Photochemical Degradation of Perfluorocarboxylic Acids Induced by Ferric Ion：Effects of pH and Carbon Chain

doi:10.6023/A14020101

Acta Chimica Sinica ›› 2014, Vol. 72 ›› Issue (6): 682-688.DOI: 10.6023/A14020101 Previous Articles Next Articles

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Fe³⁺诱导全氟羧酸的光化学降解：pH值及链长的影响

王媛^a, 石晓燕^b

a. 贵州大学化学与化工学院贵阳 550025;
b. 中国科学院生态环境研究中心北京 100085

投稿日期:2014-02-13 发布日期:2014-05-27
通讯作者: 王媛 E-mail:wangyuan08@tsinghua.org.cn
基金资助:
项目受贵州大学引进人才项目（No.贵大人基合字（2010）009号）、贵州省自然科学基金（No.黔科合J字[2011]2066号）、国家环境保护大气复合污染来源与控制重点实验室开放基金（No.SCAPC201302）和国家自然科学基金（No.21267006）资助.

Photochemical Degradation of Perfluorocarboxylic Acids Induced by Ferric Ion：Effects of pH and Carbon Chain

Wang Yuan^a, Shi Xiaoyan^b

a. School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025;
b. Research Center for Eco-Environmental Science, Chinese Academy of Sciences, Beijing 100085

Received:2014-02-13 Published:2014-05-27
Supported by:
Project supported by Guizhou University Talent Introduction Project (No.2010009), Natural Science Foundation of Guizhou Province (No.20112066), State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex (No.SCAPC201302) and National Natural Science Foundation of China (No.21267006).

Perfluorooctanoic acid (PFOA), as a typical perfluorinated compounds, is one kind of emerging persistent pollutants appearing in natural water.The existence of ferric ion in aquatic system improves the degradation of PFOA under the irradiation of 254 nm UV light.pH is an important factor for not only the distribution of photo activity species of ferric ion but also the degradation of PFOA.When the initial pH of reaction solution was 2.53, 3.04 and 3.71, respectively, PFOA was decomposed effectively and no obvious difference was observed whether for the degradation ratio of PFOA or for its corresponding defluorination ratio.On the contrary, when pH was 4.92 and 7.05, respectively, the degradation and defluorination of PFOA was inhibited markedly, which further confirmed that dissoluble iron played a key role in the decomposition of PFOA.And Fe(OH)²⁺ was the dominant species of the hydroxy complexes of Fe³⁺.At the same time, the degradation of short chain PFCAs bearing C₄～C₇ caused by ferric ions under the irradiation of 254 nm UV light was also investigated.As for PFCAs with C₆～C₈, the degradation ratio at 240 min was as follows: PFOA > PFHpA > PFHxA, which showed that the longer the carbon chain was, the easier the degradation of PFCAs was.While, for PFCAs with the number of carbon element less than 6, their degradation ratio at 240 min was as follows: PFHxA > PFBA > PFPeA.The relationship between the degradation of PFCAs and the length of carbon chain of PFCAs was not clear.More short chain PFCAs were identified by LC/MS as the primary intermediates of these short chain PFCAs.Based on these, it was proposed that the degradation of PFCAs bearing C₄～C₈ was mainly caused by the formation of complexes between ferric ion and PFCAs, and then hydroxyl radical formed from photolysis of Fe(OH)²⁺ and the redox cycle of Fe²⁺/Fe³⁺ further improved their degradation.As a result, PFCAs were decomposed step by step.

Key words: perfluorooctanoic acid, short-chain perfluorocarboxylic acid, ferric ion, UV light, decomposition mechanism

Cite this article

Wang Yuan, Shi Xiaoyan. Photochemical Degradation of Perfluorocarboxylic Acids Induced by Ferric Ion：Effects of pH and Carbon Chain[J]. Acta Chimica Sinica, 2014, 72(6): 682-688.

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Fe³⁺诱导全氟羧酸的光化学降解：pH值及链长的影响

Photochemical Degradation of Perfluorocarboxylic Acids Induced by Ferric Ion：Effects of pH and Carbon Chain

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Fe3+诱导全氟羧酸的光化学降解：pH值及链长的影响

Photochemical Degradation of Perfluorocarboxylic Acids Induced by Ferric Ion：Effects of pH and Carbon Chain

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Fe³⁺诱导全氟羧酸的光化学降解：pH值及链长的影响