LAUSR

CO2 hydrogenation to formic acid/formate has been recognized as a key reaction to realizing the CO2‐mediated hydrogen energy cycle. Herein, ultrafine and well‐dispersed Pd−CoO nanoparticles (∼1.8 nm) were encapsulated within mesoporous silica nanospheres (MSNs) via a facile one‐pot ligand‐protected synthesis strategy. The MSN‐encaged bimetallic nanocatalysts exhibit excellent catalytic activity and stability for the formate production from CO2 hydrogenation, showing high turnover frequency value up to 1824 h−1 at 373 K, which is among the top‐level reported for heterogeneous catalysts.