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Superscalar Phase Boundaries Derived Multiple Active Sites in SnO_2/Cu_6Sn_5/CuO for Tandem Electroreduction of CO2 to Formic Acid

机译:Superscalar Phase Boundaries Derived Multiple Active Sites in SnO_2/Cu_6Sn_5/CuO for Tandem Electroreduction of CO2 to Formic Acid

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摘要

The electrocatalytic CO_2 reduction reaction (CO_2RR) to fuels driven byelectrocatalysts is a viable strategy for efficient utilization of emitted CO2.CO_2RR involves multiple-steps, including adsorption, activation, hydrogenation,etc. At present, copper-tin alloy catalysts have shown the capability toreduce CO_2 to formic acid or formate. However, their poor adsorption andactivation capacities for CO_2 molecules, as well as the sluggish kinetics in*H supply restrict the proton-coupled electron transfer processes in theelectrocatalytic CO2RR to produce formic acid. In order to solve the aboveproblems, the ultra-small SnO_2/Cu_6Sn_5/CuO nanocatalysts with superscalarphase boundaries are fabricated by laser sputtering. The introduction ofSnO2 enhances the adsorption and activation of CO_2, while CuO promotesH2O decomposition and provides abundant *H intermediates, resulting intandem catalytic sites on the SnO_2/Cu_6Sn_5/CuO composite catalysts andthus leading to excellent CO_2RR activity and high selectivity to formic acid.The Faradic efficiency of formic acid (FEHCOOH) at the SnO_2/Cu_6Sn_5/CuOelectrode reaches 90.13 along with a high current density of 25.2 mA cm~(?2)at ?0.95 V versus reversible hydrogen electrode. The role of the multiphaseboundaries constructed by introduction of oxides is confirmed by in situinfrared spectroscopy and kinetic isotope effects experiments, which isconsistent with the design concept.

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