High-rate and efficient ethylene electrosynthesis using a catalyst/promoter/transport layer

Adnan Ozden; Fengwang Li; F. Pelayo Garcĺa 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; David Sinton

doi:10.1021/acsenergylett.0c01266

High-rate and efficient ethylene electrosynthesis using a catalyst/promoter/transport layer

Adnan Ozden, Fengwang Li, F. Pelayo Garcĺa 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, David Sinton^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

114 Scopus citations

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%.

Original language	English (US)
Pages (from-to)	2811-2818
Number of pages	8
Journal	ACS Energy Letters
Volume	5
Issue number	9
DOIs	https://doi.org/10.1021/acsenergylett.0c01266
State	Published - Sep 11 2020

Funding

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.

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsenergylett.0c01266

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Ozden, A., Li, F., Garcĺa De Arquer, F. P., Rosas-Hernández, A., Thevenon, A., Wang, Y., Hung, S. F., Wang, X., Chen, B., Li, J., Wicks, J., Luo, M., Wang, Z., Agapie, T., Peters, J. C., Sargent, E. H., & Sinton, D. (2020). High-rate and efficient ethylene electrosynthesis using a catalyst/promoter/transport layer. ACS Energy Letters, 5(9), 2811-2818. https://doi.org/10.1021/acsenergylett.0c01266

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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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doi = "10.1021/acsenergylett.0c01266",

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Ozden, A, Li, F, Garcĺa De Arquer, FP, Rosas-Hernández, A, Thevenon, A, Wang, Y, Hung, SF, Wang, X, Chen, B, Li, J, Wicks, J, Luo, M, Wang, Z, Agapie, T, Peters, JC, Sargent, EH & Sinton, D 2020, 'High-rate and efficient ethylene electrosynthesis using a catalyst/promoter/transport layer', ACS Energy Letters, vol. 5, no. 9, pp. 2811-2818. https://doi.org/10.1021/acsenergylett.0c01266

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T1 - High-rate and efficient ethylene electrosynthesis using a catalyst/promoter/transport layer

AU - Ozden, Adnan

AU - Li, Fengwang

AU - Garcĺa De Arquer, F. Pelayo

AU - Rosas-Hernández, Alonso

AU - Thevenon, Arnaud

AU - Wang, Yuhang

AU - Hung, Sung Fu

AU - Wang, Xue

AU - Chen, Bin

AU - Li, Jun

AU - Wicks, Joshua

AU - Luo, Mingchuan

AU - Wang, Ziyun

AU - Agapie, Theodor

AU - Peters, Jonas C.

AU - Sargent, Edward H.

AU - Sinton, David

PY - 2020/9/11

Y1 - 2020/9/11

N2 - 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%.

AB - 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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High-rate and efficient ethylene electrosynthesis using a catalyst/promoter/transport layer

Abstract

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ASJC Scopus subject areas

UN SDGs

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