Leveraging Electrons for Electrochemical CO2 Capture Using a Hemi-Labile Iron Complex
Name
Angew Chem Int Ed - 2025 - Seo - Leveraging Electrons for Electrochemical CO2 Capture Using a Hemi‐Labile Iron Complex.pdf
Description
Published version
Size
2.33 MB
Format
Adobe PDF
Checksum (MD5)
c9d8a315c76f83e22ee0bcc8d1565158
Author(s)
Seo, Hyowon
Chen, Ying
Walter, Eric
Abdinejad, Maryam
Hatton, T Alan
Date Issued
August 4, 2025
Journal
Angewandte Chemie International Edition
Publisher
Wiley
Citation
H. Seo, Y. Chen, E. Walter, M. Abdinejad, T. A. Hatton, Angew. Chem. Int. Ed. 2025, 64, e202505723.
Version
Final published version
Abstract
Climate change, driven by anthropogenic carbon emissions, demands urgent action to prevent a 2050 tipping point. With CO2 levels at 427 ppm (50% above pre-industrial levels), deploying energy-efficient carbon capture technologies is crucial. Electrochemical carbon capture processes that have been touted to have the potential to meet these needs rely on the applied cell voltage, and electron utilization (CO2 molecules separated per electron), which has generally been asserted to have a theoretical limit of one. Here, we introduce an electron-leveraging strategy to enhance electron utilization beyond this limit to 1.43 by employing Fe-EDDHA, a redox-active coordination complex having a ligand with multiple hemi-labile coordination sites. The reversibility and robustness of the system were enabled by the efficient prevention of CO2 reduction upon the introduction of nicotinamide as a guardian of the iron(2+) center. The proof-of-concept cyclic system exhibits a minimum operational energy of 22.6 kJe mol−1 and an average of 63.7 kJe mol−1 over 29 cycles, using a simulated flue gas (15% CO2). Our electron-leveraging strategy holds promise for advancing energy-efficient electrochemical carbon capture technologies, and offers an alternative to prevalent redox potential shifting methods proposed to mitigate undesired electron transfer reactions in redox-active materials across diverse operational conditions.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
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Creative Commons Attribution
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DOI of Published Version
https://doi.org/10.1002/anie.202505723
