Improving metal loading and controlling the coordination environment is nontrivial and challenging for single‐atom catalysts (SACs), which have the greatest atomic efficiency and largest number of interface sites. In this study, a matching bidentate ligand (MBL) anchoring strategy is designed for the construction of CuN4 SACs with tunable coordination environments (Cu loading range from 0.4 to15.4 wt.%). The obtained Cu SA/ZIF and Cu SA/ZIF* (0.4 wt.%) (ZIF and ZIF* = Zeolitic imidazolate framework with Matching bidentate N‐ligands) nanocomposites exhibit superior performance in homo‐coupling of phenyl acetylene under light irradiation (TON = 580, selectivity > 99%), which is 22 times higher than that of Cu SA/NC‐800 (NC = N‐doped porous carbon). Experiments and density functional theory calculations confirmed that the specific Cu five‐membered ring formed using the MBL anchoring strategy is the key to the immobilization of isolated Cu atoms. This strategy provides a basis for the construction of M SA/MOF, which has the potential to narrow the gap between experimental and theoretical catalysis, as further confirmed by the successful preparation of Fe SA/ZIF and Ni SA/ZIF.
Developing non-noble metal photocatalysts for efficient photocatalytic hydrogen evolution is crucial for exploiting renewable energy. In this study, a photocatalyst of Ni2P/CdS nanorods consisting of cadmium sulfide (CdS) nanorods (NRs) decorated with Ni2P nanoparticles (NPs) was fabricated using an in-situ solvothermal method with red phosphor (P) as the P source. Ni2P NPs were tightly anchored on the surface of CdS NRs to form a core-shell structure with a well-defined heterointerface, aiming to achieve a highly efficient photocatalytic H2 generation. The as-synthesized 2%Ni2P/CdS NRs photocatalyst exhibited the significantly improved photocatalytic H2 evolution rate of 260.2 μmol∙h−1, more than 20 folds higher than that of bare CdS NRs. Moreover, the as-synthesized 2%Ni2P/CdS NRs photocatalyst demonstrated an excellent stability, even better than that of Pt/CdS NRs. The photocatalytic performance enhancement was ascribed to the core-shell structure with the interfacial Schottky junction between Ni2P NPs and CdS NRs and the accompanying fast and effective photogenerated charge carriers’ separation and transfer. This work provides a new strategy for designing non-noble metal photocatalysts to replace the noble catalysts for photocatalytic water splitting.
Construction of heterojunction at the atomic scale to ensure efficient charge separation for improvement of photocatalytic water splitting is challenging. Herein, a facile hydrothermal method has been applied for the in situ fabrication of TiO 2 /SrTiO 3 heterojunction, using the monolayer Ti 3 C 2 MXene as the template and reactant. It is found that the sample with the hydrothermal reaction time of 60 min exhibits the highest H 2 evolution rate with the sacrificial reagent, due to the efficient charge separation of TiO 2 /SrTiO 3 heterojunction as Ti 3 C 2 derivative. In addition, the sample shows the best overall water splitting performance at a hydrothermal reaction time of 120 min, where TiO 2 is nearly converted to SrTiO 3 , due to the fast kinetic process and low structural defects of SrTiO 3 . This work not only provides a simple strategy for the fabrication of heterojunction photocatalysts but also demonstrates the difference in optimization of half-reaction and overall water splitting reaction.
Ferroelectric built-in electric fields were used for photocatalytic air purification, where the stretched PVDF dramatically enhances and stabilizes active adsorption sites.
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