An investigation of localized entropy driven cathode electrolyte interphase to a one-step complete deprotonation of ethylene carbonate on Ni-rich layered material of lithium-ion battery
Journal
Chemical Engineering Journal
Journal Volume
525
Start Page
170703
ISSN
13858947
Date Issued
2025-12-01
Author(s)
Merinda, Laurien
Yuwono, Rio Akbar
Wang, Fu-Ming
Sundari, Citra Deliana Dewi
Khotimah, Chusnul
Hsieh, Han-Pin
Chang, Jeng-Kuei
Haw, Shu-Chih
Pao, Chih-Wen
Chen, Jeng-Lung
Xu, Qunjie
Wu, Yunwen
Chen, Chi-Liang
Chan, Ting-Shan
Abstract
LiNi0.8Mn0.1Co0.1O2 (NMC811) exceeding a high specific discharge capacity of 200 mAh g−1. However, this cathode, distinct parasitic reactions with electrolyte are induced by the nucleophilic site on its surface. Here, electron-withdrawing cis-isomerism oligomers are synthesized from phenylenedimaleimide positional isomers to prevent these parasitic reactions. The para and meta substituent oligomerize through a vinyl radical mechanism, which is followed by the C-OH formation. Meanwhile, the oligomerization of ortho substituent (o-OC) gives a more electron-withdrawing carbonyl functional group due to the propagation radical polymerization pathway. This electron-withdrawing group increases the hybridization of Ni[sbnd]O according to soft X-ray absorption spectroscopy to further catalyze the polymerization of the oligomer as an artificial cathode electrolyte interphase. Interestingly, due to a smaller angular distance (~60°) between the two maleimide groups of o-CI, leading to the formation of porous organic coverage on NCM811. These unique properties of o-CI and its interaction with NCM811 lead to the entropy-driven ethylene carbonate (EC) to vinylene carbonate (VC) reaction through a direct second deprotonation mechanism. Consequently, the cycle stability is enhanced compared to pristine NCM811 after prolonged cycling. This work demonstrates a coating layer strategy to grant a beneficial conversing of EC to VC.
Subjects
Coverage
Electrolyte decomposition
Lithium-ion battery
Localized entropy driven
Ni-rich compound
One-step deprotonation
Publisher
Elsevier B.V.
Type
journal article