Abstract

AbstractSolar‐driven photocatalytic conversion of carbon dioxide (CO2) into carbon‐neutral fuels is of significance for energy sustainability. The critical challenges in this process are high charge carrier recombination and low CO2 adsorption capacity. Here, by integrating porous covalent triazine frameworks (CTFs) with cadmium sulfide (CdS) nanospheres, a CdS@CTF‐HUST‐1 heterojunction photocatalyst with core–shell structure is developed for CO2‐to‐CO conversion. Experimental investigations combined with density functional theory simulations reveal that the formation of an internal electric field provides the driving force for accelerating S‐scheme charge transfer, resulting in enhanced separation and utilization efficiency of charge carriers in photocatalysis. Together with the improved CO2 adsorption capacity contributed by the porous structure of the CTF‐HUST‐1 shell, the CdS@CTF‐HUST‐1 heterojunction photocatalyst gives an impressive CO yield rate of 168.77 µmol g−1 h−1 with high selectivity. This research furnishes a feasible strategy to construct highly active core–shell composite photocatalysts for optimizing CO2 adsorption and conversion.

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