While photocatalytic water-splitting is a promising alternative energy source, low photocatalytic efficiencies in the visible spectrum hinders its widespread deployment and commercialization. Although screening combinations of new materials and characterizing their reaction kinetics offers possible improvements to efficiency, current experiments are challenged by expensive bulky setups and slow recovery of particles downstream. Optofluidics is a good platform for screening Z-scheme catalysts cheaply and rapidly. By alleviating the problems of mass transport it can also potentially increase reaction rates and efficiencies. Here, we demonstrate a novel optofluidic device based on applying catalyst sol-gels on planar channels while measuring the reaction output by monitoring the depletion of the redox mediators. We use our setup to study the kinetics of the TiO(2)-Pt water-splitting reaction mediated by I(-)/IO(3)(-) redox pairs under different flow rates. In particular, for TiO(2)-Pt, we show ~2-fold improvements in reaction rates and efficiencies.
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http://dx.doi.org/10.1039/c2lc41129f | DOI Listing |
Nat Commun
January 2025
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, China.
Photocatalytic overall water splitting is a promising approach for a sustainable hydrogen provision using solar energy. For sufficient solar energy utilization, this reaction ought to be operated based on visible-light-active semiconductors, which is very challenging. In this work, an F-expedited nitridation strategy is applied to modify the wide-bandgap semiconductor SrTiO for visible-light-driven photocatalytic overall water splitting.
View Article and Find Full Text PDFNat Commun
January 2025
Max Planck Institute of Colloids and Interfaces, Colloid Chemistry Department, Am Mühlenberg 1, 14476, Potsdam, Germany.
Covalent semiconductors of the carbon nitride family are among the most promising systems to realize "artificial photosynthesis", that is exploiting synthetic materials which use sunlight as an energy source to split water into its elements or converting CO into added value chemicals. However, the role of surface interactions and electronic properties on the reaction mechanism remain still elusive. Here, we use in-situ spectroscopic techniques that enable monitoring surface interactions in carbon nitride under artificial photosynthetic conditions.
View Article and Find Full Text PDFNanoscale
January 2025
School of Science, Jiangsu University of Science and Technology, Zhenjiang 212001, China.
Herein, we propose a new GaN/MoSiP van der Waals (vdWs) heterostructure constructed by vertically stacking GaN and MoSiP monolayers. Its electronic, optical, and photocatalytic properties are explored DFT++BSE calculations. The calculated binding energy and phonon spectrum demonstrated the material's high stabilities.
View Article and Find Full Text PDFJ Comput Chem
January 2025
Department of Chemistry, University of Nevada Reno, Reno, Nevada, USA.
Hydrogen gas (H) can be produced via entirely solar-driven photocatalytic water splitting (PWS). A promising set of organic materials for facilitating PWS are the so-called inverted singlet-triplet, INVEST, materials. Inversion of the singlet (S) and triplet (T) energies reduces the population of triplet states, which are otherwise destructive under photocatalytic conditions.
View Article and Find Full Text PDFJ Phys Chem Lett
December 2024
Department of Chemistry, National Cheng Kung University, Tainan 701, Taiwan.
Photocatalytic water splitting holds great potential for transforming solar energy into valuable chemical products. However, obstacles such as the rapid recombination of electron-hole pairs and insufficiently active surface areas of photocatalysts remain significant challenges. In this study, we present the first demonstration that lithium bis(trifluoromethanesulfonyl)imide vapor successfully etches aluminum from NbAlC MAX phase powders while concurrently forming NbOF anchors on NbCT nanosheet (NbCTNS) MXene, leading to the in situ formation of a NbCTNS/NbOF heterostructure composite.
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