Improving CO2 photoconversion with ionic liquid and Co single atoms

Abstract

Photocatalytic CO₂ conversion promises an ideal route to store solar energy into chemical bonds. However, sluggish electron kinetics and unfavorable product selectivity remain unresolved challenges. Here, an ionic liquid, 1-ethyl-3-methylimidazolium tetrafluoroborate, and borate-anchored Co single atoms were separately loaded on ultrathin g-C₃N₄ nanosheets. The optimized nanocomposite photocatalyst produces CO and CH₄ from CO₂ and water under UV-vis light irradiation, exhibiting a 42-fold photoactivity enhancement compared with g-C₃N₄ and nearly 100% selectivity towards CO₂ reduction. Experimental and theoretical results reveal that the ionic liquid extracts electrons and facilitates CO₂ reduction, whereas Co single atoms trap holes and catalyze water oxidation. More importantly, the maximum electron transfer efficiency for CO₂ photoreduction, as measured with in-situ μs-transient absorption spectroscopy, is found to be 35.3%, owing to the combined effect of the ionic liquid and Co single atoms. This work offers a feasible strategy for efficiently converting CO₂ to valuable chemicals.