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In Situ Reconstruction of Hierarchical Sn-Cu/SnOx Core/Shell Catalyst for High-Performance CO2 Electroreduction.

Electrochemical CO 2 reduction reaction (CO 2 RR) into valuable C 1 (formate and CO) products has been identified as one of the most techno-economically achievable strategies for alleviating CO 2 emissions. However, high C 1 Faradaic efficiency and stability are generally attained at high overpotential and low current density. Herein, we demonstrate that the SnO x shell in Sn 2.7 Cu catalyst with hierarchical Sn-Cu core can be in situ reconstructed under cathodic potentials of CO 2 RR. The resulting Sn 2.7 Cu catalyst achieves a high current density of 406.7±14.4 mA cm -2 with C 1 Faradaic efficiency of 98.0±0.9% at -0.70 V versus reversible hydrogen electrode (RHE), and remains stable at 243.1±19.2 mA cm -2 with C 1 Faradaic efficiency of 99.0±0.5% for 40 h at -0.55 V vs. RHE. Density functional theory calculations indicate that the in situ reconstructed Sn/SnO x interface facilitates formic acid production by optimizing the binding of the reaction intermediate HCOO* while promotes Faradaic efficiency of C 1 products by suppressing the competitive hydrogen evolution reaction, resulting in high Faradaic efficiency, current density and stability of CO 2 RR at low overpotentials.