Journal
NATURE ENERGY
Volume 6, Issue 6, Pages 642-652Publisher
NATURE RESEARCH
DOI: 10.1038/s41560-021-00832-7
Keywords
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Funding
- Samsung Advanced Institute of Technology Global Research Outreach program
- DOE, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-AC02-76SF00515]
- DOE Office of Science User Facility [DE-AC02-05CH11231]
- STROBE, a National Science Foundation Science and Technology Center [DMR1548924]
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- National Science Foundation [ECCS-1542152, DGE-1656518]
- Stanford Graduate Fellowship
- ALS Doctoral Fellowship
- Toyota Research Institute-Accelerated Materials Design and Discovery (TRI-AMDD) program (Stanford University)
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Utilizing transmission-based X-ray absorption spectromicroscopy and ptychography, the study quantitatively profiles oxygen deficiency in layered oxide battery electrodes at the nanoscale. It reveals that oxygen vacancies in the bulk of individual particles and their diffusion are responsible for spectroscopic changes. Additionally, the arrangement of particles within secondary particles causes heterogeneity in oxygen release.
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 Li1.18-xNi0.21Mn0.53Co0.08O2-delta electrodes to quantitatively profile the oxygen deficiency over cycling at the nanoscale. The oxygen deficiency penetrates into the bulk of individual primary particles (similar to 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 (similar to 5 mu m) causes considerable heterogeneity in the extent of oxygen release between primary particles. 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.
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