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Binary Li/Na tungstates modified Mg6MnO8 as redox catalysts for enhanced performance of chemical looping oxidative dehydrogenation of ethane

文献类型：期刊论文

作者Chen, Haitao1,2; Xing, Zifan1,2; Song, Da1,2,3,4; Yu, Xiang1,2; Li, Yang3; He, Fang1,2
刊名CHEMICAL ENGINEERING JOURNAL
出版日期2024-04-01
卷号485页码:12
关键词Chemical looping oxidative dehydrogenation Ethane Oxygen carriers Binary tungstates DFT calculations
ISSN号1385-8947
DOI10.1016/j.cej.2024.150146
通讯作者He, Fang(hefang@glut.edu.cn)
英文摘要The present investigation delves into the utilization of Mg6MnO8 modified with binary Li2WO4 and Na2WO4 tungstates as oxygen carriers for the chemical looping oxidative dehydrogenation (CL-ODH) of ethane. The Mg6MnO8-LiNaW2 oxygen carrier demonstrates remarkable performance, achieving up to 77.7 % ethane conversion, 86.5 % ethylene selectivity, and 67.2 % ethylene yield. HRTEM-EDS reveals the formation of a molten binary tungstates layer covering the solid Mg6MnO8 substrate. The molten binary tungstates layer effectively modulates the release of lattice oxygen in a step-wise manner during ODH reactions. oS analysis reveals that the doping of Li/Na binary tungstates inhibits the formation of OH-/CO32- and Mn4+ species, thus preventing the deep oxidation of ethylene. The Mg6MnO8-LiNaW2 sample maintains stable reactivity and surface morphology throughout 20 redox cycles. DFT calculations further indicate that the modification with Li/Na binary tungstates promotes electron accumulation around the local environment of the Me -O bond, thereby reducing the formation energy (Eo) of oxygen vacancy in Mg6MnO8 and improving the oxygen vacancy concentration within the bulk of the oxygen carriers. The superior ethylene selectivity of the Mg6MnO8-LiNaW2 oxygen carrier can be attributed to the higher oxygen diffusion capability in the bulk of the Mg6MnO8 core, coupled with the lower oxygen transport rate through the molten tungstates layer.
WOS关键词INTENSIFIED ETHYLENE PRODUCTION ; OXYGEN CARRIER ; METHANE ; PROMOTERS ; SODIUM
资助项目Natural Science Foundation[2021GXNSFAA075036] ; Natural Science Foundation[2018GXNSFDA281005]
WOS研究方向Engineering
语种英语
WOS记录号WOS:001204364400001
出版者ELSEVIER SCIENCE SA
资助机构Natural Science Foundation
源URL[http://ir.giec.ac.cn/handle/344007/41461]  
专题中国科学院广州能源研究所
通讯作者He, Fang
作者单位1.Guilin Univ Technol, Coll Chem & Bioengn, Guilin 541006, Peoples R China
2.Guilin Univ Technol, Coll Chem & Bioengn, Guangxi Key Lab Electrochem & Magneto Chem Funct M, Guilin 541004, Peoples R China
3.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Peoples R China
4.Univ Sci & Technol China, Sch Energy Sci & Engn, Hefei, Peoples R China
推荐引用方式
GB/T 7714		 Chen, Haitao,Xing, Zifan,Song, Da,et al. Binary Li/Na tungstates modified Mg6MnO8 as redox catalysts for enhanced performance of chemical looping oxidative dehydrogenation of ethane[J]. CHEMICAL ENGINEERING JOURNAL,2024,485:12.
APA Chen, Haitao,Xing, Zifan,Song, Da,Yu, Xiang,Li, Yang,&He, Fang.(2024).Binary Li/Na tungstates modified Mg6MnO8 as redox catalysts for enhanced performance of chemical looping oxidative dehydrogenation of ethane.CHEMICAL ENGINEERING JOURNAL,485,12.
MLA Chen, Haitao,et al."Binary Li/Na tungstates modified Mg6MnO8 as redox catalysts for enhanced performance of chemical looping oxidative dehydrogenation of ethane".CHEMICAL ENGINEERING JOURNAL 485(2024):12.

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来源：广州能源研究所

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