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Metal-Support Interaction Boosts the Photocatalytic Performance of Pd/TiO2 for Acetylene Semi-Hydrogenation:
Zhidan Wang1,2, Fangxia Xie1,2, Jianxin Liu1,2
1Shanxi Key Laboratory of Complex Air Pollution Control and Carbon Reduction, College of Environmental and Ecology, Taiyuan University of Technology, Taiyuan, 030024, P. R. China.
Abstract:
Photocatalytic acetylene (C2H2) semi-hydrogenation reaction is an environmentally friendly process for ethylene (C2H4) production. However, all attempts to enhance the C2H4 yield have faced kinetic limitations. Electronic metal-support interaction (EMSI) is an effective approach to enhance kinetic constants by regulating the adsorption and desorption capabilities of intermediates and reactive species, promoting the reaction in the forward direction. Herein, Pd/TiO2 catalysts are constructed by a hydrothermal-calculation method, forming the EMSI effect between Pd and TiO2. Spectroscopy characterizations and theoretical calculations demonstrate that EMSI promotes the photo-generated charge carriers from TiO2 to Pd. The control of the local electron density on Pd nanoparticles directly influenced the Gibbs free energy of the H* reaction and the desorption energy of *C2H4. This ultimately enhances the consumption and adsorption kinetics of H*, while simultaneously suppressing H* desorption and facilitating the desorption of *C2H4. Consequently, it modulates the preferential order between H2 evolution and the C2H2 semi-hydrogenation, expediting the production of C2H4. Therefore, the Pd/TiO2 achieves 99.7% C2H2 conversion, 77.3% C2H4 selectivity, and TONC2H4 = 5960 within 3 h. This work provides a reference and guidance for the subsequent construction of efficient photocatalytic C2H2 semi-hydrogenation catalysts.
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