Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasma
This study explores an in-liquid plasma process for converting carbon dioxide into value-added organic compounds using aqueous sodium carbonate solutions derived from CO₂ captured by sodium hydroxide. The method operates without hydrogen gas or catalysts, aligning with carbon-neutral strategies. Dur...
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Elsevier
2025-09-01
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| Series: | Journal of CO2 Utilization |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S221298202500143X |
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| author | Ryota Shiba Shinfuku Nomura Akihiro Kakubo Kohei Baba Ryo Shimizu Junichi Nakajima Teruo Henmi |
| author_facet | Ryota Shiba Shinfuku Nomura Akihiro Kakubo Kohei Baba Ryo Shimizu Junichi Nakajima Teruo Henmi |
| author_sort | Ryota Shiba |
| collection | DOAJ |
| description | This study explores an in-liquid plasma process for converting carbon dioxide into value-added organic compounds using aqueous sodium carbonate solutions derived from CO₂ captured by sodium hydroxide. The method operates without hydrogen gas or catalysts, aligning with carbon-neutral strategies. During plasma treatment, the measured emission spectroscopy (ES) confirmed the formation of reactive species, including CH (431, 387 nm), CO (336, 295 nm), OH (308, 283, 282 nm), O (777, 845 nm), and H radicals (656 nm [Hα], 486 nm [Hβ]). Electron temperature estimated by [Hβ]/[Hα] of ES is in the range between 4500 and 5500 K for this plasma condition. These species are generated via vibronic coupling: interactions between molecular vibrations and orbital electronic states in CO₂ and H₂O at these plasma temperatures. CH radicals, formed by hetero-coupling of C and H, play a key role in subsequent synthesis. Gas chromatography-mass spectrometry (GC-MS) at quenching process detected acetone (retention time: 1.56 min) and ethanol (2.06 min). Ab initio calculations reveal the reaction pathways: 2 CH + 4 H + CO → CH₃COCH₃ ，2 CH + 3 H + OH → C₂H₅OH. The yield of acetone (8 mg/L) is lower compared with ethanol (14.3 mg/L) under the cooling conditions. The process proceeds through repeated plasma–quenching cycles, approaching an apparent chemical equilibrium within 60 min. This plasma method demonstrates an efficient and sustainable route for CO₂ utilization of carbonate and water, offering a promising approach for carbon-neutral fuel production and Carbon Capture, Utilization, and Storage (CCUS) process. |
| format | Article |
| id | doaj-art-72b804e5ea8e4302b7383c1bb418c7bd |
| institution | DOAJ |
| issn | 2212-9839 |
| language | English |
| publishDate | 2025-09-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Journal of CO2 Utilization |
| spelling | doaj-art-72b804e5ea8e4302b7383c1bb418c7bd2025-08-20T02:45:50ZengElsevierJournal of CO2 Utilization2212-98392025-09-019910315910.1016/j.jcou.2025.103159Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasmaRyota Shiba0Shinfuku Nomura1Akihiro Kakubo2Kohei Baba3Ryo Shimizu4Junichi Nakajima5Teruo Henmi6Graduate School of Science and Engineering, Ehime University, Matsuyama 790-8577, Japan; Institute of Environmental Sciences and Technology, Oono Associates, Tōon-shi, Ehime 791-0321, JapanGraduate School of Science and Engineering, Ehime University, Matsuyama 790-8577, Japan; Corresponding author.Graduate School of Science and Engineering, Ehime University, Matsuyama 790-8577, JapanGraduate School of Science and Engineering, Ehime University, Matsuyama 790-8577, JapanInstitute of Environmental Sciences and Technology, Oono Associates, Tōon-shi, Ehime 791-0321, JapanGraduate School of Science and Engineering, Ehime University, Matsuyama 790-8577, JapanEmeritus Professor of Ehime University, Matsuyama 790-8577, JapanThis study explores an in-liquid plasma process for converting carbon dioxide into value-added organic compounds using aqueous sodium carbonate solutions derived from CO₂ captured by sodium hydroxide. The method operates without hydrogen gas or catalysts, aligning with carbon-neutral strategies. During plasma treatment, the measured emission spectroscopy (ES) confirmed the formation of reactive species, including CH (431, 387 nm), CO (336, 295 nm), OH (308, 283, 282 nm), O (777, 845 nm), and H radicals (656 nm [Hα], 486 nm [Hβ]). Electron temperature estimated by [Hβ]/[Hα] of ES is in the range between 4500 and 5500 K for this plasma condition. These species are generated via vibronic coupling: interactions between molecular vibrations and orbital electronic states in CO₂ and H₂O at these plasma temperatures. CH radicals, formed by hetero-coupling of C and H, play a key role in subsequent synthesis. Gas chromatography-mass spectrometry (GC-MS) at quenching process detected acetone (retention time: 1.56 min) and ethanol (2.06 min). Ab initio calculations reveal the reaction pathways: 2 CH + 4 H + CO → CH₃COCH₃ ，2 CH + 3 H + OH → C₂H₅OH. The yield of acetone (8 mg/L) is lower compared with ethanol (14.3 mg/L) under the cooling conditions. The process proceeds through repeated plasma–quenching cycles, approaching an apparent chemical equilibrium within 60 min. This plasma method demonstrates an efficient and sustainable route for CO₂ utilization of carbonate and water, offering a promising approach for carbon-neutral fuel production and Carbon Capture, Utilization, and Storage (CCUS) process.http://www.sciencedirect.com/science/article/pii/S221298202500143XIn-liquid-plasmaWaterSodium-carbonateCarbon-neutralE-fuel |
| spellingShingle | Ryota Shiba Shinfuku Nomura Akihiro Kakubo Kohei Baba Ryo Shimizu Junichi Nakajima Teruo Henmi Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasma Journal of CO2 Utilization In-liquid-plasma Water Sodium-carbonate Carbon-neutral E-fuel |
| title | Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasma |
| title_full | Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasma |
| title_fullStr | Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasma |
| title_full_unstemmed | Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasma |
| title_short | Formation of selected organic compounds from aqueous sodium carbonate solution via hetero-coupling of carbon and hydrogen by in-liquid plasma |
| title_sort | formation of selected organic compounds from aqueous sodium carbonate solution via hetero coupling of carbon and hydrogen by in liquid plasma |
| topic | In-liquid-plasma Water Sodium-carbonate Carbon-neutral E-fuel |
| url | http://www.sciencedirect.com/science/article/pii/S221298202500143X |
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