文献类型：期刊文献

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

作者：Zhao, Kun[1,2];Gao, Yunfei[3];Wang, Xijun[4];Lis, Bar Mosevitzky[5];Liu, Junchen[1];Jin, Baitang[1];Smith, Jacob[1];Huang, Chuande[6];Gao, Wenpei[1];Wang, Xiaodong[6];Wang, Xin[3];Zheng, Anqing[2];Huang, Zhen[2];Hu, Jianli[7];Schoemacker, Reinhard[8];Wachs, Israel E.[5];Li, Fanxing[1]

机构：[1]North Carolina State Univ, Campus Box 7905, Raleigh, NC USA;[2]Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou, Peoples R China;[3]East China Univ Sci & Technol, Inst Clean Coal Technol, Shanghai, Peoples R China;[4]Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL USA;[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

年份：2023

卷号：14

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001316824700036)】；

基金：This work was supported by the U.S. NSF (Award No. CBET-2116724, CBET-1923468) and the Kenan Institute for Engineering, Technology and Science at the NC State University. KZ is supported by Guangdong Natural Science Fund for Distinguished Young Scholars (Grants 2023B1515020048). We also acknowledge the support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy - EXC 2008/1 (UniSysCat) - 390540038 and the Alexander von Humboldt Foundation. We acknowledge the use of the Analytical Instrumentation Facility (AIF) at the NC State University.

语种：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.