Resolving Charge Distribution for Compositionally Heterogeneous Battery Cathode Materials

Mu, Linqin; Zhang, Jin; Xu, Yahong; Wei, Chenxi; Rahman, Muhammad Mominur; Nordlund, Dennis; Liu, Yijin; Lin, Feng

doi:10.1021/acs.nanolett.1c04464

Title: Resolving Charge Distribution for Compositionally Heterogeneous Battery Cathode Materials

Journal Article · 17 January 2022 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.1c04464 · OSTI ID:1873407

^[1]; Zhang, Jin ^[2]; Xu, Yahong ^[2]; Wei, Chenxi ^[2];

^[1]; Nordlund, Dennis ^[2];

^[2];

^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

The isostructural nature of Li-layered cathodes allows for accommodating multiple transition metals (TMs). However, little is known about how the local TM stoichiometry influences the charging behavior of battery particles thus impacting battery performance. In this work, we develop heterogeneous compositional distributions in polycrystalline LiNi_1–x–yMn_xCo_yO₂ (NMC) particles to investigate the interplay between local stoichiometry and charge distribution. These NMC particles exhibit a broad, continuous distribution of local Ni/Mn/Co stoichiometry, which does not compromise the global layeredness. The local Mn and Ni concentrations in individual NMC particles are positively and negatively correlated with the electrochemically induced Ni oxidation, respectively, whereas the Co concentration does not impose a clear effect on the Ni oxidation. The resulting material delivers excellent reversible capacity, rate capability, and cycle life at high operating voltages. Engineering Ni/Mn/Co distribution in NMC particles may provide a path toward controlling the charge distribution and thus chemomechanical properties of polycrystalline battery particles.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Virginia Polytechnic Institute and State University; National Science Foundation (NSF)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1873407

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 3 Vol. 22; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (40)

Layered Na-Ion Cathodes with Outstanding Performance Resulting from the Synergetic Effect of Mixed P- and O-Type Phases Keller, Marlou; Buchholz, Daniel; Passerini, Stefano Advanced Energy Materials, Vol. 6, Issue 3 https://doi.org/10.1002/aenm.201501555	journal	November 2015
Self-Induced Concentration Gradient in Nickel-Rich Cathodes by Sacrificial Polymeric Bead Clusters for High-Energy Lithium-Ion Batteries Kim, Junhyeok; Cho, Hyeon; Jeong, Hu Young Advanced Energy Materials, Vol. 7, Issue 12 https://doi.org/10.1002/aenm.201602559	journal	January 2017
High-Capacity Concentration Gradient Li[Ni _0.865 Co _0.120 Al _0.015 ]O ₂ Cathode for Lithium-Ion Batteries Park, Kang-Joon; Choi, Min-Jae; Maglia, Filippo Advanced Energy Materials, Vol. 8, Issue 19 https://doi.org/10.1002/aenm.201703612	journal	March 2018
Quantification of Heterogeneous Degradation in Li‐Ion Batteries Yang, Yang; Xu, Rong; Zhang, Kai Advanced Energy Materials, Vol. 9, Issue 25 https://doi.org/10.1002/aenm.201900674	journal	May 2019
Ti‐Gradient Doping to Stabilize Layered Surface Structure for High Performance High‐Ni Oxide Cathode of Li‐Ion Battery Kong, Defei; Hu, Jiangtao; Chen, Zhefeng Advanced Energy Materials, Vol. 9, Issue 41 https://doi.org/10.1002/aenm.201901756	journal	September 2019
Recent Progress and Perspective of Advanced High‐Energy Co‐Less Ni‐Rich Cathodes for Li‐Ion Batteries: Yesterday, Today, and Tomorrow Choi, Ji Ung; Voronina, Natalia; Sun, Yang‐Kook Advanced Energy Materials, Vol. 10, Issue 42 https://doi.org/10.1002/aenm.202002027	journal	September 2020
Probing Dopant Redistribution, Phase Propagation, and Local Chemical Changes in the Synthesis of Layered Oxide Battery Cathodes Yang, Zhijie; Mu, Linqin; Hou, Dong Advanced Energy Materials, Vol. 11, Issue 1 https://doi.org/10.1002/aenm.202002719	journal	November 2020
A Layered P2- and O3-Type Composite as a High-Energy Cathode for Rechargeable Sodium-Ion Batteries Guo, Shaohua; Liu, Pan; Yu, Haijun Angewandte Chemie International Edition, Vol. 54, Issue 20 https://doi.org/10.1002/anie.201411788	journal	April 2015
High‐Entropy Layered Oxide Cathodes for Sodium‐Ion Batteries Zhao, Chenglong; Ding, Feixiang; Lu, Yaxiang Angewandte Chemie International Edition, Vol. 59, Issue 1 https://doi.org/10.1002/anie.201912171	journal	January 2020
Structural classification and properties of the layered oxides Delmas, C.; Fouassier, C.; Hagenmuller, P. Physica B+C, Vol. 99, Issue 1-4 https://doi.org/10.1016/0378-4363(80)90214-4	journal	January 1980
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
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
Reaction Heterogeneity in LiNi _0.8 Co _0.15 Al _0.05 O ₂ Induced by Surface Layer Grenier, Antonin; Liu, Hao; Wiaderek, Kamila M. Chemistry of Materials, Vol. 29, Issue 17 https://doi.org/10.1021/acs.chemmater.7b02236	journal	August 2017
Dopant Distribution in Co-Free High-Energy Layered Cathode Materials Mu, Linqin; Zhang, Rui; Kan, Wang Hay Chemistry of Materials, Vol. 31, Issue 23 https://doi.org/10.1021/acs.chemmater.9b03603	journal	November 2019
Heterogeneous, Defect-Rich Battery Particles and Electrodes: Why Do They Matter, and How Can One Leverage Them? Yang, Zhijie; Lin, Feng The Journal of Physical Chemistry C, Vol. 125, Issue 18 https://doi.org/10.1021/acs.jpcc.1c01703	journal	April 2021
Charge-Transfer-Induced Lattice Collapse in Ni-Rich NCM Cathode Materials during Delithiation Kondrakov, Aleksandr O.; Geßwein, Holger; Galdina, Kristina The Journal of Physical Chemistry C, Vol. 121, Issue 44 https://doi.org/10.1021/acs.jpcc.7b06598	journal	October 2017
A New Coating Method for Alleviating Surface Degradation of LiNi _0.6 Co _0.2 Mn _0.2 O ₂ Cathode Material: Nanoscale Surface Treatment of Primary Particles Kim, Hyejung; Kim, Min Gyu; Jeong, Hu Young Nano Letters, Vol. 15, Issue 3 https://doi.org/10.1021/acs.nanolett.5b00045	journal	February 2015
Facile Fabrication of Ethoxy-Functional Polysiloxane Wrapped LiNi _0.6 Co _0.2 Mn _0.2 O ₂ Cathode with Improved Cycling Performance for Rechargeable Li-Ion Battery Wang, Hao; Ge, Wujie; Li, Wen ACS Applied Materials & Interfaces, Vol. 8, Issue 28 https://doi.org/10.1021/acsami.6b04644	journal	July 2016
Targeted Surface Doping with Reversible Local Environment Improves Oxygen Stability at the Electrochemical Interfaces of Nickel-Rich Cathode Materials Steiner, James D.; Cheng, Hao; Walsh, Julia ACS Applied Materials & Interfaces, Vol. 11, Issue 41 https://doi.org/10.1021/acsami.9b14729	journal	October 2019
Distinct Surface and Bulk Thermal Behaviors of LiNi _0.6 Mn _0.2 Co _0.2 O ₂ Cathode Materials as a Function of State of Charge Tian, Chixia; Xu, Yahong; Kan, Wang Hay ACS Applied Materials & Interfaces, Vol. 12, Issue 10 https://doi.org/10.1021/acsami.9b21288	journal	February 2020
Heterogeneous Reaction Activities and Statistical Characteristics of Particle Cracking in Battery Electrodes Lin, Feng; Zhao, Kejie; Liu, Yijin ACS Energy Letters, Vol. 6, Issue 11 https://doi.org/10.1021/acsenergylett.1c02135	journal	October 2021
An Ordered P2/P3 Composite Layered Oxide Cathode with Long Cycle Life in Sodium-Ion Batteries Rahman, Muhammad Mominur; Mao, Jing; Kan, Wang Hay ACS Materials Letters, Vol. 1, Issue 5 https://doi.org/10.1021/acsmaterialslett.9b00347	journal	September 2019
In-Situ X-ray Absorption Spectroscopic Study on Variation of Electronic Transitions and Local Structure of LiNi _1/3 Co _1/3 Mn _1/3 O ₂ Cathode Material during Electrochemical Cycling Tsai, Y. W.; Hwang, B. J.; Ceder, G. Chemistry of Materials, Vol. 17, Issue 12 https://doi.org/10.1021/cm048027v	journal	June 2005
Multiprincipal Component P2-Na _0.6 (Ti _0.2 Mn _0.2 Co _0.2 Ni _0.2 Ru _0.2 )O ₂ as a High-Rate Cathode for Sodium-Ion Batteries Yang, Lufeng; Chen, Chi; Xiong, Shan JACS Au, Vol. 1, Issue 1 https://doi.org/10.1021/jacsau.0c00002	journal	December 2020
Electronic Structure of Cobalt Nanocrystals Suspended in Liquid Liu, Hongjian; Yin, Yadong Nano Letters, Vol. 7, Issue 7 https://doi.org/10.1021/nl070586o	journal	July 2007
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
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
Metal segregation in hierarchically structured cathode materials for high-energy lithium batteries Lin, Feng; Nordlund, Dennis; Li, Yuyi Nature Energy, Vol. 1, Issue 1 https://doi.org/10.1038/nenergy.2015.4	journal	January 2016
Propagation topography of redox phase transformations in heterogeneous layered oxide cathode materials Mu, Linqin; Yuan, Qingxi; Tian, Chixia Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05172-x	journal	July 2018
Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials Xu, Zhengrui; Jiang, Zhisen; Kuai, Chunguang Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-019-13884-x	journal	January 2020
Mutual modulation between surface chemistry and bulk microstructure within secondary particles of nickel-rich layered oxides Li, Shaofeng; Jiang, Zhisen; Han, Jiaxiu Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-18278-y	journal	September 2020
Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V Zhang, Jie-Nan; Li, Qinghao; Ouyang, Chuying Nature Energy, Vol. 4, Issue 7 https://doi.org/10.1038/s41560-019-0409-z	journal	June 2019
Profiling the nanoscale gradient in stoichiometric layered cathode particles for lithium-ion batteries Lin, Feng; Nordlund, Dennis; Markus, Isaac M. Energy & Environmental Science, Vol. 7, Issue 9 https://doi.org/10.1039/C4EE01400F	journal	January 2014
Elucidation of the surface characteristics and electrochemistry of high-performance LiNiO ₂ Xu, Jing; Lin, Feng; Nordlund, Dennis Chemical Communications, Vol. 52, Issue 22 https://doi.org/10.1039/C5CC09434H	journal	January 2016
A review of Ni-based layered oxides for rechargeable Li-ion batteries Xu, Jing; Lin, Feng; Doeff, Marca M. Journal of Materials Chemistry A, Vol. 5, Issue 3 https://doi.org/10.1039/C6TA07991A	journal	January 2017
Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities Rahman, Muhammad Mominur; Xu, Yahong; Cheng, Hao Energy & Environmental Science, Vol. 11, Issue 9 https://doi.org/10.1039/C8EE00309B	journal	January 2018
The synthesis, characterization and electrochemical behavior of the layered LiNi0.4Mn0.4Co0.2O2 compound Ngala, J. Katana; Chernova, Natasha A.; Ma, Miaomiao Journal of Materials Chemistry, Vol. 14, Issue 2 https://doi.org/10.1039/b309834f	journal	January 2004
Oxygen and transition metal involvement in the charge compensation mechanism of LiNi1/3Mn1/3Co1/3O2 cathodes Petersburg, Cole F.; Li, Zheng; Chernova, Natasha A. Journal of Materials Chemistry, Vol. 22, Issue 37 https://doi.org/10.1039/c2jm33392a	journal	January 2012
Resonant Soft X-Ray Emission Spectroscopy and X-Ray Absorption Spectroscopy on the Cathode Material LiNi[sub 0.65]Co[sub 0.25]Mn[sub 0.1]O[sub 2] Hollmark, H. M.; Duda, L. -C.; Dahbi, M. Journal of The Electrochemical Society, Vol. 157, Issue 8 https://doi.org/10.1149/1.3454739	journal	January 2010
Structural and Electrochemical Investigation of Li(Ni[sub 0.4]Co[sub 0.15]Al[sub 0.05]Mn[sub 0.4])O[sub 2] Cathode Material Rumble, C.; Conry, T. E.; Doeff, Marca Journal of The Electrochemical Society, Vol. 157, Issue 12 https://doi.org/10.1149/1.3494211	journal	January 2010

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