Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism

The reduction of 2,4,6-trinitrotoluene (TNT) has been studied in eight room temperature ionic liquids (RTILs) on a gold (Au) microdisk electrode and a Au thin film electrode (TFE). Three reduction peaks were observed in all RTILs, corresponding to the reductions of each of the three nitro groups in...

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Main Authors: Kang, C., Lee, J., Silvester, Debbie
Format: Journal Article
Published: American Chemical Society 2016
Online Access:http://hdl.handle.net/20.500.11937/50388
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author Kang, C.
Lee, J.
Silvester, Debbie
author_facet Kang, C.
Lee, J.
Silvester, Debbie
author_sort Kang, C.
building Curtin Institutional Repository
collection Online Access
description The reduction of 2,4,6-trinitrotoluene (TNT) has been studied in eight room temperature ionic liquids (RTILs) on a gold (Au) microdisk electrode and a Au thin film electrode (TFE). Three reduction peaks were observed in all RTILs, corresponding to the reductions of each of the three nitro groups in the TNT structure. TNT was the easiest to reduce in imidazolium RTILs, followed by pyrrolidinium and then tetraalkylphosphonium. Diffusion coefficients (D) and electron counts (n) were calculated from potential-step chronoamperometry on the first reduction peak. D's ranged from 0.7 × 10-11 to 4.1 × 10-11 m2 s-1, and a plot of D against the inverse of viscosity was linear, indicating that the Stokes-Einstein relation holds well for TNT in RTILs. The electron count was one in most RTILs-in stark contrast to the widely accepted six-electron reduction in protic solvents. An electrogenerated red solid was formed after the first reduction peak, believed to be an azo (or azoxy) compound formed by dimerization of two TNT radicals, although characterization of the product(s) proved difficult. The behavior at different concentrations revealed different degrees of chemical reversibility of reduction peak. This evidence points toward the possibility of an EC2 mechanism, which was supported by digital simulation of the experimental voltammograms. Understanding the reduction mechanism of TNT is essential if RTILs are to be used for TNT sensing applications, particularly at high concentrations.
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spelling curtin-20.500.11937-503882017-09-13T15:42:43Z Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism Kang, C. Lee, J. Silvester, Debbie The reduction of 2,4,6-trinitrotoluene (TNT) has been studied in eight room temperature ionic liquids (RTILs) on a gold (Au) microdisk electrode and a Au thin film electrode (TFE). Three reduction peaks were observed in all RTILs, corresponding to the reductions of each of the three nitro groups in the TNT structure. TNT was the easiest to reduce in imidazolium RTILs, followed by pyrrolidinium and then tetraalkylphosphonium. Diffusion coefficients (D) and electron counts (n) were calculated from potential-step chronoamperometry on the first reduction peak. D's ranged from 0.7 × 10-11 to 4.1 × 10-11 m2 s-1, and a plot of D against the inverse of viscosity was linear, indicating that the Stokes-Einstein relation holds well for TNT in RTILs. The electron count was one in most RTILs-in stark contrast to the widely accepted six-electron reduction in protic solvents. An electrogenerated red solid was formed after the first reduction peak, believed to be an azo (or azoxy) compound formed by dimerization of two TNT radicals, although characterization of the product(s) proved difficult. The behavior at different concentrations revealed different degrees of chemical reversibility of reduction peak. This evidence points toward the possibility of an EC2 mechanism, which was supported by digital simulation of the experimental voltammograms. Understanding the reduction mechanism of TNT is essential if RTILs are to be used for TNT sensing applications, particularly at high concentrations. 2016 Journal Article http://hdl.handle.net/20.500.11937/50388 10.1021/acs.jpcc.6b03018 American Chemical Society fulltext
spellingShingle Kang, C.
Lee, J.
Silvester, Debbie
Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism
title Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism
title_full Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism
title_fullStr Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism
title_full_unstemmed Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism
title_short Electroreduction of 2,4,6-Trinitrotoluene in Room Temperature Ionic Liquids: Evidence of an EC2 Mechanism
title_sort electroreduction of 2,4,6-trinitrotoluene in room temperature ionic liquids: evidence of an ec2 mechanism
url http://hdl.handle.net/20.500.11937/50388