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Zincophilic Sites Enriched Hydrogen‐Bonded Organic Framework as Multifunctional Regulating Interfacial Layers for Stable Zinc Metal Batteries

Jie Ding, Jiajing He, Ling Chen, Yi Sun, Yi Xu, Li‐Ping Lv, Yong Wang

2024Angewandte Chemie17 citationsDOI

Abstract

Abstract To construct an efficient regulating layer for Zn anodes that can simultaneously address the issues of dendritic growth and side reactions is highly demanded for stable zinc metal batteries (ZMBs). Herein, we fabricate a hydrogen‐bonded organic framework (HOF) enriched with zincophilic sites as a multifunctional layer to regulate Zn anodes with controlled spatial ion flux and stable interfacial chemistry (MA‐BTA@Zn). The framework with abundant H‐bonds helps capture H 2 O and remove the solvated shells on [Zn(H 2 O) 6 ] 2+ , leading to suppressed side reactions. The HOF layer also helps form electrolyte‐philic surfaces and expose Zn (002) crystal planes which benefit for rapid conduction and uniform deposition of Zn 2+ , and weakened sides reactions. Additionally, the electrochemically active zincophilic sites (C=O, −NH 2 and triazine groups) favor the targeted guidance and penetration of Zn 2+ and provide advantageous sites for uniform Zn deposition. High Young's modulus of the HOF layer further contributes to a high interfacial flexibility and stability against Zn plating‐associated stress. The MA‐BTA@Zn symmetric cells thereby obtain a substantially extended battery life over 1000 h at 4 mA cm −2 . The MA‐BTA@Zn||Cu half‐cell demonstrates a highly reversible Zn stripping/plating process over 1500 cycles with impressive average Coulombic efficiency (CE) of 99.5 % at 10 mA cm −2 .

Topics & Concepts

ZincMetal-organic frameworkMetalHydrogen storageHydrogenChemistryChemical engineeringMaterials scienceInorganic chemistryOrganic chemistryAdsorptionEngineeringAdvanced battery technologies researchCovalent Organic Framework ApplicationsLayered Double Hydroxides Synthesis and Applications