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Vertically aligned black reduced porous SnO2 nanosheets were succesfully developed via vacancy engineering for the first time, which simultaneously realized the promoted conductivity and active sites, hence leading to the efficient and durable CO2RR to formate.
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•Black reduced porous SnO2 nanosheets were prepared via thermal annealing.•Our electrocatalyst possessed metallic conductivity and high density of active sites.•The maximum Faradaic efficiency of 92.4% for formate was obtained in CO2RR.•Stable Faradaic efficiency of 90 ± 2% was maintained under -0.6 to -1.1 V vs. RHE.•Oxygen vacancies in SnO2 decreased the energy barrier of HCOO−* and HCOOH* for CO2RR.
The great bottleneck that lies in CO2 reduction reaction (CO2RR) electrocatalysts is to simultaneously enhance their conductivity and density of active sites. Herein, we developed a black reduced porous SnO2 nanosheets electrocatalyst that enabled possessing both metallic conductivity and high density of active sites via vacancy engineering. The black reduced porous SnO2 nanosheets showed high activity and selectivity for CO2RR to formate, with maximum Faradaic efficiency (FE) of 92.4% at the low overpotential of 0.51 V and stable FE of 90 ± 2% in the large potential range from -0.6 to -1.1 V vs. reversible hydrogen electrode (RHE). Density functional theory (DFT) calculations indicated that the introduction of oxygen vacancy increased carrier density and lowered the adsorption of HCOO- * and HCOOH by 0.29 and 0.17 eV, respectively, accounting for the improved CO2RR to formate performance.