Dual‐Domain Coupling‐Driven Interface Remodeling Enables Ultra‐Dilute Flame‐Retardant Electrolytes for High‐Voltage, Wide‐Temperature Batteries

Z Zhen‐Yi Gu (MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China) Y Yong‐Li Heng (State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory For UV Light‐Emitting Materials and Technology Department of Physics Northeast Normal University Changchun Jilin P. R. China) X Xiao‐Tong Wang (MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China) S Shuo‐Hang Zheng (State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory For UV Light‐Emitting Materials and Technology Department of Physics Northeast Normal University Changchun Jilin P. R. China) Z Zhong‐Hui Sun (State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory For UV Light‐Emitting Materials and Technology Department of Physics Northeast Normal University Changchun Jilin P. R. China) Y Yi Wu Y Yue Liu J Jie Wang (State Key Laboratory of Molecular Oncology, Beijing Key Laboratory, CAMS Key Laboratory of Translational Research on Lung Cancer, Department of Medical Oncology Cancer Hospital, Chinese Academy of Medical Sciences Beijing China) Y Yuan‐Zheng Tang (Qingdao University of Science and Technology Qingdao Shandong P. R. China) S Shu‐Yu Li (Department of Chemistry Northeast Normal University Changchun Jilin P. R. China) X Xing‐Long Wu (MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China)

Abstract

ABSTRACT The paradigm shift in electrolyte research is a critical driver for performance breakthroughs in sustainable batteries under extreme conditions. Ultra‐dilute electrolytes (UDEs) have attracted extensive attention due to their remarkable cost advantages and broad application prospects, yet excess free solvents cause trade‐offs among high‐voltage stability, wide‐temperature adaptability, longevity, and safety. In this work, we propose a dual‐domain coupling‐driven interface remodeling strategy to tailor bulk solvation and interfacial microenvironments via integrating hierarchically‐solvated carbonate ester, ether, and fluorinated cyclophosphazene. The designed UDE (0.05 M) features a more flexible solvation configuration with less restricted ion transport; concurrently, electric double layers on both electrode surfaces are regulated through molecular competitive adsorption and decomposition under electric field induction. Consequently, cross‐scale microenvironment remodeling is realized to essentially overcome the existing performance limitations. The UDE not only exhibits intrinsic flame retardancy but also significantly improves electrode compatibility (phosphate and oxide cathodes, metal anode) through a bidirectional interface stabilization mechanism. Remarkably, Na 0.67 Ni 0.33 Mn 0.67 O 2 cathode achieves desirable durability over a wide temperature range (−40∼70°C). Furthermore, this strategy is extended to potassium‐ion batteries, enabling stable operation of KVPO 4 F cathode at 4.95 V. This work establishes a universal framework for multi‐scale interfacial molecular engineering, offering a promising advancement in extreme energy storage technologies.

Article Details

Volume / Issue Vol. 1, Issue 1
Published August 05, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (11)

Z

Zhen‐Yi Gu

MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China

Y

Yong‐Li Heng

State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory For UV Light‐Emitting Materials and Technology Department of Physics Northeast Normal University Changchun Jilin P. R. China

X

Xiao‐Tong Wang

MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China

S

Shuo‐Hang Zheng

State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory For UV Light‐Emitting Materials and Technology Department of Physics Northeast Normal University Changchun Jilin P. R. China

Z

Zhong‐Hui Sun

State Key Laboratory of Integrated Optoelectronics, and MOE Key Laboratory For UV Light‐Emitting Materials and Technology Department of Physics Northeast Normal University Changchun Jilin P. R. China

Y

Yi Wu

Y

Yue Liu

J

Jie Wang

State Key Laboratory of Molecular Oncology, Beijing Key Laboratory, CAMS Key Laboratory of Translational Research on Lung Cancer, Department of Medical Oncology Cancer Hospital, Chinese Academy of Medical Sciences Beijing China

Y

Yuan‐Zheng Tang

Qingdao University of Science and Technology Qingdao Shandong P. R. China

S

Shu‐Yu Li

Department of Chemistry Northeast Normal University Changchun Jilin P. R. China

X

Xing‐Long Wu

MOE Key Laboratory For UV Light‐Emitting Materials and Technology Northeast Normal University Changchun Jilin P. R. China