The development of bifunctional photocatalysts for enhancing hydrogen (H) and hydrogen peroxide (HO) production from water is essential in addressing environmental and energy issues. However, the practical implementation of photocatalytic technology is still constrained by the inadequate separation of photo-generated charge carriers. Herein, potassium (K) atoms are introduced into the interlayers of graphitic carbon nitride (g-CN) with a hollow hexagonal structure (K-TCN) and are coordinated with N atoms in adjacent layers. The presence of K-N coordination serves as a layer bridge, facilitating the separation of charge carriers. The hollow hexagonal structure reduces the distance over which photogenerated electrons migrate to the surface, thereby enhancing the reaction kinetics. Consequently, the optimized K-TCN exhibits a dramatically improved photocatalytic H (941.6 μmol gh with platinum (Pt) as the cocatalyst) and HO (347.6 μmol gh) generation as compared to hollow g-CN (TCN) and bulk g-CN nanosheet (CN) without K-N bridge under visible light irradiation. The unique design holds promising potential for developing highly efficient bifunctional photocatalysts towards producing renewable fuels and value-added chemicals.
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http://dx.doi.org/10.1016/j.jcis.2023.08.181 | DOI Listing |
Org Biomol Chem
January 2025
State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
We report the first example of photocatalytic acceptorless dehydrogenation using cationic Eosin Y as a bifunctional photocatalyst, without metal catalysts or HAT reagents. Under Bayesian optimized conditions, a wide range of flavones were synthesized in moderate to excellent yields, many of which were reported with biological activities. Mechanistic studies suggest that flavones likely form through two HAT processes, with hydrogen release occurring photoredox.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
Laboratory of Alternative Energy Conversion Systems, Department of Mechanical Engineering, School of Engineering, University of Thessaly, Pedion Areos 38834, Greece. Electronic address:
The coupling of carbon dioxide (CO) with epoxides to produce cyclic carbonates is a desirable decarbonization approach, but its commercial applicability is still restricted by the costly catalysts required, as well as the need for high temperature and high pressure. Herein, oxygen vacancy-rich defective tungsten oxide (WO) rich in Lewis acid sites was modified by Prussian blue (PB), and the obtained composite reaches up to 94 % styrene carbonate yield (171 mmol gh) at ambient temperature and pressure, exhibiting outstanding advantages in the photocatalytic CO cycloaddition reaction compared with currently reported photocatalysts. It is found that the introduction of PB with photothermal properties significantly enhances the capability of WO to absorb and activate CO and epoxide, along with its light utilization ability.
View Article and Find Full Text PDFInorg Chem
December 2024
Henan Key Laboratory of Polyoxometalate Chemistry, College of Chemistry and Molecular Sciences, Henan University, Kaifeng, Henan 475004, P. R. China.
Amide compounds are widely present in drug molecules and natural products, which can be synthesized by acid-amine condensation. It is urgent to design new photocatalysts for achieving both nitroaromatic reduction and C-H oxidation to obtain raw materials, carboxylic acids, and aromatic amines. Herein, a novel isopolymolybdate-incorporated photoactive metal-organic framework, -TPT, was constructed by combining the oxidation catalyst [MoO], Ni(II) cation, and photosensitive ligand 2,4,6-tri(4-pyridyl)-1,3,5-triazine (TPT).
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
College of Chemistry, Zhengzhou University, Zhengzhou 450001, P. R. China.
Programming and synthesizing bifunctional materials for regulating the output of triboelectric nanogenerators (TENGs) and their photocatalytic efficiency is a promising strategy for energy harvesting to build self-powered systems. Herein, we tackle this challenge by introducing metal-organic frameworks (MOFs) as molecular catalysts and triboelectric layers for self-powered photocatalytic systems. A zeolite-like mixed-valence MOF () and a ladder-structured MOF () were obtained through structural transformation.
View Article and Find Full Text PDFNanoscale
December 2024
Key Laboratory of Applied Surface and Colloid Chemistry (Shaanxi Normal University), Ministry of Education, Xi'an, 710062, P. R. China.
Improving the rate performance is of great significance to achieve high-performance photo-assisted Li-O batteries for developing new optimized bifunctional photocatalysts. Herein, a holey etching strategy is developed to prepare porous siloxene nanosheets with a size of 10 nm and few layers (P-siloxene NSs) by a modified Ag-assisted chemical etching method, and the optimized pore-forming conditions are: Ag ion concentration 0.01 mol dm, HF concentration 0.
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