Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries

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-picoamper...

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Main Authors: Tsai, Ping-Chun, Wen, Bohua, Wolfman, Mark, Choe, Min-Ju, Pan, Menghsuan Sam, Su, Liang, Thornton, Katsuyo, Cabana, Jordi, Chiang, Yet-Ming
Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering
Format: Article
Published: Royal Society of Chemistry (RSC) 2018
Online Access:http://hdl.handle.net/1721.1/116897
https://orcid.org/0000-0002-8270-3396
https://orcid.org/0000-0002-5519-1946
https://orcid.org/0000-0002-2211-2164
https://orcid.org/0000-0002-0833-7674
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author Tsai, Ping-Chun
Wen, Bohua
Wolfman, Mark
Choe, Min-Ju
Pan, Menghsuan Sam
Su, Liang
Thornton, Katsuyo
Cabana, Jordi
Chiang, Yet-Ming
author2 Massachusetts Institute of Technology. Department of Materials Science and Engineering
author_facet Massachusetts Institute of Technology. Department of Materials Science and Engineering
Tsai, Ping-Chun
Wen, Bohua
Wolfman, Mark
Choe, Min-Ju
Pan, Menghsuan Sam
Su, Liang
Thornton, Katsuyo
Cabana, Jordi
Chiang, Yet-Ming
author_sort Tsai, Ping-Chun
collection MIT
description 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.
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spelling mit-1721.1/1168972022-09-29T12:38:04Z Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries Tsai, Ping-Chun Wen, Bohua Wolfman, Mark Choe, Min-Ju Pan, Menghsuan Sam Su, Liang Thornton, Katsuyo Cabana, Jordi Chiang, Yet-Ming Massachusetts Institute of Technology. Department of Materials Science and Engineering Tsai, Ping-Chun Wen, Bohua Pan, Menghsuan Sam Su, Liang Chiang, Yet-Ming 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. 2018-07-11T15:47:56Z 2018-07-11T15:47:56Z 2018-03 2018-01 2018-07-11T15:10:26Z Article http://purl.org/eprint/type/JournalArticle 1754-5692 1754-5706 http://hdl.handle.net/1721.1/116897 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 https://orcid.org/0000-0002-8270-3396 https://orcid.org/0000-0002-5519-1946 https://orcid.org/0000-0002-2211-2164 https://orcid.org/0000-0002-0833-7674 http://dx.doi.org/10.1039/c8ee00001h Energy & Environmental Science Creative Commons Attribution-NonCommercial 3.0 Unported https://creativecommons.org/licenses/by-nc/3.0/ application/pdf Royal Society of Chemistry (RSC) Royal Society of Chemistry
spellingShingle Tsai, Ping-Chun
Wen, Bohua
Wolfman, Mark
Choe, Min-Ju
Pan, Menghsuan Sam
Su, Liang
Thornton, Katsuyo
Cabana, Jordi
Chiang, Yet-Ming
Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
title Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
title_full Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
title_fullStr Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
title_full_unstemmed Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
title_short Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
title_sort single particle measurements of electrochemical kinetics in nmc and nca cathodes for li ion batteries
url http://hdl.handle.net/1721.1/116897
https://orcid.org/0000-0002-8270-3396
https://orcid.org/0000-0002-5519-1946
https://orcid.org/0000-0002-2211-2164
https://orcid.org/0000-0002-0833-7674
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