Simultaneous Localization of Electrons/Holes by Surface Cationic Dangling-Bonds/Vacancies for Synergistically Boosting Photocatalytic Activity

)-H thiolation), the reaction rates catalyzed by CdSe or CdS with coexisting cationic dangling bonds and vacancies are elevated to 5.5-63 times, which are much higher than those by CdS or CdSe with only cationic dangling bonds (1.7-25 times). Density functional theory calculations confirm that individual defects lower the rate-determining step barrier, and the dual-defect exhibits the most favorable adsorption energy, effectively bridging the adsorption-activation trade-off. This study clarifies the rational design, creation, function, and application of two coexisting distinct defects on a single-component nanocrystal from both the atomic level and macro-perspective, offers new ways for designing ideal photocatalysts, and provides insightful understandings for the synergy of simultaneous localization of photocarriers in photocatalysis.