Crystallinity engineering of carbon nitride protective coating for ultra-stable Zn metal anodes

Abstract

Ineffective control of dendrite growth and side reactions on Zn anodessignificantly retards commercialization of aqueous Zn-ion batteries. Unlikeconventional interfacial modification strategies that are primarilyfocused on component optimization or microstructural tuning, herein, wepropose a crystallinity engineering strategy by developing highly crystallinecarbon nitride protective layers for Zn anodes through molten salttreatment. Interestingly, the highly ordered structure along with sufficientfunctional polar groups and pre-intercalated K⁺ endows the coating withhigh ionic conductivity, strong hydrophilicity, and accelerated ion diffusionkinetics. Theoretical calculations also confirm its enhanced Znadsorption capability compared to commonly reported carbon nitridewith amorphous or semi-crystalline structure and bare Zn. Benefitingfrom the aforementioned features, the as-synthesized protective layerenables a calendar lifespan of symmetric cells for 1100 h and outstandingstability of full cells with capacity retention of 91.5% after 1500 cycles. Thiswork proposes a new conceptual strategy for Zn anode protection.

Keywords

crystalline carbon nitride / crystallinity engineering / long cycling life / uniform Zn deposition / Zn metal anode

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RIGHTS & PERMISSIONS

2024 The Authors. Electron published by Harbin Institute of Technology and John Wiley & Sons Australia, Ltd.