Operando NMR characterization of cycled and calendar aged nanoparticulate silicon anodes for Li-ion batteries

Wang, Evelyna; Rodrigues, Marco-Tulio F.; Park, Sohyun; Dogan, Fulya; Key, Baris

doi:10.1016/j.jpowsour.2024.234477

Title: Operando NMR characterization of cycled and calendar aged nanoparticulate silicon anodes for Li-ion batteries

Journal Article · 09 April 2024 · Journal of Power Sources

DOI: https://doi.org/10.1016/j.jpowsour.2024.234477 · OSTI ID:2502013

^[1];

^[1]; Park, Sohyun ^[1]; Dogan, Fulya ^[1]; Key, Baris ^[1]

Argonne National Laboratory (ANL), Argonne, IL (United States)

Replacing graphite anodes with Si anodes can greatly increase the energy of current Li-ion batteries. Detailed characterization of Si lithiation reactions, SEI formation, and reversibility are therefore active areas of research. Solid-state ⁷Li nuclear magnetic resonance (NMR) spectroscopy is useful for characterizing different lithium local environments within Si anodes. Here, we developed an operando NMR methodology to characterize aging of carbon-coated nanoparticulate Si anodes in pouch cells paired with Ni-rich cathodes. We observed a new lithiation mechanism in the Si nanoparticles: direct formation of over-lithiated Li_15+xSi₄ (x<0.6) phase. Furthermore, our novel operando cells maintained good performance with long-term cycle and calendar aging. Here we identified trapped lithium silicides as a major contributor to capacity fade with aging. Finally, we determined that the addition of Mg (TFSI)₂ to the electrolyte decreased the amount of trapped lithium silicides and therefore increased the capacity and capacity retention for the nanoparticulate Si used.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2502013

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 604; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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