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Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields

文献类型：期刊论文

作者Zhao, Kun2,3; Gao, Yunfei4; Wang, Xijun1; Lis, Bar Mosevitzky5; Liu, Junchen2; Jin, Baitang2; Smith, Jacob2; Huang, Chuande6; Gao, Wenpei2; Wang, Xiaodong6
刊名NATURE COMMUNICATIONS
出版日期2023-11-27
卷号14期号:1页码:11
DOI10.1038/s41467-023-43682-5
通讯作者Gao, Yunfei(yunfeigao@ecust.edu.cn) ; Wachs, Israel E.(iew0@lehigh.edu) ; Li, Fanxing(fli5@ncsu.edu)
英文摘要The oxidative coupling of methane to higher hydrocarbons offers a promising autothermal approach for direct methane conversion, but its progress has been hindered by yield limitations, high temperature requirements, and performance penalties at practical methane partial pressures (similar to 1 atm). In this study, we report a class of Li2CO3-coated mixed rare earth oxides as highly effective redox catalysts for oxidative coupling of methane under a chemical looping scheme. This catalyst achieves a single-pass C2+ yield up to 30.6%, demonstrating stable performance at 700 degrees C and methane partial pressures up to 1.4atm. In-situ characterizations and quantum chemistry calculations provide insights into the distinct roles of the mixed oxide core and Li2CO3 shell, as well as the interplay between the Pr oxidation state and active peroxide formation upon Li2CO3 coating. Furthermore, we establish a generalized correlation between Pr4+ content in the mixed lanthanide oxide and hydrocarbons yield, offering a valuable optimization strategy for this class of oxidative coupling of methane redox catalysts.
WOS关键词LI-DOPED MGO ; METHYL RADICALS ; OXYGEN CARRIER ; CATALYSTS ; PERFORMANCE ; ETHYLENE ; MN ; REACTIVITY ; CONVERSION ; TUNGSTEN
资助项目U.S. NSF[CBET-2116724] ; U.S. NSF[CBET-1923468] ; Kenan Institute for Engineering, Technology and Science at the NC State University ; Guangdong Natural Science Fund for Distinguished Young Scholars[2023B1515020048] ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy[EXC 2008/1] ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy[390540038] ; Alexander von Humboldt Foundation
WOS研究方向Science & Technology - Other Topics
语种英语
WOS记录号WOS:001316824700036
出版者NATURE PORTFOLIO
资助机构U.S. NSF ; Kenan Institute for Engineering, Technology and Science at the NC State University ; Guangdong Natural Science Fund for Distinguished Young Scholars ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy ; Alexander von Humboldt Foundation
源URL[http://ir.giec.ac.cn/handle/344007/43011]  
专题中国科学院广州能源研究所
通讯作者Gao, Yunfei; Wachs, Israel E.; Li, Fanxing
作者单位1.Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL USA
2.North Carolina State Univ, Campus Box 7905, Raleigh, NC USA
3.Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou, Peoples R China
4.East China Univ Sci & Technol, Inst Clean Coal Technol, Shanghai, Peoples R China
5.Lehigh Univ, Dept Chem & Biomol Engn, Operando Mol Spect & Catalysis Lab, Bethlehem, PA USA
6.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian, Peoples R China
7.West Virginia Univ, Dept Chem & Biomed Engn, Morgantown, WV USA
8.Tech Univ Berlin, Dept Chem, Str 17,Juni 124, Berlin, Germany
推荐引用方式
GB/T 7714		 Zhao, Kun,Gao, Yunfei,Wang, Xijun,et al. Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields[J]. NATURE COMMUNICATIONS,2023,14(1):11.
APA Zhao, Kun.,Gao, Yunfei.,Wang, Xijun.,Lis, Bar Mosevitzky.,Liu, Junchen.,...&Li, Fanxing.(2023).Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields.NATURE COMMUNICATIONS,14(1),11.
MLA Zhao, Kun,et al."Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields".NATURE COMMUNICATIONS 14.1(2023):11.

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来源：广州能源研究所

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