Electrochemical CO2 capture with pH-independent redox chemistry
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arXiv
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| Main Authors: | , , , , , , , , , , |
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| Format: | Preprint |
| Published: |
2025
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| _version_ | 1866912217015779328 |
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| author | Kim, Sang Cheol Gigantino, Marco Holoubek, John Matthews, Jesse E. Chen, Junjie Dho, Yaereen Jaramillo, Thomas F. Cui, Yi Majumdar, Arun Tzeng, Yan-Kai Chu, Steven |
| author_facet | Kim, Sang Cheol Gigantino, Marco Holoubek, John Matthews, Jesse E. Chen, Junjie Dho, Yaereen Jaramillo, Thomas F. Cui, Yi Majumdar, Arun Tzeng, Yan-Kai Chu, Steven |
| contents | Capture of anthropogenic CO2 is critical for mitigating climate change, and reducing the energy cost is essential for wide-scale deployment. Solubility of inorganic carbon in aqueous solutions depends on the pH, and electrochemical modulation of the pH has been investigated as a means of CO2 capture and release. However, reported methods incur unavoidable energy costs due to thermodynamic penalties. In this study, we introduce a pH-independent redox chemistry that greatly lowers the thermodynamic energy costs by changing the pH without directly changing the [H+]. We show that the redox reaction of TEMPO molecules modulates the pH for capture and release of CO2 in a flow cell with an energy cost as low as 2.6 kJ/mol of CO2 corresponding to 0.027 eV/molecule. A molecular model, supported by MD and DFT simulations, is proposed of how the pH is decreased by 7.6 while largely avoiding the entropic energy cost associated with increasing the [H+]. We believe that this work showcases the potential of pH-independent redox chemistries for practical and cost-effective CO2 capture. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2502_01028 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Electrochemical CO2 capture with pH-independent redox chemistry Kim, Sang Cheol Gigantino, Marco Holoubek, John Matthews, Jesse E. Chen, Junjie Dho, Yaereen Jaramillo, Thomas F. Cui, Yi Majumdar, Arun Tzeng, Yan-Kai Chu, Steven Chemical Physics Capture of anthropogenic CO2 is critical for mitigating climate change, and reducing the energy cost is essential for wide-scale deployment. Solubility of inorganic carbon in aqueous solutions depends on the pH, and electrochemical modulation of the pH has been investigated as a means of CO2 capture and release. However, reported methods incur unavoidable energy costs due to thermodynamic penalties. In this study, we introduce a pH-independent redox chemistry that greatly lowers the thermodynamic energy costs by changing the pH without directly changing the [H+]. We show that the redox reaction of TEMPO molecules modulates the pH for capture and release of CO2 in a flow cell with an energy cost as low as 2.6 kJ/mol of CO2 corresponding to 0.027 eV/molecule. A molecular model, supported by MD and DFT simulations, is proposed of how the pH is decreased by 7.6 while largely avoiding the entropic energy cost associated with increasing the [H+]. We believe that this work showcases the potential of pH-independent redox chemistries for practical and cost-effective CO2 capture. |
| title | Electrochemical CO2 capture with pH-independent redox chemistry |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2502.01028 |