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Title: Understanding the Mesoscale Degradation in Nickel-Rich Cathode Materials through Machine-Learning-Revealed Strain–Redox Decoupling

Abstract

The degradation of nickel-rich cathode materials for lithium-ion batteries upon prolonged electrochemical cycling features a complicated interplay among electronic structure, lattice configuration, and micro-morphology. The underlying mechanism for such an entanglement of different material properties at nano- to mesoscales is fundamental to the battery performance but not well-understood yet. Here we investigate the correlation between the local redox reaction and lattice mismatch through a nano-resolution synchrotron spectro-microscopy study of LiNi0.8Co0.1Mn0.1O2 (NCM 811) cathode particles. With assistance from a machine-learning-based data classification method, we identify local regions that demonstrate a strain–redox decoupling effect, which can be attributed to different side reactions. Overall, our results highlight the mesoscale reaction heterogeneity in the battery cathode and suggest that particle structure engineering could be a viable approach to mitigate the chemomechanical degradation of cathode materials.

Authors:
 [1];  [2];  [3];  [4];  [3];  [3]; ORCiD logo [5];  [4]; ORCiD logo [5];  [6]; ORCiD logo [4]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Shanghai Jiao Tong Univ. (China). Shanghai Electrochemical Energy Device (SEED) Research Center
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Chinese Academy of Sciences (CAS), Beijing (China). Inst. of High Energy Physics (IHEP). Beijing Synchrotron Radiation Facility
  3. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of High Energy Physics (IHEP). Beijing Synchrotron Radiation Facility
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  5. Shanghai Jiao Tong Univ. (China). Shanghai Electrochemical Energy Device (SEED) Research Center
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Research Inst. of Industrial Science and Technology (RIST), Pohang (South Korea)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Korea Institute of Energy Technology Evaluation and Planning; National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1777286
Grant/Contract Number:  
20198510050010; AC02-76SF00515; 22008154
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 2; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; nanoparticles; lattices; electrodes; extended x-ray absorption fine structure; batteries

Citation Formats

Qian, Guannan, Zhang, Jin, Chu, Sheng-Qi, Li, Jizhou, Zhang, Kai, Yuan, Qingxi, Ma, Zi-Feng, Pianetta, Piero, Li, Linsen, Jung, Keeyoung, and Liu, Yijin. Understanding the Mesoscale Degradation in Nickel-Rich Cathode Materials through Machine-Learning-Revealed Strain–Redox Decoupling. United States: N. p., 2021. Web. doi:10.1021/acsenergylett.0c02699.
Qian, Guannan, Zhang, Jin, Chu, Sheng-Qi, Li, Jizhou, Zhang, Kai, Yuan, Qingxi, Ma, Zi-Feng, Pianetta, Piero, Li, Linsen, Jung, Keeyoung, & Liu, Yijin. Understanding the Mesoscale Degradation in Nickel-Rich Cathode Materials through Machine-Learning-Revealed Strain–Redox Decoupling. United States. https://doi.org/10.1021/acsenergylett.0c02699
Qian, Guannan, Zhang, Jin, Chu, Sheng-Qi, Li, Jizhou, Zhang, Kai, Yuan, Qingxi, Ma, Zi-Feng, Pianetta, Piero, Li, Linsen, Jung, Keeyoung, and Liu, Yijin. Wed . "Understanding the Mesoscale Degradation in Nickel-Rich Cathode Materials through Machine-Learning-Revealed Strain–Redox Decoupling". United States. https://doi.org/10.1021/acsenergylett.0c02699. https://www.osti.gov/servlets/purl/1777286.
@article{osti_1777286,
title = {Understanding the Mesoscale Degradation in Nickel-Rich Cathode Materials through Machine-Learning-Revealed Strain–Redox Decoupling},
author = {Qian, Guannan and Zhang, Jin and Chu, Sheng-Qi and Li, Jizhou and Zhang, Kai and Yuan, Qingxi and Ma, Zi-Feng and Pianetta, Piero and Li, Linsen and Jung, Keeyoung and Liu, Yijin},
abstractNote = {The degradation of nickel-rich cathode materials for lithium-ion batteries upon prolonged electrochemical cycling features a complicated interplay among electronic structure, lattice configuration, and micro-morphology. The underlying mechanism for such an entanglement of different material properties at nano- to mesoscales is fundamental to the battery performance but not well-understood yet. Here we investigate the correlation between the local redox reaction and lattice mismatch through a nano-resolution synchrotron spectro-microscopy study of LiNi0.8Co0.1Mn0.1O2 (NCM 811) cathode particles. With assistance from a machine-learning-based data classification method, we identify local regions that demonstrate a strain–redox decoupling effect, which can be attributed to different side reactions. Overall, our results highlight the mesoscale reaction heterogeneity in the battery cathode and suggest that particle structure engineering could be a viable approach to mitigate the chemomechanical degradation of cathode materials.},
doi = {10.1021/acsenergylett.0c02699},
journal = {ACS Energy Letters},
number = 2,
volume = 6,
place = {United States},
year = {Wed Jan 27 00:00:00 EST 2021},
month = {Wed Jan 27 00:00:00 EST 2021}
}

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