Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation
Abstract The direct utilization of dissolved inorganic carbon in seawater for CO2 conversion promises chemical production on-demand and with zero carbon footprint. Photoelectrochemical (PEC) CO2 reduction (CO2R) devices promise the sustainable conversion of dissolved carbon in seawater to carbon pro...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56106-3 |
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| author | Bin Liu Zheng Qian Xiang Shi Haoqing Su Wentao Zhang Atsu Kludze Yuze Zheng Chengxing He Rito Yanagi Shu Hu |
| author_facet | Bin Liu Zheng Qian Xiang Shi Haoqing Su Wentao Zhang Atsu Kludze Yuze Zheng Chengxing He Rito Yanagi Shu Hu |
| author_sort | Bin Liu |
| collection | DOAJ |
| description | Abstract The direct utilization of dissolved inorganic carbon in seawater for CO2 conversion promises chemical production on-demand and with zero carbon footprint. Photoelectrochemical (PEC) CO2 reduction (CO2R) devices promise the sustainable conversion of dissolved carbon in seawater to carbon products using sunlight as the only energy input. However, the diffusion-dominant transport mechanism and the near-zero concentration of CO2(aq) (CO2 dissolved in aqueous solution) in static seawater has made it extremely challenging to achieve high solar-to-fuel (STF) efficiency and high carbon-product selectivity. Here, where CO2(aq) as a reactant generated in situ by acidification of HCO3 - flows continuously from BiVO4 photoanodes to Si photocathodes, enabling a single-step conversion of dissolved carbon into products. Our PEC device significantly increases the CO selectivity from 3% to 21%, which approaches the 30% theoretical limit according to multi-physics modeling. Meanwhile, the Si/BiVO4 PEC CO2R device achieved a STF efficiency of 0.71%. Such flow engineering achieves flow-dependent selectivity, rate, and stability in simulated seawater, thus promising practical solar fuel production at scale. |
| format | Article |
| id | doaj-art-e4addb22ea054e4498b92f99453b1071 |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-e4addb22ea054e4498b92f99453b10712025-08-20T02:13:02ZengNature PortfolioNature Communications2041-17232025-02-0116111210.1038/s41467-025-56106-3Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generationBin Liu0Zheng Qian1Xiang Shi2Haoqing Su3Wentao Zhang4Atsu Kludze5Yuze Zheng6Chengxing He7Rito Yanagi8Shu Hu9Department of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityDepartment of Chemical and Environmental Engineering, School of Engineering and Applied Sciences, Yale UniversityAbstract The direct utilization of dissolved inorganic carbon in seawater for CO2 conversion promises chemical production on-demand and with zero carbon footprint. Photoelectrochemical (PEC) CO2 reduction (CO2R) devices promise the sustainable conversion of dissolved carbon in seawater to carbon products using sunlight as the only energy input. However, the diffusion-dominant transport mechanism and the near-zero concentration of CO2(aq) (CO2 dissolved in aqueous solution) in static seawater has made it extremely challenging to achieve high solar-to-fuel (STF) efficiency and high carbon-product selectivity. Here, where CO2(aq) as a reactant generated in situ by acidification of HCO3 - flows continuously from BiVO4 photoanodes to Si photocathodes, enabling a single-step conversion of dissolved carbon into products. Our PEC device significantly increases the CO selectivity from 3% to 21%, which approaches the 30% theoretical limit according to multi-physics modeling. Meanwhile, the Si/BiVO4 PEC CO2R device achieved a STF efficiency of 0.71%. Such flow engineering achieves flow-dependent selectivity, rate, and stability in simulated seawater, thus promising practical solar fuel production at scale.https://doi.org/10.1038/s41467-025-56106-3 |
| spellingShingle | Bin Liu Zheng Qian Xiang Shi Haoqing Su Wentao Zhang Atsu Kludze Yuze Zheng Chengxing He Rito Yanagi Shu Hu Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation Nature Communications |
| title | Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation |
| title_full | Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation |
| title_fullStr | Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation |
| title_full_unstemmed | Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation |
| title_short | Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation |
| title_sort | solar driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation |
| url | https://doi.org/10.1038/s41467-025-56106-3 |
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