Journal
CHINESE PHYSICS B
Volume 29, Issue 2, Pages -Publisher
IOP PUBLISHING LTD
DOI: 10.1088/1674-1056/ab6585
Keywords
Ni-rich cathode; x-ray nanoprobe; redox heterogeneity; surface chemistry
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- National Science Foundation [DMR-1832613]
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The hierarchical structure of the composite cathodes brings in significant chemical complexity related to the interfaces, such as cathode electrolyte interphase. These interfaces account for only a small fraction of the volume and mass, they could, however, have profound impacts on the cell-level electrochemistry. As the investigation of these interfaces becomes a crucial topic in the battery research, there is a need to properly study the surface chemistry, particularly to eliminate the biased, incomplete characterization provided by techniques that assume the homogeneous surface chemistry. Herein, we utilize nano-resolution spatially-resolved x-ray spectroscopic tools to probe the heterogeneity of the surface chemistry on LiNi0.8Mn0.1Co0.1O2 layered cathode secondary particles. Informed by the nano-resolution mapping of the Ni valance state, which serves as a measurement of the local surface chemistry, we construct a conceptual model to elucidate the electrochemical consequence of the inhomogeneous local impedance over the particle surface. Going beyond the implication in battery science, our work highlights a balance between the high-resolution probing the local chemistry and the statistical representativeness, which is particularly vital in the study of the highly complex material systems.
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