Electrochemical CO2 reduction using renewable electricity can convert greenhouse gas CO2 into fuels or industrial raw materials (such as CO, CH4, C2H4, and C2H5OH), which can realize "carbon neutralization". However, the high overpotential and low selectivity of CO2 electroreduction lead to poor energy conversion efficiency, because of the high CO2 dissociation energy and the competitive hydrogen evolution reaction (HER). Cu is the only monometallic catalyst that can convert CO2 into value-added hydrocarbon and oxygenate products. Considerable attention has been paid to Cu catalysts' regulation to further increase CO2 reduction activity and selectivity. Herein, a series of CeO2-supported Cu nanocatalysts (Cuy/CeO2) with distinct interfacial characteristics are synthesized by a highly controllable synthesis, based on chemical prelithiation and galvanic displacement. Compared to pure Cu, a new strong CO2 adsorption site is generated at the interface of Cu and CeO2, which can promote the activation of CO2 and enable the conversion of CO2 to *CO intermediate on the adjacent Cu surface. With the increase of Cu loading, the C1 and C2+ products exhibited a declining and volcano-shaped trend, showing a maximum faradaic efficiency of 70% and 63%, respectively (Fig. 1). In-situ ATR-SEIRAS results showed that *CO on the surface of the catalyst had a low-frequency adsorption band (*COLFB) and a high-frequency adsorption band (*COHFB). A high percentage of the high-frequency band *COHFB promotes the C1 products, and a high percentage of the low-frequency band *COLFB facilitates the C2+ product. These findings provide a methodology for controlling the interface of heterostructured catalysts and shed light on the rational design of high-efficient catalysts toward the customizable CO2 electroreduction to target products.

Customizable CO2 electroreduction to C1 or C2+ products through Cuy/CeO2 interface engineering

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