Synergistic interaction of heteroatomic PtCu dual single-atom sites for boosting artificial photosynthesis of CH3OH

Pt Cu dual single-atom catalysts were developed for artificial photosynthesis of CH 3 OH. • Dual sites synergy: Cu promotes CO 2 activation and *CHO formation; Pt accelerates H 2 O dissociation for proton supply. • Pt Cu dual sites synergistically enhance electron transport dynamics and photogenerated carrier separation efficiency. • PtCu-DA/BOBC achieves 16.21 μmol·g −1 ·h −1 CH 3 OH yield with 96.3% electron selectivity. The rational design of photocatalysts with spatially separated dual active sites is a promising strategy to overcome the efficiency bottlenecks of artificial photosynthesis, but it remains a significant challenge. Herein, we design a dual-active site constructed from the Cu atom and Pt atom decorated on the facet junction of BiOBr 1-x Cl x (BOBC) nanosheets. This design leverages the inherently high atomic utilization and the distinct synergistic effect of PtCu dual single-atom (PtCu-DA) sites, where the Cu atoms serve as the primary sites for CO 2 adsorption and activation, while the adjacent Pt atoms function as catalytic centers for H 2 O dissociation, ensuring a steady proton supply for subsequent hydrogenation steps. Benefiting from this spatial division of labor, the optimal PtCu-DA/BOBC possesses a promising catalytic performance for CO 2 photoreduction to CH 3 OH (16.21 μmol·g −1 ·h −1 ) with 96.3% electron selectivity, significantly outperforming its single-atom photocatalysts. Mechanistic studies reveal that the synergistic interaction between Pt and Cu not only enhances the charge carrier dynamics but also lowers the energy barriers for both CO 2 activation and H 2 O dissociation. This work provides deep insights into the atomic-level engineering of material interfaces for efficient solar fuel production. Download: Download high-res image (70KB) Download: Download full-size image