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Kinetics of Water Gas Shift Reaction on Au/CeZrO4: A Comparison Between Conventional Heating and Dielectric Barrier Discharge (DBD) Plasma Activation

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Abstract

The kinetics of the low-temperature forward water gas shift (LT-WGS) reaction have been studied over a 2 wt% Au/CeZrO4 (Au/CZO) catalyst using both thermal and dielectric barrier discharge plasma heterogeneous catalyst systems. Using the energy density (ε), the apparent activation energy has been calculated under plasma and thermally activated conditions. A substantially lower apparent activation energy is observed in the plasma activated system (9.5 kJ/mol) compared with the thermal-catalysed reaction (132.9 kJ/mol). Different kinetic isotope effect (KIE) values for water were found in thermal (1.43) and plasma (1.89) activated catalytic systems which infer different mechanisms between the two activation processes and also shows the importance of water activation. Furthermore, negative and positive reaction orders with respect to CO and H2O are found for both conditions which are − 1.30, 0.28 under thermal and − 1.53, 0.35 under plasma processes, respectively. The reaction order with respect to H2O and KIE studies demonstrate that the bond cleavage in H2O molecule is a rate determining step in the plasma-assisted LT-WGS, similar to that in the thermal-assisted reaction.

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Acknowledgements

The UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC (Portfolio Grants: EP/K014706/2, EP/K014668/1, EP/K014854/1, EP/K014714/1, and EP/I019693/1). K.W. and B.I. also would like to thank Science Achievement Scholarship of Thailand (SAST), Graduate School of Chiang Mai University, Center of Excellence in Materials Science and Technology, Chiang Mai University and Thailand Research Fund (the TRF Distinguished Research Professor Award to K. Grudpan, DPG6080002) for a partial financial support.

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Authors and Affiliations

  1. School of Chemical Engineering and Analytical Science, The University of Manchester, Manchester, M13 9PL, UK

    Kanlayawat Wangkawong, Cristina E. Stere, Sarayute Chansai & Christopher Hardacre

  2. Graduate School, Chiang Mai University, Chiang Mai, 50200, Thailand

    Kanlayawat Wangkawong

  3. Department of Chemistry, Center of Excellence for Innovation in Chemistry (PERCH-CIC) and Centre of Excellence in Materials Science and Technology, Faculty of Science, Chiang Mai University, Chiang Mai, 50200, Thailand

    Kanlayawat Wangkawong, Sukon Phanichphant & Burapat Inceesungvorn

  4. School of Chemistry and Chemical Engineering, Queen’s University of Belfast, Belfast, BT9 5AG, UK

    Alexandre Goguet

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  1. Kanlayawat Wangkawong
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Correspondence to Burapat Inceesungvorn or Christopher Hardacre.

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Wangkawong, K., Phanichphant, S., Inceesungvorn, B. et al. Kinetics of Water Gas Shift Reaction on Au/CeZrO4: A Comparison Between Conventional Heating and Dielectric Barrier Discharge (DBD) Plasma Activation. Top Catal 63, 363–369 (2020). https://doi.org/10.1007/s11244-020-01245-8

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