Intrinsically Decoupled Coordination Chemistries Enable Quasi-Eutectic Electrolytes with Fast Kinetics toward Enhanced Zinc-Ion Capacitors.
Angew Chem Int Ed Engl
; 63(34): e202406906, 2024 Aug 19.
Article
em En
| MEDLINE
| ID: mdl-38819764
ABSTRACT
Eutectic electrolytes show potential beyond conventional low-concentration electrolytes (LCEs) in zinc (Zn)-ion capacitors (ZICs) yet suffer from high viscosity and sluggish kinetics. Herein, we originally propose a universal theory of intrinsically decoupling to address these issues, producing a novel electrolyte termed "quasi-eutectic" electrolyte (quasi-EE). Joint experimental and theoretical analyses confirm its unique solution coordination structure doped with near-LCE domains. This enables the quasi-EE well inherit the advanced properties at deep-eutectic states while provide facilitated kinetics as well as lower energy barriers via a vehicle/hopping-hybridized charge transfer mechanism. Consequently, a homogeneous electroplating pattern with much enhanced Sand's time is achieved on the Zn surface, followed by a twofold prolonged service-life with drastically reduced concentration polarization. More encouragingly, the quasi-EE also delivers increased capacitance output in ZICs, which is elevated by 12.4 %-144.6 % compared to that before decoupling. Furthermore, the pouch cell with a cathodic mass loading of 36.6â
mg cm-2 maintains competitive cycling performances over 600â
cycles, far exceeding other Zn-based counterparts. This work offers fresh insights into eutectic decoupling and beyond.
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Ano de publicação:
2024
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Article