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

Kun Zhao, Yunfei Gao (), Xijun Wang, Bar Mosevitzky Lis, Junchen Liu, Baitang Jin, Jacob Smith, Chuande Huang, Wenpei Gao, Xiaodong Wang, Xin Wang, Anqing Zheng, Zhen Huang, Jianli Hu, Reinhard Schömacker, Israel E. Wachs () and Fanxing Li ()
Additional contact information
Kun Zhao: North Carolina State University, Campus Box 7905
Yunfei Gao: East China University of Science and Technology
Xijun Wang: Northwestern University
Bar Mosevitzky Lis: Lehigh University
Junchen Liu: North Carolina State University, Campus Box 7905
Baitang Jin: North Carolina State University, Campus Box 7905
Jacob Smith: North Carolina State University, Campus Box 7905
Chuande Huang: Chinese Academy of Sciences
Wenpei Gao: North Carolina State University, Campus Box 7905
Xiaodong Wang: Chinese Academy of Sciences
Xin Wang: East China University of Science and Technology
Anqing Zheng: Chinese Academy of Sciences
Zhen Huang: Chinese Academy of Sciences
Jianli Hu: West Virginia University
Reinhard Schömacker: Technische Universität Berlin
Israel E. Wachs: Lehigh University
Fanxing Li: North Carolina State University, Campus Box 7905

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract 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 (~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 °C and methane partial pressures up to 1.4 atm. 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.

Date: 2023
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DOI: 10.1038/s41467-023-43682-5

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