Citation: MA Hong-Xing, GE Ting-Jie, CAI Qian-Qian, XU Ying-Hua, MA Chun-An. Catalytic Effect of Silver Cathodes on 3,4,5,6-Tetrachloropicolinic Acid Dechlorination in Aqueous Solutions[J]. Acta Physico-Chimica Sinica, ;2016, 32(7): 1715-1721. doi: 10.3866/PKU.WHXB201604121 shu

Catalytic Effect of Silver Cathodes on 3,4,5,6-Tetrachloropicolinic Acid Dechlorination in Aqueous Solutions

State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P. R. China

Received Date: 2 March 2016
Revised Date: 12 April 2016

Fund Project: The project was supported by the National Natural Science Foundation of China (21106133, 21576238), Natural Science Foundation of Zhejiang Province, China (LY16B060012), and National Key Basic Research Program of China (973) (2012CB722604).

Dechlorination of 3,4,5,6-tetrachloropicolinic acid (TeCP) on roughened silver (Ag(r)) cathodes provides an unexpected example showing extraordinary catalytic effect in aqueous solution, which is counter to what has been reported in electrochemical reduction of organic halides using aprotic media. To fully recognize this extraordinary catalytic effect of silver cathodes on electrochemical reduction of 3,4,5,6-tetrachloropicolinic acid in aqueous solutions, we conduct a comprehensive study from the aspect of surface characterization, in situ electrochemical study, and theoretical calculation. Transmission electron microscopy (TEM) images and X-ray photoelectron spectroscopy (XPS) spectra are presented to observe the surface structure and chemical state of Ag(r). Experimental results show that Ag nanoparticle can be formed in the oxidation-reduction cyclic (ORC) process, which leads to an increase in the degree of surface disorder. Density functional theory (DFT) calculations of the first electron transfer (ET) process, integrated with an in situ electrochemical surfaceenhanced Raman spectroscopy (SERS) study and a cyclic voltammetry (CV) experiment with the aid of H+, were performed to characterize various surface species in different electrode potential regions. Experimental evidence shows that the first ET process is catalyzed by silver for the radical derivate (TeCP^·-) formed by the ET process is adsorbed more strongly than TeCP. TeCP^·- ads is the key intermediate of the dechlorination process, implying that the dechlorination mechanism could drastically differ from the outer-sphere reduction at the glass carbon (GC) electrode.
- 3,4,5,6-tetrachloropicolinic acid,
- Surface-enhanced Raman spectroscopy,
- Density functional theory,
- Silver electrode,
- Electrocatalytic mechanism,
- Dechlorination,
- Adsorption
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