High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons
Abstract Electrochemical carbon dioxide (CO2) conversion to hydrocarbon fuels, such as methane (CH4), offers a promising solution for the long-term and large-scale storage of renewable electricity. To enable this technology, CO2-to-CH4 conversion must achieve high selectivity and energy efficiency a...
| Main Authors: | , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-38963-y |
| _version_ | 1797811396086333440 |
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| author | Cornelius A. Obasanjo Guorui Gao Jackson Crane Viktoria Golovanova F. Pelayo García de Arquer Cao-Thang Dinh |
| author_facet | Cornelius A. Obasanjo Guorui Gao Jackson Crane Viktoria Golovanova F. Pelayo García de Arquer Cao-Thang Dinh |
| author_sort | Cornelius A. Obasanjo |
| collection | DOAJ |
| description | Abstract Electrochemical carbon dioxide (CO2) conversion to hydrocarbon fuels, such as methane (CH4), offers a promising solution for the long-term and large-scale storage of renewable electricity. To enable this technology, CO2-to-CH4 conversion must achieve high selectivity and energy efficiency at high currents. Here, we report an electrochemical conversion system that features proton-bicarbonate-CO2 mass transport management coupled with an in-situ copper (Cu) activation strategy to achieve high CH4 selectivity at high currents. We find that open matrix Cu electrodes sustain sufficient local CO2 concentration by combining both dissolved CO2 and in-situ generated CO2 from the bicarbonate. In-situ Cu activation through alternating current operation renders and maintains the catalyst highly selective towards CH4. The combination of these strategies leads to CH4 Faradaic efficiencies of over 70% in a wide current density range (100 – 750 mA cm-2) that is stable for at least 12 h at a current density of 500 mA cm-2. The system also delivers a CH4 concentration of 23.5% in the gas product stream. |
| first_indexed | 2024-03-13T07:23:04Z |
| format | Article |
| id | doaj.art-3ce39b496593455bb74ff09fbafeedf3 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T07:23:04Z |
| publishDate | 2023-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-3ce39b496593455bb74ff09fbafeedf32023-06-04T11:33:03ZengNature PortfolioNature Communications2041-17232023-06-0114111210.1038/s41467-023-38963-yHigh-rate and selective conversion of CO2 from aqueous solutions to hydrocarbonsCornelius A. Obasanjo0Guorui Gao1Jackson Crane2Viktoria Golovanova3F. Pelayo García de Arquer4Cao-Thang Dinh5Department of Chemical Engineering, Queen’s UniversityDepartment of Chemical Engineering, Queen’s UniversityDepartment of Chemical Engineering, Queen’s UniversityICFO–Institut de Ciències Fotòniques, The Barcelona Institute of Science and TechnologyICFO–Institut de Ciències Fotòniques, The Barcelona Institute of Science and TechnologyDepartment of Chemical Engineering, Queen’s UniversityAbstract Electrochemical carbon dioxide (CO2) conversion to hydrocarbon fuels, such as methane (CH4), offers a promising solution for the long-term and large-scale storage of renewable electricity. To enable this technology, CO2-to-CH4 conversion must achieve high selectivity and energy efficiency at high currents. Here, we report an electrochemical conversion system that features proton-bicarbonate-CO2 mass transport management coupled with an in-situ copper (Cu) activation strategy to achieve high CH4 selectivity at high currents. We find that open matrix Cu electrodes sustain sufficient local CO2 concentration by combining both dissolved CO2 and in-situ generated CO2 from the bicarbonate. In-situ Cu activation through alternating current operation renders and maintains the catalyst highly selective towards CH4. The combination of these strategies leads to CH4 Faradaic efficiencies of over 70% in a wide current density range (100 – 750 mA cm-2) that is stable for at least 12 h at a current density of 500 mA cm-2. The system also delivers a CH4 concentration of 23.5% in the gas product stream.https://doi.org/10.1038/s41467-023-38963-y |
| spellingShingle | Cornelius A. Obasanjo Guorui Gao Jackson Crane Viktoria Golovanova F. Pelayo García de Arquer Cao-Thang Dinh High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons Nature Communications |
| title | High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons |
| title_full | High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons |
| title_fullStr | High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons |
| title_full_unstemmed | High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons |
| title_short | High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons |
| title_sort | high rate and selective conversion of co2 from aqueous solutions to hydrocarbons |
| url | https://doi.org/10.1038/s41467-023-38963-y |
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