Isolated copper-tin atomic interfaces tuning electrocatalytic CO2 conversion

Abstract

Direct experimental observations of the interface structure can provide vital insights into heterogeneous catalysis. Examples of interface design based on single atom and surface science are, however, extremely rare. Here, we report Cu-Sn single-atom surface alloys, where isolated Sn sites with high surface densities (up to 8%) are anchored on the Cu host, for efficient electrocatalytic CO2 reduction. The unique geometric and electronic structure of the Cu-Sn surface alloys (Cu97Sn3 and Cu99Sn1) enables distinct catalytic selectivity from pure Cu-100 and Cu70Sn30 bulk alloy. The Cu97Sn3 catalyst achieves a CO Faradaic efficiency of 98% at a tiny overpotential of 30mV in an alkaline flow cell, where a high CO current density of 100mAcm(-2) is obtained at an overpotential of 340mV. Density functional theory simulation reveals that it is not only the elemental composition that dictates the electrocatalytic reactivity of Cu-Sn alloys; the local coordination environment of atomically dispersed, isolated Cu-Sn bonding plays the most critical role. The understanding of catalytic reactions at the atomic interface is vital; however, the characterization and mechanism studies of atomically dispersed catalysts remain challenging. Here, the authors demonstrate Cu-Sn surface alloys with isolated Sn atoms on a Cu host to achieve efficient CO2 to CO conversion.