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Hydrogen production from photocatalysis via the usage of multicomponent photocatalysts represents a promising pathway for carbon peaking and carbon neutrality, owing to their structural advantages in dealing with the three crucial processes in photocatalysis, namely, light harvesting, charge transfer, and surface redox reactions. We demonstrate the fabrication of a MOF‐based multicomponent photocatalyst, denoted as semiconductor/MOF/cocatalyst, by a one‐pot electrochemical synthetic route. The as‐fabricated multicomponent photocatalyst has a clean interface among the components, leading to close connections that contribute to high‐quality heterojunction and facilitate photogenerated charge transfer and separation, thereby the efficient hydrogen evolution. The hydrogen production rate of the resultant ZrO2/Zr‐MOF/Pt is 1327 μmol ⋅ g−1 ⋅ h−1, which is much higher than that of ZrO2/Zr‐MOF (15 μmol ⋅ g−1 ⋅ h−1) and pure Zr‐MOF (10.1 μmol ⋅ g−1 ⋅ h−1), as well as the photodeposited‐Pt products ZrO2/Zr‐MOF/PtPD (287 μmol ⋅ g−1 ⋅ h−1) and Zr‐MOF/PtPD (192 μmol ⋅ g−1 ⋅ h−1) obtained by the step‐wise synthetic approach. The work gives a good inspiration for the rational design and construction of MOF‐based multicomponent photocatalysts through the one‐pot electrosynthesis. [ABSTRACT FROM AUTHOR]

Metal–organic frameworks (MOFs) represent a novel class of crystalline inorganic–organic hybrid materials with tunable semiconducting behavior. MOFs have potential for application in photocatalysis to produce sustainable solar fuels, owing to their unique structural advantages (such as clarity and modifiability) that can facilitate a deeper understanding of the structure–activity relationship in photocatalysis. This review takes the photocatalytic active sites as a particular perspective, summarizing the progress of MOF‐based photocatalysis for solar fuel production; mainly including three categories of solar‐chemical conversions, photocatalytic water splitting to hydrogen fuel, photocatalytic carbon dioxide reduction to hydrocarbon fuels, and photocatalytic nitrogen fixation to high‐energy fuel carriers such as ammonia. This review focuses on the types of active sites in MOF‐based photocatalysts and discusses their enhanced activity based on the well‐defined structure of MOFs, offering deep insights into MOF‐based photocatalysis. [ABSTRACT FROM AUTHOR]

Abstract: A wide range of light absorption and rapid electron–hole separation are desired for efficient photocatalysis. Herein, on the basis of a semiconductor‐like metal–organic framework (MOF), a Pt@MOF/Au catalyst with two types of metal–MOF interfaces integrates the surface plasmon resonance excitation of Au nanorods with a Pt‐MOF Schottky junction, which not only extends the light absorption of the MOF from the UV to the visible region but also greatly accelerates charge transfer. The spatial separation of Pt and Au particles by the MOF further steers the formation of charge flow and expedites the charge migration. As a result, the Pt@MOF/Au presents an exceptionally high photocatalytic H2 production rate by water splitting under visible light irradiation, far superior to Pt/MOF/Au, MOF/Au and other counterparts with similar Pt or Au contents, highlighting the important role of each component and the Pt location in the catalyst. [ABSTRACT FROM AUTHOR]

Improving the efficiency of electron-hole separation and charge-carrier utilization plays a central role in photocatalysis. Herein, Pt nanoparticles of ca. 3 nm are incorporated inside or supported on a representative metal-organic framework (MOF), UiO-66-NH2, denoted as Pt@UiO-66-NH2 and Pt/UiO-66-NH2, respectively, for photocatalytic hydrogen production via water splitting. Compared with the pristine MOF, both Pt-decorated MOF nanocomposites exhibit significantly improved yet distinctly different hydrogen-production activities, highlighting that the photocatalytic efficiency strongly correlates with the Pt location relative to the MOF. The Pt@UiO-66-NH2 greatly shortens the electron-transport distance, which favors the electron-hole separation and thereby yields much higher efficiency than Pt/UiO-66-NH2. The involved mechanism has been further unveiled by means of ultrafast transient absorption and photoluminescence spectroscopy. [ABSTRACT FROM AUTHOR]