Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
Author(s)
Tsai, Ping-Chun; Wen, Bohua; Wolfman, Mark; Choe, Min-Ju; Pan, Menghsuan Sam; Su, Liang; Thornton, Katsuyo; Cabana, Jordi; Chiang, Yet-Ming; ... Show more Show less
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The electrochemical kinetics of battery electrodes at the single-particle scale are measured as a function of state-of-charge, and interpreted with the aid of concurrent transmission X-ray microscopy (TXM) of the evolving particle microstructure. An electrochemical cell operating with near-picoampere current resolution is used to characterize single secondary particles of two widely-used cathode compounds, NMC333 and NCA. Interfacial charge transfer kinetics are found to vary by two orders of magnitude with state-of-charge (SOC) in both materials, but the origin of the SOC dependence differs greatly. NCA behavior is dominated by electrochemically-induced microfracture, although thin binder coatings significantly ameliorate mechanical degradation, while NMC333 demonstrates strongly increasing interfacial reaction rates with SOC for chemical reasons. Micro-PITT is used to separate interfacial and bulk transport rates, and show that for commercially relevant particle sizes, interfacial transport is rate-limiting at low SOC, while mixed-control dominates at higher SOC. These results provide mechanistic insight into the mesoscale kinetics of ion intercalation compounds, which can guide the development of high performance rechargeable batteries.
Date issued
2018-03Department
Massachusetts Institute of Technology. Department of Materials Science and EngineeringJournal
Energy & Environmental Science
Publisher
Royal Society of Chemistry (RSC)
Citation
Tsai, Ping-Chun et al. “Single-Particle Measurements of Electrochemical Kinetics in NMC and NCA Cathodes for Li-Ion Batteries.” Energy & Environmental Science 11, 4 (2018): 860–871 © 2018 Royal Society of Chemistry
Version: Final published version
ISSN
1754-5692
1754-5706