Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials

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

doi:10.1021/acs.nanolett.8b01036

Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials

Journal Article · Wed Apr 18 00:00:00 EDT 2018 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.8b01036· OSTI ID:1438313

Mu, Linqin ^[1]; Lin, Ruoqian ^[2]; Xu, Rong ^[3]; Han, Lili ^[4]; Xia, Sihao ^[5]; Sokaras, Dimosthenis ^[5]; Steiner, James D. ^[1]; Weng, Tsu -Chien ^[6]; Nordlund, Dennis ^[5]; ^[7]; ^[5]; ^[3]; ^[2]; ^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Purdue Univ., West Lafayette, IN (United States)
Tianjin Univ. of Technology, Tianjin (China)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Center for High Pressure Science & Technology Advanced Research, Shanghai (China)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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 Li_1-xNi_0.4Mn_0.4Co_0.2O₂ 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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC02-05CH11231; SC0012704

OSTI ID:: 1438313

Alternate ID(s):: OSTI ID: 1532317

Report Number(s):: BNL--205669-2018-JAAM

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 5 Vol. 18; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Journal Article · Tue Apr 23 20:00:00 EDT 2019 · Journal of Materials Chemistry. A · OSTI ID:1547284

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phase transformation

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