In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation
Summary: The direct and selective transformation of naturally abundant methane (CH4) into high-value-added oxygenates, e.g., methanol, ethanol, and formic acid, is one of the “Holy Grails” in chemistry and chemical productions. However, complex mixtures of products, often due to over-oxidations, mak...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Elsevier
2023-02-01
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| Series: | iScience |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2589004223000196 |
| _version_ | 1797903371198267392 |
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| author | Jing-Tan Han Hui Su Lida Tan Chao-Jun Li |
| author_facet | Jing-Tan Han Hui Su Lida Tan Chao-Jun Li |
| author_sort | Jing-Tan Han |
| collection | DOAJ |
| description | Summary: The direct and selective transformation of naturally abundant methane (CH4) into high-value-added oxygenates, e.g., methanol, ethanol, and formic acid, is one of the “Holy Grails” in chemistry and chemical productions. However, complex mixtures of products, often due to over-oxidations, make such transformations highly challenging. Herein, gallium nitride (GaN), a methane-active semiconductor, catalyzes the photooxidation of methane and empowers the fine-controlling of chemoselectivity toward methanol and formic acids, simply by regulating the O2 content in water. In contrast to previous methods, no overoxidation products (CO2 and CO) were observed in this process. Mechanistic investigations and the corresponding quantitative experiments indicated that the controllable generation of moderately reactive oxygen radicals (•OOH and •OH) in combination with the direct methane activation triggered by GaN is responsible for the highly selective reactivity and tunability through a photo-generated radical process. |
| first_indexed | 2024-04-10T09:31:50Z |
| format | Article |
| id | doaj.art-4018671075d844b5aab31079987c2921 |
| institution | Directory Open Access Journal |
| issn | 2589-0042 |
| language | English |
| last_indexed | 2024-04-10T09:31:50Z |
| publishDate | 2023-02-01 |
| publisher | Elsevier |
| record_format | Article |
| series | iScience |
| spelling | doaj.art-4018671075d844b5aab31079987c29212023-02-19T04:26:38ZengElsevieriScience2589-00422023-02-01262105942In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidationJing-Tan Han0Hui Su1Lida Tan2Chao-Jun Li3Department of Chemistry, and FRQNT Center for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street West, Montreal, QC H3A 0B8, CanadaDepartment of Chemistry, and FRQNT Center for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street West, Montreal, QC H3A 0B8, CanadaDepartment of Chemistry, and FRQNT Center for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street West, Montreal, QC H3A 0B8, CanadaDepartment of Chemistry, and FRQNT Center for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street West, Montreal, QC H3A 0B8, Canada; Corresponding authorSummary: The direct and selective transformation of naturally abundant methane (CH4) into high-value-added oxygenates, e.g., methanol, ethanol, and formic acid, is one of the “Holy Grails” in chemistry and chemical productions. However, complex mixtures of products, often due to over-oxidations, make such transformations highly challenging. Herein, gallium nitride (GaN), a methane-active semiconductor, catalyzes the photooxidation of methane and empowers the fine-controlling of chemoselectivity toward methanol and formic acids, simply by regulating the O2 content in water. In contrast to previous methods, no overoxidation products (CO2 and CO) were observed in this process. Mechanistic investigations and the corresponding quantitative experiments indicated that the controllable generation of moderately reactive oxygen radicals (•OOH and •OH) in combination with the direct methane activation triggered by GaN is responsible for the highly selective reactivity and tunability through a photo-generated radical process.http://www.sciencedirect.com/science/article/pii/S2589004223000196chemistrycatalysisgreen chemistry |
| spellingShingle | Jing-Tan Han Hui Su Lida Tan Chao-Jun Li In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation iScience chemistry catalysis green chemistry |
| title | In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation |
| title_full | In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation |
| title_fullStr | In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation |
| title_full_unstemmed | In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation |
| title_short | In aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation |
| title_sort | in aqua dual selective photocatalytic conversion of methane to formic acid and methanol with oxygen and water as oxidants without overoxidation |
| topic | chemistry catalysis green chemistry |
| url | http://www.sciencedirect.com/science/article/pii/S2589004223000196 |
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