Ultrathin Two-Dimensional PdMo Curved Nanosheets for Tunable CO 2 Electrocatalytic Reduction to Syngas

Syngas (CO/H2) is an essential industrial feedback. 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 reaction (CO2RR). Herein, a novel 2D PdMo curved nanosheets (PdMo CNSs) was designed for selective, efficient and stable electroreduction of CO2 to syngas. The H2/CO ratio are 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 enhance the anti-poisoning performance of the electrode to achieve more stable CO2 electroreduction. This work offers a strategy of developing new metal-based 2D nanomaterial electrocatalysts for efficient catalyzing CO2 toward syngas.