Harmonizing Nanoparticle Exsolution from Ce‐Sm Oxide Matrix for Stable Methane Dry Reforming

Catalyst deactivation hinders the application of high‐temperature catalysis such as methane dry reforming, where nanoparticle exsolution will likely clear the path. However, the harsh reaction conditions often easily unbalance the exsolution degree, leading to either sintering or insufficient exsolution of metal nanoparticles. Here, we achieve the fabrication of highly dispersed yet exposed Rh nanoparticles exsolved from the Ce‐Sm oxide matrix. Starting from examining the metal‐support interaction of Rh‐CeO2 and Rh‐Sm2O3, the exsolution dynamics of Rh nanoparticles are studied via multiple in‐situ techniques. Rapid exsolution from CeO2 induces Rh sintering and catalytic deactivation, while sluggish exsolution from Sm2O3 results in Rh encapsulation with poor activity. The balanced metal‐support interaction harmonizes the exsolution of Rh nanoparticles from the Ce‐Sm oxide matrix, fabricating an anti‐sintering and coke‐resistant catalyst for methane dry reforming. This work provides insights into the development of catalysts with structural robustness, where the essence lies in the engineering of nanoparticle exsolution.