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Boosting the photocatalytic nitrogen reduction to ammonia through adsorption-plasmonic synergistic effects
Institution:1. The Education Ministry Key Lab of Resource Chemistry, Shanghai Key Laboratory of Rare Earth Functional Materials, College of Chemistry and Materials Science, Shanghai Normal University, Shanghai 200234, China;2. School of Environmental and Geographical Sciences, Shanghai Normal University, Shanghai 200234, China;3. School of Materials Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China
Abstract:Ammonia is one of the most essential chemicals in the modern society but its production still heavily relies on energy-consuming Haber-Bosch processes. The photocatalytic reduction of nitrogen with water for ammonia production has attracted much attention recently due to its synthesis under mild conditions at room temperature and atmospheric pressure using sunlight. Herein, we report a high-performance Au/MIL-100(Cr) photocatalyst, comprising MIL-100(Cr) and Au nanoparticles in photocatalytic nitrogen reduction to ammonia at ambient conditions under visible light irradiation. The optimized photocatalyst (i.e., 0.10Au/MIL-100(Cr)) achieved the excellent ammonia production rate with 39.9 µg gcat?1 h?1 compared with pure MIL-100(Cr) (2.73 µg gcat?1 h?1), which was nearly 15 times that on pure MIL-100(Cr). The remarkable activity could be attributed to the adsorption-plasmonic synergistic effects in which the MIL-100(Cr) and Au are responsible to the strong trapping and adsorption of N2 molecules and photo-induced plasmonic hot electrons activating and decomposing the N2 molecules, respectively. This study might provide a new strategy for designing an efficient plasmonic photocatalyst to improve the photocatalytic performance of N2 fixation under visible light irradiation.
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