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Title: Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials

Abstract

Chemical and mechanical properties interplay on the nanometric scale and collectively govern the functionalities of battery materials. Understanding the relationship between the two can inform the design of battery materials with optimal chemomechanical properties for long-life lithium batteries. Herein, we report a mechanism of nanoscale mechanical breakdown in layered oxide cathode materials, originating from oxygen release at high states of charge under thermal abuse conditions. Here, we observe that the mechanical breakdown of charged Li1-xNi0.4Mn0.4Co0.2O2 materials proceeds via a two-step pathway involving intergranular and intragranular crack formation. Owing to the oxygen release, sporadic phase transformations from the layered structure to the spinel and/or rocksalt structures introduce local stress, which initiates microcracks along grain boundaries and ultimately leads to the detachment of primary particles; i.e., intergranular crack formation. Furthermore, intragranular cracks (pores and exfoliations) form, likely due to the accumulation of oxygen vacancies and continuous phase transformations at the surfaces of primary particles. Finally, finite element modeling confirms our experimental observation that the crack formation is attributable to formation of oxygen vacancies, oxygen release, and phase transformations. This study is designed to directly observe the chemomechanical behavior of layered oxide cathode materials and provides a chemical basis for strengthening primary andmore » secondary particles by stabilizing the oxygen anions in the lattice.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [5];  [1];  [6];  [5]; ORCiD logo [7]; ORCiD logo [5]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Purdue Univ., West Lafayette, IN (United States)
  4. Tianjin Univ. of Technology, Tianjin (China)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. Center for High Pressure Science & Technology Advanced Research, Shanghai (China)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1532317
Alternate Identifier(s):
OSTI ID: 1438313
Report Number(s):
BNL-205669-2018-JAAM
Journal ID: ISSN 1530-6984; ark:/13030/qt6kh823p0
Grant/Contract Number:  
AC02-05CH11231; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 5; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Layered Cathode Materials; cathode; crack; oxygen release; phase transformation

Citation Formats

Mu, Linqin, Lin, Ruoqian, Xu, Rong, Han, Lili, Xia, Sihao, Sokaras, Dimosthenis, Steiner, James D., Weng, Tsu-Chien, Nordlund, Dennis, Doeff, Marca M., Liu, Yijin, Zhao, Kejie, Xin, Huolin L., and Lin, Feng. Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials. United States: N. p., 2018. Web. https://doi.org/10.1021/acs.nanolett.8b01036.
Mu, Linqin, Lin, Ruoqian, Xu, Rong, Han, Lili, Xia, Sihao, Sokaras, Dimosthenis, Steiner, James D., Weng, Tsu-Chien, Nordlund, Dennis, Doeff, Marca M., Liu, Yijin, Zhao, Kejie, Xin, Huolin L., & Lin, Feng. Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials. United States. https://doi.org/10.1021/acs.nanolett.8b01036
Mu, Linqin, Lin, Ruoqian, Xu, Rong, Han, Lili, Xia, Sihao, Sokaras, Dimosthenis, Steiner, James D., Weng, Tsu-Chien, Nordlund, Dennis, Doeff, Marca M., Liu, Yijin, Zhao, Kejie, Xin, Huolin L., and Lin, Feng. Wed . "Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials". United States. https://doi.org/10.1021/acs.nanolett.8b01036. https://www.osti.gov/servlets/purl/1532317.
@article{osti_1532317,
title = {Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials},
author = {Mu, Linqin and Lin, Ruoqian and Xu, Rong and Han, Lili and Xia, Sihao and Sokaras, Dimosthenis and Steiner, James D. and Weng, Tsu-Chien and Nordlund, Dennis and Doeff, Marca M. and Liu, Yijin and Zhao, Kejie and Xin, Huolin L. and Lin, Feng},
abstractNote = {Chemical and mechanical properties interplay on the nanometric scale and collectively govern the functionalities of battery materials. Understanding the relationship between the two can inform the design of battery materials with optimal chemomechanical properties for long-life lithium batteries. Herein, we report a mechanism of nanoscale mechanical breakdown in layered oxide cathode materials, originating from oxygen release at high states of charge under thermal abuse conditions. Here, we observe that the mechanical breakdown of charged Li1-xNi0.4Mn0.4Co0.2O2 materials proceeds via a two-step pathway involving intergranular and intragranular crack formation. Owing to the oxygen release, sporadic phase transformations from the layered structure to the spinel and/or rocksalt structures introduce local stress, which initiates microcracks along grain boundaries and ultimately leads to the detachment of primary particles; i.e., intergranular crack formation. Furthermore, intragranular cracks (pores and exfoliations) form, likely due to the accumulation of oxygen vacancies and continuous phase transformations at the surfaces of primary particles. Finally, finite element modeling confirms our experimental observation that the crack formation is attributable to formation of oxygen vacancies, oxygen release, and phase transformations. This study is designed to directly observe the chemomechanical behavior of layered oxide cathode materials and provides a chemical basis for strengthening primary and secondary particles by stabilizing the oxygen anions in the lattice.},
doi = {10.1021/acs.nanolett.8b01036},
journal = {Nano Letters},
number = 5,
volume = 18,
place = {United States},
year = {2018},
month = {4}
}

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