Graphitic carbon nitride (g-C3N4) is an actively investigated metal-free photocatalyst for solar energy conversion. However, primary g-C3N4 usually exhibits limited utilization of visible light and fast combination of photoexcited charge carriers, resulting in low photocatalytic H2 evolution activity. Defect-modified g-C3N4 shows much enhanced photocatalytic H2 evolution activity owing to extended light absorption as well as efficient charge separation and transfer. Here, the photocatalyst simultaneously containing nitrogen vacancies and O-doping is successfully developed by using a two-step post-synthetic strategy for photocatalytic H2 evolution, resulting in a greatly-boosted H2 evolution activity (1.69 × 103 μmol g-1 h-1) compared with that of pristine g-C3N4 (1.12 × 102 μmol g-1 h-1). It is believed that the newly developed double-defect strategy may open an avenue toward obtaining molecular level comprehension of the function of a catalyst in photocatalytic H2 evolution and can be extended to the modification of other semiconductors.
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http://dx.doi.org/10.1039/c8cp01986j | DOI Listing |
Langmuir
January 2025
Key Laboratory of Thorium Energy, Chinese Academy of Science Shanghai Institute of Applied Physics, Shanghai 201800, China.
Hydrogen evolution from water, catalyzed by solar energy, is a promising yet challenging endeavor. Small-sized catalysts usually exhibit high utilization and high performance in the hydrogen evolution field. However, the high surface energy tends to make them aggregate.
View Article and Find Full Text PDFJ Hazard Mater
January 2025
Research Center for Carbon-Neutral Environmental & Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China.
Surface defect engineering has been regarded as an appealing strategy to improve photocatalytic performance, but defects are susceptible to inactivation and thus lose their function as active sites. In this study, we successfully tailored and identified the dynamic evolution of surface hydroxyl defects over ZnTi-layered double hydroxide (ZnTi-LDH) photocatalyst. The enrichment of surface hydroxyl electrons and the dynamic circulation of hydroxyl defects result in enhanced separation and transport capabilities of photogenerated carriers, thereby ensuring the perpetual activation of small molecules into •O and •OH.
View Article and Find Full Text PDFChemistry
January 2025
The Hong Kong Polytechnic University, Department of Applied Biology and Chemical Technology, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hong Hom, Hong Kong (P.R. China), 000000, Hong Kong, HONG KONG.
A series of new (donor)₂-donor-π-acceptor (D2-D-π-A) and (acceptor)₂-donor-π-acceptor (A2-D-π-A) organic photosensitizers based on the framework of (Z)-2-cyano-3-(5-(4-(diphenylamino)phenyl)thiophen-2-yl)acrylic acid have been synthesized and characterized. By incorporating groups with different electron-donating or withdrawing abilities, such as dibenzothiophene (DBT), dibenzofuran (DBF), and triazine (TA), into the triphenylamine segment, their photophysical properties have been regulated. Theoretical calculations were used to explore how various donor-acceptor combinations influence their hydrogen production performance.
View Article and Find Full Text PDFNano Converg
January 2025
Department of Energy and Material Engineering, Dongguk University-Seoul, Seoul, 04620, South Korea.
Angew Chem Int Ed Engl
January 2025
Beijing Institute of Technology, School of Chemistry and Chemical Engineering, 8th Liangxiang East Road, Room 829, Eco-Industrial Building, Beijing, 102488, Beijing, CHINA.
The structural isomerism of atomically precise nanoclusters provides a preeminent theoretical model to investigate the structure-property relationships. Herein, we synthesized three bowl-like polyoxometalate (POM)-encapsulated Ag nanoclusters (denoted as {Ag14(Sb3W30)2}-1, {Ag14(Sb3W30)2}-1a, and {Ag14(Sb3W30)2}-2) via a facile one-pot solvothermal approach. Among them, for the first time, an unprecedented isomeric {Ag14}10+ nanoclusters are obtained in polyoxoanions {Ag14(Sb3W30)2}-1 and {Ag14(Sb3W30)2}-2, which should be probably induced by the different distribution of coordinating O atoms in two isomeric bowl-like {Sb3W30} ligands.
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