Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature
The direct catalytic conversion of methane to liquid oxygenated compounds, such as methanol or dimethyl ether, at low temperature using molecular oxygen is a grand challenge in C–H activation that has never been met with synthetic, heterogeneous catalysts. We report the first demonstration of direct...
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| Format: | Article |
| Language: | en_US |
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American Chemical Society (ACS)
2017
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| Online Access: | http://hdl.handle.net/1721.1/109710 https://orcid.org/0000-0003-4111-0487 https://orcid.org/0000-0001-7638-6673 https://orcid.org/0000-0003-0657-1771 https://orcid.org/0000-0002-0025-4233 |
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| author | Narsimhan, Karthik Iyoki, Kenta Dinh, Kimberly Tam Roman, Yuriy |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Narsimhan, Karthik Iyoki, Kenta Dinh, Kimberly Tam Roman, Yuriy |
| author_sort | Narsimhan, Karthik |
| collection | MIT |
| description | The direct catalytic conversion of methane to liquid oxygenated compounds, such as methanol or dimethyl ether, at low temperature using molecular oxygen is a grand challenge in C–H activation that has never been met with synthetic, heterogeneous catalysts. We report the first demonstration of direct, catalytic oxidation of methane into methanol with molecular oxygen over copper-exchanged zeolites at low reaction temperatures (483–498 K). Reaction kinetics studies show sustained catalytic activity and high selectivity for a variety of commercially available zeolite topologies under mild conditions (e.g., 483 K and atmospheric pressure). Transient and steady state measurements with isotopically labeled molecules confirm catalytic turnover. The catalytic rates and apparent activation energies are affected by the zeolite topology, with caged-based zeolites (e.g., Cu-SSZ-13) showing the highest rates. Although the reaction rates are low, the discovery of catalytic sites in copper-exchanged zeolites will accelerate the development of strategies to directly oxidize methane into methanol under mild conditions. |
| first_indexed | 2024-09-23T15:20:35Z |
| format | Article |
| id | mit-1721.1/109710 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T15:20:35Z |
| publishDate | 2017 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1097102022-10-02T02:22:24Z Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature Narsimhan, Karthik Iyoki, Kenta Dinh, Kimberly Tam Roman, Yuriy Massachusetts Institute of Technology. Department of Chemical Engineering Narsimhan, Karthik Iyoki, Kenta Dinh, Kimberly Tam Roman, Yuriy The direct catalytic conversion of methane to liquid oxygenated compounds, such as methanol or dimethyl ether, at low temperature using molecular oxygen is a grand challenge in C–H activation that has never been met with synthetic, heterogeneous catalysts. We report the first demonstration of direct, catalytic oxidation of methane into methanol with molecular oxygen over copper-exchanged zeolites at low reaction temperatures (483–498 K). Reaction kinetics studies show sustained catalytic activity and high selectivity for a variety of commercially available zeolite topologies under mild conditions (e.g., 483 K and atmospheric pressure). Transient and steady state measurements with isotopically labeled molecules confirm catalytic turnover. The catalytic rates and apparent activation energies are affected by the zeolite topology, with caged-based zeolites (e.g., Cu-SSZ-13) showing the highest rates. Although the reaction rates are low, the discovery of catalytic sites in copper-exchanged zeolites will accelerate the development of strategies to directly oxidize methane into methanol under mild conditions. National Science Foundation (U.S.) (CHE-9808061) National Science Foundation (U.S.) (DBI-9729592) 2017-06-07T17:20:00Z 2017-06-07T17:20:00Z 2016-06 2016-05 Article http://purl.org/eprint/type/JournalArticle 2374-7943 2374-7951 http://hdl.handle.net/1721.1/109710 Narsimhan, Karthik; Iyoki, Kenta; Dinh, Kimberly and Román-Leshkov, Yuriy. “Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature.” ACS Central Science 2, no. 6 (June 2016): 424–429 © 2016 American Chemical Society https://orcid.org/0000-0003-4111-0487 https://orcid.org/0000-0001-7638-6673 https://orcid.org/0000-0003-0657-1771 https://orcid.org/0000-0002-0025-4233 en_US http://dx.doi.org/10.1021/acscentsci.6b00139 ACS Central Science Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Chemical Society (ACS) ACS |
| spellingShingle | Narsimhan, Karthik Iyoki, Kenta Dinh, Kimberly Tam Roman, Yuriy Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature |
| title | Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature |
| title_full | Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature |
| title_fullStr | Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature |
| title_full_unstemmed | Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature |
| title_short | Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature |
| title_sort | catalytic oxidation of methane into methanol over copper exchanged zeolites with oxygen at low temperature |
| url | http://hdl.handle.net/1721.1/109710 https://orcid.org/0000-0003-4111-0487 https://orcid.org/0000-0001-7638-6673 https://orcid.org/0000-0003-0657-1771 https://orcid.org/0000-0002-0025-4233 |
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