Quantification of Heterogeneous Degradation in Li-Ion Batteries

Yang, Yang; Xu, Rong; Zhang, Kai; Lee, Sang‐Jun; Mu, Linqin; Liu, Pengfei; Waters, Crystal K.; Spence, Stephanie; Xu, Zhengrui; Wei, Chenxi; Kautz, David J.; Yuan, Qingxi; Dong, Yuhui; Yu, Young‐Sang; Xiao, Xianghui; Lee, Han‐Koo; Pianetta, Piero; Cloetens, Peter; Lee, Jun‐Sik; Zhao, Kejie; Lin, Feng; Liu, Yijin

doi:10.1002/aenm.201900674

Title: Quantification of Heterogeneous Degradation in Li-Ion Batteries

Journal Article · 28 May 2019 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.201900674 · OSTI ID:1524198

Yang, Yang ^[1]; Xu, Rong ^[2]; Zhang, Kai ^[3]; Lee, Sang‐Jun ^[4]; Mu, Linqin ^[5]; Liu, Pengfei ^[2]; Waters, Crystal K. ^[5]; Spence, Stephanie ^[5]; Xu, Zhengrui ^[5]; Wei, Chenxi ^[4]; Kautz, David J. ^[5]; Yuan, Qingxi ^[6]; Dong, Yuhui ^[6]; Yu, Young‐Sang ^[7]; Xiao, Xianghui ^[8]; Lee, Han‐Koo ^[9]; Pianetta, Piero ^[4]; Cloetens, Peter ^[1]; Lee, Jun‐Sik ^[4]; Zhao, Kejie ^[2] more »

European Synchrotron Radiation Facility (ESRF), Grenoble (France)
Purdue Univ., West Lafayette, IN (United States)
Chinese Academy of Sciences (CAS), Beijing (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Chinese Academy of Sciences (CAS), Beijing (China)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Pohang Accelerator Lab. (PAL) (Korea, Republic of)

The multiscale chemomechanical interplay in lithium-ion batteries builds up mechanical stress, provokes morphological breakdown, and leads to state of charge heterogeneity. Quantifying the interplay in complex composite electrodes with multiscale resolution constitutes a frontier challenge in precisely diagnosing the fading mechanism of batteries. In this work, hard X-ray phase contrast tomography, capable of nanoprobing thousands of active particles at once, enables an unprecedented statistical analysis of the chemomechanical transformation of composite electrodes under fast charging conditions. The damage heterogeneity is demonstrated to prevail at all length scales, which stems from the unbalanced electron conduction and ionic diffusion, and collectively leads to the nonuniform utilization of active particles spatially and temporally. This research highlights that the statistical mapping of the chemomechanical transformation offers a diagnostic method for the particles utilization and fading, hence could improve electrode formulation for fast-charging batteries.

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

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

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1524198

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 25 Vol. 9; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (51)

Local State-of-Charge Mapping of Lithium-Ion Battery Electrodes Nanda, Jagjit; Remillard, Jeffrey; O'Neill, Ann Advanced Functional Materials, Vol. 21, Issue 17 https://doi.org/10.1002/adfm.201100157	journal	July 2011
Persistent State-of-Charge Heterogeneity in Relaxed, Partially Charged Li ₁₋ _x Ni _1/3 Co _1/3 Mn _1/3 O ₂ Secondary Particles Gent, William E.; Li, Yiyang; Ahn, Sungjin Advanced Materials, Vol. 28, Issue 31 https://doi.org/10.1002/adma.201601273	journal	May 2016
A Self-Forming Composite Electrolyte for Solid-State Sodium Battery with Ultralong Cycle Life Zhang, Zhizhen; Zhang, Qinghua; Shi, Jinan Advanced Energy Materials, Vol. 7, Issue 4 https://doi.org/10.1002/aenm.201601196	journal	October 2016
Multiscale Morphological and Electrical Characterization of Charge Transport Limitations to the Power Performance of Positive Electrode Blends for Lithium-Ion Batteries Besnard, Nicolas; Etiemble, Aurélien; Douillard, Thierry Advanced Energy Materials, Vol. 7, Issue 8 https://doi.org/10.1002/aenm.201602239	journal	December 2016
Dynamics of the Morphological Degradation of Si‐Based Anodes for Li‐Ion Batteries Characterized by In Situ Synchrotron X‐Ray Tomography Vanpeene, Victor; Villanova, Julie; King, Andrew Advanced Energy Materials, Vol. 9, Issue 18 https://doi.org/10.1002/aenm.201803947	journal	March 2019
Nickel-Rich Layered Lithium Transition-Metal Oxide for High-Energy Lithium-Ion Batteries Liu, Wen; Oh, Pilgun; Liu, Xien Angewandte Chemie International Edition, Vol. 54, Issue 15 https://doi.org/10.1002/anie.201409262	journal	March 2015
Disintegration of Meatball Electrodes for LiNi x Mn y Co z O2 Cathode Materials Xu, R.; de Vasconcelos, L. S.; Shi, J. Experimental Mechanics, Vol. 58, Issue 4 https://doi.org/10.1007/s11340-017-0292-0	journal	May 2017
Stabilization of the layered crystal structure of LiNiO2 by Co-substitution Zhecheva, E.; Stoyanova, R. Solid State Ionics, Vol. 66, Issue 1-2 https://doi.org/10.1016/0167-2738(93)90037-4	journal	October 1993
Autonomous filling of creep cavities in Fe-Au alloys studied by synchrotron X-ray nano-tomography Fang, H.; Versteylen, C. D.; Zhang, S. Acta Materialia, Vol. 121 https://doi.org/10.1016/j.actamat.2016.09.023	journal	December 2016
Understanding the Effect of Local Short-Range Ordering on Lithium Diffusion in Li1.3Nb0.3Mn0.4O2 Single-Crystal Cathode Kan, Wang Hay; Deng, Biao; Xu, Yahong Chem, Vol. 4, Issue 9 https://doi.org/10.1016/j.chempr.2018.05.008	journal	September 2018
High-rate and long-life lithium-ion battery performance of hierarchically hollow-structured NiCo2O4/CNT nanocomposite Wang, Jie; Wu, Jianzhong; Wu, Zexing Electrochimica Acta, Vol. 244 https://doi.org/10.1016/j.electacta.2017.05.092	journal	August 2017
Charge Heterogeneity and Surface Chemistry in Polycrystalline Cathode Materials Tian, Chixia; Xu, Yahong; Nordlund, Dennis Joule, Vol. 2, Issue 3 https://doi.org/10.1016/j.joule.2017.12.008	journal	March 2018
Synthesis and electrochemical properties of Li[Ni0.8Co0.1Mn0.1]O2 and Li[Ni0.8Co0.2]O2 via co-precipitation Kim, Myung-Hyoon; Shin, Ho-Suk; Shin, Dongwook Journal of Power Sources, Vol. 159, Issue 2 https://doi.org/10.1016/j.jpowsour.2005.11.083	journal	September 2006
Impact of Nickel agglomeration on Solid Oxide Cell operated in fuel cell and electrolysis modes Hubert, M.; Laurencin, J.; Cloetens, P. Journal of Power Sources, Vol. 397 https://doi.org/10.1016/j.jpowsour.2018.06.097	journal	September 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
The PyHST2 hybrid distributed code for high speed tomographic reconstruction with iterative reconstruction and a priori knowledge capabilities Mirone, Alessandro; Brun, Emmanuel; Gouillart, Emmanuelle Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 324 https://doi.org/10.1016/j.nimb.2013.09.030	journal	April 2014
To get the most out of high resolution X-ray tomography: A review of the post-reconstruction analysis Liu, Yijin; Kiss, Andrew M.; Larsson, Daniel H. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 117 https://doi.org/10.1016/j.sab.2016.01.002	journal	March 2016
Mesoscale Battery Science: The Behavior of Electrode Particles Caught on a Multispectral X-ray Camera Wei, Chenxi; Xia, Sihao; Huang, Hai Accounts of Chemical Research, Vol. 51, Issue 10 https://doi.org/10.1021/acs.accounts.8b00123	journal	June 2018
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
Synchrotron X-ray Analytical Techniques for Studying Materials Electrochemistry in Rechargeable Batteries Lin, Feng; Liu, Yijin; Yu, Xiqian Chemical Reviews, Vol. 117, Issue 21 https://doi.org/10.1021/acs.chemrev.7b00007	journal	September 2017
Finding a Needle in the Haystack: Identification of Functionally Important Minority Phases in an Operating Battery Zhang, Kai; Ren, Fang; Wang, Xuelong Nano Letters, Vol. 17, Issue 12 https://doi.org/10.1021/acs.nanolett.7b03985	journal	November 2017
Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials Mu, Linqin; Lin, Ruoqian; Xu, Rong Nano Letters, Vol. 18, Issue 5 https://doi.org/10.1021/acs.nanolett.8b01036	journal	April 2018
Thermal Stability of Lithium Nickel Oxide Derivatives. Part II: Li _x Ni _0.70 Co _0.15 Al _0.15 O ₂ and Li _x Ni _0.90 Mn _0.10 O ₂ ( x = 0.50 and 0.30). Comparison with Li _x Ni _1.02 O ₂ and Li _x Ni _0.89 Al _0.16 O ₂ Guilmard, M.; Croguennec, L.; Delmas, C. Chemistry of Materials, Vol. 15, Issue 23 https://doi.org/10.1021/cm030340u	journal	November 2003
Nanoscale Morphological and Chemical Changes of High Voltage Lithium–Manganese Rich NMC Composite Cathodes with Cycling Yang, Feifei; Liu, Yijin; Martha, Surendra K. Nano Letters, Vol. 14, Issue 8 https://doi.org/10.1021/nl502090z	journal	July 2014
In Situ Atomic Force Microscopy of Lithiation and Delithiation of Silicon Nanostructures for Lithium Ion Batteries Becker, Collin R.; Strawhecker, Kenneth E.; McAllister, Quinn P. ACS Nano, Vol. 7, Issue 10 https://doi.org/10.1021/nn4037909	journal	September 2013
Visualization of anisotropic-isotropic phase transformation dynamics in battery electrode particles Wang, Jiajun; Karen Chen-Wiegart, Yu-chen; Eng, Christopher Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12372	journal	August 2016
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
Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy Kuppan, Saravanan; Xu, Yahong; Liu, Yijin Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14309	journal	February 2017
Distinct charge dynamics in battery electrodes revealed by in situ and operando soft X-ray spectroscopy Liu, Xiaosong; Wang, Dongdong; Liu, Gao Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3568	journal	October 2013
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
In-operando high-speed tomography of lithium-ion batteries during thermal runaway Finegan, Donal P.; Scheel, Mario; Robinson, James B. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7924	journal	April 2015
In situ/operando synchrotron-based X-ray techniques for lithium-ion battery research Bak, Seong-Min; Shadike, Zulipiya; Lin, Ruoqian NPG Asia Materials, Vol. 10, Issue 7 https://doi.org/10.1038/s41427-018-0056-z	journal	July 2018
Quantification and modeling of mechanical degradation in lithium-ion batteries based on nanoscale imaging Müller, Simon; Pietsch, Patrick; Brandt, Ben-Elias Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04477-1	journal	June 2018
Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode Yan, Pengfei; Zheng, Jianming; Chen, Tianwu Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04862-w	journal	June 2018
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
Unsupervised Data Mining in nanoscale X-ray Spectro-Microscopic Study of NdFeB Magnet Duan, Xiaoyue; Yang, Feifei; Antono, Erin Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep34406	journal	September 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
Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries Tsai, Ping-Chun; Wen, Bohua; Wolfman, Mark Energy & Environmental Science, Vol. 11, Issue 4 https://doi.org/10.1039/C8EE00001H	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
Thermally driven mesoscale chemomechanical interplay in Li _0.5 Ni _0.6 Mn _0.2 Co _0.2 O ₂ cathode materials Wei, Chenxi; Zhang, Yan; Lee, Sang-Jun Journal of Materials Chemistry A, Vol. 6, Issue 45 https://doi.org/10.1039/C8TA08973F	journal	January 2018
LiNi _1–y Co _y O ₂ positive electrode materials: relationships between the structure, physical properties and electrochemical behaviour Saadoune, Ismael; Delmas, Claude J. Mater. Chem., Vol. 6, Issue 2 https://doi.org/10.1039/JM9960600193	journal	January 1996
Holotomography: Quantitative phase tomography with micrometer resolution using hard synchrotron radiation x rays Cloetens, P.; Ludwig, W.; Baruchel, J. Applied Physics Letters, Vol. 75, Issue 19 https://doi.org/10.1063/1.125225	journal	November 1999
Applications of Hard X‐ray Full‐Field Transmission X‐ray Microscopy at SSRL Liu, Y.; Andrews, J. C.; Meirer, F. THE 10TH INTERNATIONAL CONFERENCE ON X‐RAY MICROSCOPY, AIP Conference Proceedings https://doi.org/10.1063/1.3625377	conference	January 2011
Three-dimensional imaging of chemical phase transformations at the nanoscale with full-field transmission X-ray microscopy Meirer, Florian; Cabana, Jordi; Liu, Yijin Journal of Synchrotron Radiation, Vol. 18, Issue 5 https://doi.org/10.1107/S0909049511019364	journal	July 2011
TXM-Wizard : a program for advanced data collection and evaluation in full-field transmission X-ray microscopy Liu, Yijin; Meirer, Florian; Williams, Phillip A. Journal of Synchrotron Radiation, Vol. 19, Issue 2 https://doi.org/10.1107/S0909049511049144	journal	January 2012
A Computational Approach to Edge Detection Canny, John IEEE Transactions on Pattern Analysis and Machine Intelligence, Vol. PAMI-8, Issue 6 https://doi.org/10.1109/TPAMI.1986.4767851	journal	November 1986
Visualization and Quantification of Electrochemical and Mechanical Degradation in Li Ion Batteries Ebner, M.; Marone, F.; Stampanoni, M. Science, Vol. 342, Issue 6159 https://doi.org/10.1126/science.1241882	journal	October 2013
Efficient concentration of high-energy x-rays for diffraction-limited imaging resolution Cesar da Silva, Julio; Pacureanu, Alexandra; Yang, Yang Optica, Vol. 4, Issue 5 https://doi.org/10.1364/OPTICA.4.000492	journal	January 2017
Computational analysis of chemomechanical behaviors of composite electrodes in Li-ion batteries Xu, Rong; Scalco de Vasconcelos, Luize; Zhao, Kejie Journal of Materials Research, Vol. 31, Issue 18 https://doi.org/10.1557/jmr.2016.302	journal	August 2016
Quantification and modeling of mechanical degradation in lithium-ion batteries based on nanoscale imaging Müller, Simon; Pietsch, Patrick; Brandt, Ben-Elias ETH Zurich https://doi.org/10.3929/ethz-b-000271931	text	January 2018
PyHST2: an hybrid distributed code for high speed tomographic reconstruction with iterative reconstruction and a priori knowledge capabilities Mirone, Alessandro; Gouillart, Emmanuelle; Brun, Emmanuel arXiv https://doi.org/10.48550/arxiv.1306.1392	text	January 2013

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Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes Finegan, Donal P.; Vamvakeros, Antonis; Tan, Chun Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-14467-x	journal	January 2020
Ni‐Rich Layered Cathode Materials with Electrochemo‐Mechanically Compliant Microstructures for All‐Solid‐State Li Batteries Jung, Sung Hoo; Kim, Un‐Hyuck; Kim, Jae‐Hyung Advanced Energy Materials, Vol. 10, Issue 6 https://doi.org/10.1002/aenm.201903360	journal	December 2019
Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes Finegan, Donal P.; Vamvakeros, Antonis; Tan, Chun Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-14467-x	journal	January 2020
Probing and quantifying cathode charge heterogeneity in Li ion batteries Zhang, Yuxin; Yang, Zhijie; Tian, Chixia Journal of Materials Chemistry A, Vol. 7, Issue 41 https://doi.org/10.1039/c9ta06977a	journal	January 2019
TOPAS and TOPAS-Academic : an optimization program integrating computer algebra and crystallographic objects written in C++ Coelho, Alan A. Journal of Applied Crystallography, Vol. 51, Issue 1 https://doi.org/10.1107/S1600576718000183	journal	February 2018

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Title: Quantification of Heterogeneous Degradation in Li-Ion Batteries

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