Issue

Vol. 17 (2025)

NH4+-Modulated Cathodic Interfacial Spatial Charge Redistribution for High-Performance Dual-Ion Capacitors

https://doi.org/10.1007/s40820-025-01660-0
Yumin Chen
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, People’s Republic of China
Ziyang Song
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, People’s Republic of China
Yaokang Lv
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, People’s Republic of China
Lihua Gan
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, People’s Republic of China
Mingxian Liu
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, People’s Republic of China

Corresponding Author: Mingxian Liu

liumx@tongji.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 117

Abstract

Compared with Zn2+, the current mainly reported charge carrier for zinc hybrid capacitors, small-hydrated-sized and light-weight NH4+ is expected as a better one to mediate cathodic interfacial electrochemical behaviors, yet has not been unraveled. Here we propose an NH4+-modulated cationic solvation strategy to optimize cathodic spatial charge distribution and achieve dynamic Zn2+/NH4+ co-storage for boosting Zinc hybrid capacitors. Owing to the hierarchical cationic solvated structure in hybrid Zn(CF3SO3)2–NH4CF3SO3 electrolyte, high-reactive Zn2+ and small-hydrate-sized NH4(H2O)4+ induce cathodic interfacial Helmholtz plane reconfiguration, thus effectively enhancing the spatial charge density to activate 20% capacity enhancement. Furthermore, cathodic interfacial adsorbed hydrated NH4+ ions afford high-kinetics and ultrastable C‧‧‧H (NH4+) charge storage process due to a much lower desolvation energy barrier compared with heavy and rigid Zn(H2O)62+ (5.81 vs. 14.90 eV). Consequently, physical uptake and multielectron redox of Zn2+/NH4+ in carbon cathode enable the zinc capacitor to deliver high capacity (240 mAh g−1 at 0.5 A g−1), large-current tolerance (130 mAh g−1 at 50 A g−1) and ultralong lifespan (400,000 cycles). This study gives new insights into the design of cathode–electrolyte interfaces toward advanced zinc-based energy storage.


Highlights:
1 Hierarchical Zn2+/NH4+ solvation structure induces cathodic interfacial Helmholtz plane reconfiguration to enhance spatial charge density and capacity storage.
2 Hydrated NH4+ ions afford high-kinetics and ultrastable C‧‧‧H charge storage due to a much lower desolvation energy barrier compared with large-sized Zn(H2O)62+ (5.81 vs. 14.90 eV).
3 Interfacial Zn2+/NH4+ co-storage endow the hybrid capacitor with high capacity (240 mAh g−1), large-current tolerance (50 A g−1) and ultralong lifespan (400,000 cycles).

Keywords

NH4 -modulated cathodic interface Spatial charge redistribution Zn2 /NH4 co-storage Dual-ion capacitor
Chen, Yumin, Ziyang Song, Yaokang Lv, Lihua Gan, and Mingxian Liu. 2025. “NH4+-Modulated Cathodic Interfacial Spatial Charge Redistribution for High-Performance Dual-Ion Capacitors”. Nano-Micro Letters 17 (January):117. https://doi.org/10.1007/s40820-025-01660-0.
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