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A Self-Regulated Interface Enabled by Multi-Functional pH Buffer for Reversible Zn Electrochemistry
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DOI：10.1002/adfm.202313859.png)
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Abstract
En 中文
Aqueous Zn-ion batteries with mild acidic electrolytes are considered the promising energy storage solutions due to their outstanding merits of high energy density and cost-effectiveness. However, the rampant dendrite growth and severe parasitic reactions caused by a series of factors such as irregular Zn2+ transport pathway and pH variation would result in poor cycling stability. Herein, a self-regulated interface strategy implemented by ammonium persulfate ((NH4)2S2O8, denoted as APS) multifunctional additive is proposed to simultaneously address the above issues. The zincophilic NH4+ preferentially adsorbs on the Zn protuberance to exclude water molecules and shield the tip effect, thus inhibiting side-reactions and inducing uniform Zn deposition. Moreover, NH4+ and S2O82- can dynamically adjust H+ and OH- concentrations in a pH self-buffer manner, thus effectively mitigating hydrogen evolution reaction and formation of by-products. Consequently, with the existence of APS additive, Zn anode exhibits ultrahigh coulombic efficiency (CE) of 99.9% over 9000 cycles and ultra-long lifespan of 4300 h at 5 mA cm-2. Furthermore, even under high NH4V4O10 mass loading (9.4 mg cm-2) and thin zinc foil (10 mu m), the assembled NH4V4O10//Zn pouch cell with APS additive can still maintain stably over 210 cycles, demonstrating its excellent value for application. A trace and high-efficiency additive, ammonium persulfate, is introduced into 2 m ZnSO4 electrolyte to self-buffer pH value of H+ and OH- at the electrode-electrolyte interface, to restrain dendrite growth, formation of by-product, and corrosion behavior during cycling.image
Keywords:
ammonium persulfate
aqueous Zn-ion batteries
by-products
dendrite growth
pH buffer
Journal
IF:
19
Papers:
3.4W
Citations:
32.1W