Redistribution of Electron Density for Promoting CO2 Conversion Capacity

Abstract

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 CO₂ fixation, a hollow carbon sphere-supported catalyst of Fe_NPs/HCS (Fe_NPs, Fe nanoparticles; HCS, hollow carbon sphere) is facilely designed and fabricated. Excitingly, the experimental and calculation results reveal that Fe_NPs/HCS displays an ultrahigh activity with almost complete conversions in CO₂ cycloaddition, surpassing the performance of Fe_NPs/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 CO₂, 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 CO₂ cycloaddition.