Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters
Abstract Amine-assisted two-step CO2 hydrogenation is an efficient route for methanol production. To maximize the overall catalytic performance, both the N-formylation of amine with CO2 (i.e., first step) and the subsequent amide hydrogenation (i.e., second step) are required to be optimized. Herein...
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| Language: | English |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-55837-7 |
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| author | Desheng Su Yinming Wang Haoyun Sheng Qihao Yang Dianhui Pan Hao Liu Qiuju Zhang Sheng Dai Ziqi Tian Zhiyi Lu Liang Chen |
| author_facet | Desheng Su Yinming Wang Haoyun Sheng Qihao Yang Dianhui Pan Hao Liu Qiuju Zhang Sheng Dai Ziqi Tian Zhiyi Lu Liang Chen |
| author_sort | Desheng Su |
| collection | DOAJ |
| description | Abstract Amine-assisted two-step CO2 hydrogenation is an efficient route for methanol production. To maximize the overall catalytic performance, both the N-formylation of amine with CO2 (i.e., first step) and the subsequent amide hydrogenation (i.e., second step) are required to be optimized. Herein, a class of Al2O3-supported Ru catalysts, featuring multiple activated Ru species (i.e., metallic and oxidized Ru), are rationally fabricated. Density functional theory calculations suggest that metallic Ru forms are preferred for N-formylation step, whereas oxidized Ru species demonstrate enhanced amide hydrogenation activity. Thus, the optimal catalyst, containing unique Ru clusters with coexisting metallic and oxidized Ru species, efficiently synergize the conversion of CO2 into methanol with exceptional selectivity (>95%) in a one-pot two-step process. This work not only presents an advanced catalyst for CO2-based methanol production but also highlights the strategic design of catalysts with multiple active species for optimizing the catalytic performances of multistep reactions in the future. |
| format | Article |
| id | doaj-art-3e1320fe1c1f4e43b01b27f166a33f5e |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-3e1320fe1c1f4e43b01b27f166a33f5e2025-01-12T12:30:32ZengNature PortfolioNature Communications2041-17232025-01-0116111010.1038/s41467-025-55837-7Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clustersDesheng Su0Yinming Wang1Haoyun Sheng2Qihao Yang3Dianhui Pan4Hao Liu5Qiuju Zhang6Sheng Dai7Ziqi Tian8Zhiyi Lu9Liang Chen10Zhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesZhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesZhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesZhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesNingbo Hesheng New Materials Co., LtdZhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesZhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesSchool of Chemistry and Molecular Engineering, East China University of Science and TechnologyUniversity of Chinese Academy of SciencesZhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesZhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of SciencesAbstract Amine-assisted two-step CO2 hydrogenation is an efficient route for methanol production. To maximize the overall catalytic performance, both the N-formylation of amine with CO2 (i.e., first step) and the subsequent amide hydrogenation (i.e., second step) are required to be optimized. Herein, a class of Al2O3-supported Ru catalysts, featuring multiple activated Ru species (i.e., metallic and oxidized Ru), are rationally fabricated. Density functional theory calculations suggest that metallic Ru forms are preferred for N-formylation step, whereas oxidized Ru species demonstrate enhanced amide hydrogenation activity. Thus, the optimal catalyst, containing unique Ru clusters with coexisting metallic and oxidized Ru species, efficiently synergize the conversion of CO2 into methanol with exceptional selectivity (>95%) in a one-pot two-step process. This work not only presents an advanced catalyst for CO2-based methanol production but also highlights the strategic design of catalysts with multiple active species for optimizing the catalytic performances of multistep reactions in the future.https://doi.org/10.1038/s41467-025-55837-7 |
| spellingShingle | Desheng Su Yinming Wang Haoyun Sheng Qihao Yang Dianhui Pan Hao Liu Qiuju Zhang Sheng Dai Ziqi Tian Zhiyi Lu Liang Chen Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters Nature Communications |
| title | Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters |
| title_full | Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters |
| title_fullStr | Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters |
| title_full_unstemmed | Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters |
| title_short | Efficient amine-assisted CO2 hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters |
| title_sort | efficient amine assisted co2 hydrogenation to methanol co catalyzed by metallic and oxidized sites within ruthenium clusters |
| url | https://doi.org/10.1038/s41467-025-55837-7 |
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