TY - JOUR
T1 - Entropic electrolyte engineering for stabilizing the cathode-electrolyte interphase in high-voltage lithium-rich cathodes
AU - Che, Huiquan
AU - Su, Yuefeng
AU - Dong, Jinyang
AU - Lu, Yun
AU - Hao, Jianan
AU - Wu, Yujia
AU - Wang, Yiya
AU - Li, Ning
AU - Guan, Yibiao
AU - Wu, Feng
AU - Chen, Lai
N1 - Publisher Copyright:
© 2026 Chongqing University.
PY - 2026
Y1 - 2026
N2 - The application of lithium-rich manganese-based layered oxides (LRMOs) in high-energy lithium-ion batteries is limited by severe interfacial degradation and structural instability under high-voltage operation. Guided by theoretical calculations, a high-voltage-tolerant high-entropy (HTHE) electrolyte is designed to enable the formation of a chemically robust and functionally integrated cathode-electrolyte interphase (CEI). The electrolyte system incorporates multiple components containing fluorine, boron, sulfur, and nitrogen, which synergistically participate in interphase construction and interfacial stabilization. The CEI formed under the HTHE environment effectively mitigates oxygen release, transition metal dissolution, and irreversible phase transitions. Combined evidence from in-situ and ex-situ characterizations across multiple scales confirms that the CEI maintains the layered structure, enhances redox reversibility, and suppresses harmful phase transformation during prolonged cycling. As a result, the electrochemical performance of the LRMOs is significantly improved, with the capacity retention increasing from 73.87% in the conventional electrolyte to 85.82% in the HTHE system after 100 cycles at a cutoff voltage of 4.8 V. These findings highlight the importance of electrolyte-driven interphase engineering in stabilizing high-voltage cathodes. The proposed entropic formulation strategy provides a rational and broadly applicable approach for constructing functional CEIs and offers valuable guidance for the development of next-generation lithium-ion batteries with enhanced durability and energy density.
AB - The application of lithium-rich manganese-based layered oxides (LRMOs) in high-energy lithium-ion batteries is limited by severe interfacial degradation and structural instability under high-voltage operation. Guided by theoretical calculations, a high-voltage-tolerant high-entropy (HTHE) electrolyte is designed to enable the formation of a chemically robust and functionally integrated cathode-electrolyte interphase (CEI). The electrolyte system incorporates multiple components containing fluorine, boron, sulfur, and nitrogen, which synergistically participate in interphase construction and interfacial stabilization. The CEI formed under the HTHE environment effectively mitigates oxygen release, transition metal dissolution, and irreversible phase transitions. Combined evidence from in-situ and ex-situ characterizations across multiple scales confirms that the CEI maintains the layered structure, enhances redox reversibility, and suppresses harmful phase transformation during prolonged cycling. As a result, the electrochemical performance of the LRMOs is significantly improved, with the capacity retention increasing from 73.87% in the conventional electrolyte to 85.82% in the HTHE system after 100 cycles at a cutoff voltage of 4.8 V. These findings highlight the importance of electrolyte-driven interphase engineering in stabilizing high-voltage cathodes. The proposed entropic formulation strategy provides a rational and broadly applicable approach for constructing functional CEIs and offers valuable guidance for the development of next-generation lithium-ion batteries with enhanced durability and energy density.
KW - Cathode-electrolyte interphase
KW - Cycling stability
KW - High-entropy electrolyte
KW - High-voltage tolerant
KW - Lithium-rich oxides
UR - https://www.scopus.com/pages/publications/105034664721
U2 - 10.1016/j.nanoms.2026.01.008
DO - 10.1016/j.nanoms.2026.01.008
M3 - Article
AN - SCOPUS:105034664721
SN - 2096-6482
JO - Nano Materials Science
JF - Nano Materials Science
ER -