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Abstract
Bimetallic zeolite-imidazole frameworks with controllable flat band position, band gap and hydrogen evolution reaction characteristics were adopted as a photocatalytic hydrogen production catalyst. Furthermore, the g-C3N4–MoS2 2D–2D surface heterostructure was introduced to the ZnM-ZIF to facilitate the separation as well as utilization efficiency of the photo-exited charge carriers in the ZnM-ZIFs. On the other hand, the ZnM-ZIFs not only inhibited the aggregation of the g-C3N4–MoS2 heterostructure, but also improved the separation and transport efficiency of charge carriers in g-C3N4–MoS2. Consequently, the optimal g-C3N4–MoS2–ZnNi-ZIF exhibited an extraordinary photocatalytic hydrogen evolution activity 214.4, 37.5, and 3.7 times larger than that of the pristine g-C3N4, g-C3N4–ZnNi-ZIF and g-C3N4–MoS2, respectively, and exhibited a H2-evolution performance of 77.8 μmol h−1 g−1 under UV-Vis light irradiation coupled with oxidation of H2O into H2O2. This work will furnish a new MOF candidate for photocatalysis and provide insight into better utilization of porous MOF-based heterostructures for hydrogen production from pure water.
Highlights
powder X-ray diffraction (PXRD) pattern justi ed the successful g-C3N4–ZnMZIF–MoS2 heterostructure formation at rst and reduction of peak shows that material a er hetero-structure composite is 2D material which is amorphous in nature
Fourier Transform Infrared Spectroscopy (FTIR) spectra were further employed for con rming the formation of g-C3N4–ZnMZIF heterostructures
The systematic comparison of photocatalytic hydrogen production activity g-C3N4, g-C3N4–MoS2, ZnM-Zeolite Imidazole Frameworks (ZIFs) is showed in Fig. 3b and S10.† Under UV-Vis light irradiation, the pristine g-C3N4 and ZnNi-ZIF exhibited very limited hydrogen production rate of only 0.71 and 0.92 mmol hÀ1, respectively, and the adoption of MoS2 and ZnNi-ZIF both dramatically increased the hydrogen production rate of g-C3N4 due to the utilization and transport efficiency improving of the charge carriers, respectively
Summary
The direct conversion of sustainable solar power into ecofriendly energy over high performance photocatalysts has been extremely signi cant for powering human society.[1,2,3,4,5,6,7] Up to now, it is universally recognized that the serious recombination, underutilization and poor transport of photon-generated carriers weaken the photocatalytic activity of the photocatalyst.[8,9,10,11,12] extensive efforts have been devoted to constructing heterostructures or phase junctions, which could increase the speci c surface area of the photocatalyst,[2,13,14,15,16,17,18,19,20,21] and adopting a suitable cocatalyst for improving the separation, transport and utilization of the photo-induced charge carriers.[10,11,22,23] most of the photocatalyst systems were composed of inorganic metal oxides/sul des, which may result in poor transport and separation efficiency of charge carriers, low porosity, and limited exibility in material design.
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