Room-Temperature Synthesis of Single Iron Site by Electrofiltration for Photoreduction of CO₂ into Tunable Syngas.

Abstract

Developing a convenient and effective method to prepare single-atom catalysts at mild synthetic conditions remains a challenging task. Herein, a voltage-gauged electrofiltration method was demonstrated to synthesize single-atom site catalysts at room temperature. Under regulation of the graphene oxide membrane, a bulk Fe plate was directly converted into Fe single atoms, and the diffusion rate of Fe ions was greatly reduced, resulting in an ultralow concentration of Fe²⁺ around the working electrode, which successfully prevented the growing of nuclei and aggregating of metal atoms. Monatomic Fe atoms are homogeneously anchored on the as-prepared nitrogen-doped carbon. Owing to the fast photoelectron injection from photosensitizers to atomically dispersed Fe sites through the highly conductive supported N-C, the Fe-SAs/N-C exhibits an outstanding photocatalytic activity toward CO₂ aqueous reduction into syngas with a tunable CO/H₂ ratio under visible light irradiation. The gas evolution rates for CO and H₂ are 4500 and 4950 μmol g^-1 h^-1, respectively, and the tunable CO/H₂ ratio is from 0.3 to 8.8. This article presents an efficient strategy to develop the single-atom site catalysts and bridges the gap between heterogeneous and homogeneous catalysts toward photocatalytic CO₂ aqueous reduction into syngas.