Efficient electroreduction of CO2 to syngas over ZIF-8 derived oxygen vacancy-rich ZnO nanomaterials

NEW JOURNAL OF CHEMISTRY(2023)

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摘要
Electroreduction of CO2 is a sustainable approach to produce syngas with tunable CO/H-2 ratios, which are required as specific reactants for the optimization of desired products. Herein, ZnO-d and ZnO-n nanomaterials were derived from zeolitic imidazolate framework-8 (ZIF-8) precursors with different morphologies, which exhibit good performance for CO2 electroreduction to syngas when using 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim]PF6, 30 wt%)/acetonitrile/water (H2O, 5 wt%) as the supporting electrolyte. Regulation of the number of oxygen vacancies in different ZnO samples and the applied potentials during electrolysis can obviously affect the CO/H-2 ratios in syngas, which would be changed from 1/3 to 8.5/1. Meanwhile, ZnO-n with abundant oxygen vacancies displays the highest CO faradaic efficiency (FE) of 73.2% with the total current density of 9.8 mA cm(-2) at -1.9 V vs. Ag/Ag+. More oxygen vacancies and higher electrochemical specific surface area of ZnO-n can provide more active sites and facilitate the adsorption of CO2 and its intermediates. The smaller charge transfer impedance of ZnO-n can accelerate the electron and proton transfer, and thus improve the catalytic activity and the selectivity of products. In addition, the good synergistic effect between the [Bmim]PF6-containing electrolyte and ZnO-n can enhance the formation of syngas.
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