Constructing Cu1-Ti dual sites for highly efficient photocatalytic hydrogen evolution

Constructing dual sites is promising to break scaling relations between the adsorption energetics of reaction intermediates and ultimately improves the activity and selectivity due to the synergistic effect. However, it is a grand challenge to precisely form a dual-site configuration with one metal site adjacent to another active site. Loading single atoms onto oxides with pre-introduction of surface oxygen vacancies may be an alternative strategy to overcome such challenge. Motivated by our theoretical calculations that the dual sites formed by single Cu atoms and unsaturated Ti sites on TiO 2 enables a higher activity towards hydrogen evolution from water splitting than corresponding single site, we successfully synthesized a Cu 1 -Ti dual-site catalyst by depositing Cu single atoms on TiO 2 nanoparticles with abundant surface oxygen vacancies. The designed target catalyst significantly outperforms the benchmark Pt nanoparticle decorated TiO 2 with a high and stable activity towards photocatalytic hydrogen production. • Theoretical calculations revealed that Ovs and single Cu atoms respectively promote water dissociation and hydrogen formation, synergistically providing active sites to catalyze hydrogen production. • The designed target catalyst exhibited extraordinarily high activity and excellent stability for photocatalytic hydrogen evolution. • The developed method provide a paradigm that precisely combines single metal atoms with substrate unsaturated metal sites to generate highly active dual sites.