Resolving Chemical and Spatial Heterogeneities at Complex Electrochemical Interfaces in Li-Ion Batteries

Hestenes, Julia C.; May, Richard; Sadowski, Jerzy T.; Munich, Naiara; Marbella, Lauren E.

doi:10.1021/acs.chemmater.1c03185

Title: Resolving Chemical and Spatial Heterogeneities at Complex Electrochemical Interfaces in Li-Ion Batteries

Journal Article · 27 December 2021 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.1c03185 · OSTI ID:1841112

Hestenes, Julia C. ^[1]; May, Richard ^[1];

^[2]; Munich, Naiara ^[1];

^[1]

Columbia Univ., New York, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

The high specific capacities of Ni-rich transition metal oxides have garnered immense interest for improving the energy density of Li-ion batteries (LIBs). Despite the potential of these materials, Ni-rich cathodes suffer from interfacial instabilities that lead to crystallographic rearrangement of the active material surface as well as the formation of a cathode electrolyte interphase (CEI) layer on the composite during electrochemical cycling. While changes in crystallographic structure can be detected with diffraction-based methods, probing the chemistry of the disordered, heterogeneous CEI layer is challenging. In this work, we use a combination of ex situ solid-state nuclear magnetic resonance (SSNMR) spectroscopy and X-ray photoemission electron microscopy (XPEEM) to provide chemical and spatial information, on the nanometer length scale, on the CEI deposited on LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) composite cathode films. XPEEM elemental maps offer insight into the lateral arrangement of the electrolyte decomposition products that comprise the CEI and paramagnetic interactions (assessed with electron paramagnetic resonance (EPR) and relaxation measurements) in ¹³C SSNMR provide information on the radial arrangement of the CEI from the NMC811 particles outward. Using this approach, here we find that LiF, Li₂CO₃, and carboxy-containing structures are directly appended to NMC811 active particles, whereas soluble species detected during in situ ¹H and ¹⁹F solution NMR experiments (e.g., alkyl carbonates, HF, and vinyl compounds) are randomly deposited on the composite surface. We show that the combined approach of ex situ SSNMR and XPEEM, in conjunction with in situ solution NMR, allows spatially-resolved, molecular-level characterization of paramagnetic surfaces and new insights into electrolyte oxidation mechanisms in porous electrode films.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1841112

Report Number(s):: BNL--222610-2022-JAAM

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 1 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (89)

Crossover Effects in Batteries with High‐Nickel Cathodes and Lithium‐Metal Anodes Langdon, Jayse; Manthiram, Arumugam Advanced Functional Materials, Vol. 31, Issue 17 https://doi.org/10.1002/adfm.202010267	journal	February 2021
What Can We Learn from Solid State NMR on the Electrode-Electrolyte Interface? Haber, Shira; Leskes, Michal Advanced Materials, Vol. 30, Issue 41 https://doi.org/10.1002/adma.201706496	journal	June 2018
Kinetic Stability of Bulk LiNiO ₂ and Surface Degradation by Oxygen Evolution in LiNiO ₂ -Based Cathode Materials Kong, Fantai; Liang, Chaoping; Wang, Luhua Advanced Energy Materials, Vol. 9, Issue 2 https://doi.org/10.1002/aenm.201802586	journal	November 2018
Cross Talk between Transition Metal Cathode and Li Metal Anode: Unraveling Its Influence on the Deposition/Dissolution Behavior and Morphology of Lithium Betz, Johannes; Brinkmann, Jan‐Paul; Nölle, Roman Advanced Energy Materials, Vol. 9, Issue 21 https://doi.org/10.1002/aenm.201900574	journal	April 2019
A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries Li, Jianyu; Manthiram, Arumugam Advanced Energy Materials, Vol. 9, Issue 45 https://doi.org/10.1002/aenm.201902731	journal	October 2019
Probing Dynamic Processes in Lithium-Ion Batteries by In Situ NMR Spectroscopy: Application to Li _1.08 Mn _1.92 O ₄ Electrodes Zhou, Lina; Leskes, Michal; Liu, Tao Angewandte Chemie International Edition, Vol. 54, Issue 49 https://doi.org/10.1002/anie.201507632	journal	October 2015
Modified High-Nickel Cathodes with Stable Surface Chemistry Against Ambient Air for Lithium-Ion Batteries You, Ya; Celio, Hugo; Li, Jianyu Angewandte Chemie International Edition, Vol. 57, Issue 22 https://doi.org/10.1002/anie.201801533	journal	April 2018
Fundamental Concepts of NMR in Paramagnetic Systems. Part II: Relaxation Effects Satterlee, James D. Concepts in Magnetic Resonance, Vol. 2, Issue 3 https://doi.org/10.1002/cmr.1820020302	journal	July 1990
Instability of PVDF Binder in the LiFePO ₄ versus Li ₄ Ti ₅ O ₁₂ Li‐Ion Battery Cell Leanza, Daniela; Vaz, C. A. F.; Novák, Petr Helvetica Chimica Acta, Vol. 104, Issue 1 https://doi.org/10.1002/hlca.202000183	journal	December 2020
On the gassing behavior of lithium-ion batteries with NCM523 cathodes Berkes, Balázs B.; Schiele, Alexander; Sommer, Heino Journal of Solid State Electrochemistry, Vol. 20, Issue 11 https://doi.org/10.1007/s10008-016-3362-9	journal	August 2016
Degradation Mechanisms and Mitigation Strategies of Nickel-Rich NMC-Based Lithium-Ion Batteries Li, Tianyu; Yuan, Xiao-Zi; Zhang, Lei Electrochemical Energy Reviews, Vol. 3, Issue 1 https://doi.org/10.1007/s41918-019-00053-3	journal	October 2019
The cathode–electrolyte interface in the Li-ion battery Edström, K.; Gustafsson, T.; Thomas, J. O. Electrochimica Acta, Vol. 50, Issue 2-3 https://doi.org/10.1016/j.electacta.2004.03.049	journal	November 2004
Breaking Free from Cobalt Reliance in Lithium-Ion Batteries Gourley, Storm William D.; Or, Tyler; Chen, Zhongwei iScience, Vol. 23, Issue 9 https://doi.org/10.1016/j.isci.2020.101505	journal	September 2020
Magnetic properties of LixNiyMnyCo1−2yO2 (0.2≤1−2y≤0.5, 0≤x≤1) Mauger, A.; Gendron, F.; Julien, C. M. Journal of Alloys and Compounds, Vol. 520 https://doi.org/10.1016/j.jallcom.2011.12.055	journal	April 2012
Hydrolysis in the system LiPF6—propylene carbonate—dimethyl carbonate—H2O Plakhotnyk, Andriy V.; Ernst, Ludger; Schmutzler, Reinhard Journal of Fluorine Chemistry, Vol. 126, Issue 1 https://doi.org/10.1016/j.jfluchem.2004.09.027	journal	January 2005
Deciphering the multi-step degradation mechanisms of carbonate-based electrolyte in Li batteries Gachot, Gregory; Grugeon, Sylvie; Armand, Michel Journal of Power Sources, Vol. 178, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.11.110	journal	March 2008
Evolution of the LiFePO4 positive electrode interface along cycling monitored by MAS NMR Cuisinier, Marine; Dupré, Nicolas; Martin, Jean-Frédéric Journal of Power Sources, Vol. 224 https://doi.org/10.1016/j.jpowsour.2012.08.099	journal	February 2013
Comparison of the structural and electrochemical properties of layered Li[NixCoyMnz]O2 (x = 1/3, 0.5, 0.6, 0.7, 0.8 and 0.85) cathode material for lithium-ion batteries Noh, Hyung-Joo; Youn, Sungjune; Yoon, Chong Seung Journal of Power Sources, Vol. 233 https://doi.org/10.1016/j.jpowsour.2013.01.063	journal	July 2013
A high performance layered transition metal oxide cathode material obtained by simultaneous aluminum and iron cationic substitution El Mofid, Wassima; Ivanov, Svetlozar; Konkin, Alexander Journal of Power Sources, Vol. 268 https://doi.org/10.1016/j.jpowsour.2014.06.048	journal	December 2014
Anode-originated SEI migration contributes to formation of cathode-electrolyte interphase layer Fang, Shuyu; Jackson, David; Dreibelbis, Mark L. Journal of Power Sources, Vol. 373 https://doi.org/10.1016/j.jpowsour.2017.09.050	journal	January 2018
Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries Xia, Sihao; Mu, Linqin; Xu, Zhengrui Nano Energy, Vol. 53 https://doi.org/10.1016/j.nanoen.2018.09.051	journal	November 2018
Unveiling decaying mechanism through quantitative structure-activity relationship in electrolytes for lithium-ion batteries Su, Chi-Cheung; He, Meinan; Amine, Rachid Nano Energy, Vol. 83 https://doi.org/10.1016/j.nanoen.2021.105843	journal	May 2021
Paramagnetic NMR in solution and the solid state Pell, Andrew J.; Pintacuda, Guido; Grey, Clare P. Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 111 https://doi.org/10.1016/j.pnmrs.2018.05.001	journal	April 2019
Cationic distribution and electrochemical performance of LiCo_1/3Ni_1/3Mn_1/3O₂ electrodes for lithium-ion batteries Shinova, E.; Stoyanova, R.; Zhecheva, E. Solid State Ionics, Vol. 179, Issue 38, p. 2198-2208 https://doi.org/10.1016/j.ssi.2008.07.026	journal	November 2008
Quantitative MAS NMR characterization of the LiMn1/2Ni1/2O2 electrode/electrolyte interphase Cuisinier, M.; Martin, J. -F.; Moreau, P. Solid State Nuclear Magnetic Resonance, Vol. 42 https://doi.org/10.1016/j.ssnmr.2011.09.001	journal	April 2012
Leveraging Cation Identity to Engineer Solid Electrolyte Interphases for Rechargeable Lithium Metal Anodes May, Richard; Zhang, Yumin; Denny, Steven R. Cell Reports Physical Science, Vol. 1, Issue 11 https://doi.org/10.1016/j.xcrp.2020.100239	journal	November 2020
Electrochemical Characteristics of Layered Transition Metal Oxide Cathode Materials for Lithium Ion Batteries: Surface, Bulk Behavior, and Thermal Properties Tian, Chixia; Lin, Feng; Doeff, Marca M. Accounts of Chemical Research, Vol. 51, Issue 1 https://doi.org/10.1021/acs.accounts.7b00520	journal	December 2017
Post Mortem and Operando XPEEM: a Surface-Sensitive Tool for Studying Single Particles in Li-Ion Battery Composite Electrodes Mirolo, Marta; Leanza, Daniela; Höltschi, Laura Analytical Chemistry, Vol. 92, Issue 4 https://doi.org/10.1021/acs.analchem.9b04124	journal	January 2020
Long-Term Cyclability of NCM-811 at High Voltages in Lithium-Ion Batteries: an In-Depth Diagnostic Study Li, Wangda; Liu, Xiaoming; Xie, Qiang Chemistry of Materials, Vol. 32, Issue 18 https://doi.org/10.1021/acs.chemmater.0c02398	journal	August 2020
Voltage Dependent Solid Electrolyte Interphase Formation in Silicon Electrodes: Monitoring the Formation of Organic Decomposition Products Michan, Alison L.; Leskes, Michal; Grey, Clare P. Chemistry of Materials, Vol. 28, Issue 1 https://doi.org/10.1021/acs.chemmater.5b04408	journal	December 2015
Fluoroethylene Carbonate and Vinylene Carbonate Reduction: Understanding Lithium-Ion Battery Electrolyte Additives and Solid Electrolyte Interphase Formation Michan, Alison L.; Parimalam, Bharathy. S.; Leskes, Michal Chemistry of Materials, Vol. 28, Issue 22 https://doi.org/10.1021/acs.chemmater.6b02282	journal	November 2016
Impact of Microcrack Generation and Surface Degradation on a Nickel-Rich Layered Li[Ni _0.9 Co _0.05 Mn _0.05 ]O ₂ Cathode for Lithium-Ion Batteries Sun, Ho-Hyun; Manthiram, Arumugam Chemistry of Materials, Vol. 29, Issue 19 https://doi.org/10.1021/acs.chemmater.7b03268	journal	September 2017
Capacity Fading of Ni-Rich Li[Ni _x Co _y Mn _{1– x – y} ]O ₂ (0.6 ≤ x ≤ 0.95) Cathodes for High-Energy-Density Lithium-Ion Batteries: Bulk or Surface Degradation? Ryu, Hoon-Hee; Park, Kang-Joon; Yoon, Chong S. Chemistry of Materials, Vol. 30, Issue 3 https://doi.org/10.1021/acs.chemmater.7b05269	journal	January 2018
Evolution of Structure and Lithium Dynamics in LiNi _0.8 Mn _0.1 Co _0.1 O ₂ (NMC811) Cathodes during Electrochemical Cycling Märker, Katharina; Reeves, Philip J.; Xu, Chao Chemistry of Materials, Vol. 31, Issue 7 https://doi.org/10.1021/acs.chemmater.9b00140	journal	March 2019
Cation Ordering and Redox Chemistry of Layered Ni-Rich Li _x Ni _{1–2 y} Co _y Mn _y O ₂ : An Operando Raman Spectroscopy Study Flores, Eibar; Novák, Petr; Aschauer, Ulrich Chemistry of Materials, Vol. 32, Issue 1 https://doi.org/10.1021/acs.chemmater.9b03202	journal	November 2019
Sample Dependence of Magnetism in the Next-Generation Cathode Material LiNi _0.8 Mn _0.1 Co _0.1 O ₂ Mukherjee, Paromita; Paddison, Joseph A. M.; Xu, Chao Inorganic Chemistry, Vol. 60, Issue 1 https://doi.org/10.1021/acs.inorgchem.0c02899	journal	December 2020
Operando Monitoring of Early Ni-mediated Surface Reconstruction in Layered Lithiated Ni–Co–Mn Oxides Streich, Daniel; Erk, Christoph; Guéguen, Aurelie The Journal of Physical Chemistry C, Vol. 121, Issue 25 https://doi.org/10.1021/acs.jpcc.7b02303	journal	June 2017
Decomposition Reactions of Anode Solid Electrolyte Interphase (SEI) Components with LiPF ₆ Parimalam, Bharathy S.; MacIntosh, Alex D.; Kadam, Rahul The Journal of Physical Chemistry C, Vol. 121, Issue 41 https://doi.org/10.1021/acs.jpcc.7b08433	journal	October 2017
Coupled LiPF ₆ Decomposition and Carbonate Dehydrogenation Enhanced by Highly Covalent Metal Oxides in High-Energy Li-Ion Batteries Yu, Yang; Karayaylali, Pinar; Katayama, Yu The Journal of Physical Chemistry C, Vol. 122, Issue 48 https://doi.org/10.1021/acs.jpcc.8b07848	journal	October 2018
Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights Gauthier, Magali; Carney, Thomas J.; Grimaud, Alexis The Journal of Physical Chemistry Letters, Vol. 6, Issue 22 https://doi.org/10.1021/acs.jpclett.5b01727	journal	October 2015
Surface-Sensitive NMR Detection of the Solid Electrolyte Interphase Layer on Reduced Graphene Oxide Leskes, Michal; Kim, Gunwoo; Liu, Tao The Journal of Physical Chemistry Letters, Vol. 8, Issue 5 https://doi.org/10.1021/acs.jpclett.6b02590	journal	February 2017
Operando EPR for Simultaneous Monitoring of Anionic and Cationic Redox Processes in Li-Rich Metal Oxide Cathodes Tang, Mingxue; Dalzini, Annalisa; Li, Xiang The Journal of Physical Chemistry Letters, Vol. 8, Issue 17 https://doi.org/10.1021/acs.jpclett.7b01425	journal	August 2017
Chemical Reactivity Descriptor for the Oxide-Electrolyte Interface in Li-Ion Batteries Giordano, Livia; Karayaylali, Pinar; Yu, Yang The Journal of Physical Chemistry Letters, Vol. 8, Issue 16 https://doi.org/10.1021/acs.jpclett.7b01655	journal	August 2017
Do Increased Ni Contents in LiNi _x Mn _y Co _z O ₂ (NMC) Electrodes Decrease Structural and Thermal Stability of Li Ion Batteries? A Thorough Look by Consideration of the Li ⁺ Extraction Ratio Kasnatscheew, Johannes; Röser, Stephan; Börner, Markus ACS Applied Energy Materials, Vol. 2, Issue 11 https://doi.org/10.1021/acsaem.9b01440	journal	October 2019
Insights into the Cathode–Electrolyte Interphases of High-Energy-Density Cathodes in Lithium-Ion Batteries Erickson, Evan M.; Li, Wangda; Dolocan, Andrei ACS Applied Materials & Interfaces, Vol. 12, Issue 14 https://doi.org/10.1021/acsami.0c00900	journal	March 2020
Probing Depth-Dependent Transition-Metal Redox of Lithium Nickel, Manganese, and Cobalt Oxides in Li-Ion Batteries Yu, Yang; Karayaylali, Pinar; Giordano, Livia ACS Applied Materials & Interfaces, Vol. 12, Issue 50 https://doi.org/10.1021/acsami.0c16285	journal	December 2020
Revealing the Dual Surface Reactions on a HE-NCM Li-Ion Battery Cathode and Their Impact on the Surface Chemistry of the Counter Electrode Leanza, Daniela; Vaz, Carlos A. F.; Melinte, Georgian ACS Applied Materials & Interfaces, Vol. 11, Issue 6 https://doi.org/10.1021/acsami.8b19511	journal	January 2019
An Outlook on Lithium Ion Battery Technology Manthiram, Arumugam ACS Central Science, Vol. 3, Issue 10 https://doi.org/10.1021/acscentsci.7b00288	journal	September 2017
Rechargeable Batteries from the Perspective of the Electron Spin Nguyen, Howie; Clément, Raphaële J. ACS Energy Letters, Vol. 5, Issue 12 https://doi.org/10.1021/acsenergylett.0c02074	journal	November 2020
Structural Stability of LiNiO ₂ Cycled above 4.2 V Yoon, Chong S.; Jun, Do-Wook; Myung, Seung-Taek ACS Energy Letters, Vol. 2, Issue 5 https://doi.org/10.1021/acsenergylett.7b00304	journal	April 2017
A Combined Computational/Experimental Study on LiNi _1/3 Co _1/3 Mn _1/3 O ₂ Hwang, B. J.; Tsai, Y. W.; Carlier, D. Chemistry of Materials, Vol. 15, Issue 19 https://doi.org/10.1021/cm030299v	journal	September 2003
Layered Li _x Ni _y Mn _y Co _1-2 _y O ₂ Cathodes for Lithium Ion Batteries: Understanding Local Structure via Magnetic Properties Chernova, Natasha A.; Ma, Miaomiao; Xiao, Jie Chemistry of Materials, Vol. 19, Issue 19 https://doi.org/10.1021/cm0708867	journal	September 2007
NMR Studies of Cathode Materials for Lithium-Ion Rechargeable Batteries Grey, Clare P.; Dupré, Nicolas Chemical Reviews, Vol. 104, Issue 10 https://doi.org/10.1021/cr020734p	journal	October 2004
High-Frequency Electron Paramagnetic Resonance Analysis of the Oxidation State and Local Structure of Ni and Mn Ions in Ni,Mn-Codoped LiCoO₂ Stoyanova, R.; Barra, A.-L.; Yoncheva, M. Inorganic Chemistry, Vol. 49, Issue 4, p. 1932-1941 https://doi.org/10.1021/ic902351u	journal	February 2010
Soft x-ray absorption spectroscopy. Electronic and morphological structure of poly(vinylidene fluoride) Williams, R. S.; Denley, D.; Shirley, D. A. Journal of the American Chemical Society, Vol. 102, Issue 18 https://doi.org/10.1021/ja00538a003	journal	August 1980
Electrolyte Oxidation Pathways in Lithium-Ion Batteries Rinkel, Bernardine L. D.; Hall, David S.; Temprano, Israel Journal of the American Chemical Society, Vol. 142, Issue 35 https://doi.org/10.1021/jacs.0c06363	journal	July 2020
Solid Electrolyte Interphase Growth and Capacity Loss in Silicon Electrodes Michan, Alison L.; Divitini, Giorgio; Pell, Andrew J. Journal of the American Chemical Society, Vol. 138, Issue 25 https://doi.org/10.1021/jacs.6b02882	journal	June 2016
Identifying the Structural Basis for the Increased Stability of the Solid Electrolyte Interphase Formed on Silicon with the Additive Fluoroethylene Carbonate Jin, Yanting; Kneusels, Nis-Julian H.; Magusin, Pieter C. M. M. Journal of the American Chemical Society, Vol. 139, Issue 42 https://doi.org/10.1021/jacs.7b06834	journal	October 2017
Residual Lithium Carbonate Predominantly Accounts for First Cycle CO ₂ and CO Outgassing of Li-Stoichiometric and Li-Rich Layered Transition-Metal Oxides Renfrew, Sara E.; McCloskey, Bryan D. Journal of the American Chemical Society, Vol. 139, Issue 49 https://doi.org/10.1021/jacs.7b08461	journal	November 2017
Understanding Fluoroethylene Carbonate and Vinylene Carbonate Based Electrolytes for Si Anodes in Lithium Ion Batteries with NMR Spectroscopy Jin, Yanting; Kneusels, Nis-Julian H.; Marbella, Lauren E. Journal of the American Chemical Society, Vol. 140, Issue 31 https://doi.org/10.1021/jacs.8b03408	journal	July 2018
Intragranular cracking as a critical barrier for high-voltage usage of layer-structured cathode for lithium-ion batteries Yan, Pengfei; Zheng, Jianming; Gu, Meng Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14101	journal	January 2017
Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries Li, Wangda; Dolocan, Andrei; Oh, Pilgun Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14589	journal	April 2017
Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries Lin, Feng; Markus, Isaac M.; Nordlund, Dennis Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4529	journal	March 2014
Identifying the components of the solid–electrolyte interphase in Li-ion batteries Wang, Luning; Menakath, Anjali; Han, Fudong Nature Chemistry, Vol. 11, Issue 9 https://doi.org/10.1038/s41557-019-0304-z	journal	August 2019
Bulk fatigue induced by surface reconstruction in layered Ni-rich cathodes for Li-ion batteries Xu, Chao; Märker, Katharina; Lee, Juhan Nature Materials, Vol. 20, Issue 1 https://doi.org/10.1038/s41563-020-0767-8	journal	August 2020
Solid electrolyte interphase on graphite Li-ion battery anodes studied by soft X-ray spectroscopy Augustsson, A.; Herstedt, M.; Guo, J. -H. Phys. Chem. Chem. Phys., Vol. 6, Issue 16 https://doi.org/10.1039/B313434B	journal	January 2004
Performance and design considerations for lithium excess layered oxide positive electrode materials for lithium ion batteries Hy, Sunny; Liu, Haodong; Zhang, Minghao Energy & Environmental Science, Vol. 9, Issue 6 https://doi.org/10.1039/C5EE03573B	journal	January 2016
Spatially resolved surface valence gradient and structural transformation of lithium transition metal oxides in lithium-ion batteries Liu, Hanshuo; Bugnet, Matthieu; Tessaro, Matteo Z. Physical Chemistry Chemical Physics, Vol. 18, Issue 42 https://doi.org/10.1039/C6CP05262B	journal	January 2016
Mechanistic insights into lithium ion battery electrolyte degradation – a quantitative NMR study Wiemers-Meyer, S.; Winter, M.; Nowak, S. Physical Chemistry Chemical Physics, Vol. 18, Issue 38 https://doi.org/10.1039/C6CP05276B	journal	January 2016
A battery cell for in situ NMR measurements of liquid electrolytes Wiemers-Meyer, Simon; Winter, Martin; Nowak, Sascha Physical Chemistry Chemical Physics, Vol. 19, Issue 7 https://doi.org/10.1039/C6CP08653E	journal	January 2017
Transition metal dissolution and deposition in Li-ion batteries investigated by operando X-ray absorption spectroscopy Wandt, Johannes; Freiberg, Anna; Thomas, Rowena Journal of Materials Chemistry A, Vol. 4, Issue 47 https://doi.org/10.1039/C6TA08865A	journal	January 2016
Breathing and oscillating growth of solid-electrolyte-interphase upon electrochemical cycling Zhuo, Zengqing; Lu, Peng; Delacourt, Charles Chemical Communications, Vol. 54, Issue 7 https://doi.org/10.1039/C7CC07082A	journal	January 2018
Chemomechanical behaviors of layered cathode materials in alkali metal ion batteries Xu, Zhengrui; Rahman, Muhammad Mominur; Mu, Linqin Journal of Materials Chemistry A, Vol. 6, Issue 44 https://doi.org/10.1039/C8TA06875E	journal	January 2018
Revealing electrolyte oxidation via carbonate dehydrogenation on Ni-based oxides in Li-ion batteries by in situ Fourier transform infrared spectroscopy Zhang, Yirui; Katayama, Yu; Tatara, Ryoichi Energy & Environmental Science, Vol. 13, Issue 1 https://doi.org/10.1039/C9EE02543J	journal	January 2020
Detection of surface layers using 7Li MAS NMR Dupré, Nicolas; Martin, Jean-Frédéric; Guyomard, Dominique Journal of Materials Chemistry, Vol. 18, Issue 36 https://doi.org/10.1039/b807778a	journal	January 2008
Probing the electrode/electrolyte interface in the lithium excess layered oxide Li1.2Ni0.2Mn0.6O2 Carroll, Kyler J.; Qian, Danna; Fell, Chris Physical Chemistry Chemical Physics, Vol. 15, Issue 26 https://doi.org/10.1039/c3cp51927a	journal	January 2013
Monitoring local redox processes in LiNi _0.5 Mn _1.5 O ₄ battery cathode material by in operando EPR spectroscopy Niemöller, Arvid; Jakes, Peter; Eurich, Svitlana The Journal of Chemical Physics, Vol. 148, Issue 1 https://doi.org/10.1063/1.5008251	journal	January 2018
Interfacial properties in energy storage systems studied by soft x-ray absorption spectroscopy and resonant inelastic x-ray scattering Li, Qinghao; Yan, Shishen; Yang, Wanli The Journal of Chemical Physics, Vol. 152, Issue 14 https://doi.org/10.1063/5.0003311	journal	April 2020
Multi-length-scale x-ray spectroscopies for determination of surface reactivity at high voltages of LiNi _0.8 Co _0.15 Al _0.05 O ₂ vs Li ₄ Ti ₅ O ₁₂ Mirolo, Marta; Vaz, Carlos A. F.; Novák, Petr The Journal of Chemical Physics, Vol. 152, Issue 18 https://doi.org/10.1063/5.0006269	journal	May 2020
Electrochemistry and Structural Chemistry of LiNiO[sub 2] (R3m) for 4 Volt Secondary Lithium Cells Ohzuku, Tsutomu Journal of The Electrochemical Society, Vol. 140, Issue 7 https://doi.org/10.1149/1.2220730	journal	January 1993
Aging of the LiNi[sub 1∕2]Mn[sub 1∕2]O[sub 2] Positive Electrode Interface in Electrolyte Dupré, Nicolas; Martin, Jean-Frédéric; Oliveri, Julie Journal of The Electrochemical Society, Vol. 156, Issue 5 https://doi.org/10.1149/1.3098494	journal	January 2009
On the Performance of LiNi[sub 1/3]Mn[sub 1/3]Co[sub 1/3]O[sub 2] Nanoparticles as a Cathode Material for Lithium-Ion Batteries Sclar, Hadar; Kovacheva, Daniela; Zhecheva, Ekaterina Journal of The Electrochemical Society, Vol. 156, Issue 11 https://doi.org/10.1149/1.3212850	journal	January 2009
Oxygen Release and Its Effect on the Cycling Stability of LiNi _x Mn _y Co _z O ₂ (NMC) Cathode Materials for Li-Ion Batteries Jung, Roland; Metzger, Michael; Maglia, Filippo Journal of The Electrochemical Society, Vol. 164, Issue 7 https://doi.org/10.1149/2.0021707jes	journal	January 2017
Review—Recent Advances and Remaining Challenges for Lithium Ion Battery Cathodes: I. Nickel-Rich, LiNi Schipper, Florian; Erickson, Evan M.; Erk, Christoph Journal of The Electrochemical Society, Vol. 164, Issue 1 https://doi.org/10.1149/2.0351701jes	journal	December 2016
LiNi _0.4 Mn _1.6 O ₄ /Electrolyte and Carbon Black/Electrolyte High Voltage Interfaces: To Evidence the Chemical and Electronic Contributions of the Solvent on the Cathode-Electrolyte Interface Formation Demeaux, Julien; Caillon-Caravanier, Magaly; Galiano, Hervé Journal of The Electrochemical Society, Vol. 159, Issue 11 https://doi.org/10.1149/2.052211jes	journal	January 2012
Anodic Oxidation of Conductive Carbon and Ethylene Carbonate in High-Voltage Li-Ion Batteries Quantified by On-Line Electrochemical Mass Spectrometry Metzger, Michael; Marino, Cyril; Sicklinger, Johannes Journal of The Electrochemical Society, Vol. 162, Issue 7 https://doi.org/10.1149/2.0951506jes	journal	January 2015
The Role of Oxygen Release from Li- and Mn-Rich Layered Oxides during the First Cycles Investigated by On-Line Electrochemical Mass Spectrometry Strehle, Benjamin; Kleiner, Karin; Jung, Roland Journal of The Electrochemical Society, Vol. 164, Issue 2 https://doi.org/10.1149/2.1001702jes	journal	December 2016
Electrode/Electrolyte Interface Studies in Lithium Batteries Using NMR Dupre, N.; Cuisinier, M.; Guyomard, D. Interface magazine, Vol. 20, Issue 3 https://doi.org/10.1149/2.F06113if	journal	January 2011
Reversible Deposition and Stripping of the Cathode Electrolyte Interphase on Li2RuO3 Hestenes, Julia C.; Ells, Andrew W.; Navarro Goldaraz, Mateo Frontiers in Chemistry, Vol. 8 https://doi.org/10.3389/fchem.2020.00681	journal	August 2020

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