Redistribution of Electron Density for Promoting CO Conversion Capacity.

There is a need to design substrate-supported catalysts for the heterogeneous fields, especially with large porosity, which can facilitate mass transport. Herein, aiming at enhancing the performance of CO fixation, a hollow carbon sphere-supported catalyst of Fe/HCS (Fe, Fe nanoparticles; HCS, hollow carbon sphere) is facilely designed and fabricated. Excitingly, the experimental and calculation results reveal that Fe/HCS displays an ultrahigh activity with almost complete conversions in CO cycloaddition, surpassing the performance of Fe/CS (CS, carbon sphere); this demonstrates that the HCS plays a key role, which may be attributed to the hollow structure tuning the electron density and enhancing the enrichment of the substrate and CO, consequently lowering the barrier associated with mass transfer. The work not only provides a novel strategy to construct an efficient catalyst but also proposes, for the first time, an electron redistribution tactic to influence the catalytic process for CO cycloaddition.