Electrochemical Reduction of Carbon Dioxide to Methanol on Hierarchical Pd/SnO2 Nanosheets with Abundant Pd–O–Sn Interfaces

Electrochemical conversion of CO2 into fuels using electricity generated from renewable sources helps to create an artificial carbon cycle. However, the low efficiency and poor stability hinder the practical use of most conventional electrocatalysts. In this work, a 2D hierarchical Pd/SnO2 structure, ultrathin Pd nanosheets partially capped by SnO2 nanoparticles, is designed to enable multi‐electron transfer for selective electroreduction of CO2 into CH3OH. Such a structure design not only enhances the adsorption of CO2 on SnO2, but also weakens the binding strength of CO on Pd due to the as‐built Pd–O–Sn interfaces, which is demonstrated to be critical to improve the electrocatalytic selectivity and stability of Pd catalysts. This work provides a new strategy to improve electrochemical performance of metal‐based catalysts by creating metal oxide interfaces for selective electroreduction of CO2. Elektrochemische CO2‐Umwandlung: Eine Pd/SnO2‐Struktur aus ultradünnen, partiell mit SnO2‐Nanopartikeln bedeckten Pd‐Nanoschichten ermöglicht Multielektronentransfer für die Elektroreduktion von CO2 zu CH3OH. Die verstärkte Adsorption von CO2 auf der SnO2‐Oberfläche, die richtige Bindung von CO an Pd und die Pd‐O‐Sn‐Grenzflächen sind entscheidend für die elektrokatalytische Selektivität und Stabilität.