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Cascade CO₂ electroreduction enables efficient carbonate-free production of ethylene

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.

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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.

Item Type:Article
Related URLs:
URLURL TypeDescription
Ozden, Adnan0000-0002-6924-1967
Wang, Yuhang0000-0001-5336-5183
Li, Fengwang0000-0003-1531-2966
Thevenon, Arnaud0000-0002-5543-6595
Rosas-Hernández, Alonso0000-0002-0812-5591
Agapie, Theodor0000-0002-9692-7614
Peters, Jonas C.0000-0002-6610-4414
Sargent, Edward H.0000-0003-0396-6495
Sinton, David0000-0003-2714-6408
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.
Funding AgencyGrant Number
Ontario Research FoundationUNSPECIFIED
Natural Sciences and Engineering Research Council of Canada (NSERC)UNSPECIFIED
Canadian Institute for Advanced Research (CIFAR)UNSPECIFIED
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE-SC0004993
Marie Curie Fellowship793471
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
Record Number:CaltechAUTHORS:20210216-140504601
Persistent URL:
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, (
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108073
Deposited By: George Porter
Deposited On:16 Feb 2021 23:53
Last Modified:16 Nov 2021 19:08

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