Catalyst surface reconstruction under reaction conditions is ubiquitous and crucial for creating unusual active sites, thereby enhancing catalytic performance. Here, we report the surface reconstruction of supported Ni3InC0.5 nanoparticles, leading to the formation of defective In2O3-x overlayers and inverse In2O3-x/Ni interfaces, driven by CO2-induced selective surface oxidation during CO2 hydrogenation. The synergy between In2O3-x overlayers and inverse In2O3-x/Ni interfaces facilitates CO2 adsorption and activation, as well as the following hydrogenation of HCOO* and CHxO* intermediates, enabling efficient methanol synthesis from CO2. Accordingly, the optimized LDH-NiInCAl catalyst achieves an impressive CO2 conversion of 19% with 65% methanol selectivity and 508.4 mg g cat - 1 h - 1 methanol space-time yield at 260 °C, 5 MPa, and 12000 mL g cat - 1 h - 1 , outperforming commercial Cu/ZnO/Al2O3 catalysts. This work showcases how structural evolution and surface reconstruction enhance catalytic performance, providing new insights into the dynamic structure-activity relationship.
Chen et al. (Mon,) studied this question.