Precisely Constructed Silver Active Sites in Gold Nanoclusters for Chemical Fixation of CO2

Abstract

AbstractPrecise control of the composition and structure of active sites in an atom‐by‐atom fashion remains insuperable for heterogeneous catalysts. Here, we introduce tailor‐made catalytic sites for the cycloaddition of CO2 to epoxides achieved by implementing Ag atoms at different levels of liberation in atomically precise Au nanoclusters. Our results reveal that a single open Ag site on the Au19Ag4 cluster improves the ring‐opening of epoxides and sequent CO2 insertion, while the partially exposed Ag site on the Au20Ag1 cluster exhibits a weak affinity for epoxides and poor efficiency for CO2 capture. Structural tunability imparted by the atom‐by‐atom tailoring and unusual atomic charges distributed on Au and Ag atoms of the three clusters seem to be crucial for promoting challenging bond cleavages and formations in the chemical utilization of CO2.