Regulation of d‐Band Center of Ruthenium Sites via Electronic Complementary Effect of C60 Fullerene Molecules and Manganese Atoms for Efficient Alkaline Hydrogen Evolution

Abstract Developing advanced electrocatalysts is crucial for alkaline hydrogen evolution reaction (HER). A balance in adsorption energy for each reaction intermediate on the catalyst determines the overall catalytic rate. This balance is closely linked to the d‐band center, which is, in turn, controlled by the electronic structure of the active sites. Herein, C 60 molecules with electron‐withdrawing properties and manganese (Mn) atoms with electron‐donating properties to drive charge redistribution on Ru active sites are strategically utilized. The synergistic and complementary effects of C 60 and Mn regulate the d‐band centers of Ru sites to an optimal position, optimizing both the water adsorption and hydrogen desorption of the synthesized Ru catalysts. The constructed MnRu/C 60 ‐3 catalyst exhibits a low overpotential of 8 mV at 10 mA cm −2 , a large TOF value of 15.5 s −1 , and a high mass activity of 2.39 A mg −1 Ru at an overpotential of 100 mV in 1.0 m KOH. The anion exchange membrane water electrolyzer, assembled with MnRu/C 60 ‐3 as the cathode, demonstrates excellent water electrolysis performance and high stability under industrial operational conditions. This work offers a fresh perspective on catalyst design principles by manipulating the d‐band centers of active sites using two complementary components.