The coupling of efficient adsorption and effective charge separation with photocatalysts enables the use of sunlight for photocatalytic reduction of carbon dioxide (CO) into high-value-added products. In this work, we used a straightforward solid-phase hydrothermal technique to build an oxygen-vacancy-rich, heterogeneous interface-coupled CeO/mesoporous TiO framework structural system. The heterogeneous structure was constructed by introducing oxygen-vacancy-rich CeO into mesoporous TiO, which may encourage the transfer of charges and increase the number of active sites and CO adsorption by utilizing the coupled synergistic effect of oxygen vacancies and heterogeneous interfaces, and it can also regulate the pathway of the photocatalytic reaction and the selectivity of the products. The composite of CeO with different morphologies and oxygen-rich vacancies regulated the system's active sites and degree of exposure and enhanced photocatalytic CO reduction. The highest CO yield of 6.25 mmol g was obtained by use of the rod CeO/mesoporous TiO composite photocatalyst (R-CeO/TiO), and this yield was 1.6 times higher than that of pure mesoporous TiO and 1.84 times higher than that of pure R-CeO. Also, the product selectivity increased by 4.3% compared to a single sample. Combining the Mott-Schottky plot results and the energy-barrier perspective to further explore the photocatalytic reduction of the CO reaction mechanism as well as the product selectivity, it appears that the construction of the composite system of oxygen-rich vacancies and heterogeneous boundary-coupled photocatalysis provides a practical pathway for the photocatalytic reaction, which may contribute to the photocatalytic reaction's high efficiency and yield selectivity.
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http://dx.doi.org/10.1039/d4dt02014f | DOI Listing |
Adv Sci (Weinh)
January 2025
School of Resources and Environment, University of Electronic Science and Technology of China, Chengdu, 611731, China.
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr-CsPbBr polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface.
View Article and Find Full Text PDFNanomaterials (Basel)
January 2025
Institute of Materials Science & Devices, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China.
Carbon catalysts have shown promise as an alternative to the currently available energy-intensive approaches for nitrogen fixation (NF) to urea, NH, or related nitrogenous compounds. The primary challenges for NF are the natural inertia of nitrogenous molecules and the competitive hydrogen evolution reaction (HER). Recently, carbon-based materials have made significant progress due to their tunable electronic structure and ease of defect formation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Friedrich Alexander University Erlangen Nuremberg: Friedrich-Alexander-Universitat Erlangen-Nurnberg, Department of Materials Science, GERMANY.
Bottom-up syntheses of carbon nanodots (CND) using solvothermal treatment of citric acid are known to afford nanometer-sized, amorphous polycitric acid-based materials. The addition of suitable co-reactants in the form of in-situ synthesized N-hetero-π-conjugated chromophores facilitates hereby the overall functionalization. Our incentive was to design a CND model that features phenazine (P-CND) - a well-known N-hetero-π-conjugated chromophore - to investigate the influence of the CND matrix on its redox chemistry as well as photochemistry.
View Article and Find Full Text PDFChem Commun (Camb)
January 2025
Coordination Chemistry Institute, State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing National Laboratory of Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, China.
The design of efficient photocatalysts is crucial for photocatalytic CO reduction. This study developed photocatalysts based on MIL-101(Cr) composited with a facet-engineered Pt/Pd nanoalloy (PPNA). Photocatalytic performance evaluations show that MIL-101(Cr) loaded with PPNA exposing {111} facets, namely M-A(111), exhibits a CO to CH conversion rate of 9.
View Article and Find Full Text PDFNanoscale Adv
December 2024
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University Nanchang 330063 P. R. China.
Photocatalytic reduction of CO to produce organic fuels is a promising strategy for addressing carbon reduction and energy scarcity. Transition metal carbides (TiCT ) are of particular interest due to their unique layered structures and excellent electrical conductivity. However, the practical application of TiCT is limited by the poor separation efficiency of photogenerated charge carriers and the low migration ability of photogenerated electrons.
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