Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface
Abstract Photo-oxidation of methane (CH4) using hydrogen peroxide (H2O2) synthesized in situ from air and water under sunlight offers an attractive route for producing green methanol while storing intermittent solar energy. However, in commonly used aqueous-phase systems, photocatalysis efficiency i...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56180-7 |
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| author | Yuchen Hao Liwei Chen Haodong Liu Wenfeng Nie Xiangjie Ge Jiani Li Hui-Zi Huang Chao Sun Cuncai Lv Shangbo Ning Linjie Gao Yaguang Li Shufang Wang An-Xiang Yin Bo Wang Jinhua Ye |
| author_facet | Yuchen Hao Liwei Chen Haodong Liu Wenfeng Nie Xiangjie Ge Jiani Li Hui-Zi Huang Chao Sun Cuncai Lv Shangbo Ning Linjie Gao Yaguang Li Shufang Wang An-Xiang Yin Bo Wang Jinhua Ye |
| author_sort | Yuchen Hao |
| collection | DOAJ |
| description | Abstract Photo-oxidation of methane (CH4) using hydrogen peroxide (H2O2) synthesized in situ from air and water under sunlight offers an attractive route for producing green methanol while storing intermittent solar energy. However, in commonly used aqueous-phase systems, photocatalysis efficiency is severely limited due to the ultralow availability of CH4 gas and H2O2 intermediate at the flooded interface. Here, we report an atomically modified metal-organic framework (MOF) membrane nanoreactor that promotes direct CH4 photo-oxidation to methanol at the gas-solid interface in a reticular open framework. We show that the domino synergy between colocalized single-atom palladium and iron on MOF nodes enables efficient generation and in situ utilization of H2O2 in the absence of liquid water, thus circumventing H2O2 dilution. Meanwhile, the “breathable” MOF membrane, optimized by solar-driven interfacial water management, provides high-flux channels to facilitate efficient gas diffusion and rapid methanol desorption and transfer. As a result, we demonstrate over 210 hours of continuous photosynthesis of 0.25 M methanol with unity selectivity, achieving an exceptional methanol productivity of 14.4 millimoles per gram of catalyst per hour. |
| format | Article |
| id | doaj-art-421a72b2627c4f04b28df2348c198964 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj-art-421a72b2627c4f04b28df2348c1989642025-01-19T12:29:56ZengNature PortfolioNature Communications2041-17232025-01-0116111310.1038/s41467-025-56180-7Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interfaceYuchen Hao0Liwei Chen1Haodong Liu2Wenfeng Nie3Xiangjie Ge4Jiani Li5Hui-Zi Huang6Chao Sun7Cuncai Lv8Shangbo Ning9Linjie Gao10Yaguang Li11Shufang Wang12An-Xiang Yin13Bo Wang14Jinhua Ye15Research Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityMinistry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Frontiers Science Center for High Energy Material, School of Chemistry and Chemical Engineering, Beijing Institute of TechnologyResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityMinistry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Frontiers Science Center for High Energy Material, School of Chemistry and Chemical Engineering, Beijing Institute of TechnologyMinistry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Frontiers Science Center for High Energy Material, School of Chemistry and Chemical Engineering, Beijing Institute of TechnologyMinistry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Frontiers Science Center for High Energy Material, School of Chemistry and Chemical Engineering, Beijing Institute of TechnologyResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityMinistry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Frontiers Science Center for High Energy Material, School of Chemistry and Chemical Engineering, Beijing Institute of TechnologyMinistry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Frontiers Science Center for High Energy Material, School of Chemistry and Chemical Engineering, Beijing Institute of TechnologyResearch Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, In-stitute of Life Science and Green Development, Hebei UniversityAbstract Photo-oxidation of methane (CH4) using hydrogen peroxide (H2O2) synthesized in situ from air and water under sunlight offers an attractive route for producing green methanol while storing intermittent solar energy. However, in commonly used aqueous-phase systems, photocatalysis efficiency is severely limited due to the ultralow availability of CH4 gas and H2O2 intermediate at the flooded interface. Here, we report an atomically modified metal-organic framework (MOF) membrane nanoreactor that promotes direct CH4 photo-oxidation to methanol at the gas-solid interface in a reticular open framework. We show that the domino synergy between colocalized single-atom palladium and iron on MOF nodes enables efficient generation and in situ utilization of H2O2 in the absence of liquid water, thus circumventing H2O2 dilution. Meanwhile, the “breathable” MOF membrane, optimized by solar-driven interfacial water management, provides high-flux channels to facilitate efficient gas diffusion and rapid methanol desorption and transfer. As a result, we demonstrate over 210 hours of continuous photosynthesis of 0.25 M methanol with unity selectivity, achieving an exceptional methanol productivity of 14.4 millimoles per gram of catalyst per hour.https://doi.org/10.1038/s41467-025-56180-7 |
| spellingShingle | Yuchen Hao Liwei Chen Haodong Liu Wenfeng Nie Xiangjie Ge Jiani Li Hui-Zi Huang Chao Sun Cuncai Lv Shangbo Ning Linjie Gao Yaguang Li Shufang Wang An-Xiang Yin Bo Wang Jinhua Ye Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface Nature Communications |
| title | Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface |
| title_full | Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface |
| title_fullStr | Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface |
| title_full_unstemmed | Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface |
| title_short | Continuous photo-oxidation of methane to methanol at an atomically tailored reticular gas-solid interface |
| title_sort | continuous photo oxidation of methane to methanol at an atomically tailored reticular gas solid interface |
| url | https://doi.org/10.1038/s41467-025-56180-7 |
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