Abstract
AbstractThe visible light‐driven transformation of chemical compounds in combination with the liberation of H2 is highly attractive. Herein, we report on a photocatalyst that allows the acceptorless dehydrogenation of benzylamine. Upon light absorption, free charge carriers are generated and used for the concerted imine formation and liberation of H2. Our photocatalyst consists of CdS as a light harvesting semiconductor supported on colloidal metal‐organic framework crystallites. The decoration with co‐catalytic nickel nanoparticles promotes hydrogen evolution and, in addition, stabilizes the CdS component under irradiation.
Highlights
The solar-driven upgrading of organic compounds is a promising and sustainable way to produce value-added products.[1]The simultaneous liberation of H2 during such upgrading processes generates an additional, highly attractive byproduct.a well investigated approach is the photocatalytic acceptorless dehydrogenation of alcohols to yield carbonyl compounds (Scheme 1, top).[2]
The visible light-mediated aerobic amine oxidation is catalyzed by semiconductor materials including CdS,[3] graphitic carbon nitride,[4] Nb2O5,[5] WS2,[6] WO3[7]
Ni/CdS@MIL-101 is composed of three components. a) The metal organic framework (MOF) known as MIL-101(Cr) is used as the visible light inactive support material that acts as a molecular sponge permitting the semiconductor and catalyst synthesis and determines the overall size of the photocatalyst for efficient recycling.[14] b) CdS is the visible light absorbing semiconductor material. c) Nickel nanoparticles are an efficient
Summary
The solar-driven upgrading of organic compounds is a promising and sustainable way to produce value-added products.[1]. A) The metal organic framework (MOF) known as MIL-101(Cr) is used as the visible light inactive support material that acts as a molecular sponge permitting the semiconductor and catalyst synthesis and determines the overall size of the photocatalyst for efficient recycling.[14] b) CdS is the visible light absorbing semiconductor material. (η3-Allyl)(η5cyclopentadienyl)-palladium(II) [Pd(C3H5)(C5H5)] was used to generate 5 wt.% Pd0 nanoparticles by sublimation at 32 °C in dynamic vacuum and reduction at 70 °C and 70 bar H2.[19] The modification with 5 wt.% Pt0 proceeds via the gas phase loading of trimethyl-(methylcyclopentadienyl)-palladium(IV) [Me3Pt(CH3C5H4)] into the pores of CdS@MIL-101 at 37 °C in static vacuum, followed by a reduction step at 80 °C and 50 bar H2.[20] TEM analysis (Scheme 2; Supporting Information, Figure S3) indicated a homogeneous distribution of metallic nanoparticles smaller than 2 nm which are located on the CdS particles, forming an interface with the visible light-absorbing semiconducting material. DFT calculations suggest a stronger substrate binding of the amine to the Ni than to Pd nanoparticles
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