Highly Selective Photocatalytic CO2Reduction to CH4by Ball-Milled Cubic Silicon Carbide Nanoparticles under Visible-Light Irradiation

Abstract

The ultimate goal of photocatalytic CO2 reduction is to achieve high selectivity for a single product with high efficiency. One of the most significant challenges is that expensive catalysts prepared through complex processes are usually used. Herein, gram-scale cubic silicon carbide (3C-SiC) nanoparticles are prepared through a top-down ball-milling approach from low-priced 3C-SiC powders. This facile mechanical milling strategy ensures large-scale production of 3C-SiC nanoparticles with an amorphous silicon oxide (SiOx) shell and simultaneously induces abundant surface states. The surface states are demonstrated to trap the photogenerated carriers, thus remarkably enhancing the charge separation, while the thin SiOx shell prevents 3C-SiC from corrosion under visible light. The unique electronic structure of 3C-SiC tackles the challenge associated with low selectivity of photocatalytic CO2 reduction to C1 compounds. In conjugation with efficient water oxidation, 3C-SiC nanoparticles can reduce CO2 into CH4 with selectivity over 90%.