Regulating the metal‐support interaction of highly efficient Ni/ <scp>TUD</scp> ‐1 catalysts for low‐temperature <scp> CO ₂ </scp> methanation

Abstract Metal‐support interaction (MSI) imposes significant influences on the performance of CO 2 methanation; however, its precise regulation remains confusing. Herein, we design two Ni cooperated with mesoporous TUD‐1 catalysts differing in strength of MSI to investigate the relationship between their structure and activity. It is found that the optimal Ni/TUD‐1‐GEL catalyst prepared by a gel‐assisted one‐pot synthesis method possesses a smaller particle size. Additionally, its moderate MSI restrains the migration and coalescence of active species. This ultimately results in a superior performance with CO 2 conversion of 65.4% without evident deactivation for 156 h on stream at an ultra‐low temperature of 225°C, which is one of the best performances of catalysts in published works under the given conditions. In situ diffuse reflectance infrared Fourier transforms reveal that CO 2 is sequentially converted into formate and carbonate and, finally, CH 4 . Moreover, the formation and evolution of the active phase during catalyst synthesis and reaction processes are probed by in situ x‐ray diffraction.