Ta3N5 is regarded as a promising candidate material with adequate visible light absorption and band structure for photoelectrochemical water splitting. However, the performance of Ta3N5 is severely limited by the...

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Cu-based materials are promising catalysts for the electrochemical CO 2 reduction reaction (CO 2 RR). However, they frequently have a low Faradaic efficiency (FE) and selectivity for a specific single product. Particularly, the precise construction of a Cu microenvironment is a great challenge in the design and fabrication of excellent Cu-based CO 2 RR catalysts. In order to systematically regulate the Cu metal site environment, the classic HKUST-1 containing paddlewheel Cu coordination nodes was used as a template and modified with the atomic layer infiltration (ALI) technique in this work. A detailed structural analysis shows that a uniform distribution of Zn−O−Zn sites is introduced into HKUST-1 and linked to neighboring Cu nodes without changing the original morphology and structure. In comparison with pristine HKUST-1, the FE for CO increases from 20−30% to 70−80% for the ALI-modified HKUST-1 within the tested overpotential range. Density functional theory (DFT) simulations prove that the modification with Zn−O−Zn by ALI enhances the adsorption enthalpy of CO 2 and strengthens the bonding interaction between the COOH* intermediate and the adsorption center, thereby reducing the whole reaction barrier and accelerating CO formation. The proposed ALI technique elucidates the reliance of CO 2 RR selectivity on the Cu microenvironment and provides a platform for regulating the coordination environments of Cu or other metal-based electrocatalysts to facilitate the high selectivity of CO 2 RR in the future.