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Transition Metal Ion Doping on ZIF?8 for Enhanced the Electrochemical CO2 Reduction Reaction

The electrochemical reduction of CO2 to diverse value?added chemicals is a unique, environmentally friendly approach for curbing greenhouse gas emissions while addressing sluggish catalytic activity and low Faradaic efficiency (FE) of electrocatalysts. Here, zeolite?imidazolate?frameworks?8 (ZIF?8) containing various transition metal ions—Ni, Fe, and Cu—at varying concentrations upon doping were fabricated for the electrocatalytic CO2 reduction reaction (CO2RR) to CO without further processing. Atom coordination environments and theoretical electrocatalytic performance were scrutinized via X?ray absorption spectroscopy and density functional theory calculations. Upon optimized Cu doping on ZIF?8, Cu0.5Zn0.5/ZIF?8 achieved a high partial current density of 11.57 mA cm–2 and maximum FE for CO of 88.5% at –1.0 V (versus RHE) with a stable catalytic activity over 6 h. Furthermore, the electron?rich sp2 C atom facilitated COOH* promotion after Cu doping of ZIF?8, leading to a local effect between the Zn–N4 and Cu–N4 moieties. Additionally, advanced CO2RR pathway was illustrated from various perspectives, including the pre?H?covered state under the CO2RR. Our findings expand the pool of efficient MOF?based CO2RR catalysts, deeming them viable alternatives to conventional catalysts.This article is protected by copyright. All rights reserved

Publication date: 02/12/2022

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This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 870292.