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Electrocatalytic Reduction Of Co2 To Formate By An Iron Schiff Base Complex

INORGANIC CHEMISTRY(2018)

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摘要
The synthesis, structural characterization, and reactivity of an iron(III) chloride compound of 6,6'-di(3,5-ditert-butyl-2-hydroxybenzene)-2,2'-bipyridine (Fe((tbu)dhbpy)-Cl), under electrochemically reducing conditions is reported. In the presence of carbon dioxide (CO2) under anhydrous conditions in N,N-dimethylformamide (DMF), this complex mediates the 2(e-) reductive disproportionation of two equivalents of CO2 to carbon monoxide (CO) and carbonate (CO32-). Upon addition of phenol (PhOH) as a proton source under CO2 saturation, catalytic current is observed; product analysis from controlled potential electrolysis experiments shows the majority product is formate (68 +/- 4% Faradaic efficiency), with H-2 as a minor product (30 +/- 10% efficiency) CO (1.1 +/- 0.3% efficiency). On the basis of data obtained from cyclic voltammetry and infrared spectroelectrochemistry (IR-SEC), the release of CO from intermediate Fe carbonyl species is extremely slow and undergoes competitive degradation, limiting the activity and lifetime of this catalyst. Mechanistic studies also indicate the phenolate moieties coordinated to Fe are sensitive to protonation in the reduced state, suggesting the possibility of cooperative pendent proton interactions being involved in CO2 reduction.
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关键词
CO2 Reduction,CO2 Capture,Heterogeneous Electrocatalysts,Electrocatalysis,Electrochemical Conversion
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