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Title:Low temperature electrocatalytic reduction of carbon dioxide utilizing room temperature ionic liquids
Author(s):Rosen, Brian
Director of Research:Kenis, Paul J.A.
Doctoral Committee Chair(s):Kenis, Paul J.A.
Doctoral Committee Member(s):Masel, Richard I.; Harley, Brendan A.; Dlott, Dana D.
Department / Program:Chemical & Biomolecular Engr
Discipline:Chemical Engineering
Degree Granting Institution:University of Illinois at Urbana-Champaign
Degree:Ph.D.
Genre:Dissertation
Subject(s):Carbon Dioxide (CO2)
ionic liquid
overpotential
catalysis
overpotential
Abstract:Artificial photosynthesis, where one uses electricity from the sun, or wind, to convert water and carbon dioxide into a hydrocarbon fuel could provide a viable route to renewable fuels but so far the results have been stymied because of the lack of a CO2 conversion catalyst that operates at low overpotentials. In this study we report a catalyst system that shows CO2 conversion at low overpotentials. The system uses two different catalysts to achieve the conversion. First an ionic liquid or ionic salt is used to catalyze the formation of a “(CO2)-” intermediate. Then a transition metal is used to catalyze the conversion of the “(CO2)-” intermediate into useful products. CO formation is first observed at -450mV with respect to a standard hydrogen electrode (SHE), compared to 800mV in the absence of the ionic liquid. Thus, CO2 conversion to CO can occur without the large energy loss associated with a high overpotential, raising the possibility of practical artificial photosynthesis. The reduction of CO2 in 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIM BF4) was studied in an H-type electrochemical cell, an in-situ SFG cell, in and in an EXAFS cell. This diagnostic data enabled the design of a continuous flow CO2 electrolysis cell. Results from these experiments suggest that the EMIM BF4 is able to catalyze the reaction in such a way that opens the door for the practical low potential and temperature conversion of CO2.
Issue Date:2013-05-24
URI:http://hdl.handle.net/2142/44382
Rights Information:Copyright 2013 Brian Rosen
Date Available in IDEALS:2013-05-24
Date Deposited:2013-05


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