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Elucidating the origins of phase transformation hysteresis during electrochemical cycling of Li-Sb electrodes

Chang, Donghee; Huo, Hua; Johnston, Karen E.; Ménétrier, Michel; Monconduit, Laure; Grey, Clare P.; Van der Ven, Anton

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Authors

Donghee Chang

Hua Huo

Michel Ménétrier

Laure Monconduit

Clare P. Grey

Anton Van der Ven



Abstract

We investigate the origins of phase transformation hysteresis in electrodes of Li-ion batteries, focusing on the alloying reaction of Li with Sb. Electrochemical measurements confirm that the reaction path followed during Li insertion into Sb electrodes differs from that followed upon subsequent Li extraction. Results from first-principles calculations and NMR measurements indicate that Li3Sb is capable of tolerating high Li-vacancy concentrations. An unusually high Li mobility in Li3Sb facilitates over potentials during charging, which leads to a substantially larger driving force for the nucleation of Sb compared to that of Li2Sb. The differences in nucleation driving forces arise from a lever effect that favors phases with large changes in Li concentration over phases that are closer in composition along the equilibrium path. These properties provide an explanation for the observed path hysteresis between charge and discharge in the Li–Sb system and likely also play a role in intercalation compounds and other alloying reactions exhibiting similar phase transformation hysteresis.

Citation

Chang, D., Huo, H., Johnston, K. E., Ménétrier, M., Monconduit, L., Grey, C. P., & Van der Ven, A. (2015). Elucidating the origins of phase transformation hysteresis during electrochemical cycling of Li-Sb electrodes. Journal of Materials Chemistry A: materials for energy and sustainability, 3(37), 18928-18943. https://doi.org/10.1039/c5ta06183k

Journal Article Type Article
Acceptance Date Aug 11, 2015
Online Publication Date Aug 11, 2015
Publication Date Aug 11, 2015
Deposit Date Sep 30, 2016
Publicly Available Date Aug 28, 2018
Journal Journal of Materials Chemistry A: materials for energy and sustainability
Print ISSN 2050-7488
Electronic ISSN 2050-7496
Publisher Royal Society of Chemistry
Peer Reviewed Peer Reviewed
Volume 3
Issue 37
Pages 18928-18943
DOI https://doi.org/10.1039/c5ta06183k

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