Persistent and partially mobile oxygen vacancies in Li-rich layered oxides

Csernica, Peter M.; Kalirai, Samanbir S.; Gent, William E.; Lim, Kipil; Yu, Young-Sang; Liu, Yunzhi; Ahn, Sung-Jin; Kaeli, Emma; Xu, Xin; Stone, Kevin H.; Marshall, Ann F.; Sinclair, Robert; Shapiro, David A.; Toney, Michael F.; Chueh, William C.

doi:10.1038/s41560-021-00832-7

Persistent and partially mobile oxygen vacancies in Li-rich layered oxides

Journal Article · Mon Jun 14 04:00:00 EDT 2021 · Nature Energy

DOI:https://doi.org/10.1038/s41560-021-00832-7· OSTI ID:1807552

^[1]; Kalirai, Samanbir S. ^[2]; ^[1]; Lim, Kipil ^[3]; ^[4]; Liu, Yunzhi ^[1]; Ahn, Sung-Jin ^[5]; ^[1]; ^[1]; ^[6]; Marshall, Ann F. ^[1]; Sinclair, Robert ^[1]; ^[4]; ^[7]; ^[3]

Stanford Univ., CA (United States)
Stanford Univ., CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Samsung Advanced Inst. of Technology, Suwon-si (South Korea)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Colorado, Boulder, CO (United States)

Increasing the energy density of layered oxide battery electrodes is challenging as accessing high states of delithiation often triggers voltage degradation and oxygen release. Here we utilize transmission-based X-ray absorption spectromicroscopy and ptychography on mechanically cross-sectioned Li_1.18–xNi_0.21Mn_0.53Co_0.08O_2–δ electrodes to quantitatively profile the oxygen deficiency over cycling at the nanoscale. The oxygen deficiency penetrates into the bulk of individual primary particles (~200 nm) and is well-described by oxygen vacancy diffusion. Using an array of characterization techniques, we demonstrate that, surprisingly, bulk oxygen vacancies that persist within the native layered phase are indeed responsible for the observed spectroscopic changes. We additionally show that the arrangement of primary particles within secondary particles (~5 μm) causes considerable heterogeneity in the extent of oxygen release between primary particles. Finally, our work merges an ensemble of length-spanning characterization methods and informs promising approaches to mitigate the deleterious effects of oxygen release in lithium-ion battery electrodes.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231

OSTI ID:: 1807552

Alternate ID(s):: OSTI ID: 1841719

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 6 Vol. 6; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Main Text Data for "Persistent and Partially Mobile Oxygen Vacancies in Li-Rich Layered Oxides" Csernica, Peter M. Zenodo https://doi.org/10.5281/zenodo.4697951	dataset	January 2021
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