Inverse In2O3-x/Ni interfaces via Ni3InC0.5 surface reconstruction for efficient CO2 hydrogenation to methanol

作者：Jiyi Chen, Tian‐Tian Xiao, Bingqing Yao, Maoshuai Li, Heng Zhang, Mingwu Tan, Shibo Xi, Shixiong Tang, Wenyan Jia, Qi Yang, Ziwen Hao, Zhenmei Zhang, Kang Hui Lim, Xiaoyu Han, Xiaohui Zi, Yue Wang, Yue Wang, Jing Lv, Qian He, Yong Wang, Yong Wang, Sibudjing Kawi, Xinbin Ma · 发表于：Nature Communications · 年份：2025 · DOI：10.1038/s41467-025-65929-z · 被引用次数：21 · 研究领域：Catalysts for Methane Reforming、Catalysis for Biomass Conversion、CO2 Reduction Techniques and Catalysts

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 $${{\rm{mg}}}{{{\rm{g}}}}_{{{\rm{cat}}}}^{-1}{{{\rm{h}}}}^{-1}$$ methanol space-time yield at 260 °C, 5 MPa, and 12000 $${{\rm{mL}}}{{{\rm{g}}}}_{{{\rm{cat}}}}^{-1}{{{\rm{h}}}}^{-1}$$ , 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. Surface reconstruction during reactions often generates unique active sites that boost catalytic performance. Here, the authors show that supported Ni₃InC₀.₅ nanoparticles undergo CO₂-induced surface oxidation, forming defective In₂O₃₋ₓ layers and inverse In₂O₃₋ₓ/Ni interfaces during CO2 hydrogenation.