▌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
探究局域熵驅動的正極電解質界面層及乙烯碳酸酯在鋰離子電池鎳富層狀材料上的一步完全去質子化
L. Merinda, R. A. Yuwono, F. M. Wang*, N. L. Wu*, C. D. D. Sundari, C. Khotimah, J. K. Chang, S. C. Haw, C. W. Pao, J. L. Chen, Q. Xu, Y. Wu, C. L. Chen and T. S. Chan
https://doi.org/10.1016/j.cej.2025.170703
SEED Member: F. M. Wang, J. K. Chang
Major Contributions
1. A localized entropy-driven mechanism is identified for cathode electrolyte interphase (CEI) formation on Ni-rich layered cathodes, linking configurational and vibrational entropy effects to interphase composition, thickness, and stability.
2. A one-step complete deprotonation pathway of ethylene carbonate (EC) on the Ni-rich cathode surface is revealed, elucidating the molecular-level mechanism of EC solvent decomposition at high-voltage interfaces.
3. The mechanistic framework provides guidance for rational electrolyte formulation to tune CEI chemistry, improving interfacial stability and cycling performance of Ni-rich Li-ion batteries.
主要貢獻
1. 在鎳富層狀正極上識別出局域熵驅動機制主導正極電解質界面層（CEI）的形成，將組態熵與振動熵效應與界面層組成、厚度及穩定性相連結。
2. 揭示乙烯碳酸酯（EC）在鎳富正極表面的一步完全去質子化路徑，闡明高壓界面上 EC 溶劑分解的分子層面機制。
3. 機制框架為理性設計電解液以調控 CEI 化學提供指導，改善鎳富鋰離子電池的界面穩定性與循環性能。
