Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields
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)....
| Main Authors: | , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2023-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-43682-5 |
| _version_ | 1797414653658136576 |
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| author | 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 Fanxing Li |
| author_facet | 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 Fanxing Li |
| author_sort | Kun Zhao |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-09T05:36:37Z |
| format | Article |
| id | doaj.art-541024f90735452094967dc217685606 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-09T05:36:37Z |
| publishDate | 2023-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-541024f90735452094967dc2176856062023-12-03T12:27:59ZengNature PortfolioNature Communications2041-17232023-11-0114111110.1038/s41467-023-43682-5Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yieldsKun Zhao0Yunfei Gao1Xijun Wang2Bar Mosevitzky Lis3Junchen Liu4Baitang Jin5Jacob Smith6Chuande Huang7Wenpei Gao8Xiaodong Wang9Xin Wang10Anqing Zheng11Zhen Huang12Jianli Hu13Reinhard Schömacker14Israel E. Wachs15Fanxing Li16North Carolina State University, Campus Box 7905Institute of Clean Coal Technology, East China University of Science and TechnologyDepartment of Chemical and Biological Engineering, Northwestern UniversityOperando Molecular Spectroscopy & Catalysis Laboratory, Department of Chemical & Biomolecular Engineering, Lehigh UniversityNorth Carolina State University, Campus Box 7905North Carolina State University, Campus Box 7905North Carolina State University, Campus Box 7905Dalian Institute of Chemical Physics, Chinese Academy of SciencesNorth Carolina State University, Campus Box 7905Dalian Institute of Chemical Physics, Chinese Academy of SciencesInstitute of Clean Coal Technology, East China University of Science and TechnologyCAS Key Laboratory of Renewable Energy, Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou Institute of Energy Conversion, Chinese Academy of SciencesCAS Key Laboratory of Renewable Energy, Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou Institute of Energy Conversion, Chinese Academy of SciencesDepartment of Chemical & Biomedical Engineering, West Virginia UniversityDepartment of Chemistry, Technische Universität BerlinOperando Molecular Spectroscopy & Catalysis Laboratory, Department of Chemical & Biomolecular Engineering, Lehigh UniversityNorth Carolina State University, Campus Box 7905Abstract 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.https://doi.org/10.1038/s41467-023-43682-5 |
| spellingShingle | 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 Fanxing Li Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields Nature Communications |
| title | Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields |
| title_full | Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields |
| title_fullStr | Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields |
| title_full_unstemmed | Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields |
| title_short | Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields |
| title_sort | lithium carbonate promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields |
| url | https://doi.org/10.1038/s41467-023-43682-5 |
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