column_1_of_2:white [255, 255, 255] white False False [64.74, 267.04, 201.34, 78.67] Figure 6. (a) Overview of the cathode after 60 cycles with small domains of spinel nucleated. (b and c) The nucleated spinel crystal domains have been found to be in di ff erent crystal orientation: [111] zone spinel is… Figure 6. (a) Overview of the cathode after 60 cycles with small domains of spinel nucleated. (b and c) The nucleated spinel crystal domains have been found to be in di ff erent crystal orientation: [111] zone spinel is… Figure 6. (a) Overview of the cathode after 60 cycles with small domains of spinel nucleated. (b and c) The nucleated spinel crystal domains have been found to be in di ff erent crystal orientation: [111] zone spinel is cycled in green, [001] zone spinel is labeled with a red square; area circled by blue is amorphous; the dashed lines indicate a dislocation. (d) FFT of the TEM image in panel c showing that the region is polycrystalline and the elongation of the di ff raction spots indicates distortions of the lattices. Figure 6. (a) Overview of the cathode after 60 cycles with small domains of spinel nucleated. (b and c) The nucleated spinel crystal domains have been found to be in di ff erent crystal orientation: [111] zone spinel is cycled in green, [001] zone spinel is labeled with a red square; area circled by blue is amorphous; the dashed lines indicate a dislocation. (d) FFT of the TEM image in panel c showing that the region is polycrystalline and the elongation of the di ff raction spots indicates distortions of the lattices. 5 9 5 55 #/texts/71 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 [64.29, 760.66, 34.51, 7.08] GU ET AL . GU ET AL . GU ET AL . GU ET AL . 5 2 6 56 #/texts/64 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:white [255, 255, 255] white False False [540.13, 47.17, 28.39, 112.47] ARTICLE ARTICLE ARTICLE ARTICLE 5 6 7 57 #/texts/68 caption caption False low outside_body_flow_caption outside_body_flow_caption True p5:body_region:1 page_body column_2_of_2 2 2 p5:page_body:column_2_of_2:white [255, 255, 255] white False False [283.92, 317.44, 201.3, 78.73] Figure 7. LNMO after 100 cycles (a) TEM images shows the distorted and polycrystalline lattices and (b) FFT of the image in panel a shows amorphous rings and di ff ractions spots corresponding to the LiMn2O4-type spinel… Figure 7. LNMO after 100 cycles (a) TEM images shows the distorted and polycrystalline lattices and (b) FFT of the image in panel a shows amorphous rings and di ff ractions spots corresponding to the LiMn2O4-type spinel… Figure 7. LNMO after 100 cycles (a) TEM images shows the distorted and polycrystalline lattices and (b) FFT of the image in panel a shows amorphous rings and di ff ractions spots corresponding to the LiMn2O4-type spinel in the [001] zone and [111] zone; the elongated circular spot region of 001 zone spots shows that there is a big amount of lattice distortions, which can also be observed in image c. The region highlighted in red in the TEM image (c) illustrates the lattice distortions. Figure 7. LNMO after 100 cycles (a) TEM images shows the distorted and polycrystalline lattices and (b) FFT of the image in panel a shows amorphous rings and di ff ractions spots corresponding to the LiMn2O4-type spinel in the [001] zone and [111] zone; the elongated circular spot region of 001 zone spots shows that there is a big amount of lattice distortions, which can also be observed in image c. The region highlighted in red in the TEM image (c) illustrates the lattice distortions. 5 11 9 59 #/texts/73 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 [551.96, 758.01, 14.85, 10.27] 764 764 764 764 5 10 10 60 #/texts/72 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 [323.72, 759.15, 141.77, 8.55] VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 5 8 11 61 #/texts/70 text page_margin_footer False low page_margin_footer page_margin_footer False None bottom_margin column_2_of_2 2 2 p5:bottom_margin:column_2_of_2:white [255, 255, 255] white False True [473.22, 779.07, 59.2, 1.67] www.acsnano.org www.acsnano.org 6 4 2 63 #/texts/75 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 [64.74, 494.46, 201.34, 70.48] Figure 8. (a d) Cycled LNMO and (e) LNMCO samples showing porosity formation after 60 cycles. (a) Z -contrast image; (b) bright fi eld image; (c) higher magni fi cation Z-contrast and (d) bright fi eld image showing t… Figure 8. (a d) Cycled LNMO and (e) LNMCO samples showing porosity formation after 60 cycles. (a) Z -contrast image; (b) bright fi eld image; (c) higher magni fi cation Z-contrast and (d) bright fi eld image showing t… Figure 8. (a d) Cycled LNMO and (e) LNMCO samples showing porosity formation after 60 cycles. (a) Z -contrast image; (b) bright fi eld image; (c) higher magni fi cation Z-contrast and (d) bright fi eld image showing the contrast comparison of the pores in LNMO sample; (e) STEM Zcontrast image and EDS maps of cycled LNMCO sample. Thescale bar in panel e is 30 nm and can be applied to all the elemental maps therein. Figure 8. (a d) Cycled LNMO and (e) LNMCO samples showing porosity formation after 60 cycles. (a) Z -contrast image; (b) bright fi eld image; (c) higher magni fi cation Z-contrast and (d) bright fi eld image showing the contrast comparison of the pores in LNMO sample; (e) STEM Zcontrast image and EDS maps of cycled LNMCO sample. Thescale bar in panel e is 30 nm and can be applied to all the elemental maps therein. 6 6 3 64 #/texts/77 caption caption False low docling_caption docling_caption False None bottom_margin column_1_of_2 1 2 p6:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [64.74, 728.63, 420.48, 15.91] Figure 9. STEMandMn,Ni,Co, O, C, EDS maps showing the crack formation in LNMCO after 60 cycles; the red arrows indicate the crack locations in the image and maps. Figure 9. STEMandMn,Ni,Co, O, C, EDS maps showing the crack formation in LNMCO after 60 cycles; the red arrows indicate the crack locations in the image and maps. Figure 9. STEMandMn,Ni,Co, O, C, EDS maps showing the crack formation in LNMCO after 60 cycles; the red arrows indicate the crack locations in the image and maps. Figure 9. STEMandMn,Ni,Co, O, C, EDS maps showing the crack formation in LNMCO after 60 cycles; the red arrows indicate the crack locations in the image and maps. 6 8 4 65 #/texts/79 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_1_of_2 1 2 p6:bottom_margin:column_1_of_2:white [255, 255, 255] white False False [64.29, 760.66, 34.51, 7.08] GU ET AL . GU ET AL . GU ET AL . GU ET AL . 6 3 5 66 #/texts/74 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:white [255, 255, 255] white False False [540.13, 47.17, 28.39, 112.47] ARTICLE ARTICLE ARTICLE ARTICLE 6 10 8 69 #/texts/81 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_2_of_2 2 2 p6:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [551.96, 758.01, 14.85, 10.27] 765 765 765 765 6 9 9 70 #/texts/80 page_footer page_footer False low docling_page_footer docling_page_footer True p6:body_region:0 bottom_margin column_2_of_2 2 2 p6:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [323.72, 759.15, 141.77, 8.55] VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 6 7 10 71 #/texts/78 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_page_footer False None bottom_margin column_2_of_2 2 2 p6:bottom_margin:column_2_of_2:white [255, 255, 255] white False True [473.22, 779.07, 59.2, 1.67] www.acsnano.org www.acsnano.org 7 3 1 72 #/texts/83 caption caption False low outside_body_flow_caption outside_body_flow_caption True p7:body_region:0 body_zone column_1_of_2 1 2 p7:body_zone:column_1_of_2:white [255, 255, 255] white False False [64.74, 228.88, 201.31, 51.74] Figure 10. Schematic drawing showing that the initial material is composed of three phases: R 3 m , C 2/ m , and nanocompsite of intergrowth of R 3 m and C 2/ m . The transition from the R 3 m and C 2/ m layered structu… Figure 10. Schematic drawing showing that the initial material is composed of three phases: R 3 m , C 2/ m , and nanocompsite of intergrowth of R 3 m and C 2/ m . The transition from the R 3 m and C 2/ m layered structu… Figure 10. Schematic drawing showing that the initial material is composed of three phases: R 3 m , C 2/ m , and nanocompsite of intergrowth of R 3 m and C 2/ m . The transition from the R 3 m and C 2/ m layered structure to the spinel follows di ff erent routes, leading to di ff erent structural features of the spinel grains. Figure 10. Schematic drawing showing that the initial material is composed of three phases: R 3 m , C 2/ m , and nanocompsite of intergrowth of R 3 m and C 2/ m . The transition from the R 3 m and C 2/ m layered structure to the spinel follows di ff erent routes, leading to di ff erent structural features of the spinel grains. 7 4 3 74 #/texts/84 section_header body_heading False low body_heading body_heading True p7:body_region:0 body_zone column_1_of_2 1 2 p7:body_zone:column_1_of_2:white [255, 255, 255] white False True [64.74, 576.08, 42.93, 7.65] METHODS METHODS METHODS METHODS 7 11 5 76 #/texts/91 page_footer page_footer False low docling_page_footer docling_page_footer 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 [64.29, 760.66, 34.51, 7.08] GU ET AL . GU ET AL . GU ET AL . GU ET AL . 7 2 6 77 #/texts/82 page_header page_header False low docling_page_header docling_page_header False None top_margin column_2_of_2 2 2 p7:top_margin:column_2_of_2:white [255, 255, 255] white False False [540.13, 47.17, 28.39, 112.47] ARTICLE ARTICLE ARTICLE ARTICLE 7 7 8 79 #/texts/87 section_header body_heading False low body_heading body_heading True p7:body_region:1 body_zone column_2_of_2 2 2 p7:body_zone:column_2_of_2:white [255, 255, 255] white False False [283.92, 219.32, 61.7, 7.65] CONCLUSIONS CONCLUSIONS CONCLUSIONS CONCLUSIONS 7 14 11 82 #/texts/94 page_footer page_footer False low docling_page_footer docling_page_footer False None bottom_margin column_2_of_2 2 2 p7:bottom_margin:column_2_of_2:white [255, 255, 255] white False False [551.96, 758.01, 14.85, 10.27] 766 766 766 766 7 12 12 83 #/texts/92 page_footer page_footer False low docling_page_footer docling_page_footer 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 [323.72, 759.15, 117.92, 8.55] VOL. 7 ' NO. 1 ' 760 -767 ' VOL. 7 ' NO. 1 ' 760 -767 ' VOL. 7 ' NO. 1 ' 760 -767 ' VOL. 7 ' NO. 1 ' 760 -767 ' 7 13 13 84 #/texts/93 page_footer page_footer False low docling_page_footer docling_page_footer 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 [447.76, 766.03, 17.73, 1.67] 2013 2013 2013 2013 7 10 14 85 #/texts/90 page_footer page_footer False low outside_body_flow_page_footer outside_body_flow_page_footer False None bottom_margin column_2_of_2 2 2 p7:bottom_margin:column_2_of_2:white [255, 255, 255] white False True [473.22, 779.07, 59.2, 1.67] www.acsnano.org www.acsnano.org 8 3 2 87 #/texts/96 text back_matter_heading False low back_matter_heading back_matter_heading stop_trigger 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 [64.74, 103.87, 201.2, 15.69] Conflict of Interest: The authors declare no competing fi nancial interest. Conflict of Interest: The authors declare no competing fi nancial interest. Conflict of Interest: The authors declare no competing fi nancial interest. Conflict of Interest: The authors declare no competing fi nancial interest. 8 4 3 88 #/texts/97 text back_matter_heading False low 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 [64.74, 133.98, 201.38, 177.09] Acknowledgment. The research described in this paper is part of the Chemical Imaging Initiative at Paci fi c Northwest National Laboratory (PNNL). It was conducted under the Laboratory Directed Research and Development … Acknowledgment. The research described in this paper is part of the Chemical Imaging Initiative at Paci fi c Northwest National Laboratory (PNNL). It was conducted under the Laboratory Directed Research and Development … Acknowledgment. The research described in this paper is part of the Chemical Imaging Initiative at Paci fi c Northwest National Laboratory (PNNL). It was conducted under the Laboratory Directed Research and Development Program at PNNL, a multiprogram national laboratory operated by Battelle under Contract DE-AC05-76RLO1830 for the U.S. Department of Energy (DOE). The work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scienti fi c user facility sponsored by DOE's O ffi ce of Biological and Environmental Research and located at PNNL. J. Zhang and J. Xiao would like to acknowledge the support of the Assistant Secretary for Energy E ffi ciency and Renewable Energy, O ffi ce of Vehicle Technologies of DOE under Contract No. DE-AC02-05CH11231, Subcontract No. 18769 under the Batteries for Advanced Transportation Technologies (BATT) program. J. Liu would like to acknowledge the support of the DOE Offi ce of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award KC020105-FWP12152. I. Belharouak and K. Amine would like to acknowledge the support from DOE's Freedom CAR and Vehicle Technologies O ffi ce. Acknowledgment. The research described in this paper is part of the Chemical Imaging Initiative at Paci fi c Northwest National Laboratory (PNNL). It was conducted under the Laboratory Directed Research and Development Program at PNNL, a multiprogram national laboratory operated by Battelle under Contract DE-AC05-76RLO1830 for the U.S. Department of Energy (DOE). The work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scienti fi c user facility sponsored by DOE's O ffi ce of Biological and Environmental Research and located at PNNL. J. Zhang and J. Xiao would like to acknowledge the support of the Assistant Secretary for Energy E ffi ciency and Renewable Energy, O ffi ce of Vehicle Technologies of DOE under Contract No. DE-AC02-05CH11231, Subcontract No. 18769 under the Batteries for Advanced Transportation Technologies (BATT) program. J. Liu would like to acknowledge the support of the DOE Offi ce of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award KC020105-FWP12152. I. Belharouak and K. Amine would like to acknowledge the support from DOE's Freedom CAR and Vehicle Technologies O ffi ce. 8 5 4 89 #/texts/98 text back_matter_heading False low 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 [64.74, 316.46, 201.39, 33.66] Supporting Information Available: The Supporting Information includes STEM image of the prestine LNMCO cathode nanoparticles. No cracks are visible in the pristine particles. This material is available free of charge vi… Supporting Information Available: The Supporting Information includes STEM image of the prestine LNMCO cathode nanoparticles. No cracks are visible in the pristine particles. This material is available free of charge vi… Supporting Information Available: The Supporting Information includes STEM image of the prestine LNMCO cathode nanoparticles. No cracks are visible in the pristine particles. This material is available free of charge via the Internet at http://pubs.acs.org. Supporting Information Available: The Supporting Information includes STEM image of the prestine LNMCO cathode nanoparticles. No cracks are visible in the pristine particles. This material is available free of charge via the Internet at 8 6 5 90 #/texts/99 section_header back_matter_heading False low 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 True [64.74, 370.18, 106.92, 7.65] REFERENCES AND NOTES REFERENCES AND NOTES REFERENCES AND NOTES REFERENCES AND NOTES 8 7 6 91 #/texts/100 list_item reference False low 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 [71.21, 382.63, 194.8, 24.96] Armstrong, A. R.; Bruce, P. G. Synthesis of Layered LiMnO2 as an Electrode for Rechargeable Lithium Batteries. Nature 1996 , 381 , 499 -500. Armstrong, A. R.; Bruce, P. G. Synthesis of Layered LiMnO2 as an Electrode for Rechargeable Lithium Batteries. Nature 1996 , 381 , 499 -500. Armstrong, A. R.; Bruce, P. G. 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