Interfacial coordination bonds accelerate charge separation for unprecedented hydrogen evolution over S-scheme heterojunction
Inspired by natural photosynthesis,fabricating high-performance S-scheme heterojunction is re-garded as a successful tactic to address energy and environmental issues.Herein,NH2-MIL-125(Ti)/Zn0.5Cd0.5S/NiS(NMT/ZCS/NiS)S-scheme heterojunction with interfacial coordi-nation bonds is successfully synthesized through in-situ solvothermal strategy.Notably,the optimal NMT/ZCS/NiS S-scheme heterojunction exhibits comparable photocatalytic H2 evolution(PHE)rate of about 14876.7 μmol h-1 g-1 with apparent quantum yield of 24.2％at 420 nm,which is signifi-cantly higher than that of recently reported MOFs-based photocatalysts.The interfacial coordina-tion bonds(Zn-N,Cd-N,and Ni-N bonds)accelerate the separation and transfer of photogenerated charges,and the NiS as cocatalyst can provide more catalytically active sites,which synergistically improve the photocatalytic performance.Moreover,theoretical calculation results display that the construction of NMT/ZCS/NiS S-scheme heterojunction also optimize the binding energy of active site-adsorbed hydrogen atoms to enable fast adsorption and desorption.Photoassisted Kelvin probe force microscopy,in-situ irradiation X-ray photoelectron spectroscopy,femtosecond transient ab-sorption spectroscopy,and theoretical calculations provide sufficient evidence of the S-scheme charge migration mechanism.This work offers unique viewpoints for simultaneously accelerating the charge dynamics and optimizing the binding strength between the active sites and hydrogen adsorbates over S-scheme heterojunction.
Interfacial coordination bondS-scheme heterojunctionPhotocatalytic H2 evolutionCharge dynamicsFree energy barrier
万方数据
