Synchrotron Operando Depth Profiling Studies of State-of-Charge Gradients in Thick Li(Ni0.8Mn0.1Co0.1)O2 Cathode Films

Li, Zhuo; Yin, Liang; Mattei, Gerard S.; Cosby, Monty R.; Lee, Byoung-Sun; Wu, Zhaohui; Bak, Seong-Min; Chapman, Karena W.; Yang, Xiao-Qing; Liu, Ping; Khalifah, Peter G.

doi:10.1021/acs.chemmater.0c00983

Synchrotron Operando Depth Profiling Studies of State-of-Charge Gradients in Thick Li(Ni_0.8Mn_0.1Co_0.1)O₂ Cathode Films

Journal Article · Sun Jul 05 00:00:00 EDT 2020 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.0c00983· OSTI ID:1677676

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Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Department of NanoEngineering, University of California San Diego, La Jolla, California 92093, United States
Univ. of California, San Diego, CA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Higher energy densities in rechargeable batteries can be achieved using thicker cathode films, though it is a challenging endeavor since the electrochemical performance of thick electrodes is substantially worse than that of the conventional thin electrodes due to a variety of transport limitations, which are thus far poorly understood. For the first time, operando synchrotron studies have been applied to thick film samples to determine the depth-dependent state of charge (SOC) distribution inside 170 micron thick Li(Ni_0.8Mn_0.1Co_0.1)O₂ cathode films using an unconventional radial diffraction experiment geometry, allowing the SOC to be probed with both high spatial resolution (20 microns) and high temporal resolution (hundreds of time steps) in a single experiment. The resulting data allow the evolution of vertical inhomogeneity within these thick cathode films to be determined during cycling and they reveal a number of unexpected phenomena, such as the continuation of charging at some heights within the cathode during the discharge cycle of the cell. The new availability of comprehensive depth-dependent SOC data will drive the parameterization and advancement of whole-cell models, leading to an improved understanding of large-scale transport phenomena and enhanced capabilities for the rational design of thick electrodes with improved performance.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: SC0012704

OSTI ID:: 1677676

Alternate ID(s):: OSTI ID: 1648358

Report Number(s):: BNL-219945-2020--JAAM

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 15 Vol. 32; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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