Dual-antenna@reactor with active “hot spots” for full-spectrum driven CO2 cycloaddition studied at single-particle level

Plasmon-enhanced CO 2 cycloaddition is a viable strategy for converting CO 2 into value-added chemicals under mild conditions. However, it remains challenging to construct catalysts with desirable activity and uncover the detailed mechanisms of plasmon-enhanced CO 2 cycloaddition. Herein, dual-antenna@reactor with active “hot spots”, Au@AgPt yolk-shell, was designed and achieved a styrene carbonate (SC) yield of 12257   mmol   g -1 h -1 , which was at least two orders of magnitude higher than reported catalysts. Theoretical and experimental analyses demonstrated that the dual-antenna structure with enriched “hot spots” dramatically enhanced the light-harvesting, generation and transfer of hot carriers, as well as adsorption and activation of styrene oxide (SO) and CO 2 . The spatially specific dual-antenna structure realized full-spectrum harvesting. The nanocavities located between Au yolk and AgPt shell and on AgPt shell served as reaction chambers for reactants enrichment and formed active “hot spots” by plasmon coupling, resulting in the extremely enhanced electric field, approximately 71 and 14 times stronger than AgPt alloy and Au@AgPt core-shell, respectively. Notably, in situ single-particle photoluminescence (PL) quenching proved the effective carrier transfer between Au@AgPt yolk-shell and SO. This study offers guidance for designing plasmonic photocatalysts to enhance CO 2 cycloaddition efficiency.