ACS Catalysis · 2019 · 94 citations · 37 references
Natural SciencesChemical EngineeringChemistryCatalysisGreen ChemistryRedox BiochemistryCatalytic MechanismsPhotocatalysisPhotochemical SynthesisPhotochemistryPhotoelectrochemistryRedox-active MaterialsConduction BandPhotocatalytic MaterialsPhotocatalytic OxidationPhotocatalytic SynthesisPhotochemical Redox ReactionsSolar Energy StorageTandem ReactionsVisible-light Photocatalysis
Photocatalytic H2 evolution from organic feedstocks with simultaneous utilization of photogenerated holes achieves solar energy storage and coproduces value-added chemicals. Here we show visible-light H2 production from benzyl alcohol (BAL) with controllable generation of deoxybenzoin (DOB) or benzoin (BZ) through tandem redox reactions. Particularly, DOB synthesis circumvents the use of expensive feedstocks and environmentally unfriendly catalysts that are required previously. Under the irradiation of blue LEDs, the key of steering the major product to DOB rather than BZ is to decrease the conduction band bottom potentials of the ZnIn sulfide catalysts by increasing the Zn/In ratio, which results in the dehydration of intermediate hydrobenzoin (HB) to DOB proceeding in a redox-neutral mechanism and consuming an electron–hole pair. As a proof of concept, this method is used to synthesize DOB derivatives in gram scale.
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