Ozden, Adnan and Wang, Yuhang and Li, Fengwang and Luo, Mingchuan and Sisler, Jared and Thevenon, Arnaud and Rosas-Hernández, Alonso and Burdyny, Thomas and Lum, Yanwei and Yadegari, Hossein and Agapie, Theodor and Peters, Jonas C. and Sargent, Edward H. and Sinton, David (2021) Cascade CO₂ electroreduction enables efficient carbonate-free production of ethylene. Joule, 5 (3). pp. 706-719. ISSN 2542-4351. doi:10.1016/j.joule.2021.01.007. https://resolver.caltech.edu/CaltechAUTHORS:20210216-140504601
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Abstract
CO₂ electroreduction provides a route to convert waste emissions into chemicals such as ethylene (C₂H₄). However, the direct transformation of CO₂-to-C₂H₄ suffers from CO₂ loss to carbonate, consuming up to 72% of energy input. A cascade approach—coupling a solid-oxide CO₂-to-CO electrochemical cell (SOEC) with a CO-to-C₂H₄ membrane electrode assembly (MEA)—would eliminate CO₂ loss to carbonate. However, this approach requires a CO-to-C₂H₄ MEA with energy efficiency well beyond demonstrations to date. Focusing on the MEA, we find that an N-tolyl substituted tetrahydro-bipyridine film improves the stabilization of key reaction intermediates, while an SSC ionomer enhances CO transport to the Cu surface, enabling a C₂H₄ faradaic efficiency of 65% at 150 mA cm⁻² for 110 h. Demonstrating a cascade SOEC-MEA approach, we achieve CO₂-to-C₂H₄ with a ~48% reduction in energy intensity compared with the direct route. We further reduce the energy intensity by coupling CO electroreduction (CORR) with glucose electrooxidation.
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Alternate Title: | Cascade CO2 electroreduction enables efficient carbonate-free production of ethylene | ||||||||||||||||||||
Additional Information: | © 2021 Elsevier. Received 19 October 2020, Revised 1 December 2020, Accepted 21 January 2021, Available online 15 February 2021. The authors acknowledge Ontario Centre for the Characterization of Advanced Materials (OCCAM) for sample preparation and characterization facilities. Funding: this work received financial support from the Ontario Research Foundation: Research Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, the CIFAR Bio-Inspired Solar Energy program and TOTAL S.E. and the Joint Centre of Artificial Synthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under award no. DE-SC0004993. D.S. acknowledges the NSERC E.W.R Steacie Memorial Fellowship. A.T. acknowledges Marie Skłodowska-Curie Fellowship H2020-MSCA-IF-2017 (793471). The authors thank Dr. Y.-F. Liao for the GIWAXS measurements at Spring-8 BL-12B2 beamline of NSRRC. The authors also thank Dr. T. Regier for their assistance at the SGM beamline of CLS. Author contributions. D.S. and E.H.S. supervised the project. A.O. carried out all the electrochemical experiments with advice from Y.W. and F.L. A.T., A.R.-H., J.C.P., and T.A. designed and synthesized the N-tolylpyridinium molecule and contributed to the manuscript editing. A.O. and F.L. carried out Raman spectroscopies. Y.W. performed the SEM and TEM analysis. A.O. performed the nuclear magnetic resonance spectroscopies. A.O. and Y.W. co-wrote the manuscript. J.S. performed the TEA modeling. T.B. conducted the CO diffusion modeling. M.L., Y.L., and H.Y. contributed to the discussions and manuscript editing. A.O., Y.W., and F.L. provided equal contributions to this study. All authors contributed to the manuscript. Declaration of interests. A.O., Y.W., F.L., D.S., and E.H.S. have filled provisional patent application no. 63/135,277 regarding Cascade CO2 electroreduction systems. | ||||||||||||||||||||
Group: | JCAP | ||||||||||||||||||||
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Subject Keywords: | CO electroreduction; carbon utilization; ethylene electrolysis; electrolyser; membrane electrode assembly; solid-oxide electrolyser; catalyst design; molecular catalyst; energy efficiency | ||||||||||||||||||||
Issue or Number: | 3 | ||||||||||||||||||||
DOI: | 10.1016/j.joule.2021.01.007 | ||||||||||||||||||||
Record Number: | CaltechAUTHORS:20210216-140504601 | ||||||||||||||||||||
Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20210216-140504601 | ||||||||||||||||||||
Official Citation: | Adnan Ozden, Yuhang Wang, Fengwang Li, Mingchuan Luo, Jared Sisler, Arnaud Thevenon, Alonso Rosas-Hernández, Thomas Burdyny, Yanwei Lum, Hossein Yadegari, Theodor Agapie, Jonas C. Peters, Edward H. Sargent, David Sinton, Cascade CO2 electroreduction enables efficient carbonate-free production of ethylene, Joule, Volume 5, Issue 3, 2021, Pages 706-719, ISSN 2542-4351, https://doi.org/10.1016/j.joule.2021.01.007. (https://www.sciencedirect.com/science/article/pii/S2542435121000386) | ||||||||||||||||||||
Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||
ID Code: | 108073 | ||||||||||||||||||||
Collection: | CaltechAUTHORS | ||||||||||||||||||||
Deposited By: | George Porter | ||||||||||||||||||||
Deposited On: | 16 Feb 2021 23:53 | ||||||||||||||||||||
Last Modified: | 16 Nov 2021 19:08 |
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