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Title: Detection of a Cobalt-Containing Interphase at the Li6PS5Cl-NMC111 Interface by In Situ μXANES and EIS

Journal Article · · Journal of the Electrochemical Society
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  1. Northeastern Univ., Boston, MA (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
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Sulfide electrolyte all-solid-state lithium batteries (ASLBs) with uncoated Li-NixMnyCo1–x–yO2 (NMC) cathodes suffer from a large capacity loss during initial cycling and an increase in cell impedance. Decomposition reactions are known to occur at the Li6PS5Cl-NMC111 interface due to incompatibility between the two materials. If a stabilizing coating is applied to the NMC, it delivers full capacity during initial charge. However, the loss in capacity during discharge still occurs. The interface was studied by μXANES and through EIS analysis. A chemically-formed interphase was detected by μXANES, evident from reduction of Co at an uncoated NMC particle surface. This interphase was produced by decomposition at rest. To study the effect of the interphase on electrochemically active surface area, piecewise in situ EIS was performed and the data was modeled using a transmission line model (TLM). The charge transfer resistance RCT was used to estimate the volume specific active surface area (aact). The median value for aact was 296 cm–1, a factor of 7.5 lower than the theoretical value of 2216 cm–1. This provided evidence of a lower electrochemically active surface area in the ASLB.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
SC0012704; AC02-06CH11357
OSTI ID:
2333671
Report Number(s):
BNL--225454-2024-JAAM
Journal Information:
Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 3 Vol. 171; ISSN 0013-4651
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

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