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Electrochemical activation of persulfates at BDD anode: Radical or nonradical oxidation?
Water Res. 2018 Jan 01; 128:393-401.WR

Abstract

The combination of persulfates (peroxydisulfate (PDS) and peroxymonosulfate (PMS)) and electrolysis using boron-doped diamond (BDD) anode is a promising green advanced oxidation process. In comparison with electrolysis alone, electrochemical activation of persulfates at BDD anode considerably enhanced the degradation of carbamazepine (CBZ). The experimental results indicate that the surface-adsorbed hydroxyl radical (HO) played the dominant role. The generally proposed nonradical oxidation mechanism ignored hydroxyl radical (HO) oxidation because low concentration of radical scavenger (<10 M methanol or 5 M tertbutanol) could not effectively scavenge the surface-adsorbed HO. The quasi steady-state concentration of HO was estimated to be about 5.0-9.1 × 10-12 M for electrolysis with BDD anode, and it was increased to 1.1-1.6 × 10-11 M and 3.2-5.0 × 10-11 M for addition of 5 mM PDS and PMS, respectively. The results of cyclic voltammetry (CV) and chronoamperometry as well as evolution of dissolved oxygen (DO) reveal that the electrochemically activated persulfates molecule (PDS∗/PMS∗) promoted the production of HO via water dissociation at BDD anode and enhanced the direct electron transfer (DET) reaction, which otherwise inhibited the oxygen evolution side reaction. Therefore, higher current efficiency was achieved in electrochemical activation of persulfates process compared with electrolysis process. Additionally, the transformation products of CBZ were also investigated and their formation pathways were proposed.

Authors+Show Affiliations

State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China. Electronic address: jiangjinhit@126.com.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China. Electronic address: majun@hit.edu.cn.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China.State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China.

Pub Type(s)

Evaluation Study
Journal Article

Language

eng

PubMed ID

29127807

Citation

Song, Haoran, et al. "Electrochemical Activation of Persulfates at BDD Anode: Radical or Nonradical Oxidation?" Water Research, vol. 128, 2018, pp. 393-401.
Song H, Yan L, Jiang J, et al. Electrochemical activation of persulfates at BDD anode: Radical or nonradical oxidation? Water Res. 2018;128:393-401.
Song, H., Yan, L., Jiang, J., Ma, J., Zhang, Z., Zhang, J., Liu, P., & Yang, T. (2018). Electrochemical activation of persulfates at BDD anode: Radical or nonradical oxidation? Water Research, 128, 393-401. https://doi.org/10.1016/j.watres.2017.10.018
Song H, et al. Electrochemical Activation of Persulfates at BDD Anode: Radical or Nonradical Oxidation. Water Res. 2018 Jan 1;128:393-401. PubMed PMID: 29127807.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Electrochemical activation of persulfates at BDD anode: Radical or nonradical oxidation? AU - Song,Haoran, AU - Yan,Linxia, AU - Jiang,Jin, AU - Ma,Jun, AU - Zhang,Zhongxiang, AU - Zhang,Jiaming, AU - Liu,Pingxin, AU - Yang,Tao, Y1 - 2017/10/12/ PY - 2017/06/05/received PY - 2017/08/28/revised PY - 2017/10/08/accepted PY - 2017/11/12/pubmed PY - 2018/7/19/medline PY - 2017/11/12/entrez KW - BDD anode KW - Electrochemical activation of persulfates KW - Nonradical oxidation KW - Surface-adsorbed HO SP - 393 EP - 401 JF - Water research JO - Water Res. VL - 128 N2 - The combination of persulfates (peroxydisulfate (PDS) and peroxymonosulfate (PMS)) and electrolysis using boron-doped diamond (BDD) anode is a promising green advanced oxidation process. In comparison with electrolysis alone, electrochemical activation of persulfates at BDD anode considerably enhanced the degradation of carbamazepine (CBZ). The experimental results indicate that the surface-adsorbed hydroxyl radical (HO) played the dominant role. The generally proposed nonradical oxidation mechanism ignored hydroxyl radical (HO) oxidation because low concentration of radical scavenger (<10 M methanol or 5 M tertbutanol) could not effectively scavenge the surface-adsorbed HO. The quasi steady-state concentration of HO was estimated to be about 5.0-9.1 × 10-12 M for electrolysis with BDD anode, and it was increased to 1.1-1.6 × 10-11 M and 3.2-5.0 × 10-11 M for addition of 5 mM PDS and PMS, respectively. The results of cyclic voltammetry (CV) and chronoamperometry as well as evolution of dissolved oxygen (DO) reveal that the electrochemically activated persulfates molecule (PDS∗/PMS∗) promoted the production of HO via water dissociation at BDD anode and enhanced the direct electron transfer (DET) reaction, which otherwise inhibited the oxygen evolution side reaction. Therefore, higher current efficiency was achieved in electrochemical activation of persulfates process compared with electrolysis process. Additionally, the transformation products of CBZ were also investigated and their formation pathways were proposed. SN - 1879-2448 UR - https://www.unboundmedicine.com/medline/citation/29127807/Electrochemical_activation_of_persulfates_at_BDD_anode:_Radical_or_nonradical_oxidation L2 - https://linkinghub.elsevier.com/retrieve/pii/S0043-1354(17)30847-3 DB - PRIME DP - Unbound Medicine ER -