“…The apparent peak attributable to the Co–O scattering path in the Fe-CoMoB active layer demonstrates the oxidation effect during the modification process, and the decreased amplitude of the Co–Co and Co–Mo paths indicate the appearance of Co site defects. , The EXAFS fitting analysis at the Co K-edge indicates the decreasing of the Co coordination number in Fe-CoMoB compared with CoMoB, which further demonstrates that the electrochemical modification induces multiple Co vacancy sites (Table S2). To sum up, as for the unmodified CoMoB active layer, element B acts as an electron donor to generate electron-rich Co, and Mo provides a small amount of oxygen vacancies in the form of high-valent oxides, which plays as electron promoter to transfer electrons to surface Co atoms. , By further electrochemical modification, the introduction of Fe elements intensifies the electron enrichment of Co, and a large number of Co and O vacancies are introduced through the directional migration of atoms . The above increases the number of catalytic active sites and electronic modulation of metallic sites (Co), and the effective kinetic activation of H 2 O on the electron-rich Co allows an easier dissociation into OH and H, which is the rate-determining step of a reaction step of AB hydrolysis. , The above multilevel synergistic from electron transfer to vacancy generation to micromorphology leads to a significant performance enhancement of the Fe-CoMoB active layer, providing an ∼3-fold catalytic activity in hydrolytic dehydrogenation of AB (Figure S8).…”