Ozden, Adnan and Li, Fengwang and Garcı́a de Arquer, F. Pelayo and Rosas-Hernández, Alonso and Thevenon, Arnaud and Wang, Yuhang and Hung, Sung-Fu and Wang, Xue and Chen, Bin and Li, Jun and Wicks, Joshua and Luo, Mingchuan and Wang, Ziyun and Agapie, Theodor and Peters, Jonas C. and Sargent, Edward H. and Sinton, David (2020) High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer. ACS Energy Letters, 5 (9). pp. 2811-2818. ISSN 2380-8195. doi:10.1021/acsenergylett.0c01266. https://resolver.caltech.edu/CaltechAUTHORS:20200818-072409036
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Abstract
Carbon dioxide (CO₂) electroreduction to valuable chemicals such as ethylene is an avenue to store renewable electricity and close the carbon cycle. Membrane electrode assembly (MEA) electrolyzers have attracted recent interest in light of their high stability and despite low productivity (a modest partial current density in CO₂-to-ethylene conversion of approximately 100 mA cm⁻²). Here we present an adlayer functionalization catalyst design: a catalyst/tetrahydro-phenanthrolinium/ionomer (CTPI) interface in which the catalytically active copper is functionalized using a phenanthrolinium-derived film and a perfluorocarbon-based polymeric ionomer. We find, using electroanalytical tools and operando spectroscopies, that this hierarchical adlayer augments both the local CO₂ availability and the adsorption of the key reaction intermediate CO on the catalyst surface. Using this CTPI catalyst, we achieve an ethylene Faradaic efficiency of 66% at a partial current density of 208 mA cm⁻²—a 2-fold increase over the best prior MEA electrolyzer report—and an improved full-cell energy efficiency of 21%.
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| Additional Information: | © 2020 American Chemical Society. Received: June 10, 2020; Accepted: August 6, 2020; Published: August 14, 2020. This work was financially supported by the Ontario Research Fund: Research Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, the CIFAR Bio-Inspired Solar Energy program 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. X-ray absorption spectra were performed on SXRMB beamlines at the Canadian Light Source (CLS), which is supported by the Canada Foundation for Innovation, Natural Sciences and Engineering Research Council of Canada, the University of Saskatchewan, the Government of Saskatchewan, Western Economic Diversification Canada, the National Research Council Canada, and the Canadian Institutes of Health Research. The authors acknowledge Ontario Centre for the Characterization of Advanced Materials (OCCAM) for sample preparation and characterization facilities and thank Dr. Alexander H. Ip, Dr. Christine Gabardo and Mr. Colin P. O’Brien for useful discussions. A.T. acknowledges Marie Skłodowska-Curie Fellowship H2020-MSCA-IF-2017 (793471). J.L. acknowledges the Banting postdoctoral fellowship. D.S. acknowledges the NSERC E.W.R. Steacie Memorial Fellowship. Author Contributions: A.O. and F.L. contributed equally to this work. D.S. and E.H.S. supervised the project. A.O. conceived the idea and carried out the electrochemical experiments with advice from F.L.. A.T. and A.R.-H. synthesized and characterized the tetrahydro-phenanthrolinium. A.O. carried out Raman and EIS measurements. Y.W. and A.O. carried out SEM imaging. F.L. and S.F.H. designed the XAS measurements. S.-F.H. performed the XAS measurements. X.W. performed the NMR analysis and provided help in EIS measurements. B.C. and Y.W. performed the TEM analysis. J.W. performed XPS measurements. M.L., J.L., and Z.W. provided help in electrochemical experiments. A.O. and F.L. wrote the manuscript. F.P.G.A. provided help in manuscript writing. All authors discussed the results and assisted during manuscript preparation. The authors declare no competing financial interest. | ||||||||||||||||||||||||||||
| Group: | JCAP | ||||||||||||||||||||||||||||
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| Issue or Number: | 9 | ||||||||||||||||||||||||||||
| DOI: | 10.1021/acsenergylett.0c01266 | ||||||||||||||||||||||||||||
| Record Number: | CaltechAUTHORS:20200818-072409036 | ||||||||||||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20200818-072409036 | ||||||||||||||||||||||||||||
| Official Citation: | High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer. Adnan Ozden, Fengwang Li, F. Pelayo Garcı́a de Arquer, Alonso Rosas-Hernández, Arnaud Thevenon, Yuhang Wang, Sung-Fu Hung, Xue Wang, Bin Chen, Jun Li, Joshua Wicks, Mingchuan Luo, Ziyun Wang, Theodor Agapie, Jonas C. Peters, Edward H. Sargent, and David Sinton. ACS Energy Letters 2020 5 (9), 2811-2818; DOI: 10.1021/acsenergylett.0c01266 | ||||||||||||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||||||||||
| ID Code: | 104987 | ||||||||||||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||||||||||||
| Deposited By: | Tony Diaz | ||||||||||||||||||||||||||||
| Deposited On: | 18 Aug 2020 15:32 | ||||||||||||||||||||||||||||
| Last Modified: | 16 Nov 2021 18:38 |
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