Excluded Docling blocks

这里是差集：Docling 全量解析 text block 减去最终会进入正文的 block。优先人工检查 risk=high / medium。

layout_review.html excluded_blocks.json excluded_blocks.tsv final_body_blocks.tsv visual_assets.tsv original.pdf

Diff Summary

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Truncation

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Excluded Page Overlays

这些框显示被排除块，同时叠加真实图表资产框。青色虚线表示该 text block 被图表资产 caption 吸收；红色 STOP 是截断触发点，红色框是截断后被排除的块。

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Visual Assets

这是实际图表资产输出，不是审计层重新推断。

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1figureFig. 12nearby_text_caption0.82[303.89, 48.4, 254.45, 213.72]Fig. 1 | Structural characterization and electrochemical data for Li 1.2 Ni0.13 Co0.13 Mn0.54 O2. a , Li 1.2 Ni0.13 Co0.13 Mn0.54 O2 with a layered R 3m structure, in-plane ordering of Li/Ni and Co/Mn giving rise to the honeycomb superstructure ordering. Li atoms are represented in blue, TM in purple and oxygen in red. b , PXRD data and refinement to the R 3m crystal structure. c , Load curves for Li 1.2 Ni0.13 Co0.13 Mn0.54 O2, cycled between 2.0 V and 4.8 V at 100 mA g -1 for 100 cycles.
2figureFig. 23sequence_or_inferred_caption0.82[95.03, 49.21, 410.23, 456.31]Fig. 2 | Evolution in bulk O-redox activity over 2nd and 100th cycles. a , d , Load curves for the 2nd ( a ) and 100th ( d ) cycles for Li 1.2 Mn0.54 Co0.13 Ni0.13 O2, with the states of charge studied. b , e , RIXS spectra at 531.5 eV collected over the 2nd ( b ) and 100th ( e ) cycles. c , f , Variation in intensity of the molecular O 2 signal in the RIXS spectra over the 2nd ( c ) and 100th ( f ) cycles, as determined by principal component analysis (Methods). Data are presented as mean ± standard deviation with a sample size of 15. P, pristine.
3figureFig. 33nearby_text_caption0.82[347.62, 572.31, 181.51, 123.37]Fig. 3 | Evolution in amount of trapped O 2 over cycling. Variation in intensity of the molecular O 2 signal from RIXS over cycling in the fully charged (FC) and fully discharged (FD) states. The amount of O 2 formed in the charged materials decreases with cycling and there is increasing evidence of O 2 that is not reduced on discharge. Data are presented as mean ± standard deviation with a sample size of 15.
4figureFig. 44sequence_or_inferred_caption0.82[84.76, 55.16, 430.21, 324.23]Fig. 4 | Formation of voids and large diamagnetic Li-rich regions over cycling. a -c , ADF-STEM images showing single grains of the pristine ( a ), 2nd discharge ( b ) and 100th discharge ( c ) material showing the formation of voids about 4-12 nm in diameter over extended cycling. d , 129 Xe NMR experiments. Samples were extracted from cells and infiltrated with Xe gas to probe the open porosity. e , 129 Xe NMR of the pristine, 2nd discharge and 100th discharge materials. The orange region highlighted indicates the presence of open voids of 17 nm diameter and greater after 100 cycles. δ iso , isotropic chemical shift. f , g , 6 Li ( f ) and 17 O ( g ) NMR isolating slow and fast relaxing environments. The sharp peaks at 0 ppm in the 6 Li and slow relaxing 17 O NMR spectra indicate the formation of large diamagnetic Li-rich regions on extended cycling.
5figureFig. 55sequence_or_inferred_caption0.82[90.45, 53.92, 422.97, 266.9]Fig. 5 | Partial reduction of O 2 trapped in voids to form Li-coordinated O 2on the 100th discharge. a , b , 17 O NMR spectra isolating fast ( a ) and slow ( b ) relaxing 17 O environments. The sharp peaks in a are assigned to trapped molecular O2, which decrease in intensity on discharge. There is still evidence of some residual molecular O 2 in the discharged sample, δ cg ( 17 O2) = 2,770 ppm. In b the slow relaxation 17 O is dominated by oxide environments coordinated to paramagnetic TM ions (TM-O 2-), δ cg = 2,100-2,300 ppm. After discharge, a new 17 O environment is formed corresponding to oxide surrounded by Li (that is, Li-O 2) created by the reduction of O 2 in the voids and reinsertion of Li + into the voids coordinated by the O 2, centred at δ cg = 0 ppm. D 1 , relaxation delay. c , Large voids accommodating O2 are partially repopulated by Li + on discharge. Most O 2 is reduced to O 2but some residual O 2 remains.
6figureFig. 66direct_caption_ref0.82[90.07, 51.04, 426.68, 451.81]Fig. 6 | Voltage fade mechanism. a , b , Second cycle: reversible O-redox involves the formation of molecular O 2 trapped in small vacancy clusters throughout the particle. O 2 molecules are fully reduced to O 2on discharge forming small diamagnetic Li-rich regions. c , d , One-hundreth cycle: further TM migration
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white		[39.68, 115.3, 498.52, 52.07]Trapped O2 and the origin of voltage fade in layered Li-rich cathodesTrapped O2 and the origin of voltage fade in layered Li-rich cathodes
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white		[306.14, 232.57, 241.98, 17.77]Publisher's note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.Publisher's note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
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white		[306.14, 641.05, 256.79, 71.53]J.-J.M. conducted the synthesis and characterization work. J.-J.M. prepared the 129 Xe-infiltrated samples, R.A.H. prepared the 17 O-labelled samples and G.J.R. performed and fitted the MAS NMR. R.A.H. and J.-J.M. in close collaboration with S.A., M.G.-F. and K.-J.Z. conducted the RIXS measurements. A.W.R. and J.C. conducted the ADF-STEM measurements. M.J. performed the BET measurements. J.-J.M., R.A.H. and P.G.B. wrote the paper with contributions from all authors.J.-J.M. conducted the synthesis and characterization work. J.-J.M. prepared the 129 Xe-infiltrated samples, R.A.H. prepared the 17 O-labelled samples and G.J.R. performed and fitted the MAS NMR. R.A.H. and J.-J.M. in close collaboration with S.A., M.G.-F. and K.-J.Z. conducted the RIXS measurements. A.W.R. and J.C. conducted the ADF-STEM measurements. M.J. performed the BET measurements. J.-J.M., R.A.H. and P.G.B. wrote the paper with contributions from all authors.
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white		[306.14, 49.8, 233.31, 28.52]Peer review information Nature Materials thanks William Chueh, Naoaki Yabuuchi and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.Peer review information Nature Materials thanks William Chueh, Naoaki Yabuuchi and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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white		[39.69, 210.69, 113.18, 7.44]Received: 15 December 2021Received: 15 December 2021
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white		[39.69, 726.36, 448.43, 7.62]1 Department of Materials, University of Oxford, Oxford, UK. 2 The Faraday Institution, Didcot, UK. 3 Diamond Light Source, Didcot, UK.1 Department of Materials, University of Oxford, Oxford, UK. 2 The Faraday Institution, Didcot, UK. 3 Diamond Light Source, Didcot, UK.
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white		[39.69, 737.11, 465.54, 7.62]4 Department of Chemistry, University of Oxford, Oxford, UK. e-mail: robert.house@materials.ox.ac.uk; peter.bruce@materials.ox.ac.uk4 Department of Chemistry, University of Oxford, Oxford, UK. e-mail: robert.house@materials.ox.ac.uk; peter.bruce@materials.ox.ac.uk
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white		[39.69, 284.25, 157.2, 21.97]Voltage fade characteristics in Li 1.2 Ni0.13 Co0.13Mn0.54O2Voltage fade characteristics in Li 1.2 Ni0.13 Co0.13Mn0.54O2
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white		[436.42, 191.42, 5.7, 38.67]Voltage vs LiVoltage vs Li
low254textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[240, 240, 240]
gray		[307.4, 191.78, 3.95, 2.64]55
low255textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[239, 239, 239]
gray		[537.35, 194.1, 12.04, 4.82]20th20th
low256textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[308.97, 194.42, 5.7, 39.98]Intensity (×10Intensity (×10
low257textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[321.73, 197.29, 2.2, 4.82]11
low258textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[243, 243, 243]
gray		[448.01, 198.75, 8.1, 4.82]3.53.5
low259textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[224, 224, 224]
gray		[537.35, 199.77, 12.4, 4.82]60th60th
low260textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:off_white[247, 247, 247]
off_white		[537.35, 205.42, 14.93, 4.82]100th100th
low261textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[248, 248, 248]
white		[447.5, 211.29, 8.62, 4.82]3.03.0
low262textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[448.29, 223.84, 7.83, 4.82]2.52.5
low263textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[243, 243, 243]
gray		[320.18, 227.66, 3.75, 4.82]00
low264textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[447.77, 236.37, 8.35, 4.82]2.02.0
low265textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[244, 244, 244]
gray		[331.2, 244.0, 6.79, 4.82]2020
low266textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[215, 215, 215]
gray		[343.56, 244.0, 7.07, 4.82]3030
low267textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[254, 254, 254]
white		[356.02, 244.0, 7.14, 4.82]4040
low268textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[237, 237, 237]
gray		[368.6, 244.0, 6.97, 4.82]5050
low269textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[243, 243, 243]
gray		[381.01, 244.0, 7.15, 4.82]6060
low270textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[254, 254, 254]
white		[393.76, 244.0, 6.63, 4.82]7070
low271textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[195, 195, 195]
gray		[406.03, 244.0, 7.08, 4.82]8080
low272textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[228, 228, 228]
gray		[418.5, 244.0, 7.16, 4.82]9090
low273textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[248, 248, 248]
white		[458.99, 244.0, 3.75, 4.82]00
low274textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[228, 228, 228]
gray		[470.64, 244.0, 6.97, 4.82]5050
low275textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[241, 241, 241]
gray		[482.56, 244.0, 9.69, 4.82]100100
low276textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[239, 239, 239]
gray		[496.09, 244.0, 9.17, 4.82]150150
low277textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[254, 254, 254]
white		[508.67, 244.0, 50.23, 4.82]200 250 300 350200 250 300 350
low278textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[478.95, 253.6, 54.58, 7.27]Capacity (mAh g -1Capacity (mAh g -1
low279textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[236, 236, 236]
gray		[533.53, 255.17, 2.09, 5.7])
low280textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[357.26, 255.26, 3.6, 5.7]22
low281textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[232, 232, 232]
gray		[360.86, 255.26, 3.98, 5.7]θ
low282textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[364.84, 255.26, 18.04, 5.7](Cu K(Cu K
low283textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:white[250, 250, 250]
white		[391.19, 255.26, 2.09, 5.7])
low284textvisual_textvisual_textvisual_text
p2:body_region:1p2:body_zone:column_2_of_2:gray[219, 219, 219]
gray		[382.89, 258.69, 8.31, 3.95]α1,2α1,2
low285captioncaptiondocling_captiondocling_caption
p2:body_region:1p2:body_zone:column_2_of_2:white[255, 255, 255]
white		[306.14, 269.16, 254.8, 66.5]Fig. 1 | Structural characterization and electrochemical data for Li 1.2 Ni0.13 Co0.13 Mn0.54 O2. a , Li 1.2 Ni0.13 Co0.13 Mn0.54 O2 with a layered R 3m structure, in-plane ordering of Li/Ni and Co/Mn giving rise to the honeycomb superstructure ordering. Li atoms are represented in blue, TM in purple and oxygen in red. b , PXRD data and refinement to the R 3m crystal structure. c , Load curves for Li 1.2 Ni0.13 Co0.13 Mn0.54 O2, cycled between 2.0 V and 4.8 V at 100 mA g -1 for 100 cycles.Fig. 1 | Structural characterization and electrochemical data for Li 1.2 Ni0.13 Co0.13 Mn0.54 O2. a , Li 1.2 Ni0.13 Co0.13 Mn0.54 O2 with a layered R 3m structure, in-plane ordering of Li/Ni and Co/Mn giving rise to the honeycomb superstructure ordering. Li atoms are represented in blue, TM in purple and oxygen in red. b , PXRD data and refinement to the R 3m crystal structure. c , Load curves for Li 1.2 Ni0.13 Co0.13 Mn0.54 O2, cycled between 2.0 V and 4.8 V at 100 mA g -1 for 100 cycles.
low290page_footerpage_footerdocling_page_footerdocling_page_footer
p2:body_region:1p2:bottom_margin:column_2_of_2:gray[238, 238, 238]
gray		[548.66, 764.06, 14.02, 6.99]819819
low391page_headerpage_headerdocling_page_headerdocling_page_header
p3:body_region:0p3:top_margin:left:white[255, 255, 255]
white		[39.69, 24.45, 31.06, 8.75]ArticleArticle
low392page_headerpage_headerdocling_page_headerdocling_page_header
p3:top_margin:right:off_white[243, 247, 250]
off_white		[392.65, 25.88, 176.63, 6.99]https://doi.org/10.1038/s41563-024-01833-z
low393textvisual_textvisual_textvisual_text
p3:body_region:0p3:top_margin:left:white[255, 255, 255]
white		[96.86, 50.07, 5.44, 8.12]aa
low394textvisual_textvisual_textvisual_text
p3:body_region:0p3:top_margin:left:white[250, 250, 250]
white		[117.02, 52.2, 3.23, 4.82]55
low395textvisual_textvisual_textvisual_text
p3:body_region:0p3:top_margin:left:gray[245, 245, 245]
gray		[260.54, 56.98, 7.01, 4.82]FCFC
low396textvisual_textvisual_textvisual_text
p3:top_margin:right:white[252, 252, 252]
white		[310.13, 50.07, 6.0, 8.12]dd
low397textvisual_textvisual_textvisual_text
p3:top_margin:right:gray[234, 234, 234]
gray		[322.81, 52.27, 3.23, 4.82]55
low398textvisual_textvisual_textvisual_text
p3:top_margin:right:white[255, 255, 255]
white		[462.72, 57.95, 7.01, 4.82]FCFC
low399textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:off_white[247, 247, 247]
off_white		[134.41, 61.13, 25.16, 4.82]2nd cycle2nd cycle
low3100textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[244, 244, 244]
gray		[235.73, 66.39, 11.8, 4.82]3QC3QC
low3101textvisual_textvisual_textvisual_text
p3:page_body:right:gray[240, 240, 240]
gray		[341.01, 61.13, 30.3, 4.82]100th cycle100th cycle
low3102textvisual_textvisual_textvisual_text
p3:page_body:right:gray[245, 245, 245]
gray		[437.75, 73.0, 11.8, 4.82]3QC3QC
low3103textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[104.98, 100.41, 3.95, 2.34]+
low3104textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[106.55, 82.5, 5.7, 17.91]/Li (V)/Li (V)
low3105textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[254, 254, 254]
white		[116.86, 92.5, 3.39, 4.82]44
low3106textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[227, 227, 227]
gray		[158.83, 91.55, 8.47, 4.82]QCQC
low3107textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[196.14, 82.56, 8.02, 4.82]HCHC
low3108textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[311.21, 85.19, 5.7, 17.91]/Li (V)/Li (V)
low3109textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[322.65, 92.55, 3.39, 4.82]44
low3110textvisual_textvisual_textvisual_text
p3:page_body:right:white[251, 251, 251]
white		[366.64, 98.48, 8.47, 4.82]QCQC
low3111textvisual_textvisual_textvisual_text
p3:page_body:right:gray[191, 191, 191]
gray		[403.36, 84.89, 8.02, 4.82]HCHC
low3112textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[106.55, 102.75, 5.7, 38.86]Voltage vs LiVoltage vs Li
low3113textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[235, 235, 235]
gray		[116.93, 132.81, 3.32, 4.82]33
low3114textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[252, 252, 252]
white		[127.18, 105.23, 3.05, 4.82]22
low3115textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[216, 216, 216]
gray		[130.23, 103.67, 4.29, 3.07]ndnd
low3116textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[134.51, 105.24, 4.65, 4.82]PP
low3117textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[214, 214, 214]
gray		[157.45, 135.52, 11.61, 4.82]3QD3QD
low3118textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[196.96, 122.94, 7.84, 4.82]HDHD
low3119textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[213, 213, 213]
gray		[239.44, 102.74, 8.28, 4.82]QDQD
low3120textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[309.64, 103.11, 3.95, 2.34]+
low3121textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[311.21, 105.44, 5.7, 38.86]Voltage vs LiVoltage vs Li
low3122textvisual_textvisual_textvisual_text
p3:page_body:right:gray[211, 211, 211]
gray		[322.72, 132.95, 3.32, 4.82]33
low3123textvisual_textvisual_textvisual_text
p3:page_body:right:gray[241, 241, 241]
gray		[332.53, 111.34, 9.7, 4.82]100100
low3124textvisual_textvisual_textvisual_text
p3:page_body:right:gray[194, 194, 194]
gray		[342.22, 109.76, 3.31, 3.07]thth
low3125textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[345.53, 111.33, 4.65, 4.82]PP
low3126textvisual_textvisual_textvisual_text
p3:page_body:right:white[254, 254, 254]
white		[441.12, 126.78, 8.28, 4.82]QDQD
low3127textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[364.59, 150.44, 11.61, 4.82]3QD3QD
low3128textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[403.68, 142.69, 7.84, 4.82]HDHD
low3129textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[252, 252, 252]
white		[117.2, 173.11, 3.05, 4.82]22
low3130textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[132.47, 168.15, 6.83, 4.82]FDFD
low3131textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[322.99, 173.22, 3.05, 4.82]22
low3132textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[340.6, 166.73, 6.83, 4.82]FDFD
low3133textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[243, 243, 243]
gray		[126.12, 180.59, 3.75, 4.82]00
low3134textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[200, 200, 200]
gray		[150.72, 180.59, 6.98, 4.82]5050
low3135textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[252, 252, 252]
white		[175.59, 180.59, 9.7, 4.82]100100
low3136textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[235, 235, 235]
gray		[202.07, 180.59, 9.18, 4.82]150150
low3137textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[235, 235, 235]
gray		[227.61, 180.59, 10.55, 4.82]200200
low3138textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[235, 235, 235]
gray		[254.09, 180.59, 10.03, 4.82]250250
low3139textvisual_textvisual_textvisual_text
p3:page_body:right:gray[200, 200, 200]
gray		[332.71, 180.59, 3.75, 4.82]00
low3140textvisual_textvisual_textvisual_text
p3:page_body:right:gray[237, 237, 237]
gray		[365.96, 180.59, 6.98, 4.82]5050
low3141textvisual_textvisual_textvisual_text
p3:page_body:right:gray[219, 219, 219]
gray		[399.46, 180.59, 9.7, 4.82]100100
low3142textvisual_textvisual_textvisual_text
p3:page_body:right:gray[239, 239, 239]
gray		[434.57, 180.59, 9.18, 4.82]150150
low3143textvisual_textvisual_textvisual_text
p3:page_body:right:gray[243, 243, 243]
gray		[468.74, 180.59, 10.55, 4.82]200200
low3144textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[173.24, 190.42, 54.98, 7.27]Capacity (mAh g -1Capacity (mAh g -1
low3145textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[239, 239, 239]
gray		[228.22, 191.99, 2.09, 5.7])
low3146textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[379.35, 190.42, 54.98, 7.27]Capacity (mAh g -1Capacity (mAh g -1
low3147textvisual_textvisual_textvisual_text
p3:page_body:right:white[254, 254, 254]
white		[434.33, 191.99, 2.09, 5.7])
low3148textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[96.86, 209.88, 6.01, 8.12]bb
low3149textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[311.22, 209.88, 5.62, 8.12]ee
low3150textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[241, 241, 241]
gray		[134.81, 223.31, 25.16, 4.82]2nd cycle2nd cycle
low3151textvisual_textvisual_textvisual_text
p3:page_body:right:gray[240, 240, 240]
gray		[343.72, 220.31, 30.3, 4.82]100th cycle100th cycle
low3152textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:off_white[247, 247, 247]
off_white		[279.75, 238.74, 3.05, 4.82]22
low3153textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:gray[210, 210, 210]
gray		[282.8, 237.17, 4.29, 3.07]ndnd
low3154textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:white[255, 255, 255]
white		[287.09, 238.74, 4.65, 4.82]PP
low3155textvisual_textvisual_textvisual_text
p3:page_body:right:white[251, 251, 251]
white		[486.95, 236.11, 9.7, 4.82]100100
low3156textvisual_textvisual_textvisual_text
p3:page_body:right:gray[199, 199, 199]
gray		[496.65, 234.54, 3.31, 3.07]thth
low3157textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[499.96, 236.11, 4.65, 4.82]PP
low3158textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:off_white[247, 247, 247]
off_white		[279.76, 249.19, 8.47, 4.82]QCQC
low3159textvisual_textvisual_textvisual_text
p3:page_body:right:gray[243, 243, 243]
gray		[486.96, 247.96, 8.47, 4.82]QCQC
low3160textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:white[248, 248, 248]
white		[279.76, 260.2, 8.02, 4.82]HCHC
low3161textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[486.96, 260.12, 8.02, 4.82]HCHC
low3162textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:white[253, 253, 253]
white		[279.76, 272.44, 11.8, 4.82]3QC3QC
low3163textvisual_textvisual_textvisual_text
p3:page_body:right:gray[239, 239, 239]
gray		[486.96, 272.02, 11.8, 4.82]3QC3QC
low3164textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:gray[245, 245, 245]
gray		[279.76, 284.31, 7.01, 4.82]FCFC
low3165textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[486.96, 283.28, 7.01, 4.82]FCFC
low3166textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:white[254, 254, 254]
white		[279.76, 295.26, 8.28, 4.82]QDQD
low3167textvisual_textvisual_textvisual_text
p3:page_body:right:gray[235, 235, 235]
gray		[486.96, 294.26, 8.28, 4.82]QDQD
low3168textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:white[248, 248, 248]
white		[279.76, 307.01, 7.84, 4.82]HDHD
low3169textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[486.96, 306.52, 7.84, 4.82]HDHD
low3170textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:white[251, 251, 251]
white		[279.76, 317.15, 11.61, 4.82]3QD3QD
low3171textvisual_textvisual_textvisual_text
p3:page_body:right:gray[235, 235, 235]
gray		[486.96, 318.04, 11.61, 4.82]3QD3QD
low3172textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left_crossing:white[255, 255, 255]
white		[279.76, 327.7, 6.83, 4.82]FDFD
low3173textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[486.96, 329.64, 6.83, 4.82]FDFD
low3174textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[253, 253, 253]
white		[125.88, 339.79, 3.75, 4.82]00
low3175textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[161.11, 339.79, 7.83, 4.82]2.52.5
low3176textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[254, 254, 254]
white		[198.03, 339.79, 8.52, 4.82]5.05.0
low3177textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[235.73, 339.79, 7.67, 4.82]7.57.5
low3178textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[271.21, 339.79, 11.24, 4.82]10.010.0
low3179textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[334.36, 339.79, 3.75, 4.82]00
low3180textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[369.22, 339.79, 7.83, 4.82]2.52.5
low3181textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[405.78, 339.79, 8.52, 4.82]5.05.0
low3182textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[443.11, 339.79, 7.67, 4.82]7.57.5
low3183textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[478.24, 339.79, 11.24, 4.82]10.010.0
low3184textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[175.98, 350.09, 48.86, 5.7]Energy loss (eV)Energy loss (eV)
low3185textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[382.02, 350.09, 48.86, 5.7]Energy loss (eV)Energy loss (eV)
low3186textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[96.86, 367.5, 5.45, 8.12]cc
low3187textvisual_textvisual_textvisual_text
p3:page_body:right_crossing:white[255, 255, 255]
white		[302.23, 367.02, 3.65, 8.12]ff
low3188textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[237, 237, 237]
gray		[109.7, 382.56, 10.55, 4.82]200200
low3189textvisual_textvisual_textvisual_text
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low3190textvisual_textvisual_textvisual_text
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low3191textvisual_textvisual_textvisual_text
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gray		[341.01, 381.59, 30.3, 4.82]100th cycle100th cycle
low3192textvisual_textvisual_textvisual_text
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white		[97.72, 398.66, 5.29, 59.84]signal intensity (a.u.)signal intensity (a.u.)
low3193textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[241, 241, 241]
gray		[110.55, 435.33, 9.7, 4.82]100100
low3194textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[111.07, 408.95, 9.18, 4.82]150150
low3195textvisual_textvisual_textvisual_text
p3:page_body:right_crossing:white[255, 255, 255]
white		[303.09, 397.57, 5.29, 59.84]signal intensity (a.u.)signal intensity (a.u.)
low3196textvisual_textvisual_textvisual_text
p3:page_body:right:gray[238, 238, 238]
gray		[316.19, 434.59, 9.7, 4.82]100100
low3197textvisual_textvisual_textvisual_text
p3:page_body:right:gray[245, 245, 245]
gray		[316.71, 407.75, 9.18, 4.82]150150
low3198textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[97.72, 458.5, 6.96, 7.12]O 2O 2
low3199textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[249, 249, 249]
white		[113.27, 461.71, 6.98, 4.82]5050
low3200textvisual_textvisual_textvisual_text
p3:page_body:right_crossing:white[255, 255, 255]
white		[303.09, 457.41, 6.96, 7.12]O 2O 2
low3201textvisual_textvisual_textvisual_text
p3:page_body:right:gray[240, 240, 240]
gray		[318.91, 461.41, 6.98, 4.82]5050
low3202textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[248, 248, 248]
white		[116.5, 488.1, 3.75, 4.82]00
low3203textvisual_textvisual_textvisual_text
p3:page_body:right:gray[243, 243, 243]
gray		[322.14, 488.1, 3.75, 4.82]00
low3204textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[126.67, 499.56, 14.44, 4.82]2nd P2nd P
low3205textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[251, 251, 251]
white		[146.74, 499.55, 8.47, 4.82]QCQC
low3206textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:gray[226, 226, 226]
gray		[164.04, 499.55, 8.02, 4.82]HCHC
low3207textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[179.24, 499.55, 11.8, 4.82]3QC3QC
low3208textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[198.72, 499.55, 7.01, 4.82]FCFC
low3209textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[215.17, 499.55, 8.28, 4.82]QDQD
low3210textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[248, 248, 248]
white		[232.47, 499.55, 7.84, 4.82]HDHD
low3211textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[247.67, 499.55, 11.61, 4.82]3QD3QD
low3212textvisual_textvisual_textvisual_text
p3:body_region:0p3:page_body:left:white[255, 255, 255]
white		[267.14, 499.55, 6.83, 4.82]FDFD
low3213textvisual_textvisual_textvisual_text
p3:page_body:right:white[253, 253, 253]
white		[329.54, 499.55, 19.58, 4.82]100th P100th P
low3214textvisual_textvisual_textvisual_text
p3:page_body:right:white[254, 254, 254]
white		[352.25, 499.55, 8.47, 4.82]QCQC
low3215textvisual_textvisual_textvisual_text
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gray		[369.41, 499.55, 8.02, 4.82]HCHC
low3216textvisual_textvisual_textvisual_text
p3:page_body:right:white[253, 253, 253]
white		[384.46, 499.55, 11.8, 4.82]3QC3QC
low3217textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[403.79, 499.55, 7.01, 4.82]FCFC
low3218textvisual_textvisual_textvisual_text
p3:page_body:right:gray[241, 241, 241]
gray		[420.09, 499.55, 8.28, 4.82]QDQD
low3219textvisual_textvisual_textvisual_text
p3:page_body:right:gray[228, 228, 228]
gray		[437.25, 499.55, 7.84, 4.82]HDHD
low3220textvisual_textvisual_textvisual_text
p3:page_body:right:white[249, 249, 249]
white		[452.3, 499.55, 11.61, 4.82]3QD3QD
low3221textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[471.63, 499.55, 6.83, 4.82]FDFD
low3222captioncaptionoutside_body_flow_captionoutside_body_flow_caption
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white		[39.68, 515.49, 253.49, 37.32]Fig. 2 | Evolution in bulk O-redox activity over 2nd and 100th cycles. a , d , Load curves for the 2nd ( a ) and 100th ( d ) cycles for Li 1.2 Mn0.54 Co0.13 Ni0.13 O2, with the states of charge studied. b , e , RIXS spectra at 531.5 eV collected over the 2nd ( b ) and 100th ( e ) cycles. c , f , Variation in intensity of the molecular O 2 signal inFig. 2 | Evolution in bulk O-redox activity over 2nd and 100th cycles. a , d , Load curves for the 2nd ( a ) and 100th ( d ) cycles for Li 1.2 Mn0.54 Co0.13 Ni0.13 O2, with the states of charge studied. b , e , RIXS spectra at 531.5 eV collected over the 2nd ( b ) and 100th ( e ) cycles. c , f , Variation in intensity of the molecular O 2 signal in
low3223captioncaptionoutside_body_flow_captionoutside_body_flow_caption
p3:page_body:right_crossing:white[255, 255, 255]
white		[306.47, 515.49, 254.96, 26.5]the RIXS spectra over the 2nd ( c ) and 100th ( f ) cycles, as determined by principal component analysis (Methods). Data are presented as mean ± standard deviation with a sample size of 15. P, pristine.the RIXS spectra over the 2nd ( c ) and 100th ( f ) cycles, as determined by principal component analysis (Methods). Data are presented as mean ± standard deviation with a sample size of 15. P, pristine.
low3225captioncaptiondocling_captiondocling_caption
p3:bottom_margin:right_crossing:white[255, 255, 255]
white		[306.14, 700.46, 255.03, 44.5]Fig. 3 | Evolution in amount of trapped O 2 over cycling. Variation in intensity of the molecular O 2 signal from RIXS over cycling in the fully charged (FC) and fully discharged (FD) states. The amount of O 2 formed in the charged materials decreases with cycling and there is increasing evidence of O 2 that is not reduced on discharge. Data are presented as mean ± standard deviation with a sample size of 15.Fig. 3 | Evolution in amount of trapped O 2 over cycling. Variation in intensity of the molecular O 2 signal from RIXS over cycling in the fully charged (FC) and fully discharged (FD) states. The amount of O 2 formed in the charged materials decreases with cycling and there is increasing evidence of O 2 that is not reduced on discharge. Data are presented as mean ± standard deviation with a sample size of 15.
low3226textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[349.66, 587.7, 5.7, 72.26]O2 signal intensity (a.u.)O2 signal intensity (a.u.)
low3227textvisual_textvisual_textvisual_text
p3:page_body:right:gray[235, 235, 235]
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low3228textvisual_textvisual_textvisual_text
p3:page_body:right:gray[240, 240, 240]
gray		[361.76, 625.17, 9.7, 4.82]100100
low3229textvisual_textvisual_textvisual_text
p3:page_body:right:white[253, 253, 253]
white		[362.28, 603.82, 9.18, 4.82]150150
low3230textvisual_textvisual_textvisual_text
p3:page_body:right:white[248, 248, 248]
white		[364.49, 646.51, 6.97, 4.82]5050
low3231textvisual_textvisual_textvisual_text
p3:page_body:right:white[248, 248, 248]
white		[367.71, 667.86, 3.75, 4.82]00
low3232textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[378.54, 679.05, 3.75, 4.82]00
low3233textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[405.57, 679.05, 6.8, 4.82]2020
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p3:page_body:right:white[255, 255, 255]
white		[431.21, 689.17, 43.08, 5.7]Cycle numberCycle number
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p3:page_body:right:white[255, 255, 255]
white		[433.95, 679.05, 7.14, 4.82]4040
low3236textvisual_textvisual_textvisual_text
p3:page_body:right:white[250, 250, 250]
white		[462.5, 679.05, 7.16, 4.82]6060
low3237textvisual_textvisual_textvisual_text
p3:page_body:right:gray[245, 245, 245]
gray		[473.85, 606.76, 7.02, 4.82]FCFC
low3238textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[473.86, 652.3, 6.83, 4.82]FDFD
low3239textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[491.08, 679.05, 7.09, 4.82]8080
low3240textvisual_textvisual_textvisual_text
p3:page_body:right:white[255, 255, 255]
white		[518.33, 679.05, 9.7, 4.82]100100
low3241page_footerpage_footerdocling_page_footerdocling_page_footer
p3:body_region:0p3:bottom_margin:left:white[255, 255, 255]
white		[39.69, 763.46, 185.86, 7.0]Nature Materials | Volume 23 | June 2024 | 818-825Nature Materials | Volume 23 | June 2024 | 818-825
low3242page_footerpage_footerdocling_page_footerdocling_page_footer
p3:bottom_margin:right:white[255, 255, 255]
white		[546.3, 763.81, 15.75, 6.99]820820
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white		[39.69, 24.45, 31.06, 8.75]ArticleArticle
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white		[87.18, 54.88, 5.44, 8.12]aa
low4245textvisual_textvisual_textvisual_text
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white		[143.04, 59.91, 22.56, 5.7]PristinePristine
low4246textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_1_of_2:gray[108, 108, 108]
gray		[96.76, 184.93, 16.56, 4.82]20 nm20 nm
low4247textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[87.19, 208.88, 6.0, 8.12]dd
low4248textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[162.28, 232.54, 27.75, 5.7]EvacuateEvacuate
low4249textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[92.38, 244.87, 29.44, 5.7]ElectrodeElectrode
low4250textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[123.65, 265.28, 30.04, 5.7]NMR tubeNMR tube
low4251textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[162.28, 275.04, 27.85, 5.7]Xe purgeXe purge
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white		[93.98, 342.98, 21.55, 5.7]CycledCycled
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p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[92.18, 350.78, 25.16, 5.7]cathodecathode
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p4:body_region:0p4:page_body:column_1_of_2:white[254, 254, 254]
white		[93.08, 358.58, 23.35, 5.7]particleparticle
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p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[154.83, 359.12, 32.84, 5.7]Open poreOpen pore
low4256captioncaptionoutside_body_flow_captionoutside_body_flow_caption
p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[39.67, 385.51, 252.98, 56.5]Fig. 4 | Formation of voids and large diamagnetic Li-rich regions over cycling. a -c , ADF-STEM images showing single grains of the pristine ( a ), 2nd discharge ( b ) and 100th discharge ( c ) material showing the formation of voids about 4-12 nm in diameter over extended cycling. d , 129 Xe NMR experiments. Samples were extracted from cells and infiltrated with Xe gas to probe the open porosity. e , 129 Xe NMR of the pristine, 2nd discharge and 100th discharge materials.Fig. 4 | Formation of voids and large diamagnetic Li-rich regions over cycling. a -c , ADF-STEM images showing single grains of the pristine ( a ), 2nd discharge ( b ) and 100th discharge ( c ) material showing the formation of voids about 4-12 nm in diameter over extended cycling. d , 129 Xe NMR experiments. Samples were extracted from cells and infiltrated with Xe gas to probe the open porosity. e , 129 Xe NMR of the pristine, 2nd discharge and 100th discharge materials.
low4258section_headerbody_headingbody_headingbody_heading
p4:body_region:0p4:page_body:column_1_of_2:white[255, 255, 255]
white		[39.69, 499.25, 132.67, 9.95]Void formation on cyclingVoid formation on cycling
low4261page_footerpage_footerdocling_page_footerdocling_page_footer
p4:body_region:0p4:bottom_margin:column_1_of_2:white[255, 255, 255]
white		[39.69, 763.46, 185.86, 7.0]Nature Materials | Volume 23 | June 2024 | 818-825Nature Materials | Volume 23 | June 2024 | 818-825
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p4:body_region:1p4:top_margin:column_2_of_2:off_white[244, 248, 251]
off_white		[392.65, 25.88, 176.63, 6.99]https://doi.org/10.1038/s41563-024-01833-z
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white		[237.0, 54.88, 6.01, 8.12]bb
low4264textvisual_textvisual_textvisual_text
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white		[384.55, 54.88, 5.45, 8.12]cc
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gray		[396.38, 184.93, 16.56, 4.82]20 nm20 nm
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p4:body_region:0p4:page_body:column_2_of_2:white[255, 255, 255]
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white		[422.45, 208.89, 5.99, 8.12]gg
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white		[231.75, 212.63, 31.18, 7.27]129 Xe NMR129 Xe NMR
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white		[342.67, 212.63, 23.99, 7.27]6 Li NMR6 Li NMR
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white		[454.08, 212.63, 25.67, 7.27]17 O NMR17 O NMR
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gray		[425.29, 247.69, 19.1, 4.82]PristinePristine
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low4279textvisual_textvisual_textvisual_text
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white		[174.18, 316.39, 7.96, 5.7]XeXe
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low4288textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[252, 252, 252]
white		[174.18, 324.19, 10.72, 5.7]gasgas
low4289textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:gray[223, 223, 223]
gray		[425.29, 326.01, 25.53, 4.82]dischargedischarge
low4290textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[248, 248, 248]
white		[318.03, 328.29, 14.93, 4.82]100th100th
low4291textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:gray[240, 240, 240]
gray		[205.15, 328.29, 14.93, 4.82]100th100th
low4292textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:gray[234, 234, 234]
gray		[318.03, 334.79, 25.53, 4.82]dischargedischarge
low4293textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:gray[225, 225, 225]
gray		[205.15, 334.79, 25.53, 4.82]dischargedischarge
low4294textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[255, 255, 255]
white		[197.93, 359.66, 8.99, 4.82]120120
low4295textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:gray[219, 219, 219]
gray		[221.34, 359.66, 7.08, 4.82]8080
low4296textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[255, 255, 255]
white		[243.78, 359.66, 7.14, 4.82]4040
low4297textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[255, 255, 255]
white		[267.93, 359.66, 3.75, 4.82]00
low4298textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[255, 255, 255]
white		[287.25, 359.66, 10.03, 4.82]-40-40
low4299textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[305.84, 359.66, 16.18, 4.82]4,0004,000
low4300textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[335.58, 359.66, 15.83, 4.82]2,0002,000
low4301textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[254, 254, 254]
white		[371.2, 359.66, 3.75, 4.82]00
low4302textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[393.29, 359.66, 18.73, 4.82]-2,000-2,000
low4303textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[249, 249, 249]
white		[425.97, 359.66, 16.13, 4.82]8,0008,000
low4304textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[449.7, 359.66, 16.18, 4.82]4,0004,000
low4305textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[479.67, 359.66, 3.75, 4.82]00
low4306textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[495.77, 359.66, 19.07, 4.82]-4,000-4,000
low4307textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[255, 255, 255]
white		[235.57, 369.51, 37.21, 7.27]129 Xe (ppm))129 Xe (ppm))
low4308textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:gray[225, 225, 225]
gray		[349.89, 369.51, 2.79, 3.95]66
low4309textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[457.58, 369.51, 31.71, 7.27]17 O (ppm))17 O (ppm))
low4310textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[249, 249, 249]
white		[221.9, 371.08, 3.83, 5.7]δ
low4311textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:white[255, 255, 255]
white		[231.76, 371.08, 3.82, 5.7](
low4312textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:gray[233, 233, 233]
gray		[336.86, 371.08, 3.83, 5.7]δ
low4313textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[346.07, 371.08, 3.82, 5.7](
low4314textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[352.67, 371.08, 27.24, 5.7]Li (ppm))Li (ppm))
low4315textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[249, 249, 249]
white		[444.55, 371.08, 3.83, 5.7]δ
low4316textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[453.76, 371.08, 3.82, 5.7](
low4317textvisual_textvisual_textvisual_text
p4:body_region:0p4:page_body:column_2_of_2:gray[234, 234, 234]
gray		[225.73, 374.51, 6.03, 3.95]isoiso
low4318textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:gray[207, 207, 207]
gray		[340.69, 374.51, 5.39, 3.95]cgcg
low4319textvisual_textvisual_textvisual_text
p4:body_region:1p4:page_body:column_2_of_2:gray[232, 232, 232]
gray		[448.38, 374.51, 5.39, 3.95]cgcg
low4320captioncaptiondocling_captiondocling_caption
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[306.47, 385.51, 255.16, 46.5]The orange region highlighted indicates the presence of open voids of 17 nm diameter and greater after 100 cycles. δ iso , isotropic chemical shift. f , g , 6 Li ( f ) and 17 O ( g ) NMR isolating slow and fast relaxing environments. The sharp peaks at 0 ppm in the 6 Li and slow relaxing 17 O NMR spectra indicate the formation of large diamagnetic Li-rich regions on extended cycling.The orange region highlighted indicates the presence of open voids of 17 nm diameter and greater after 100 cycles. δ iso , isotropic chemical shift. f , g , 6 Li ( f ) and 17 O ( g ) NMR isolating slow and fast relaxing environments. The sharp peaks at 0 ppm in the 6 Li and slow relaxing 17 O NMR spectra indicate the formation of large diamagnetic Li-rich regions on extended cycling.
low4322section_headerbody_headingbody_headingbody_heading
p4:body_region:1p4:page_body:column_2_of_2:white[255, 255, 255]
white		[306.14, 692.75, 163.24, 9.95]The contents of the closed voidsThe contents of the closed voids
low4324page_footerpage_footerdocling_page_footerdocling_page_footer
p4:body_region:1p4:bottom_margin:column_2_of_2:white[255, 255, 255]
white		[549.18, 764.06, 13.5, 6.99]821821
low5325page_headerpage_headerdocling_page_headerdocling_page_header
p5:body_region:0p5:top_margin:column_1_of_2:white[255, 255, 255]
white		[39.69, 24.45, 31.06, 8.75]ArticleArticle
low5326textvisual_textvisual_textvisual_text
p5:body_region:0p5:top_margin:column_1_of_2:white[255, 255, 255]
white		[92.94, 55.58, 5.44, 8.12]aa
low5327textvisual_textvisual_textvisual_text
p5:body_region:0p5:top_margin:column_1_of_2:white[255, 255, 255]
white		[146.54, 57.66, 44.51, 5.7]Fast relaxationFast relaxation
low5328textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[161.42, 65.46, 23.17, 5.7]= 2 ms)= 2 ms)
low5329textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[254, 254, 254]
white		[152.99, 65.46, 2.09, 5.7](
low5330textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[155.09, 65.46, 4.54, 5.7]DD
low5331textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:gray[203, 203, 203]
gray		[159.63, 68.89, 1.8, 3.95]11
low5332textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[99.28, 92.87, 40.68, 5.7]100th charge100th charge
low5333textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[249, 249, 249]
white		[92.29, 174.28, 18.03, 4.82]12,00012,000
low5334textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:gray[237, 237, 237]
gray		[123.3, 174.28, 16.13, 4.82]8,0008,000
low5335textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[249, 249, 249]
white		[153.32, 174.28, 16.18, 4.82]4,0004,000
low5336textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[159.46, 184.18, 31.7, 7.27]17 O (ppm))17 O (ppm))
low5337textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[248, 248, 248]
white		[146.43, 185.75, 3.83, 5.7]δ
low5338textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:gray[204, 204, 204]
gray		[157.37, 185.75, 2.09, 5.7](
low5339textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:gray[238, 238, 238]
gray		[150.26, 189.18, 5.39, 3.95]cgcg
low5340textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[98.82, 222.18, 49.53, 5.7]100th discharge100th discharge
low5341textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[249, 249, 249]
white		[92.29, 300.95, 18.03, 4.82]12,00012,000
low5342textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:gray[237, 237, 237]
gray		[123.3, 300.95, 16.13, 4.82]8,0008,000
low5343textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[249, 249, 249]
white		[153.32, 300.95, 16.18, 4.82]4,0004,000
low5344textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[159.46, 311.15, 31.7, 7.27]17 O (ppm))17 O (ppm))
low5345textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[146.43, 312.72, 3.83, 5.7]δ
low5346textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:gray[201, 201, 201]
gray		[157.37, 312.72, 2.09, 5.7](
low5347textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_1_of_2:gray[223, 223, 223]
gray		[150.26, 316.15, 5.39, 3.95]cgcg
low5348captioncaptionoutside_body_flow_captionoutside_body_flow_caption
p5:body_region:0p5:page_body:column_1_of_2:white[255, 255, 255]
white		[39.68, 327.16, 248.35, 56.5]Fig. 5 | Partial reduction of O 2 trapped in voids to form Li-coordinated O 2on the 100th discharge. a , b , 17 O NMR spectra isolating fast ( a ) and slow ( b ) relaxing 17 O environments. The sharp peaks in a are assigned to trapped molecular O2, which decrease in intensity on discharge. There is still evidence of some residual molecular O 2 in the discharged sample, δ cg ( 17 O2) = 2,770 ppm. In b the slow relaxation 17 O is dominated by oxide environments coordinated toFig. 5 | Partial reduction of O 2 trapped in voids to form Li-coordinated O 2on the 100th discharge. a , b , 17 O NMR spectra isolating fast ( a ) and slow ( b ) relaxing 17 O environments. The sharp peaks in a are assigned to trapped molecular O2, which decrease in intensity on discharge. There is still evidence of some residual molecular O 2 in the discharged sample, δ cg ( 17 O2) = 2,770 ppm. In b the slow relaxation 17 O is dominated by oxide environments coordinated to
low5352page_footerpage_footerdocling_page_footerdocling_page_footer
p5:body_region:0p5:bottom_margin:column_1_of_2:white[255, 255, 255]
white		[39.69, 763.46, 185.86, 7.0]Nature Materials | Volume 23 | June 2024 | 818-825Nature Materials | Volume 23 | June 2024 | 818-825
low5353page_headerpage_headerdocling_page_headerdocling_page_header
p5:body_region:1p5:top_margin:column_2_of_2:off_white[243, 247, 250]
off_white		[392.65, 25.88, 176.63, 6.99]https://doi.org/10.1038/s41563-024-01833-z
low5354textvisual_textvisual_textvisual_text
p5:body_region:0p5:top_margin:column_2_of_2:white[255, 255, 255]
white		[249.0, 55.58, 6.01, 8.12]bb
low5355textvisual_textvisual_textvisual_text
p5:body_region:1p5:top_margin:column_2_of_2:white[255, 255, 255]
white		[403.65, 55.58, 5.45, 8.12]cc
low5356textvisual_textvisual_textvisual_text
p5:body_region:1p5:top_margin:column_2_of_2:white[252, 252, 252]
white		[301.12, 57.98, 47.17, 5.7]Slow relaxationSlow relaxation
low5357textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[488.35, 65.27, 7.76, 7.38]O2O2
low5358textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[313.43, 65.78, 30.98, 5.7]= 100 ms)= 100 ms)
low5359textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[305.0, 65.78, 2.09, 5.7](
low5360textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[307.1, 65.78, 4.54, 5.7]DD
low5361textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:gray[210, 210, 210]
gray		[311.63, 69.21, 1.8, 3.95]11
low5362textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[403.65, 69.52, 22.76, 7.27]TM-O 2-TM-O 2-
low5363textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[255, 255, 255]
white		[211.06, 89.47, 22.76, 7.27]TM-O 2-TM-O 2-
low5364textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[255, 255, 255]
white		[258.78, 92.87, 40.68, 5.7]100th charge100th charge
low5365textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[255, 255, 255]
white		[224.01, 104.24, 7.76, 7.38]O2O2
low5366textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[368.07, 106.84, 22.76, 7.27]TM-O 2-TM-O 2-
low5367textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[248, 248, 248]
white		[189.59, 174.28, 3.75, 4.82]00
low5368textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[254, 254, 254]
white		[211.97, 174.28, 19.07, 4.82]-4,000-4,000
low5369textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[250, 250, 250]
white		[248.38, 174.28, 18.03, 4.82]12,00012,000
low5370textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:gray[245, 245, 245]
gray		[279.21, 174.28, 16.13, 4.82]8,0008,000
low5371textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[248, 248, 248]
white		[309.06, 174.28, 16.18, 4.82]4,0004,000
low5372textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[248, 248, 248]
white		[345.15, 174.28, 3.75, 4.82]00
low5373textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[253, 253, 253]
white		[367.36, 174.28, 19.07, 4.82]-4,000-4,000
low5374textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[315.37, 184.18, 31.7, 7.27]17 O (ppm))17 O (ppm))
low5375textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[248, 248, 248]
white		[302.33, 185.75, 3.83, 5.7]δ
low5376textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[254, 254, 254]
white		[313.27, 185.75, 2.09, 5.7](
low5377textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[465.19, 187.65, 36.5, 5.7]DischargingDischarging
low5378textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:gray[223, 223, 223]
gray		[306.17, 189.18, 5.39, 3.95]cgcg
low5379textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[417.2, 203.81, 18.69, 7.27]Li-O 2-Li-O 2-
low5380textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[488.2, 207.16, 7.76, 7.38]O2O2
low5381textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[255, 255, 255]
white		[258.33, 222.18, 49.53, 5.7]100th discharge100th discharge
low5382textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[251, 251, 251]
white		[385.1, 235.41, 4.86, 3.95]2-2-
low5383textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[372.52, 236.98, 12.58, 5.7]Li-OLi-O
low5384textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[248, 248, 248]
white		[189.59, 300.95, 3.75, 4.82]00
low5385textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[254, 254, 254]
white		[211.97, 300.95, 19.07, 4.82]-4,000-4,000
low5386textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:white[250, 250, 250]
white		[248.38, 300.95, 18.03, 4.82]12,00012,000
low5387textvisual_textvisual_textvisual_text
p5:body_region:0p5:page_body:column_2_of_2:gray[245, 245, 245]
gray		[279.21, 300.95, 16.13, 4.82]8,0008,000
low5388textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[248, 248, 248]
white		[309.06, 300.95, 16.18, 4.82]4,0004,000
low5389textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[248, 248, 248]
white		[345.15, 300.95, 3.75, 4.82]00
low5390textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[253, 253, 253]
white		[367.36, 300.95, 19.07, 4.82]-4,000-4,000
low5391textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[315.37, 311.15, 31.7, 7.27]17 O (ppm))17 O (ppm))
low5392textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[250, 250, 250]
white		[302.33, 312.72, 3.83, 5.7]δ
low5393textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:white[254, 254, 254]
white		[313.27, 312.72, 2.09, 5.7](
low5394textvisual_textvisual_textvisual_text
p5:body_region:1p5:page_body:column_2_of_2:gray[206, 206, 206]
gray		[306.17, 316.15, 5.39, 3.95]cgcg
low5395captioncaptiondocling_captiondocling_caption
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[306.47, 326.2, 254.19, 58.27]paramagnetic TM ions (TM-O 2-), δ cg = 2,100-2,300 ppm. After discharge, a new 17 O environment is formed corresponding to oxide surrounded by Li (that is, Li-O 2) created by the reduction of O 2 in the voids and reinsertion of Li + into the voids coordinated by the O 2, centred at δ cg = 0 ppm. D 1 , relaxation delay. c , Large voids accommodating O2 are partially repopulated by Li + on discharge. Most O 2 is reduced to O 2but some residual O 2 remains.paramagnetic TM ions (TM-O 2-), δ cg = 2,100-2,300 ppm. After discharge, a new 17 O environment is formed corresponding to oxide surrounded by Li (that is, Li-O 2) created by the reduction of O 2 in the voids and reinsertion of Li + into the voids coordinated by the O 2, centred at δ cg = 0 ppm. D 1 , relaxation delay. c , Large voids accommodating O2 are partially repopulated by Li + on discharge. Most O 2 is reduced to O 2but some residual O 2 remains.
low5397section_headerbody_headingbody_headingbody_heading
p5:body_region:1p5:page_body:column_2_of_2:white[255, 255, 255]
white		[306.14, 585.25, 199.96, 20.7]O2 loss and residual trapped O 2 explain voltage fadeO2 loss and residual trapped O 2 explain voltage fade
low5400page_footerpage_footerdocling_page_footerdocling_page_footer
p5:body_region:1p5:bottom_margin:column_2_of_2:white[255, 255, 255]
white		[547.16, 763.81, 14.9, 6.99]822822
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white		[39.69, 24.45, 31.06, 8.75]ArticleArticle
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[91.33, 59.54, 5.44, 8.12]aa
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[153.83, 65.59, 26.03, 5.7]VacancyVacancy
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p6:body_region:0p6:page_body:column_1_of_2:white[249, 249, 249]
white		[154.74, 73.39, 24.2, 5.7]clustersclusters
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p6:body_region:0p6:page_body:column_1_of_2:white[250, 251, 253]
white		[154.6, 231.31, 7.76, 7.38]O2O2
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p6:body_region:0p6:page_body:column_1_of_2:white[249, 250, 252]
white		[145.69, 239.11, 25.58, 5.7]reducedreduced
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[96.15, 243.54, 43.45, 5.7]2nd discharge2nd discharge
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[149.4, 245.34, 18.16, 7.27]to O 2-to O 2-
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[91.33, 274.27, 5.45, 8.12]cc
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[165.7, 342.72, 16.28, 5.48]OpenOpen
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[167.52, 350.21, 12.64, 5.48]voidvoid
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p6:body_region:0p6:page_body:column_1_of_2:white[254, 254, 254]
white		[91.33, 478.61, 49.53, 5.7]100th discharge100th discharge
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[146.06, 480.51, 27.1, 7.38]Some O 2Some O 2
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[146.83, 488.31, 25.55, 5.7]reducedreduced
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[163.79, 494.54, 4.86, 3.95]2-2-
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[150.57, 496.11, 13.23, 5.7]to Oto O
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p6:body_region:0p6:page_body:column_1_of_2:white[255, 255, 255]
white		[39.68, 514.96, 251.36, 36.5]Fig. 6 | Voltage fade mechanism. a , b , Second cycle: reversible O-redox involves the formation of molecular O 2 trapped in small vacancy clusters throughout the particle. O 2 molecules are fully reduced to O 2on discharge forming small diamagnetic Li-rich regions. c , d , One-hundreth cycle: further TM migrationFig. 6 | Voltage fade mechanism. a , b , Second cycle: reversible O-redox involves the formation of molecular O 2 trapped in small vacancy clusters throughout the particle. O 2 molecules are fully reduced to O 2on discharge forming small diamagnetic Li-rich regions. c , d , One-hundreth cycle: further TM migration
low6420page_footerpage_footerdocling_page_footerdocling_page_footer
p6:body_region:0p6:bottom_margin:column_1_of_2:white[255, 255, 255]
white		[39.69, 763.46, 185.86, 7.0]Nature Materials | Volume 23 | June 2024 | 818-825Nature Materials | Volume 23 | June 2024 | 818-825
low6421page_headerpage_headerdocling_page_headerdocling_page_header
p6:body_region:1p6:top_margin:column_2_of_2:off_white[243, 247, 250]
off_white		[392.65, 25.88, 176.63, 6.99]https://doi.org/10.1038/s41563-024-01833-z
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p6:body_region:0p6:top_margin:column_2_of_2:off_white[247, 247, 247]
off_white		[251.98, 54.06, 28.51, 5.7]DensifiedDensified
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[310.35, 59.54, 6.01, 8.12]bb
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[243.64, 61.86, 45.18, 5.7]rocksalt/spinelrocksalt/spinel
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[254.94, 69.66, 22.61, 5.7]surfacesurface
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[433.72, 93.58, 34.6, 5.7]2nd charge2nd charge
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p6:body_region:0p6:page_body:column_2_of_2:off_white[251, 246, 247]
off_white		[196.28, 102.72, 7.76, 7.38]O2O2
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[432.28, 108.59, 46.71, 5.7]O2 formation inO2 formation in
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[419.85, 108.59, 2.16, 5.7]•
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p6:body_region:0p6:page_body:column_2_of_2:off_white[251, 246, 247]
off_white		[188.06, 110.52, 24.22, 5.7]trappedtrapped
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[257.16, 110.55, 34.6, 5.7]2nd charge2nd charge
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[414.81, 116.39, 69.21, 5.7]small vacancy clusterssmall vacancy clusters
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[189.95, 118.32, 20.42, 5.7]in bulkin bulk
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[176.21, 160.25, 29.78, 5.7]2nd cycle2nd cycle
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[215.56, 189.44, 19.01, 5.7]Li-richLi-rich
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p6:body_region:1p6:page_body:column_2_of_2:white[252, 252, 252]
white		[338.55, 190.17, 43.45, 5.7]2nd discharge2nd discharge
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p6:body_region:0p6:page_body:column_2_of_2:white[254, 254, 254]
white		[215.56, 197.24, 19.71, 5.7]regionregion
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[327.94, 212.68, 2.16, 5.7]•
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p6:body_region:1p6:page_body:column_2_of_2:white[254, 254, 254]
white		[340.38, 212.68, 57.25, 5.7]Formation of smallFormation of small
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[321.19, 220.48, 83.2, 5.7]diamagnetic Li-rich regionsdiamagnetic Li-rich regions
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[334.61, 227.7, 2.16, 5.7]•
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[347.05, 227.7, 43.92, 5.7]Dense particleDense particle
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[335.84, 235.5, 53.9, 5.7]structure remainsstructure remains
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[310.35, 274.27, 6.0, 8.12]dd
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[203.96, 275.43, 7.76, 7.38]O2O2
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[232.61, 284.71, 52.86, 5.7]O2 loss from voidO2 loss from void
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p6:body_region:0p6:page_body:column_2_of_2:white[250, 250, 250]
white		[235.5, 292.51, 47.09, 5.7]coarsening andcoarsening and
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[245.59, 300.31, 26.89, 5.7]openingopening
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[267.53, 318.33, 7.76, 7.38]O2O2
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[435.53, 322.37, 40.68, 5.7]100th charge100th charge
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[426.28, 337.38, 2.16, 5.7]•
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[438.71, 337.38, 46.73, 5.71]O2 formation inO2 formation in
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[257.19, 342.26, 40.68, 5.7]100th charge100th charge
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[420.36, 345.19, 70.99, 5.7]larger vacancy clusterslarger vacancy clusters
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white		[425.13, 352.4, 2.16, 5.7]•
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[437.56, 352.4, 49.02, 5.7]Particle fractureParticle fracture
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p6:body_region:0p6:page_body:column_2_of_2:white[254, 254, 254]
white		[185.72, 353.41, 20.6, 5.48]ClosedClosed
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[425.44, 359.91, 73.26, 5.7]O2 loss from open voidsO2 loss from open voids
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white		[413.01, 359.91, 2.16, 5.7]•
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[189.7, 360.91, 12.64, 5.48]voidvoid
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p6:body_region:0p6:page_body:column_2_of_2:white[251, 251, 251]
white		[175.55, 403.36, 35.81, 5.7]100th cycle100th cycle
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[342.57, 430.31, 49.53, 5.7]100th discharge100th discharge
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[334.27, 445.24, 2.16, 5.7]•
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[346.71, 445.24, 58.96, 5.7]Formation of largerFormation of larger
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[328.37, 453.04, 83.2, 5.7]diamagnetic Li-rich regionsdiamagnetic Li-rich regions
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white		[328.75, 460.25, 2.16, 5.7]•
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[341.18, 460.25, 74.17, 5.7]Incomplete reduction ofIncomplete reduction of
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[371.22, 468.05, 49.21, 5.7]in larger closedin larger closed
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p6:body_region:1p6:page_body:column_2_of_2:white[255, 255, 255]
white		[323.67, 468.05, 45.0, 5.7]trapped Otrapped O
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p6:body_region:1p6:page_body:column_2_of_2:gray[191, 191, 191]
gray		[368.73, 471.48, 2.49, 3.95]22
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[232.9, 474.16, 25.86, 5.7]ResidualResidual
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p6:body_region:1p6:page_body:column_2_of_2:white[253, 253, 253]
white		[363.92, 475.85, 16.25, 5.7]voidsvoids
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p6:body_region:0p6:page_body:column_2_of_2:white[255, 255, 255]
white		[228.97, 481.96, 33.72, 7.38]trapped O 2trapped O 2
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p6:body_region:1p6:bottom_margin:column_2_of_2:white[252, 252, 252]
white		[547.53, 764.06, 15.15, 6.99]823823
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white		[39.69, 24.45, 31.06, 8.75]ArticleArticle
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white		[39.69, 252.0, 66.19, 9.95]ImplicationsImplications
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white		[39.69, 520.75, 77.44, 9.95]Online contentOnline content
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white		[306.14, 415.35, 77.35, 7.02]© The Author(s) 2024© The Author(s) 2024
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p8:body_region:0p8:bottom_margin:column_2_of_2:white[249, 249, 249]
white		[547.69, 764.06, 14.98, 6.99]825825
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white		[39.69, 24.45, 31.06, 8.75]ArticleArticle
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p9:body_region:0p9:top_margin:column_1_of_2:white[255, 255, 255]
white		[39.69, 47.75, 45.99, 9.95]MethodsMethods
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p9:body_region:0p9:body_zone:column_1_of_2:white[255, 255, 255]
white		[39.69, 59.95, 109.91, 8.11]Co-precipitation synthesisCo-precipitation synthesis
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p9:body_region:0p9:body_zone:column_1_of_2:white[255, 255, 255]
white		[39.69, 264.2, 138.36, 8.11]Electrochemical characterizationElectrochemical characterization
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p9:body_region:0p9:body_zone:column_1_of_2:white[255, 255, 255]
white		[39.69, 446.95, 240.37, 8.11]Inductively coupled plasma optical emission spectroscopyInductively coupled plasma optical emission spectroscopy
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p9:body_region:0p9:body_zone:column_1_of_2:white[255, 255, 255]
white		[39.69, 532.95, 23.86, 8.11]PXRDPXRD
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p9:body_region:0p9:body_zone:column_1_of_2:white[255, 255, 255]
white		[39.69, 575.95, 43.72, 8.11]ADF-STEMADF-STEM
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p9:body_region:0p9:body_zone:column_1_of_2:white[255, 255, 255]
white		[39.69, 672.7, 19.95, 8.11]RIXSRIXS
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gray		[39.69, 763.46, 61.32, 7.0]Nature MaterialsNature Materials
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gray		[392.65, 25.82, 167.85, 7.4]https://doi.org/10.1038/s41563-024-01833-z
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white		[306.14, 112.51, 186.78, 9.3]Solid-state 17 O and 6 Li MAS NMR spectroscopySolid-state 17 O and 6 Li MAS NMR spectroscopy
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p9:body_region:1p9:body_zone:column_2_of_2:white[255, 255, 255]
white		[306.14, 241.51, 65.28, 9.3]129 Xe static NMR129 Xe static NMR
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white		[306.14, 350.2, 16.42, 8.11]BETBET
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stop_triggerp9:body_region:1p9:body_zone:column_2_of_2:white[255, 255, 255]
white		[306.14, 402.5, 85.11, 9.95]Data availabilityData availability
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white		[306.14, 555.05, 257.0, 60.78]P.G.B. is indebted to the EPSRC, the Henry Royce Institute for Advanced Materials (EP/R00661X/1, EP/S019367/1, EP/R010145/1 and EP/L019469/1) and the Faraday Institution (FIRG016) for financial support. R.A.H. acknowledges funding from the Royal Academy of Engineering under the Research Fellowship scheme. We acknowledge Diamond Light Source for time on I21 under proposal MM25785.P.G.B. is indebted to the EPSRC, the Henry Royce Institute for Advanced Materials (EP/R00661X/1, EP/S019367/1, EP/R010145/1 and EP/L019469/1) and the Faraday Institution (FIRG016) for financial support. R.A.H. acknowledges funding from the Royal Academy of Engineering under the Research Fellowship scheme. We acknowledge Diamond Light Source for time on I21 under proposal MM25785.
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white		[306.14, 628.25, 111.43, 9.95]Author contributionsAuthor contributions
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white		[306.14, 725.0, 106.08, 9.95]Competing interestsCompeting interests
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white		[306.14, 737.8, 160.03, 7.02]The authors declare no competing interests.The authors declare no competing interests.
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white		[39.69, 24.45, 31.06, 8.75]ArticleArticle
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white		[39.69, 47.75, 120.86, 9.95]Additional informationAdditional information
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white		[39.69, 60.55, 157.48, 7.02]Extended data is available for this paper atExtended data is available for this paper at
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white		[39.69, 71.3, 161.21, 7.02]https://doi.org/10.1038/s41563-024-01833-z.
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white		[39.69, 92.8, 249.6, 17.77]Correspondence and requests for materials should be addressed to Robert A. House or Peter G. Bruce.Correspondence and requests for materials should be addressed to Robert A. House or Peter G. Bruce.
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gray		[39.69, 763.46, 61.32, 7.0]Nature MaterialsNature Materials
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gray		[392.65, 25.82, 167.85, 7.4]https://doi.org/10.1038/s41563-024-01833-z
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gray		[392.65, 25.82, 167.85, 7.4]https://doi.org/10.1038/s41563-024-01833-z
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white		[39.68, 225.57, 503.0, 16.5]Extended Data Fig. 1 | SEM and EDX images for Li 1.2 Ni0.13 Co0.13Mn0.54O2showing elemental distribution. Spherical particles of 3-4 μm in diameter can be seen, while the EDX elemental analysis confirms a homogenous distribution of metals within the grains.Extended Data Fig. 1 | SEM and EDX images for Li 1.2 Ni0.13 Co0.13Mn0.54O2showing elemental distribution. Spherical particles of 3-4 μm in diameter can be seen, while the EDX elemental analysis confirms a homogenous distribution of metals within the grains.
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gray		[39.69, 763.46, 61.32, 7.0]Nature MaterialsNature Materials
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white		[39.68, 467.25, 498.47, 16.5]Extended Data Fig. 2 | Electrochemical cycling data at different rates. ( a ) Cycling data collected at different current rates of 100 and 20 mA/g (C/3 and C/15). A similar degree of voltage ( b ) and capacity ( c ) fade is observed.Extended Data Fig. 2 | Electrochemical cycling data at different rates. ( a ) Cycling data collected at different current rates of 100 and 20 mA/g (C/3 and C/15). A similar degree of voltage ( b ) and capacity ( c ) fade is observed.
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gray		[392.65, 25.82, 167.85, 7.4]https://doi.org/10.1038/s41563-024-01833-z
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white		[39.69, 651.69, 508.14, 16.5]Extended Data Fig. 3 | SEM and EDX for the mixed metal carbonate precursor. Spherical particles of 3-4 μm in diameter can be seen in the SEM and EDX shows a homogenous distribution of metals within grains and between particles.Extended Data Fig. 3 | SEM and EDX for the mixed metal carbonate precursor. Spherical particles of 3-4 μm in diameter can be seen in the SEM and EDX shows a homogenous distribution of metals within grains and between particles.
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white		[39.69, 223.06, 521.81, 17.45]Extended Data Fig. 4 | Additional ADF-STEM images. ( a ) Pristine, ( b ) 2 nd cycle and ( c ) 100 th cycle. Again, well defined atomic layers can be seen within the grains in the pristine and 2 nd cycles, while the images from the 100 th cycle highlight the presence of voids.Extended Data Fig. 4 | Additional ADF-STEM images. ( a ) Pristine, ( b ) 2 nd cycle and ( c ) 100 th cycle. Again, well defined atomic layers can be seen within the grains in the pristine and 2 nd cycles, while the images from the 100 th cycle highlight the presence of voids.
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white		[39.68, 433.78, 522.6, 17.45]Extended Data Fig. 5 | ADF-STEM images for samples collected after the 100 th cycle. Voids are outlined in orange and range in dimensions from 4 to 12 nm. The likely interconnection of several of these voids is apparent.Extended Data Fig. 5 | ADF-STEM images for samples collected after the 100 th cycle. Voids are outlined in orange and range in dimensions from 4 to 12 nm. The likely interconnection of several of these voids is apparent.
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white		[39.68, 306.34, 501.57, 17.45]Extended Data Fig. 6 | 129 Xe NMR data. 129 Xe NMR data at different stages of cycling alongside a plot of void size vs chemical shift 45 . The minimum void size in the samples is around ~17 nm, as taken from a maximum chemical shift of 50 ppm.Extended Data Fig. 6 | 129 Xe NMR data. 129 Xe NMR data at different stages of cycling alongside a plot of void size vs chemical shift 45 . The minimum void size in the samples is around ~17 nm, as taken from a maximum chemical shift of 50 ppm.
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white		[39.68, 219.82, 514.04, 27.45]Extended Data Fig. 7 | BET data. ( a ) BET data showing the pore size distributions for the pristine, 2 nd cycle and 100 th cycle samples. To remove the contribution from carbon and binder which were present in all samples, the pristine data were subtracted from the 2 nd and 100 th cycle data to better observe the changes in cathode particle porosity, ( b ).Extended Data Fig. 7 | BET data. ( a ) BET data showing the pore size distributions for the pristine, 2 nd cycle and 100 th cycle samples. To remove the contribution from carbon and binder which were present in all samples, the pristine data were subtracted from the 2 nd and 100 th cycle data to better observe the changes in cathode particle porosity, ( b ).
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white		[39.69, 303.22, 494.49, 7.45]Extended Data Fig. 8 | RIXS line scans. RIXS line scans collected at 531.5 eV at different sample locations for the charged samples of ( a ) 2 nd and ( b ) 100 th cycles.Extended Data Fig. 8 | RIXS line scans. RIXS line scans collected at 531.5 eV at different sample locations for the charged samples of ( a ) 2 nd and ( b ) 100 th cycles.
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white		[39.69, 49.89, 261.87, 9.1]Extended Data Table 1 | ICP-OES data for Li 1.2 Ni0.13 Co0.13Mn0.54O2Extended Data Table 1 | ICP-OES data for Li 1.2 Ni0.13 Co0.13Mn0.54O2
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white		[39.69, 49.89, 478.99, 9.1]Extended Data Table 2 | Rietveld Refinement parameters of powder X-ray diffraction data for Li 1.2 Ni0.13 Co0.13Mn0.54O2Extended Data Table 2 | Rietveld Refinement parameters of powder X-ray diffraction data for Li 1.2 Ni0.13 Co0.13Mn0.54O2
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