Water-gas-shift reaction over Au single-atom catalysts with reversible oxide supports: A density functional theory study |
| |
| Affiliation: | 1. State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China;2. Institute of Engineering Technology, SINOPEC Catalyst Co., Ltd., Beijing 110112, China;1. São Carlos Federal University (UFSCar), Chemical Engineering Department (DEQ), Rod. Washington Luiz, km 235 – SP 310, CEP 13565-905, São Carlos, SP, Brazil;2. São Carlos Institute of Chemistry (IQSC), University of São Paulo (USP), Av. Trabalhador São-Carlense 400, CEP 13566-590, São Carlos, SP, Brazil;1. Institute of Nanoscience and Nanotechnology, National Center for Scientific Research Demokritos, Aghia Paraskevi, 153 10, Athens, Greece;2. Department of Industrial Engineering, University of Padova, Via F. Marzolo, 9, 35131, Padova, Italy;3. Department of Chemical Sciences, University of Padova, Via F. Marzolo, 1, 35131 Padua, Italy;4. CNR-ICMATE, Via F. Marzolo, 1, 35131 Padua, Italy;1. High-Performance Computing Unit (CECC-HCU), Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok 10330, Thailand;2. Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok 10330, Thailand;3. Saelee Research Group, Bangkok 10330, Thailand;4. Rittiruam Research Group, Bangkok 10330, Thailand;5. Khajondetchairit Research Group, Bangkok 10330, Thailand;6. Extreme Conditions Physics Research Laboratory and Center of Excellence in Physics of Energy Materials (CE: PEM), Department of Physics, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand;7. Theoretical Physics Division, Department of Physics, Chemistry and Biology (IFM), Linköping University, SE-581 83 Linköping, Sweden |
| |
| Abstract: | The low-temperature water-gas-shift (LT-WGS) reaction has shown remarkable activity for Au single-atom supported on reducible oxide catalysts. The water dissociation step of the WGS reaction is calculated using density functional theory (DFT) over four single Au atom (Au1)-pristine reversible oxides support systems Au1/MaOb-Ov (Au1/TiO2-x, Au1/ZrO2-x, Au1/CeO2-x and Au1/Co3O4-x) system and four Au1-supports with O vacancy (Ov) systems Au1/MaOb (Au1/TiO2, Au1/ZrO2, Au1/CeO2 and Au1/Co3O4). According to its greatest H2O adsorption energy, lowest water dissociation barrier, and slightest structural distortion, Au1/CeO2-x is chosen as the most beneficial catalyst for the WGS process. Afterwards, for Au1/CeO2-x, three reaction pathways (redox path, formate path and carboxyl path) are calculated. The predominant reaction pathway is the carboxyl pathway, and hydrogen production is the rate-determining step (RDS). For the purpose of designing single metal-support catalysts for the LT-WGS reaction, this paper gives information on the strong metal-support interaction (SMSI). |
| |
| Keywords: | Low-temperature water-gas-shift reaction Reaction mechanism Metal-support synergistic effect DFT |
| 本文献已被 ScienceDirect 等数据库收录！ |
|
