Journal
ACS ENERGY LETTERS
Volume 5, Issue 9, Pages 2811-2818Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c01266
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Funding
- Ontario Research Fund: Research Excellence Program
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- CIFAR Bio-Inspired Solar Energy program
- Joint Centre of Artificial Synthesis, a DOE Energy Innovation Hub through the Office of Science of the US Department of Energy [DE-SC0004993]
- Canada Foundation for Innovation
- Natural Sciences and Engineering Research Council of Canada
- University of Saskatchewan
- Government of Saskatchewan
- Western Economic Diversification Canada
- National Research Council Canada
- Canadian Institutes of Health Research
- Marie Sklodowska-Curie Fellowship H2020-MSCA-IF-2017 [793471]
- Banting postdoctoral fellowship
- NSERC E.W.R. Steacie Memorial Fellowship
- Marie Curie Actions (MSCA) [793471] Funding Source: Marie Curie Actions (MSCA)
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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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