Conversion of Interfacial Chemical Bonds for Inducing Efficient Photoelectrocatalytic Water Splitting.

Abstract

Sp-C-hybridized alkyne bonds present the natural advantages of interacting with metal atoms and have the ability to generate a large number of new catalytic active sites on the surface and the interfaces, thus greatly promoting the efficient progress of various light/electrochemical reactions. In this work, we have successfully fabricated a novel type of interfacial structure containing sp-C-Mo/O bonds and mixed Mo valence states with outstanding catalytic activity and stability for photoelectrocatalytic (PEC) overall water splitting in a wide pH range (0-14), due to the presence of sp-carbon-rich graphdiyne. For example, in alkaline conditions (pH = 14), the overpotentials of oxygen and hydrogen evolution reactions at 10 mA cm-2 are 165 and 8 mV. When being used as an electrolyzer, the cell voltage of this catalyst is only 1.40 V to achieve 10 mA cm-2. The high PEC activity of graphdiyne@molybdenum oxide originates from the conversion of chemical bonds at the sp-C hybrid interface and the coexistence of multivalent states of molybdenum, triggering a large number of catalytic active sites, greatly promoting charge transfer and lowering water dissociation energy.