Abstract
Producing hydrogen from organic/inorganic hydrides is an innovative clean energy alternative to fossil fuels, addressing the increasing energy demands. Here, we first propose coupled photocatalytic water hydrogen production and N,N-dimethylformamide (DMF, C3H7NO) dehydrogenation technology to obtain high value-added H2 and N,N-dimethylcarbamic acid (C3H7NO2). ZnIn2S4@MIL-125(Ti) nanoheterostructures were synthesized using a simple solvothermal method and resulting in a photocatalytic H2 production rate of 2.135 mmol h−1 g−1 (apparent quantum efficiency at 380 nm was 2.6 %) which is 2.77 times higher than pure ZnIn2S4. Liquid-phase mass spectrometry indicates that the DMF oxidation activity of ZIS@MIL heterojunction is double pure ZnIn2S4 and only microcrystalline CO2 is produced. Isotopes indicate that the production pathway of H2 results from the coupling of the –CHO bond in DMF and the –H in water. The improved photocatalytic activity of the ZnIn2S4@MIL-125(Ti) heterostructure is attributed to facilitating efficient charge carrier transfer and separation and DMF depletion of holes accelerates electron transfer.
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