Novel B-site substituted KCuTa3-xNbxO9 solid solution photocatalysts with modulated band structure for visible-light-driven hydrogen evolution |
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| Affiliation: | 1. College of Chemistry, Northeast Normal University, Changchun 130024, PR China;2. College of Environmental and Chemical Engineering, Xi''an Polytechnic University, Xi''an 710048, PR China;1. Dr. S. S. Bhatnagar University Institute of Chemical Engineering and Technology (Formerly Department of Chemical Engineering & Technology), Panjab University, Chandigarh, 160014, India;2. Department of Physics, Sunrise University, Alwar, Rajasthan, 301028, India;3. Cipla Limited, Malpur Upper, Baddi, Dist, Solan, 173205, India;4. Computational Physics & Materials Science Lab, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900, Saudi Arabia;5. Centre for Nanoscience & Nanotechnology, University Institute for Emerging Areas in Science and Technology, Panjab University, Chandigarh, 160014, India;6. Energy Research Centre, Panjab University, Chandigarh, 160014, India;1. Fuel Cell Institute, Universiti Kebangsaan Malaysia, Bangi, Malaysia;2. Department of Chemical and Process Engineering, Faculty of Engineering and Built Environment, Universiti Kebangsaan Malaysia, Bangi, Malaysia;1. Graduate School of Advanced Science and Engineering, Hiroshima University, 1-4-1 Kagamiyama, Higashi-Hiroshima 739-8527, Japan;2. Hydrolabo Inc., 3-10-31, Kagamiyama, Higashi-Hiroshima 739-0046, Japan;3. Faculty of Science, University of the Ryukyus, 1 Senbaru, Nishihara-cho, Okinawa 903-0213, Japan;4. Natural Science Centre for Basic Research & Development, Hiroshima University, 1-3-1 Kagamiyama, Higashi-Hiroshima 739-8530, Japan |
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| Abstract: | Perovskite-like metal oxides (PLMOs), featuring unique structural and optical properties, exhibit great potential in photocatalytic water splitting field. However, the wide bandgap and strong carrier recombination severely suppress their photocatalytic hydrogen production activity. Thus, design and development of novel PLMO photocatalyst with extended photo-response range and enhanced photo-generated charge separation/transport efficiency remains an ongoing challenge. Herein, a series of novel B-site substituted KCuTa3-xNbxO9 solid solution photocatalysts were synthesized via a simple solid-state reaction method. With an increased content of Nb, a distinct red-shifted of the optical absorption edge of KCuTa3-xNbxO9 solid solution was observed, leading to a decreased bandgap (from 2.69 to 1.91 eV), and a positive shift of the conduction band bottom (from −0.54 to −0.49 eV vs RHE). All of the Nb-substituted KCuTa3O9 solid solutions exhibit enhanced separation efficiency of photoinduced charge carriers, which leads to increased hydrogen evolution activity, among which KCuTa0.75Nb2.25O9 exhibits the highest hydrogen evolution rate of 2.16 μmol h−1 under the visible light irradiation (λ > 420 nm), which is approximately 7-fold higher than that of the pure KCuTa3O9. This study demonstrates the potential of modulating band structure through constructing solid solutions for efficient perovskite-like metal oxides photocatalysis. |
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| Keywords: | Photocatalysis Hydrogen evolution Perovskite oxides Solid solution Visible light absorption |
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