Highly efficient and mild electrochemical mineralization of long-chain perfluorocarboxylic acids (C9-C10) by Ti/SnO2-Sb-Ce, Ti/SnO 2-Sb/Ce-PbO2, and Ti/BDD electrodes

Hui Lin, Junfeng Niu, Jiale Xu, Haiou Huang, Duo Li, Zhihan Yue, Chenghong Feng

Research output: Contribution to journalArticle

Abstract

The electrochemical mineralization of environmentally persistent long-chain perfluorinated carboxylic acids (PFCAs), i.e., perfluorononanoic acid (C 8F17COOH, PFNA) and perfluorodecanoic acid (C 9F19COOH, PFDA) was investigated in aqueous solutions (0.25 mmol L-1) over Ti/SnO2-Sb-Ce (SnO2), Ti/SnO2-Sb/Ce-PbO2 (PbO2), and Ti/BDD (BDD) anodes under galvanostatic control at room temperature. Based on PFCA decay rate, total organic carbon (TOC) reduction, defluorination ratio, safety, and energy consumption, the performance of PbO2 electrode was comparable with that of BDD electrode. After 180 min electrolysis, the PFNA removals on BDD and PbO2 electrodes were 98.7 ± 0.4% and 97.1 ± 1.0%, respectively, while the corresponding PFDA removals were 96.0 ± 1.4% and 92.2 ± 1.9%. SnO2 electrode yielded lower PFCA removals and led to notable secondary pollution by Sb ions. The primary mineralization product, F-, as well as trace amounts of intermediate PFCAs with shortened chain lengths, were detected in aqueous solution after electrolysis. On the basis of these results, a degradation mechanism including three potential routes is proposed: via formation of short-chain PFCAs by stepwise removal of CF2; direct mineralization to CO2 and HF; conversion to volatile fluorinated organic compounds. The results presented here demonstrate that electrochemical technique exhibits high efficiency in mineralizing PFNA and PFDA under mild conditions, and is promising for the treatment of long-chain PFCAs in wastewater.

Original languageEnglish (US)
Pages (from-to)13039-13046
Number of pages8
JournalEnvironmental Science and Technology
Volume47
Issue number22
DOIs
StatePublished - Nov 19 2013
Externally publishedYes

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carboxylic acid
Carboxylic Acids
Electrodes
electrode
mineralization
Acids
acid
Electrolysis
electrokinesis
aqueous solution
Electrochemical Techniques
Volatile Organic Compounds
Waste Water
Organic carbon
Volatile organic compounds
Chain length
total organic carbon
volatile organic compound
7,7'-dimethoxy-(4,4'-bi-1,3-benzodioxole)-5,5'-dicarboxylic acid dimethyl ester
Anodes

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Medicine(all)

Cite this

Highly efficient and mild electrochemical mineralization of long-chain perfluorocarboxylic acids (C9-C10) by Ti/SnO2-Sb-Ce, Ti/SnO 2-Sb/Ce-PbO2, and Ti/BDD electrodes. / Lin, Hui; Niu, Junfeng; Xu, Jiale; Huang, Haiou; Li, Duo; Yue, Zhihan; Feng, Chenghong.

In: Environmental Science and Technology, Vol. 47, No. 22, 19.11.2013, p. 13039-13046.

Research output: Contribution to journalArticle

Lin, Hui ; Niu, Junfeng ; Xu, Jiale ; Huang, Haiou ; Li, Duo ; Yue, Zhihan ; Feng, Chenghong. / Highly efficient and mild electrochemical mineralization of long-chain perfluorocarboxylic acids (C9-C10) by Ti/SnO2-Sb-Ce, Ti/SnO 2-Sb/Ce-PbO2, and Ti/BDD electrodes. In: Environmental Science and Technology. 2013 ; Vol. 47, No. 22. pp. 13039-13046.
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abstract = "The electrochemical mineralization of environmentally persistent long-chain perfluorinated carboxylic acids (PFCAs), i.e., perfluorononanoic acid (C 8F17COOH, PFNA) and perfluorodecanoic acid (C 9F19COOH, PFDA) was investigated in aqueous solutions (0.25 mmol L-1) over Ti/SnO2-Sb-Ce (SnO2), Ti/SnO2-Sb/Ce-PbO2 (PbO2), and Ti/BDD (BDD) anodes under galvanostatic control at room temperature. Based on PFCA decay rate, total organic carbon (TOC) reduction, defluorination ratio, safety, and energy consumption, the performance of PbO2 electrode was comparable with that of BDD electrode. After 180 min electrolysis, the PFNA removals on BDD and PbO2 electrodes were 98.7 ± 0.4{\%} and 97.1 ± 1.0{\%}, respectively, while the corresponding PFDA removals were 96.0 ± 1.4{\%} and 92.2 ± 1.9{\%}. SnO2 electrode yielded lower PFCA removals and led to notable secondary pollution by Sb ions. The primary mineralization product, F-, as well as trace amounts of intermediate PFCAs with shortened chain lengths, were detected in aqueous solution after electrolysis. On the basis of these results, a degradation mechanism including three potential routes is proposed: via formation of short-chain PFCAs by stepwise removal of CF2; direct mineralization to CO2 and HF; conversion to volatile fluorinated organic compounds. The results presented here demonstrate that electrochemical technique exhibits high efficiency in mineralizing PFNA and PFDA under mild conditions, and is promising for the treatment of long-chain PFCAs in wastewater.",
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T1 - Highly efficient and mild electrochemical mineralization of long-chain perfluorocarboxylic acids (C9-C10) by Ti/SnO2-Sb-Ce, Ti/SnO 2-Sb/Ce-PbO2, and Ti/BDD electrodes

AU - Lin, Hui

AU - Niu, Junfeng

AU - Xu, Jiale

AU - Huang, Haiou

AU - Li, Duo

AU - Yue, Zhihan

AU - Feng, Chenghong

PY - 2013/11/19

Y1 - 2013/11/19

N2 - The electrochemical mineralization of environmentally persistent long-chain perfluorinated carboxylic acids (PFCAs), i.e., perfluorononanoic acid (C 8F17COOH, PFNA) and perfluorodecanoic acid (C 9F19COOH, PFDA) was investigated in aqueous solutions (0.25 mmol L-1) over Ti/SnO2-Sb-Ce (SnO2), Ti/SnO2-Sb/Ce-PbO2 (PbO2), and Ti/BDD (BDD) anodes under galvanostatic control at room temperature. Based on PFCA decay rate, total organic carbon (TOC) reduction, defluorination ratio, safety, and energy consumption, the performance of PbO2 electrode was comparable with that of BDD electrode. After 180 min electrolysis, the PFNA removals on BDD and PbO2 electrodes were 98.7 ± 0.4% and 97.1 ± 1.0%, respectively, while the corresponding PFDA removals were 96.0 ± 1.4% and 92.2 ± 1.9%. SnO2 electrode yielded lower PFCA removals and led to notable secondary pollution by Sb ions. The primary mineralization product, F-, as well as trace amounts of intermediate PFCAs with shortened chain lengths, were detected in aqueous solution after electrolysis. On the basis of these results, a degradation mechanism including three potential routes is proposed: via formation of short-chain PFCAs by stepwise removal of CF2; direct mineralization to CO2 and HF; conversion to volatile fluorinated organic compounds. The results presented here demonstrate that electrochemical technique exhibits high efficiency in mineralizing PFNA and PFDA under mild conditions, and is promising for the treatment of long-chain PFCAs in wastewater.

AB - The electrochemical mineralization of environmentally persistent long-chain perfluorinated carboxylic acids (PFCAs), i.e., perfluorononanoic acid (C 8F17COOH, PFNA) and perfluorodecanoic acid (C 9F19COOH, PFDA) was investigated in aqueous solutions (0.25 mmol L-1) over Ti/SnO2-Sb-Ce (SnO2), Ti/SnO2-Sb/Ce-PbO2 (PbO2), and Ti/BDD (BDD) anodes under galvanostatic control at room temperature. Based on PFCA decay rate, total organic carbon (TOC) reduction, defluorination ratio, safety, and energy consumption, the performance of PbO2 electrode was comparable with that of BDD electrode. After 180 min electrolysis, the PFNA removals on BDD and PbO2 electrodes were 98.7 ± 0.4% and 97.1 ± 1.0%, respectively, while the corresponding PFDA removals were 96.0 ± 1.4% and 92.2 ± 1.9%. SnO2 electrode yielded lower PFCA removals and led to notable secondary pollution by Sb ions. The primary mineralization product, F-, as well as trace amounts of intermediate PFCAs with shortened chain lengths, were detected in aqueous solution after electrolysis. On the basis of these results, a degradation mechanism including three potential routes is proposed: via formation of short-chain PFCAs by stepwise removal of CF2; direct mineralization to CO2 and HF; conversion to volatile fluorinated organic compounds. The results presented here demonstrate that electrochemical technique exhibits high efficiency in mineralizing PFNA and PFDA under mild conditions, and is promising for the treatment of long-chain PFCAs in wastewater.

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