We demonstrate the rational design and construction of sandwich-like ZnInS-InO hierarchical tubular heterostructures by growing ZnInS nanosheets on both inner and outer surfaces of InO microtubes as photocatalysts for efficient CO photoreduction. The unique design integrates InO and ZnInS into hierarchical one-dimensional (1D) open architectures with double-heterojunction shells and ultrathin two-dimensional (2D) nanosheet subunits. This design accelerates the separation and transfer of photogenerated charges, offers large surface area for CO adsorption, and exposes abundant active sites for surface catalysis. Benefiting from the structural and compositional merits, the optimized ZnInS-InO photocatalyst exhibits outstanding performance for reductive CO deoxygenation with considerable CO generation rate (3075 μmol h g) and high stability.
Here we demonstrate the delicate design and construction of hierarchical Co 9 S 8 @ZnIn 2 S 4 heterostructured cages as an efficient photocatalyst for hydrogen evolution with visible light. Two photoactive sulfide semiconductors are rationally integrated into a hierarchical hollow structure with strongly coupled heterogeneous shells and two-dimensional ultrathin subunits. The unique architecture can efficiently facilitate the separation and transfer of light-induced charges, offer large surface area, and expose rich active sites for photocatalytic redox reactions. Owing to the distinctive structural and compositional benefits, the hierarchical Co 9 S 8 @ZnIn 2 S 4 hollow heterostructures without using any cocatalysts show remarkable activity with a hydrogen-producing rate of 6250 μmol h -1 g -1 and high stability for photocatalytic water splitting.
We demonstrate rational design and fabrication of hierarchical InS-CdInS heterostructured nanotubes as efficient and stable photocatalysts for visible light CO reduction. The novel self-templated strategy, including sequential anion- and cation-exchange reactions, integrates two distinct sulfide semiconductors into hierarchical tubular hybrids with homogeneous interfacial contacts and ultrathin two-dimensional (2D) nanosheet subunits. Accordingly, the hierarchical heterostructured nanotubes facilitate separation and migration of photoinduced charge carriers, enhance the adsorption and concentration of CO molecules, and offer rich active sites for surface redox reactions. Benefiting from these structural and compositional features, the optimized hierarchical InS-CdInS nanotubes without employing noble metal cocatalysts in the catalytic system manifest remarkable performance for deoxygenative reduction of CO with high CO generation rate (825 μmol h g) and outstanding stability under visible light irradiation.
Metal-organic frameworks (MOFs) have shown great promise for CO2 capture and storage. However, the operation of chemical redox functions of framework substances and organic CO2 -trapping entities which are spatially linked together to catalyze CO2 conversion has had much less attention. Reported herein is a cobalt-containing zeolitic imidazolate framework (Co-ZIF-9) which serves as a robust MOF cocatalyst to reduce CO2 by cooperating with a ruthenium-based photosensitizer. The catalytic turnover number of Co-ZIF-9 was about 450 within 2.5 hours under mild reaction conditions, while still keeping its original reactivity during prolonged operation.
Metal-organic frameworks (MOFs) have attracted significant research attention in diverse areas due to their unique physical and chemical characteristics that allow their innovative application in various research fields. Recently, the application of MOFs in heterogeneous photocatalysis for water splitting, CO2 reduction, and organic transformation have emerged, aiming at providing alternative solutions to address the world-wide energy and environmental problems by taking advantage of the unique porous structure together with ample physicochemical properties of the metal centers and organic ligands in MOFs. In this review, the latest progress in MOF-involved solar-to-chemical energy conversion reactions are summarized according to their different roles in the photoredox chemical systems, e.g., photocatalysts, co-catalysts, and hosts. The achieved progress and existing problems are evaluated and proposed, and the opportunities and challenges of MOFs and their related materials for their advanced development in photocatalysis are discussed and anticipated.
Ternary boron carbon nitride (BCN) semiconductors have been developed as emerging metal-free photocatalysts for visiblelight reduction of CO 2 , but the achieved efficiency is still not satisfying. Herein, we report that the CO 2 photoreduction performance of a bulk BCN semiconductor can be substantially improved by surface engineering with CdS nanoparticles. The CdS/BCN photocatalysts are characterized completely by diverse tests (e.g., XRD, FTIR, XPS, DRS, SEM, TEM, N 2 sorption, PL, and transient photocurrent spectroscopy). Performance of the CdS/BCN heterostructures is evaluated by reductive CO 2 conversion reactions with visible light under benign reaction conditions. Compared with bare BCN material, the optimized CdS/BCN photocatalyst exhibits a 10-fold-enhanced CO 2 reduction activity and high stability, delivering a considerable CO production rate of 12.5 μmol h −1 (250 μmol h −1 g −1 ) with triethanolamine (TEOA) as the reducing agent. The reinforced photocatalytic CO 2 reduction activity is mainly assigned to the obviously improved visible-light harvesting and the greatly accelerated separation/transport kinetics of light-triggered electron−hole pairs. Furthermore, a possible visible-light-induced CO 2 reduction mechanism is proposed on the basis of photocatalytic and photo(electro)chemical results.
Rational design and synthesis of highly active and robust bifunctional non‐noble electrocatalysts for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are urgently required for efficient rechargeable metal–air batteries. Herein, abundant MnO/Co heterointerfaces are engineered in porous graphitic carbon (MnO/Co/PGC) polyhedrons via a facile hydrothermal‐calcination route with a bimetal–organic framework as the precursor. The in situ generated Co nanocrystals not only create well‐defined heterointerfaces with high conductivity to overcome the poor OER activity but also promote the formation of robust graphitic carbon. Owing to the desired composition and formation of the heterostructures, the resulting MnO/Co/PGC exhibits superior activity and stability toward both OER and ORR, which makes it an efficient air cathode for the rechargeable Zn–air battery. Importantly, the homemade Zn–air battery is able to deliver excellent performance including a peak power density of 172 mW cm−2 and a specific capacity of 872 mAh g−1, as well as excellent cycling stability (350 cycles), outperforming commercial mixed Pt/C||RuO2 catalysts. This work highlights the synergy from heterointerfaces in oxygen electrocatalysis, thus providing a promising approach for advanced metal–air cathode materials.
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