Highly Selective Photocatalytic CO2 Reduction to CH4 by Ball-Milled Cubic Silicon Carbide Nanoparticles under Visible-Light Irradiation

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 3C-SiC tackles the challenge associated with low selectivity of photocatalytic CO2 reduction to C-1 compounds. In conjugation with efficient water oxidation, 3C-SiC nanoparticles can reduce CO2 into CH4 with selectivity over 90%.

Automated summary

Gram-scale cubic silicon carbide nanoparticles with amorphous silicon oxide shell and abundant surface states are prepared through a simple mechanical milling approach, which enhances charge separation and prevents corrosion under visible light. The unique electronic properties of 3C-SiC nanoparticles address the challenge of low selectivity in photocatalytic CO2 reduction to C-1 compounds, achieving over 90% selectivity for CH4 production with efficient water oxidation.