期刊
TOPICS IN CATALYSIS
卷 63, 期 3-4, 页码 363-369出版社
SPRINGER/PLENUM PUBLISHERS
DOI: 10.1007/s11244-020-01245-8
关键词
Non-thermal plasma; Kinetics; Dielectric barrier discharge; Water gas shift (WGS); Au; CeZrO4
资金
- EPSRC [EP/K014706/2, EP/K014668/1, EP/K014854/1, EP/K014714/1, EP/I019693/1]
- Science Achievement Scholarship of Thailand (SAST)
- Graduate School of Chiang Mai University
- Center of Excellence in Materials Science and Technology
- Chiang Mai University
- Thailand Research Fund [DPG6080002]
- EPSRC [EP/I019693/1, EP/K014706/2, EP/K014854/1, EP/K014668/1, EP/K014714/1] Funding Source: UKRI
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 (epsilon), 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. Graphic
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