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 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 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 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… 1 4 4 3 #/texts/3 text body True None body_before_non_intro_heading body_before_non_intro_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, 202.65, 430.22, 47.68] † Environmental Molecular Science Laboratory, ^ Fundamental and Computational Science Directorate, and # Energy and Environmental Directorate, Paci fi c Northwest National Laboratory, 902 Battelle Boulevard, Richland, W… † Environmental Molecular Science Laboratory, ^ Fundamental and Computational Science Directorate, and # Energy and Environmental Directorate, Paci fi c Northwest National Laboratory, 902 Battelle Boulevard, Richland, W… 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. 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 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… 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… 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… 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 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… 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. 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. 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 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 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. - 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 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 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… 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… 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 2 5 4 21 #/texts/38#prov0 text body True None body body 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 [64.74, 617.25, 201.28, 127.49] Electrochemical Performance Measurements. Cycling performance and the corresponding charge/discharge profile evolution of the lithium-rich cathode material LNMO and AlF3-coated LNMCO are shown in Figure 1. During format… Electrochemical Performance Measurements. Cycling performance and the corresponding charge/discharge profile evolution of the lithium-rich cathode material LNMO and AlF3-coated LNMCO are shown in Figure 1. During format… 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 . 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 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. 2 6 8 25 #/texts/38#prov1 text body True None body body 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 [283.92, 437.69, 201.28, 306.71] of 82.8%. However, the material shows faster capacity fading after 100 cycles, which would be ascribed to the spinel transformation, lattice break down, and possible deteriorated electrode/electrolyte interface that ham… of 82.8%. However, the material shows faster capacity fading after 100 cycles, which would be ascribed to the spinel transformation, lattice break down, and possible deteriorated electrode/electrolyte interface that ham… 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 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 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 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… 3 1 2 30 #/texts/38#prov2 text body True None body body 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, 365.41, 201.31, 175.18] involving lattice breakdown and phase transformation from layered to spinel during initial activation and subsequent cycling. 15,23 This structural transformation leads to a layered-spinel intergrowth structure and the … involving lattice breakdown and phase transformation from layered to spinel during initial activation and subsequent cycling. 15,23 This structural transformation leads to a layered-spinel intergrowth structure and the … 3 4 3 31 #/texts/46#prov0 text body True None body body 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 [64.74, 545.53, 201.27, 199.27] Structure of the Pristine Materials. The layered LNMO is a nanocomposite composed of the intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases (M denotes transiton metal cations) as shown in Figure 2 and Figure 3. 7,13 Th… Structure of the Pristine Materials. The layered LNMO is a nanocomposite composed of the intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases (M denotes transiton metal cations) as shown in Figure 2 and Figure 3. 7,13 Th… 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 . 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 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… 3 5 7 35 #/texts/46#prov1 text body True None body body 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, 366.2, 201.28, 103.47] scale Z -contrast image in Figure 2c clearly shows that Li channels have the least intensity compared to the O sites or the brightest TM sites. The atomic resolution imagein Figure 2c belongs to the [010] zone projectio… scale Z -contrast image in Figure 2c clearly shows that Li channels have the least intensity compared to the O sites or the brightest TM sites. The atomic resolution imagein Figure 2c belongs to the [010] zone projectio… 3 7 8 36 #/texts/48 text body True None body body 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 [283.92, 473.8, 201.28, 270.87] The cation ordered Li2MO3 C 2/ m phase has been observed to coexist with the LiMO2 R 3 m phase even in a single nanoparticle. The atomic structural model of Li2MO3 C 2/ m phase is shown in Figure 3. A comparison of Li2M… The cation ordered Li2MO3 C 2/ m phase has been observed to coexist with the LiMO2 R 3 m phase even in a single nanoparticle. The atomic structural model of Li2MO3 C 2/ m phase is shown in Figure 3. A comparison of Li2M… 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 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 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 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… 4 6 2 41 #/texts/58 text body True None body body 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, 375.76, 201.27, 248.57] Formation of Spinel Phase from R 3 m Phase. The formation of LiMn2O4-type cubic spinel in the cycled sample has been identified by aberration corrected TEM along the [001] zone axis as shown in Figure 4a e. After 300 … Formation of Spinel Phase from R 3 m Phase. The formation of LiMn2O4-type cubic spinel in the cycled sample has been identified by aberration corrected TEM along the [001] zone axis as shown in Figure 4a e. After 300 … 4 7 3 42 #/texts/59#prov0 text body True None body body 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 [64.74, 628.46, 201.26, 115.42] To trace the origin of the spinel formation, chemically sensitive Z -contrast imaging is utilized to analyze the atomic structure of the cycled samples. Migration of the TM cations into the Li layers has been detected a… To trace the origin of the spinel formation, chemically sensitive Z -contrast imaging is utilized to analyze the atomic structure of the cycled samples. Migration of the TM cations into the Li layers has been detected a… 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 . 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 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… 4 3 7 46 #/texts/55 text body True None body body 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 [283.92, 366.14, 201.27, 378.43] ions also show visible contrast. The Li layer in the pristine LNMO nanoparticle shows no visible contrast as illustrated in Figures 2c and 5d. However, following the charge/discharge cycles, the atomic columns in the Li… ions also show visible contrast. The Li layer in the pristine LNMO nanoparticle shows no visible contrast as illustrated in Figures 2c and 5d. However, following the charge/discharge cycles, the atomic columns in the Li… 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 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 ' 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 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 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… 5 1 2 52 #/texts/59#prov1 text body True None body body 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, 365.01, 201.29, 115.42] Associated with these structural transformation characteristics, the spinels formed within a parental layered particle show features of a mosaic structure as seen in Figure 4. Formation of spinel destroyed the layered c… Associated with these structural transformation characteristics, the spinels formed within a parental layered particle show features of a mosaic structure as seen in Figure 4. Formation of spinel destroyed the layered c… 5 4 3 53 #/texts/66 text body True None body body 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, 484.58, 201.27, 163.22] Ni concentration appears to play a role on the layered structure to spinel transformation. 27 Gu et al . used STEM and EDS mapping to analyze the composition and phase distribution in pristine LNMO. 7 The Li2MO3 phase c… Ni concentration appears to play a role on the layered structure to spinel transformation. 27 Gu et al . used STEM and EDS mapping to analyze the composition and phase distribution in pristine LNMO. 7 The Li2MO3 phase c… 5 5 4 54 #/texts/67 text body True None body body 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 [64.74, 652.79, 201.25, 91.66] Disoriented Spinel Domains Generation, Porosity and Crack Formation. In the cycled sample, spinel particles that are typically several nanometers show random orientation and are often found to be dispersed in an amorpho… Disoriented Spinel Domains Generation, Porosity and Crack Formation. In the cycled sample, spinel particles that are typically several nanometers show random orientation and are often found to be dispersed in an amorpho… 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 . 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 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… 5 7 8 58 #/texts/69#prov0 text body True None body body 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 [283.92, 413.93, 201.27, 330.63] These spinel domains are in different orientations with each other. For example, there are spinel domains in the [111] zone and [001] zone in Figure 6b,c. In between these domains are distorted lattice/amorphous phases … These spinel domains are in different orientations with each other. For example, there are spinel domains in the [111] zone and [001] zone in Figure 6b,c. In between these domains are distorted lattice/amorphous phases … 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 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 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 6 1 1 62 #/texts/69#prov1 text body True None body body 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, 67.15, 201.25, 91.56] circled in red) and [111] (diffraction spots circled in blue) zone axis. The amorphous ring patterns indicate that amorphous regions must exist in this region in the TEM image in Figure 7a. A higher magnification TEM im… circled in red) and [111] (diffraction spots circled in blue) zone axis. The amorphous ring patterns indicate that amorphous regions must exist in this region in the TEM image in Figure 7a. A higher magnification TEM im… 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… 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. 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 . 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 6 2 6 67 #/texts/69#prov2 text body True None body body True p6:body_region:0 page_body column_2_of_2 2 2 p6:page_body:column_2_of_2:white [255, 255, 255] white False False [283.92, 67.14, 201.31, 306.71] in both the LNMO and LNMCO cathode nanoparticles. As shown in Figure 8, simultaneously taken Z -contrast and bright field images have been used to map the porosity formation in the cathode nanoparticles after cycling. P… in both the LNMO and LNMCO cathode nanoparticles. As shown in Figure 8, simultaneously taken Z -contrast and bright field images have been used to map the porosity formation in the cathode nanoparticles after cycling. P… 6 5 7 68 #/texts/76#prov0 text body True None body body True p6:body_region:0 page_body column_2_of_2 2 2 p6:page_body:column_2_of_2:white [255, 255, 255] white False False [283.92, 377.99, 201.28, 187.14] Last but not least, crack formation has been found to exist as evidenced by the results of S/TEM imaging and EDS mapping in the cycled LNMCO samples in Figure 9. A comparison of the STEM Z-contrast image of the pristine… Last but not least, crack formation has been found to exist as evidenced by the results of S/TEM imaging and EDS mapping in the cycled LNMCO samples in Figure 9. A comparison of the STEM Z-contrast image of the pristine… 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 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 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 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… 7 1 2 73 #/texts/76#prov1 text body True None body body 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, 294.94, 201.28, 234.99] and lattice break-up in the LiMO2 R 3 m phase region duetotheLi þ removal during high voltage cycling. The overall phase transformation characteristic of the layer structured materials is schematically shown in Figure 1… and lattice break-up in the LiMO2 R 3 m phase region duetotheLi þ removal during high voltage cycling. The overall phase transformation characteristic of the layer structured materials is schematically shown in Figure 1… 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 7 5 4 75 #/texts/85 text body True None body body 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 [64.74, 589.16, 201.27, 155.38] The LNMO and LNMCO were synthesized via a coprecipitation method. 29 Nickel sulfate hexahydrate (NiSO4.6H2O), manganese sulfate monohydrate (MnSO4.H2O), sodium hydroxide (NaOH), and ammonium hydroxide (NH3.H2O) were use… The LNMO and LNMCO were synthesized via a coprecipitation method. 29 Nickel sulfate hexahydrate (NiSO4.6H2O), manganese sulfate monohydrate (MnSO4.H2O), sodium hydroxide (NaOH), and ammonium hydroxide (NH3.H2O) were use… 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 . 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 7 6 7 78 #/texts/86 text body True None body body True p7:body_region:1 front_matter column_2_of_2 2 2 p7:front_matter:column_2_of_2:white [255, 255, 255] white False False [283.92, 67.14, 201.3, 139.35] surface coating or the chemical additive is not clear. Typically, in the present work, a thin layer of AlF3 coating on the surface of the LNMCO leads to a better capacity retention as illustrated in Figure 1. The surfac… surface coating or the chemical additive is not clear. Typically, in the present work, a thin layer of AlF3 coating on the surface of the LNMCO leads to a better capacity retention as illustrated in Figure 1. The surfac… 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 7 8 9 80 #/texts/88 text body True None body body 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, 235.01, 201.32, 294.74] The LNMO and LNMCO layered cathode materials consist of an intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases. Migration of TM cations into the Li layer initiated the transformation to spinel for the R 3 m phase region… The LNMO and LNMCO layered cathode materials consist of an intergrowth of LiMO2 R 3 m and Li2MO3 C 2/ m phases. Migration of TM cations into the Li layer initiated the transformation to spinel for the R 3 m phase region… 7 9 10 81 #/texts/89#prov0 text body True None body body 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 [283.92, 576.24, 201.39, 168.31] dissolved in ethyl carbonate (EC) and dimethyl carbonate (DMC) (1:2 in volume) as electrolyte in an argon- fi lled MBraun glovebox. The electrochemical performance tests were performed galvanostatically between 2.0 and … dissolved in ethyl carbonate (EC) and dimethyl carbonate (DMC) (1:2 in volume) as electrolyte in an argon- fi lled MBraun glovebox. The electrochemical performance tests were performed galvanostatically between 2.0 and … 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 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 ' 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 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 8 1 1 86 #/texts/89#prov1 text body True None body body 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, 67.99, 201.41, 33.66] models are built using the VESTA software suite. The cycled samples are carried to the TEM within a sealed Ar atmosphere andtheturbo-pumpoftheS/TEMmicroscopeisprepumpedtofull speed so that the total air exposure time is… models are built using the VESTA software suite. The cycled samples are carried to the TEM within a sealed Ar atmosphere andtheturbo-pumpoftheS/TEMmicroscopeisprepumpedtofull speed so that the total air exposure time is… 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. 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 … 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… 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 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. 8 8 7 92 #/texts/101 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, 410.01, 194.79, 42.94] Armstrong, A. R.; Holzapfel, M.; Novák, P.; Johnson, C. S.; Kang, S.-H.; Thackeray, M. M.; Bruce, P. G. Demonstrating Oxygen Loss and Associated Structural Reorganization in the Lithium Battery Cathode Li[Ni0.2Li0.2Mn0.… Armstrong, A. R.; Holzapfel, M.; Novák, P.; Johnson, C. S.; Kang, S.-H.; Thackeray, M. M.; Bruce, P. G. Demonstrating Oxygen Loss and Associated Structural Reorganization in the Lithium Battery Cathode Li[Ni0.2Li0.2Mn0.… 8 9 8 93 #/texts/102 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, 455.37, 194.79, 33.92] Armstrong, A. R.; Lyness, C.; Panchmatia, P. M.; Islam, M. S.; Bruce, P. G. The Lithium Intercalation Process in the LowVoltage Lithium Battery Anode Li1 þ X V1 X O2. Nat. Mater. 2011 , 10 , 223 -229. Armstrong, A. R.; Lyness, C.; Panchmatia, P. M.; Islam, M. S.; Bruce, P. G. The Lithium Intercalation Process in the LowVoltage Lithium Battery Anode Li1 þ X V1 X O2. Nat. Mater. 2011 , 10 , 223 -229. 8 10 9 94 #/texts/103 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, 491.71, 194.75, 33.98] Ceder, G.; Chiang, Y. M.; Sadoway, D. R.; Aydinol, M. K.; Jang, Y. I.; Huang, B. Identi fi cation of Cathode Materials for Lithium Batteries Guided by First-Principles Calculations. Nature 1998 , 392 , 694 -696. Ceder, G.; Chiang, Y. M.; Sadoway, D. R.; Aydinol, M. K.; Jang, Y. I.; Huang, B. Identi fi cation of Cathode Materials for Lithium Batteries Guided by First-Principles Calculations. Nature 1998 , 392 , 694 -696. 8 11 10 95 #/texts/104 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, 527.52, 194.79, 16.28] Chiang, Y.-M. Building a Better Battery. Science 2010 , 330 , 1485 -1486. Chiang, Y.-M. Building a Better Battery. Science 2010 , 330 , 1485 -1486. 8 12 11 96 #/texts/105 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, 546.53, 194.8, 42.56] Gu, M.; Li, Y.; Li, X.; Hu, S.; Zhang, X.; Xu, W.; Thevuthasan, S.; Baer, D. R.; Zhang, J.-G.; Liu, J.; et al . In situ Tem Study of Lithiation Behavior of Silicon Nanoparticles Attached to and Embedded in a Carbon Matr… Gu, M.; Li, Y.; Li, X.; Hu, S.; Zhang, X.; Xu, W.; Thevuthasan, S.; Baer, D. R.; Zhang, J.-G.; Liu, J.; et al . In situ Tem Study of Lithiation Behavior of Silicon Nanoparticles Attached to and Embedded in a Carbon Matr… 8 13 12 97 #/texts/106 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, 591.82, 194.79, 33.98] Gu, M.; Belharouak, I.; Genc, A.; Wang, D.; Wang, Z.; Amine, K.; Gao, F.; Zhou, G.; Thevuthasan, S.; Baer, D. R.; et al . Con fl icting Roles of Ni in Controlling Cathode Performance in Li-Ion Batteries. Nano Lett. 2012… Gu, M.; Belharouak, I.; Genc, A.; Wang, D.; Wang, Z.; Amine, K.; Gao, F.; Zhou, G.; Thevuthasan, S.; Baer, D. R.; et al . Con fl icting Roles of Ni in Controlling Cathode Performance in Li-Ion Batteries. Nano Lett. 2012… 8 14 13 98 #/texts/107 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, 628.22, 194.8, 34.33] Yu, C.; Guan, X.; Li, G.; Zheng, J.; Li, L.; Novel, A. Approach to Composite Electrode 0.3Li2MnO3 0.7LiMn1/3Ni1/3Co1/3O2 in Lithium-Ion Batteries with an Anomalous Capacity and Cycling Stability at 45.4 ° C. Scr. Mate… Yu, C.; Guan, X.; Li, G.; Zheng, J.; Li, L.; Novel, A. Approach to Composite Electrode 0.3Li2MnO3 0.7LiMn1/3Ni1/3Co1/3O2 in Lithium-Ion Batteries with an Anomalous Capacity and Cycling Stability at 45.4 ° C. Scr. Mate… 8 15 14 99 #/texts/108 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, 664.56, 194.75, 42.94] Ito, A.; Shoda, K.; Sato, Y.; Hatano, M.; Horie, H.; Ohsawa, Y. Direct Observation of the Partial Formation of a Framework Structure for Li-Rich Layered Cathode Material Li[Ni0.17Li0.2Co0.07Mn0.56]O2 Upon the First Char… Ito, A.; Shoda, K.; Sato, Y.; Hatano, M.; Horie, H.; Ohsawa, Y. Direct Observation of the Partial Formation of a Framework Structure for Li-Rich Layered Cathode Material Li[Ni0.17Li0.2Co0.07Mn0.56]O2 Upon the First Char… 8 16 15 100 #/texts/109 list_item reference 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 [67.35, 710.37, 198.62, 33.98] Hong, J.; Seo, D.-H.; Kim, S.-W.; Gwon, H.; Oh, S.-T.; Kang, K. Structural Evolution of Layered Li1.2Ni0.2Mn0.6O2 Upon Electrochemical Cycling in a Li Rechargeable Battery. J. Mater. Chem. 2010 , 20 , 10179 -10186. Hong, J.; Seo, D.-H.; Kim, S.-W.; Gwon, H.; Oh, S.-T.; Kang, K. Structural Evolution of Layered Li1.2Ni0.2Mn0.6O2 Upon Electrochemical Cycling in a Li Rechargeable Battery. J. Mater. Chem. 2010 , 20 , 10179 -10186. 8 37 16 101 #/texts/130 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 [64.29, 760.66, 34.51, 7.08] GU ET AL . GU ET AL . 8 2 17 102 #/texts/95 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 p8:top_margin:column_2_of_2:white [255, 255, 255] white False False [540.13, 47.17, 28.39, 112.47] ARTICLE ARTICLE 8 17 18 103 #/texts/110 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 67.99, 198.64, 33.67] Kim, J. H.; Sun, Y. K. Electrochemical Performance of Li[LixNi (1 3 x )/2Mn(1 þ X )/2]O2 Cathode Materials Synthesized by a Sol Gel Method. J. Power Sources 2003 , 119 121 , 166 -170. Kim, J. H.; Sun, Y. K. Electrochemical Performance of Li[LixNi (1 3 x )/2Mn(1 þ X )/2]O2 Cathode Materials Synthesized by a Sol Gel Method. J. Power Sources 2003 , 119 121 , 166 -170. 8 18 19 104 #/texts/111 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.52, 103.64, 198.67, 34.66] Fell, C. R.; Carroll, K. J.; Chi, M.; Meng, Y. S. Synthesis Structure Property Relations in Layered, Li-Excess Oxides Electrode Materials Li[Li [1/3 -2 x /3]NixMn[2/3 -X /3]]O2 ( X = 1/3, 1/4, and 1/5). J. Electroch… Fell, C. R.; Carroll, K. J.; Chi, M.; Meng, Y. S. Synthesis Structure Property Relations in Layered, Li-Excess Oxides Electrode Materials Li[Li [1/3 -2 x /3]NixMn[2/3 -X /3]]O2 ( X = 1/3, 1/4, and 1/5). J. Electroch… 8 19 20 105 #/texts/112 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 140.72, 198.64, 33.67] Lu, Z.; Beaulieu, L. Y.; Donaberger, R. A.; Thomas, C. L.; Dahn, J. R. Synthesis, Structure, and Electrochemical Behavior of Li[Ni x Li [1/3 -2 x /3]Mn[2/3 -X /3]]O2. J. Electrochem. Soc. 2002 , 149 , A778 -A791. Lu, Z.; Beaulieu, L. Y.; Donaberger, R. A.; Thomas, C. L.; Dahn, J. R. Synthesis, Structure, and Electrochemical Behavior of Li[Ni x Li [1/3 -2 x /3]Mn[2/3 -X /3]]O2. J. Electrochem. Soc. 2002 , 149 , A778 -A791. 8 20 21 106 #/texts/113 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.52, 177.12, 198.65, 24.96] Seo, H.; Lee, E.; Yi, C.-W.; Kim, K. The Synthesis and Electrochemical Properties of Lithium Manganese Oxide (Li2MnO3). J. Electrochem. Sci. Technol. 2011 , 2 , 180 -185. Seo, H.; Lee, E.; Yi, C.-W.; Kim, K. The Synthesis and Electrochemical Properties of Lithium Manganese Oxide (Li2MnO3). J. Electrochem. Sci. Technol. 2011 , 2 , 180 -185. 8 21 22 107 #/texts/114 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 204.5, 198.62, 42.93] Xu, B.; Fell, C. R.; Chi, M.; Meng, Y. S. Identifying Surface Structural Changes in Layered Li-Excess Nickel Manganese Oxides in High Voltage Lithium Ion Batteries: A Joint Experimental and Theoretical Study. Energy Env… Xu, B.; Fell, C. R.; Chi, M.; Meng, Y. S. Identifying Surface Structural Changes in Layered Li-Excess Nickel Manganese Oxides in High Voltage Lithium Ion Batteries: A Joint Experimental and Theoretical Study. Energy Env… 8 22 23 108 #/texts/115 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 249.8, 198.66, 33.98] Deng, Z. Q.; Manthiram, A. In fl uence of Cationic Substitutions on the Oxygen Loss and Reversible Capacity of Lithium-Rich Layered Oxide Cathodes. J. Phys. Chem. C 2011 , 115 , 7097 -7103. Deng, Z. Q.; Manthiram, A. In fl uence of Cationic Substitutions on the Oxygen Loss and Reversible Capacity of Lithium-Rich Layered Oxide Cathodes. J. Phys. Chem. C 2011 , 115 , 7097 -7103. 8 23 24 109 #/texts/116 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 286.2, 198.66, 24.97] Yu, D. Y. W.; Yanagida, K. Structural Analysis of Li2MnO3 and Related Li Mn O Materials. J. Electrochem. Soc. 2011 , 158 , A1015 -A1022. Yu, D. Y. W.; Yanagida, K. Structural Analysis of Li2MnO3 and Related Li Mn O Materials. J. Electrochem. Soc. 2011 , 158 , A1015 -A1022. 8 24 25 110 #/texts/117 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 313.58, 198.62, 24.96] Pennycook, S. J. Z -contrast Transmission Electron Microscopy ; Direct Atomic Imaging of Materials. Annu. Rev. Mater. Sci. 1992 , 22 , 171 -195. Pennycook, S. J. Z -contrast Transmission Electron Microscopy ; Direct Atomic Imaging of Materials. Annu. Rev. Mater. Sci. 1992 , 22 , 171 -195. 8 25 26 111 #/texts/118 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 340.96, 198.66, 42.62] Zheng, J. M.; Zhang, Z. R.; Wu, X. B.; Dong, Z. X.; Zhu, Z.; Yang, Y. The E ff ects of AlF3 Coating on the Performance of Li[Li0.2Mn0.54Ni0.13Co0.13]O2 Positive Electrode Material for Lithium-Ion Battery. J. Electrochem… Zheng, J. M.; Zhang, Z. R.; Wu, X. B.; Dong, Z. X.; Zhu, Z.; Yang, Y. The E ff ects of AlF3 Coating on the Performance of Li[Li0.2Mn0.54Ni0.13Co0.13]O2 Positive Electrode Material for Lithium-Ion Battery. J. Electrochem… 8 26 27 112 #/texts/119 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 386.32, 198.66, 33.92] Zheng, J. M.; Wu, X. B.; Yang, Y. A Comparison of Preparation Method on the Electrochemical Performance of Cathode Material Li[Li0.2Mn0.54Ni0.13Co0.13]O2 for Lithium Ion Battery. Electrochim. Acta 2011 , 56 , 3071 -3078. Zheng, J. M.; Wu, X. B.; Yang, Y. A Comparison of Preparation Method on the Electrochemical Performance of Cathode Material Li[Li0.2Mn0.54Ni0.13Co0.13]O2 for Lithium Ion Battery. Electrochim. Acta 2011 , 56 , 3071 -3078. 8 27 28 113 #/texts/120 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 422.66, 198.66, 43.42] Zheng, J.; Zhu, D.; Yang, Y.; Fung, Y. The E ff ects of N -MethylN -Butylpyrrolidinium Bis(Tri fl uoromethylsulfonyl)Imide-Based Electrolyte on the Electrochemical Performance of High Capacity Cathode Material Li[Li 0.2… Zheng, J.; Zhu, D.; Yang, Y.; Fung, Y. The E ff ects of N -MethylN -Butylpyrrolidinium Bis(Tri fl uoromethylsulfonyl)Imide-Based Electrolyte on the Electrochemical Performance of High Capacity Cathode Material Li[Li 0.2… 8 28 29 114 #/texts/121 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 468.01, 198.62, 33.92] Lu, Z.; Dahn, J. R. Understanding the Anomalous Capacity of Li/Li[Ni X Li (1/3 -2 x /3)Mn(2/3 -X /3)]O2 Cells Using in situ X-ray Di ff raction and Electrochemical Studies. J. Electrochem. Soc. 2002 , 149 , A815. Lu, Z.; Dahn, J. R. Understanding the Anomalous Capacity of Li/Li[Ni X Li (1/3 -2 x /3)Mn(2/3 -X /3)]O2 Cells Using in situ X-ray Di ff raction and Electrochemical Studies. J. Electrochem. Soc. 2002 , 149 , A815. 8 29 30 115 #/texts/122 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 503.9, 198.66, 34.4] Johnson, C. S.; Li, N.; Le fi ef, C.; Vaughey, J. T.; Thackeray, M. M. Synthesis, Characterization and Electrochemistry of Lithium Battery Electrodes: XLi2MnO3 3 (1 X )LiMn0.333 Ni0.333 -Co0.333O2 (0 e X e 0.7). Chem.… Johnson, C. S.; Li, N.; Le fi ef, C.; Vaughey, J. T.; Thackeray, M. M. Synthesis, Characterization and Electrochemistry of Lithium Battery Electrodes: XLi2MnO3 3 (1 X )LiMn0.333 Ni0.333 -Co0.333O2 (0 e X e 0.7). Chem.… 8 30 31 116 #/texts/123 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 539.73, 198.64, 33.98] Jarvis, K. A.; Deng, Z.-Q.; Allard, L. F.; Manthiram, A.; Ferreira, P. J. Atomic Structure of a Lithium-Rich Layered Oxide Material for Lithium-Ion Batteries: Evidence of a Solid Solution. Chem. Mater. 2011 , 23 , 3614 … Jarvis, K. A.; Deng, Z.-Q.; Allard, L. F.; Manthiram, A.; Ferreira, P. J. Atomic Structure of a Lithium-Rich Layered Oxide Material for Lithium-Ion Batteries: Evidence of a Solid Solution. Chem. Mater. 2011 , 23 , 3614 … 8 31 32 117 #/texts/124 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 575.61, 198.61, 24.97] Reed, J.; Ceder, G. Charge, Potential, and Phase Stability of Layered Li(Ni0.5Mn0.5)O2. Electrochem. Solid State Lett. 2002 , 5 , A145 -A148. Reed, J.; Ceder, G. Charge, Potential, and Phase Stability of Layered Li(Ni0.5Mn0.5)O2. Electrochem. Solid State Lett. 2002 , 5 , A145 -A148. 8 32 33 118 #/texts/125 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 602.49, 198.64, 33.66] Xiao, J.; Chernova, N. A.; Whittingham, M. S. Layered Mixed Transition Metal Oxide Cathodes with Reduced Cobalt Content for Lithium Ion Batteries. Chem. Mater. 2008 , 20 , 7454 -7464. Xiao, J.; Chernova, N. A.; Whittingham, M. S. Layered Mixed Transition Metal Oxide Cathodes with Reduced Cobalt Content for Lithium Ion Batteries. Chem. Mater. 2008 , 20 , 7454 -7464. 8 33 34 119 #/texts/126 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 638.37, 198.64, 24.97] Sun, Y.-K.; Myung, S.-T.; Park, B.-C.; Prakash, J.; Belharouak, I.; Amine, K. High-Energy Cathode Material for Long-Life and Safe Lithium Batteries. Nat. Mater. 2009 , 8 , 320 -324. Sun, Y.-K.; Myung, S.-T.; Park, B.-C.; Prakash, J.; Belharouak, I.; Amine, K. High-Energy Cathode Material for Long-Life and Safe Lithium Batteries. Nat. Mater. 2009 , 8 , 320 -324. 8 34 35 120 #/texts/127 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.53, 665.24, 198.62, 33.98] Lei, C. H.; Bareno, J.; Wen, J. G.; Petrov, I.; Kang, S. H.; Abraham, D. P. Local Structure and Composition Studies of Li1.2Ni0.2Mn0.6O2 by Analytical Electron Microscopy. J. Power Sources 2008 , 178 , 422 -433. Lei, C. H.; Bareno, J.; Wen, J. G.; Petrov, I.; Kang, S. H.; Abraham, D. P. Local Structure and Composition Studies of Li1.2Ni0.2Mn0.6O2 by Analytical Electron Microscopy. J. Power Sources 2008 , 178 , 422 -433. 8 35 36 121 #/texts/128 list_item reference False low after_back_matter_stop after_back_matter_stop after_stop False None page_body column_2_of_2 2 2 p8:page_body:column_2_of_2:white [255, 255, 255] white False False [286.52, 701.13, 198.64, 33.61] Wang, D.; Belharouak, I.; Koenig, G. M.; Zhou, G.; Amine, K. Growth Mechanism of Ni0.3Mn0.7CO3 Precursor for High Capacity Li-Ion Battery Cathodes. J. Mater. Chem. 2011 , 21 , 9290 -9295. Wang, D.; Belharouak, I.; Koenig, G. M.; Zhou, G.; Amine, K. Growth Mechanism of Ni0.3Mn0.7CO3 Precursor for High Capacity Li-Ion Battery Cathodes. J. Mater. Chem. 2011 , 21 , 9290 -9295. 8 39 37 122 #/texts/132 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 [551.96, 758.01, 14.85, 10.27] 767 767 8 38 38 123 #/texts/131 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 [323.72, 759.15, 141.77, 8.55] VOL. 7 ' NO. 1 ' 760 -767 ' 2013 VOL. 7 ' NO. 1 ' 760 -767 ' 2013 8 36 39 124 #/texts/129 text page_margin_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 True [473.22, 779.07, 59.2, 1.67] www.acsnano.org