Spatio-dipolar synergy modulated interfacial molecular bridge for calendar-aging-resistant aqueous zinc-ion batteriesOA
Short calendar-aging life and interfacial degradation hinder the applications of aqueous Zn-ion batteries.Herein,trimorpholinophosphine oxide(TPO),featuring a high topological polar surface area(TPSA),is introduced as an electrolyte additive that modulates interfacial ions via steric-dipolar synergism.Specifically,the topological polarity of TPO facilitates Zn^(2+)coordination and strong surface adsorption,creating migration channels within solvation-interfacial networks.Moreover,the steric hindrance of TPO disrupts the solvation sheath of Zn^(2+),forming H_(3)O+-repelled layers.Consequently,TPO-containing cells achieve an exceptional average Coulombic efficiency(CE)of 99.91%and operate steadily at ultrahigh current densities(280 mA cm^(-2)).At-20℃,TPO-containing cells retain 177 mAh g^(-1) after 6000 cycles,yet additive-free cells fail after 1400 cycles(84 mAh g^(-1)).Most importantly,TPO-containing cells maintain a high CE exceeding 95%for over 2500 h under intermittent calendar-aging,far exceeding the 72 h of additive-free cells.This work offers molecular-level insights into TPSA-induced steric-dipole synergism for ultra-stable batteries.
Zimin Yang;Yilun Sun;Jianwei Li;Mingqiang Wu;Siting Deng;Xinbin Nie;Yifan Su;Hao Tong;Pengpeng Guo;Jingkui Gao;Guoliang Chai
State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China Fujian College,University of Chinese Academy of Sciences,Fuzhou 350002,China School of Chemical Science,University of Chinese Academy of Sciences,Beijing 100049,ChinaState Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,ChinaSchool of Chemical Science,University of Chinese Academy of Sciences,Beijing 100049,China Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources,Qinghai Province Key Laboratory of Resources and Chemistry of Salt Lakes,Qinghai Institute of Salt Lakes,Chinese Academy of Sciences,Xining 810008,ChinaState Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China College of Chemistry,Fuzhou University,Fuzhou 350108,ChinaState Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,ChinaKey Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources,Qinghai Province Key Laboratory of Resources and Chemistry of Salt Lakes,Qinghai Institute of Salt Lakes,Chinese Academy of Sciences,Xining 810008,ChinaKey Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources,Qinghai Province Key Laboratory of Resources and Chemistry of Salt Lakes,Qinghai Institute of Salt Lakes,Chinese Academy of Sciences,Xining 810008,ChinaState Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,ChinaCollege of Chemistry,Fuzhou University,Fuzhou 350108,ChinaCollege of Chemistry,Fuzhou University,Fuzhou 350108,ChinaState Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China Fujian College,University of Chinese Academy of Sciences,Fuzhou 350002,China School of Chemical Science,University of Chinese Academy of Sciences,Beijing 100049,China
信息技术与安全科学
aqueous Zn-ion batteriesadditivecalendar agingspatio-dipolar synergy
《National Science Review》 2026 (12)
P.214-226,13
supported by the National Key Research and Development Program of China(2018YFA0704502)the Na-tional Natural Science Foundation of China(U22A20436 and 52403365)the Special Program for Guiding Local Science and Technology Development by the Central Government(2022L3090)supported by the Strategic Priority Research Program of the Chinese Academy of Sci-ences(XDB1170000)the Major Science and Technology Spe-cial Project of Xining(2024-Z-1)the Science and Technol-ogy Program of Qinghai Province,China(2025-ZJ-960M).
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