Two-dimensional PdMo curved nanosheets for tunable CO2 electrocatalytic reduction to syngas

Summary Syngas (CO/H2) is an essential industrial feedstock. Electroreduction of CO2 to syngas is a desirable solution to energy and environmental challenges. Two-dimensional (2D) nanomaterials have been identified as promising electrocatalysts in CO2 reduction reactions (CO2RRs). Here, we report 2D PdMo curved nanosheets (PdMo CNSs) as the electrocatalyst for efficient, tunable, selective, and stable electroreduction of CO2 to syngas. The H2/CO ratio is tunable from 0.15:1 to 4:1. The current density can be as high as 65.6 mA cm–2 with a H2/CO ratio of 1:1. Density functional theory calculations illustrate that alloying Mo can optimize the electronic structure around Pd and significantly reduce the kinetic energy barrier, thus improving the migration ability of CO∗ and enhancing the anti-poisoning performance of the electrode to achieve more stable CO2 electroreduction. This work offers a strategy for developing new metal-based 2D nanomaterial electrocatalysts for efficient catalysis of CO2 to syngas.