Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
[2];
[3];
[4];
[4];
[3];
[2]
- Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, USA, Department of Materials Science and Engineering
- Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, USA
- Department of Chemistry, University of Illinois at Chicago, Chicago, USA
- Department of Materials Science and Engineering, University of Michigan, Ann Arbor, USA
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.
- Research Organization:
- State Univ. of New York (SUNY), Binghamton, NY (United States). Energy Frontier Research Center (EFRC) NorthEast Center for Chemical Energy Storage (NECCES)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- SC0012583; AC02-76SF00515; AC02-06CH11357; SC0001294
- OSTI ID:
- 1426310
- Alternate ID(s):
- OSTI ID: 1470238
- Journal Information:
- Energy & Environmental Science, Journal Name: Energy & Environmental Science Vol. 11 Journal Issue: 4; ISSN 1754-5692
- Publisher:
- Royal Society of Chemistry (RSC)Copyright Statement
- Country of Publication:
- United Kingdom
- Language:
- English
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