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Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid
Photochemical conversion of CO(2) into fuels has promise as a strategy for storage of intermittent solar energy in the form of chemical bonds. However, higher-energy-value hydrocarbons are rarely produced by this strategy, because of kinetic challenges. Here we demonstrate a strategy for green-light...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2019
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6494896/ https://www.ncbi.nlm.nih.gov/pubmed/31043604 http://dx.doi.org/10.1038/s41467-019-10084-5 |
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author | Yu, Sungju Jain, Prashant K. |
author_facet | Yu, Sungju Jain, Prashant K. |
author_sort | Yu, Sungju |
collection | PubMed |
description | Photochemical conversion of CO(2) into fuels has promise as a strategy for storage of intermittent solar energy in the form of chemical bonds. However, higher-energy-value hydrocarbons are rarely produced by this strategy, because of kinetic challenges. Here we demonstrate a strategy for green-light-driven synthesis of C(1)–C(3) hydrocarbons from CO(2) and H(2)O. In this approach, plasmonic excitation of Au nanoparticles produces a charge-rich environment at the nanoparticle/solution interface conducive for CO(2) activation, while an ionic liquid stabilizes charged intermediates formed at this interface, facilitating multi-step reduction and C–C coupling. Methane, ethylene, acetylene, propane, and propene are photosynthesized with a C(2+) selectivity of ~50% under the most optimal conditions. Hydrocarbon turnover exhibits a volcano relationship as a function of the ionic liquid concentration, the kinetic analysis of which coupled with density functional theory simulations provides mechanistic insights into the synergy between plasmonic excitation and the ionic liquid. |
format | Online Article Text |
id | pubmed-6494896 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-64948962019-05-03 Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid Yu, Sungju Jain, Prashant K. Nat Commun Article Photochemical conversion of CO(2) into fuels has promise as a strategy for storage of intermittent solar energy in the form of chemical bonds. However, higher-energy-value hydrocarbons are rarely produced by this strategy, because of kinetic challenges. Here we demonstrate a strategy for green-light-driven synthesis of C(1)–C(3) hydrocarbons from CO(2) and H(2)O. In this approach, plasmonic excitation of Au nanoparticles produces a charge-rich environment at the nanoparticle/solution interface conducive for CO(2) activation, while an ionic liquid stabilizes charged intermediates formed at this interface, facilitating multi-step reduction and C–C coupling. Methane, ethylene, acetylene, propane, and propene are photosynthesized with a C(2+) selectivity of ~50% under the most optimal conditions. Hydrocarbon turnover exhibits a volcano relationship as a function of the ionic liquid concentration, the kinetic analysis of which coupled with density functional theory simulations provides mechanistic insights into the synergy between plasmonic excitation and the ionic liquid. Nature Publishing Group UK 2019-05-01 /pmc/articles/PMC6494896/ /pubmed/31043604 http://dx.doi.org/10.1038/s41467-019-10084-5 Text en © The Author(s) 2019 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
spellingShingle | Article Yu, Sungju Jain, Prashant K. Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid |
title | Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid |
title_full | Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid |
title_fullStr | Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid |
title_full_unstemmed | Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid |
title_short | Plasmonic photosynthesis of C(1)–C(3) hydrocarbons from carbon dioxide assisted by an ionic liquid |
title_sort | plasmonic photosynthesis of c(1)–c(3) hydrocarbons from carbon dioxide assisted by an ionic liquid |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6494896/ https://www.ncbi.nlm.nih.gov/pubmed/31043604 http://dx.doi.org/10.1038/s41467-019-10084-5 |
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