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Electrocatalytic dechlorination of volatile organic compounds at a copper cathode. Part I: Polychloromethanes

Paper ID Volume ID Publish Year Pages File Format Full-Text
46561 46441 2012 8 PDF Available
Title
Electrocatalytic dechlorination of volatile organic compounds at a copper cathode. Part I: Polychloromethanes
Abstract

The electrochemical reductive dehalogenation of CCl4, CHCl3, CH2Cl2 and CH3Cl was investigated at Cu in dimethylformamide (DMF). The principal aim of the study was to check whether Cu has good electrocatalytic properties and is stable to fouling in preparative-scale electrolyses. All polychloromethanes (PCMs) have been investigated by cyclic voltammetry in DMF + 0.1 M Pr4NBF4 in order to evaluate the reduction mechanism and the catalytic activity of Cu. The electrochemical reduction of CCl4 and CHCl3 has also been studied by controlled-potential electrolysis in DMF + 0.1 M Pr4NBF4 both in the absence and presence of H2O or CH3CO2H, using chromatographic techniques to determine the intermediates and final products of the process. Cu exhibits a good electrocatalytic activity, in some cases the positive shifts of the reduction potentials with respect to GC being comparable with those at Ag, which is considered to be one of the best candidates for environmental applications in dehalogenation reactions. The results point out that the reduction mechanism at Cu is similar to what was already observed for Ag on which reduction of PCMs takes place through two competing reaction pathways: hydrodehalogenation and hydrogenolysis of carbenes. The proton availability of the medium affects drastically both the catalytic effect of Cu and the distribution of reduction products. The presence of an added proton donor promotes the hydrodehalogenation pathway, enhancing the concentration of intermediate PCMs and the final yield of methane, which is the main product of the exhaustive electrolysis.

Graphical abstractFigure optionsDownload full-size imageDownload as PowerPoint slideHighlights▸ Like Ag, Cu is a good electrocatalyst for the reduction of polychloromethanes, PCMs. ▸ Complete dechlorination of any PCM can be achieved at Cu without electrode fouling. ▸ Both potentiostatic and galvanostatic electrolyses give high yields of methane. ▸ Addition of a good proton donor highly favors the hydrodehalogenation reaction route. ▸ Cu is a promising cathode for large scale applications and pollution remediation.

Keywords
Polychloromethanes; Copper cathode; Electrocatalysis; Pollutant degradation; Hydrodehalogenation
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Electrocatalytic dechlorination of volatile organic compounds at a copper cathode. Part I: Polychloromethanes
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volume 126, 25 September 2012, Pages 347–354
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
Full-text PDF Download
Online Support
Any Questions? feel free to contact us