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Comprehending the catalytic reaction implementation for heterostructure photocatalysts is crucial by scrutinizing the spatial separation and transfer process of photoexcited charges at nanoscale junctions. Herein, we fabricated the F-doped TiO/ZnInS-based S-scheme heterostructure using a direct liquid-assembly method. The optimum hydrogen evolution rate (HER) of ∼ 1.58 mmol gh was acquired for 30-FT@ZIS, which was about 15 and 2 times superior to the pristine F-doped TiO and ZnInS, respectively. The interaction between F-doped TiO and ZnInS facilitated the charge transfer from ZIS to FT which was confirmed through XPS. UV-vis spectroscopy and Mott-Schottky validated that F-doped TiO and ZnInS retain the suitable energy band alignment for the S-scheme heterostructure. In situ, KPFM and EPR analysis revealed that F-doped TiO and ZnInS possess a spontaneous photoelectrochemical response, and their junction significantly improves the internal electric field by separating photoexcited charge carriers. This work provides a conclusive experimental and theoretical validation for an internal electric field and charge flow direction in non-noble-metal-based heterostructure photocatalysts.
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http://dx.doi.org/10.1016/j.jcis.2024.11.124 | DOI Listing |
Phys Rev Lett
May 2025
University of Vienna, Faculty of Physics and Center for Computational Materials Science, Vienna, Austria.
Polarons are crucial for charge transport in semiconductors, significantly impacting material properties and device performance. The dynamics of small polarons can be investigated using first-principles molecular dynamics. However, the limited timescale of these simulations presents a challenge for adequately sampling infrequent polaron hopping events.
View Article and Find Full Text PDFNanomaterials (Basel)
May 2025
Department of Chemical and Physical Sciences, Walter Sisulu University, Private Bag X1, Mthatha 5117, South Africa.
In this work, a density functional theory (DFT) with Hubbard correction (U) approaches implemented through the Quantum ESPRESSO code is utilized to investigate the effects of fluorine (F) doping on the structural, electronic, and optical properties of rutile TiO. Rutile TiO is a promising material for renewable energy production and environmental remediation, but its wide bandgap limits its application to the UV spectrum, which is narrow and expensive. To extend the absorption edge of TiO into the visible light range, different concentrations of F were substituted at oxygen atom sites.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2025
School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 211816, Jiangsu, China.
The complete catalytic oxidation of propane (CH) at low temperatures remains challenging due to the competitive adsorption between the oxidation of the O and CH molecules. In this study, we propose an innovative approach to enhance CH oxidation by strategically designing active Pt sites with modulated electronic structures on F-doped TiO-supported Pt catalyst (Pt/F-TiO), which exhibits 50 and 90% of propane conversion at 200 and 320 °C. Our mechanistic study reveals that the electron coupling between Pt 5d and F 2p alters the d orbital electron property, which leads to generation of abundant efficient electron-enriched Pt species.
View Article and Find Full Text PDFNanoscale
April 2025
Departamento de Química Inorgánica, Facultad de Ciencias, Calle Francisco Tomás y Valiente, 7, Universidad Autónoma de Madrid, Ciudad Universitaria de Cantoblanco, 28049, Madrid, Spain.
We present the design and synthesis of a new quinoline-based covalent triazine framework (Quin-CTF) that combines two photoactive fragments within its structure (triazine and quinoline moieties). By hybridizing this CTF material with fluorine-doped titanium dioxide (F-TiO2), we prepared and characterized photocatalysts with enhanced performance that leverage the synergy between the two components for pollutant photodegradation in water. This F-TiO2@CTF hybrid system was evaluated for the photocatalytic degradation of methylene blue dye and a pharmaceutical compound such as ciprofloxacin as model water pollutants.
View Article and Find Full Text PDFSci Rep
January 2025
Department of Physics, Wolkite University, P. O. Box: 07, Wolkite, Ethiopia.
This study uses the Quantum ESPRESSO code to introduce Hubbard correction (U) to the density functional theory (DFT) in order to examine the effects of non-metals (C, F, N, and S) doping on the structural, electronic, and optical characteristics of rutile TiO. Rutile TiO is a substance that shows promise for use in renewable energy production, including fuels and solar energy, as well as environmental cleanup. Its wide bandgap, however, restricts their uses to areas with UV light.
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