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Efficient electrocatalytic conversion of CO2 to ethanol enabled by imidazolium-functionalized ionomer confined molybdenum phosphide

Journal Article · · Applied Catalysis. B, Environmental
 [1];  [1];  [2];  [3];  [3];  [1];  [3];  [3];  [2];  [1];  [1]
  1. Illinois Institute of Technology, Chicago, IL (United States)
  2. Argonne National Laboratory (ANL), Argonne, IL (United States)
  3. Univ. of Illinois, Chicago, IL (United States)
+ Show Author Affiliations
An effective electrochemical carbon dioxide reduction reaction (eCO2RR) requires the discovery of a catalytic system that is highly active and selective for multi-carbon products together with superior CO2 diffusion at a catalyst layer to minimize the reduction barriers. Here, we found a catalytic system that uses molybdenum phosphide (MoP) nanoparticles covered by imidazolium-functionalized ionomer (Im) that promotes CO2 diffusion at the catalyst layer toward the catalyst surface, where CO2 is reduced to ethanol (C2H5OH). The electrochemical results with the MoP-Im co-catalyst show a C2H5OH production Faradaic efficiency and a cathodic energy efficiency of 77.4% and 63.3%, respectively, at a potential as low as - 200 mV vs. RHE. The electrochemical experiments along with our physicochemical characterizations indicate that the Im improves CO2 diffusion and balances water content resulting in a higher CO2-to-water ratio at the catalyst layer and fine-tunes the electronic properties of Mo atoms at the MoP surface. Finally, in-situ Raman spectroscopy reveals that a high number of adsorbed *CO intermediates on the surface and a higher binding strength of *CO intermediates on the Mo surface sites in the presence of imidazolium molecules are the main reasons for a superior C-C coupling and thereby the improved C2H5OH formation.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
Grant/Contract Number:
AC02-06CH11357; AR0001581
OSTI ID:
2439556
Journal Information:
Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 317; ISSN 0926-3373
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 reduction reaction
ethanol electrosynthesis
imidazolium
in-situ Raman
transition metal phosphides