Acid- and Gas-Scavenging Electrolyte Additive Improving the Electrochemical Reversibility of Ni-Rich Cathodes in Li-Ion Batteries

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In view of their high theoretical capacities, nickel-rich layered oxides are promising cathode materials for high-energy Li-ion batteries. However, the practical applications of these oxides are hindered by transition metal dissolution, microcracking, and gas/reactive compound formation due to the undesired reactions of residual lithium species. Herein, we show that the interfacial degradation of the LiNi0.9CoxMnyAlzO2 (NCMA, x + y + z = 0.1) cathode and the graphite (Gr) anode of a representative Li-ion battery by HF can be hindered by supplementing the electrolyte with tert-butyldimethylsilyl glycidyl ether (tBS-GE). The silyl ether moiety of tBS-GE scavenges HF and PF5, thus stabilizing the interfacial layers on both electrodes, while the epoxide moiety reacts with CO2 released by the parasitic reaction between HF and Li2CO3 on the NCMA surface to afford cyclic carbonates and thus suppresses battery swelling. NCMA/Gr full cells fabricated by supplementing the baseline electrolyte with 0.1 wt % tBS-GE feature an increased capacity retention of 85.5% and deliver a high discharge capacity of 162.9 mAh/g after 500 cycles at 1 C and 25 degrees C. Thus, our results reveal that the molecular aspect-based design of electrolyte additives can be efficiently used to eliminate reactive species and gas components from Li-ion batteries and increase their performance.
Publisher
AMER CHEMICAL SOC
Issue Date
2023-05
Language
English
Article Type
Article
Citation

ACS APPLIED MATERIALS & INTERFACES, v.15, no.18, pp.22157 - 22166

ISSN
1944-8244
DOI
10.1021/acsami.3c02231
URI
http://hdl.handle.net/10203/306888
Appears in Collection
CBE-Journal Papers(저널논문)
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