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Dual-atom catalysts possess a significant potential for promoting CO2 photoreduction to lucrative solar fuels. However, the precise construction of the diatomic sites that simultaneously foster light absorption and catalytic activity is a formidable challenge, as both processes follow distinct pathways in the photocatalyst. Herein, a facile electrostatic-driven self-assembling approach is employed to realize a bifunctional architecture of a diatomic LaNi-Phen (Phenanthroline)/covalent organic framework (COF-5) photocatalyst. The La site acts as an optically active center for the photoinduced generation of carriers, while the Ni site serves as the catalytically active center for highly selective CO2-to-CO reduction enabled by directional charge transfer via COF-5. Density functional theory (DFT) calculations and in-situ characterization reveal the efficient synergistic effect of the La-Ni double-atomic sites, leading to decreased reaction energy barriers of *COOH intermediate and enhanced CO2-to-CO conversion. As a result, in the absence of any additional photosensitizers, a 15.2 times enhancement of the CO2 reduction rate (605.8 µmol·g− 1·h− 1) over that of pristine COF-5 colloid (39.9 µmol·g− 1·h− 1) and an improvement in CO selectivity to 98.2% are achieved. This work presents a novel strategy for integrating optically and catalytically active centers, which results in a diatomic synergy effect enabling high-performance photocatalytic CO2 reduction. more...

Halide perovskite quantum dots (HP QDs) have been widely used in the field of photocatalysis due to their excellent performance. However, the issues of lead toxicity and instability prevent their process in the photocatalysis application. Herein, the lead-free Cs2AgInCl6 perovskite quantum dots (CAIC QDs) are synthesized by the hot-injection method, and CAIC QDs@Ag composites with various Ag loading amounts are self-assembled by adjusting the Cl source in the synthesis process, which is used to improve the CO2 photoreduction efficiency by using the surface plasmon resonance (SPR) effect of Ag nanoparticles. In addition, the surface ligand density of CAIC QDs@Ag composites is regulated by the purification processing treatment to release the influence of organic ligands on the charge transport performance. It is found that the CAIC QDs@Ag composite with the optimal ligands density possesses fast electron transport and effective carrier separation efficiency, which are crucial for the improvement of the photocatalysis reaction. As a result, the CAIC QDs@Ag-2 composite after purification processing achieves the highest yield of 26.4 μmol g−1 and 28.9 μmol g−1 for CO and CH4, respectively, during the CO2 photoreduction process. In addition, there is no significant decline of CO2 photoreduction performance after the photocatalysis cycling test for 9 h, indicating the good stability of the CAIC QDs@Ag composite in the photocatalysis process. more...