Screening the optimal Cox/CeO2(110)(x=1-6)catalyst for methane activation in coalbed gas
Li'nan Huang1
Danyang Li1
Lei Jiang1
Zhiqiang Li1
Dong Tian2
Kongzhai Li2
1.Engineering Research Center of Metallurgical Energy Conservation and Emission Reduction,Ministry of Education,Kunming University of Science and Technology,Kunming 650093,China;Faculty of Metallurgical and Energy Engineering,Kunming University of Science and Technology,Kunming 650093,China2.Engineering Research Center of Metallurgical Energy Conservation and Emission Reduction,Ministry of Education,Kunming University of Science and Technology,Kunming 650093,China;Faculty of Metallurgical and Energy Engineering,Kunming University of Science and Technology,Kunming 650093,China;State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization,Kunming University of Science and Technology,Kunming 650093,China
摘要：The challenges posed by energy and environmental issues have forced mankind to explore and utilize unconventional energy sources.It is imperative to convert the abundant coalbed gas(CBG)into high value-added products,i.e.,selective and efficient conversion of methane from CBG.Methane activation,known as the"holy grail",poses a challenge to the design and development of catalysts.The structural complexity of the active metal on the carrier is of particular concern.In this work,we have studied the nucleation growth of small Co clusters(up to Co6)on the surface of CeO2(110)using density functional theory,from which a stable loaded Co/CeO2(110)structure was selected to investigate the methane activation mechanism.Despite the relatively small size of the selected Co clusters,the obtained Cox/CeO2(110)exhibits interesting properties.The optimized Co5/CeO2(110)structure was selected as the optimal structure to study the activation mechanism of methane due to its competitive electronic structure,adsorption energy and binding energy.The energy bar-riers for the stepwise dissociation of methane to form CH3*,CH2*,CH*,and C*radical fragments are 0.44,0.55,0.31,and 1.20 eV,respectively,indicating that CH*dissociative dehydrogenation is the rate-determining step for the system under investigation here.This fundamental study of metal-support interactions based on Co growth on the CeO2(110)surface contributes to the understanding of the essence of Co/CeO2 catalysts with promising catalytic behavior.It provides theoretical guidance for better designing the optimal Co/CeO2 catalyst for tailored catalytic reactions.
机标关键词：screeningoptimalcatalystactivationcoalbedmethane
论文发表日期：2024-06-28
在线出版日期：2025-08-15（本平台首次上网日期，不代表文献的发表时间）
页数：16( 256-271 )
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