Complete mineralization of perfluorooctanoic acid (PFOA) by γ-irradiation in aqueous solution

被引:85
作者
Zhang, Ze [1 ]
Chen, Jie-Jie [1 ]
Lyu, Xian-Jin [1 ]
Yin, Hao [2 ]
Sheng, Guo-Ping [1 ]
机构
[1] Univ Sci & Technol China, Dept Chem, CAS Key Lab Urban Pollutant Convers, Hefei 230026, Peoples R China
[2] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
关键词
RADIATION-INDUCED DEGRADATION; SULFONATE PFOS; PERFLUOROCARBOXYLIC ACIDS; REDUCTIVE DEFLUORINATION; DRINKING-WATER; DECOMPOSITION; PERFLUOROALKYL; SURFACTANTS; MECHANISMS; CONVERSION;
D O I
10.1038/srep07418
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Decomposition of perfluorooctanoic acid (C7F15COOH, PFOA) has been gaining increasing interests because it is a ubiquitous environmental contaminant and resistant to the most conventional treatment processes. In this work, the rapid and complete mineralization of PFOA and simultaneous defluorination were achieved by gamma-ray irradiation with a Co-60 source. The degradation rate of PFOA by gamma-ray irradiation would be high, and a pseudo-first-order kinetic rate constant of 0.67 h(-1) could be achieved in the N-2 satured condition at pH 13.0. The experimental results and quantum chemical calculation confirmed that two radicals, i.e., hydroxyl radical ((OH)-O-center dot) and aqueous electrons (e(aq)(-)), were responsible for the degradation of PFOA, while only either e(aq)(-) or (OH)-O-center dot might not be able to accomplish complete mineralization of PFOA. The synergistic effects of (OH)-O-center dot and e(aq)(-) involved in the cleavage of C-C and C-F bonds, and therefore complete mineralization of PFOA were achieved. The intermediate products were identified and the degradation pathway was also proposed. The results of this study may offer a useful, high-efficient approach for complete mineralizing fluorochemicals and other persistent pollutants.
引用
收藏
页数:6
相关论文
共 42 条
[1]  
Aal SEA, 2001, J RADIOANAL NUCL CH, V250, P329
[2]   Modeling global-scale fate and transport of perfluorooctanoate emitted from direct sources [J].
Armitage, James ;
Cousins, Ian T. ;
Buck, Robert C. ;
Prevedouros, Konstantinos ;
Russell, Mark H. ;
MacLeod, Matthew ;
Korzeniowski, Stephen H. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (22) :6969-6975
[3]  
Bartels DM, 2006, ABSTR PAP AM CHEM S, V231
[4]  
Buxton G. V., 2010, CHARGED PARTICLE PHO, P331
[5]   Effects of titanate nanotubes synthesized by a microwave hydrothermal method on photocatalytic decomposition of perfluorooctanoic acid [J].
Chen, Ying-Chu ;
Lo, Shang-Lien ;
Kuo, Jeff .
WATER RESEARCH, 2011, 45 (14) :4131-4140
[6]   Radiation-induced degradation of methyl orange in aqueous solutions [J].
Chen, You-Peng ;
Liu, Shao-Yang ;
Yu, Han-Qing ;
Yin, Hao ;
Li, Qian-Rong .
CHEMOSPHERE, 2008, 72 (04) :532-536
[7]   Radiolysis of aqueous phenol solutions with nanoparticles.: 1.: Phenol degradation and TOC removal in solutions containing TiO2 induced by UV, γ-ray and electron beams [J].
Chitose, N ;
Ueta, S ;
Seino, S ;
Yamamoto, TA .
CHEMOSPHERE, 2003, 50 (08) :1007-1013
[8]   Fast calculation of electrostatics in crystals and large molecules [J].
Delley, B .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (15) :6107-6110
[9]   From molecules to solids with the DMol3 approach [J].
Delley, B .
JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (18) :7756-7764
[10]   Radiation-induced degradation of water pollutants - State of the art [J].
Getoff, N .
RADIATION PHYSICS AND CHEMISTRY, 1996, 47 (04) :581-593