biostudies-literatureChen JNational Research Foundation Singapore (National Research Foundation-Prime Minister's office, Republic of Singapore)National Natural Science Foundation of China (National Science Foundation of China)10935https://www.ebi.ac.uk/biostudies/studies/S-EPMC12686540biostudies-literatureUnknown16(1)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 Ni₃InC_0.5 nanoparticles, leading to the formation of defective In₂O_3-x overlayers and inverse In₂O_3-x/Ni interfaces, driven by CO₂-induced selective surface oxidation during CO₂ hydrogenation. The synergy between In₂O_3-x overlayers and inverse In₂O_3-x/Ni interfaces facilitates CO₂ adsorption and activation, as well as the following hydrogenation of HCOO^* and CH_xO^* 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 mggcat-1h-1 methanol space-time yield at 260 °C, 5 MPa, and 12000 mLgcat-1h-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.Nature communicationsInverse In<sub>2</sub>O<sub>3-x</sub>/Ni interfaces via Ni<sub>3</sub>InC<sub>0.5</sub> surface reconstruction for efficient CO<sub>2</sub> hydrogenation to methanol.PMC1268654022438010U2102d201122378310U2102d200622178265Tan MChen JZhang HLim KHMa XHan XXiao THe QXi SZi XLi MLv JKawi SHao ZZhang ZTang SYao BJia WYang QWang YfalseInverse In<sub>2</sub>O<sub>3-x</sub>/Ni interfaces via Ni<sub>3</sub>InC<sub>0.5</sub> surface reconstruction for efficient CO<sub>2</sub> hydrogenation to methanol.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 Ni₃InC_0.5 nanoparticles, leading to the formation of defective In₂O_3-x overlayers and inverse In₂O_3-x/Ni interfaces, driven by CO₂-induced selective surface oxidation during CO₂ hydrogenation. The synergy between In₂O_3-x overlayers and inverse In₂O_3-x/Ni interfaces facilitates CO₂ adsorption and activation, as well as the following hydrogenation of HCOO^* and CH_xO^* 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 mggcat-1h-1 methanol space-time yield at 260 °C, 5 MPa, and 12000 mLgcat-1h-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.2025-01-01T00:00:00Z2025 Dec2026-06-05T23:48:28.528Z2026-05-23T03:13:57.814ZS-EPMC126865404136078310.1038/s41467-025-65929-z