Redistribution\nof Electron Density for Promoting CO<sub>2</sub> Conversion Capacity

There is a need to design substrate-supported catalysts\nfor the\nheterogeneous fields, especially with large porosity, which can facilitate\nmass transport. Herein, aiming at enhancing the performance of CO<sub>2</sub> fixation, a hollow carbon sphere-supported catalyst of Fe<sub>NPs</sub>/HCS (Fe<sub>NPs</sub>, Fe nanoparticles; HCS, hollow carbon\nsphere) is facilely designed and fabricated. Excitingly, the experimental\nand calculation results reveal that Fe<sub>NPs</sub>/HCS displays\nan ultrahigh activity with almost complete conversions in CO<sub>2</sub> cycloaddition, surpassing the performance of Fe<sub>NPs</sub>/CS\n(CS, carbon sphere); this demonstrates that the HCS plays a key role,\nwhich may be attributed to the hollow structure tuning the electron\ndensity and enhancing the enrichment of the substrate and CO<sub>2</sub>, consequently lowering the barrier associated with mass transfer.\nThe work not only provides a novel strategy to construct an efficient\ncatalyst but also proposes, for the first time, an electron redistribution\ntactic to influence the catalytic process for CO<sub>2</sub> cycloaddition.