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Title: A Bifunctional Ionic Liquid for Capture and Electrochemical Conversion of CO2 to CO over Silver

Journal Article · · ACS Catalysis
ORCiD logo [1]; ORCiD logo [1];  [1];  [2];  [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Case Western Reserve University, Cleveland, OH (United States)
  2. University of California, Davis, CA (United States)
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Electrochemical conversion of CO2 requires selective catalysts and high solubility of CO2 in the electrolyte to reduce the energy requirement and increase the current efficiency. In this study, the CO2 reduction reaction (CO2RR) over Ag electrodes in acetonitrile-based electrolytes containing 0.1 M [EMIM][2-CNpyr] (1-ethyl-3-methylimidazolium 2-cyanopyrolide), a reactive ionic liquid (IL), is shown to selectively (>94%) convert CO2 to CO with a stable current density (6 mA·cm–2) for at least 12 h. The linear sweep voltammetry experiments show the onset potential of CO2 reduction in acetonitrile shifts positively by 240 mV when [EMIM][2-CNpyr] is added. This is attributed to the pre-activation of CO2 through the carboxylate formation via the carbene intermediate of the [EMIM]+ cation and the carbamate formation via binding to the nucleophilic [2-CNpyr]– anion. The analysis of the electrode–electrolyte interface by surface-enhanced Raman spectroscopy (SERS) confirms the catalytic role of the functionalized IL where the accumulation of the IL-CO2 adduct between –1.7 and –2.3 V vs Ag/Ag+ and the simultaneous CO formation are captured. Furthermore, this study reveals the electrode surface species and the role of the functionalized ions in lowering the energy requirement of CO2RR for the design of multifunctional electrolytes for the integrated capture and conversion.

Research Organization:
Case Western Reserve Univ., Cleveland, OH (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); American Chemical Society Petroleum Research; National Institutes of Health (NIH)
Grant/Contract Number:
SC0022214; PRF 59520-DNI4; R35GM126961; SC0023427
OSTI ID:
1985644
Alternate ID(s):
OSTI ID: 1975317
Journal Information:
ACS Catalysis, Vol. 13, Issue 12; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
electrochemical CO2 reduction
ionic liquid
faradaic efficiency
carbon monoxide
carbon capture and utilization
anions
electrodes
electrolysis
electrolytes
inorganic carbon compounds