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维生素B12催化纳米零价铁仿生降解全氟辛磺酸
Biomimetic degradation of PFOS catalyzed by vitamin B12 using nanoscale zero-valent iron as reductants
研究了维生素B12（VB12）催化纳米零价铁（nFe0）仿生还原降解工业级全氟辛磺酸（PFOS）.结果表明，VB12催化nFe0不仅能够降解支链PFOS，而且也能够同时降解直链PFOS，这是首次报道直链PFOS的仿生还原降解.PFOS降解过程可用准一级动力学模型模拟，且升高温度有利于PFOS的还原降解去除和脱氟.超高效液相色谱-四级杆飞行时间质谱（UPLC-QTOF）定性分析表明，PFOS仿生降解产物包括4种全氟磺酸类（全氟碳链长度为C4~C7）、9种全氟羧酸类（全氟碳链长度为C2~C7、C10、C11和C13）和5种多氟代酸类（即H-全氟己酸、H-全氟庚酸、H-全氟辛酸、H2-全氟辛酸和H-全氟辛磺酸）化合物.全氟磺酸类和全氟羧酸类化合物首次在VB12仿生催化降解PFOS的产物之中检出，其中全氟十一烷酸（C10）、全氟十二烷酸（C11）和全氟十四烷酸（C13）等长链化合物第一次在降解PFOS过程中被发现.在降解样中检出的H-全氟烷烃（链长为C2~C7、C10、C11和C13）是否是PFOS的仿生降解产物，还有待进一步研究确认.
The reductive degradation of technical perfluorooctanesulfonate (PFOS) were investigated in a biomimetic system consisting of vitamin B12(VB12) as catalyst and nanoscale zero-valent iron (nFe0) as reductants. Both branched and linear PFOS could be degraded simultaneously, and the biomimetic degradation of linear PFOS was first reported. The degradation was well described by a pseudo-first-order kinetic model, and increasing the incubation temperature was favorable for the removal of PFOS and for its defluorination. Three types of PFOS degradation products, including 4 perfluoroalkylsulfonates (perfluorocarbon chain length:C4~C7), 9perfluorocarboxylates (perfluorocarbon chain length:C2~C7, C10, C11, and C13), and 5 polyfluorinated acids (i.e. H-perfluorohexanoate, H-perfluoroheptanoate, H-perfluorooctanoate, H2-perfluorooctanoate, and H-perfluorooctanesulfonate) have been qualitatively determined by ultra-performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UPLC-QTOF). For the first time, Perfluoroalkylsulfonates and perfluorocarboxylates were detected among the biomimetic reduction products of PFOS catalyzed by VB12, while some long-chain perfluorocarboxylates, including perfluoroundecanoate (C10), perfluorodocecanoate (C11) and perfluorotetradecanoate (C13), were first reported as the degradation products during decomposition of PFOS. It was unclear whether H-perfluoroalkanes (carbon chain length:C2~C7, C10, C11, and C13) were the biomimetic degradation products of PFOS, and further investigation is warranted.
仿生降解 / 还原脱氟 / 纳米零价铁 / 全氟辛磺酸 / 维生素B12
biomimetic degradation / nanoscale zero-valent iron / PFOS / reductive defluorination / vitamin B12
[1] Kissa E. Fluorinated surfactants and repellents[M]. New York:Marcel Dekker Inc, 2001.
[2] Li B, Hu L, Yang Y, et al. Contamination profiles and health risks of PFASs in groundwater of the Maozhou River basin[J]. Environmental Pollution, 2020,260:113996.
[3] Bao J, Yu W, Liu Y, et al. Perfluoroalkyl substances in groundwater and home-produced vegetables and eggs around a fluorochemical industrial park in China[J]. Ecotoxicology and Environmental Safety, 2019,171:199-205.
[4] Liu Y, Ma L, Yang Q, et al. Occurrence and spatial distribution of perfluorinated compounds in groundwater receiving reclaimed water through river bank infiltration[J]. Chemosphere, 2018,211:1203-1211.
[5] Ji B, Kang P, Wei T, et al. Challenges of aqueous per-and polyfluoroalkyl substances (PFASs) and their foreseeable removal strategies[J]. Chemosphere, 2020,250:126316.
[6] Ateia M, Maroli A, Tharayil N, et al. The overlooked short-and ultrashort-chain poly-and perfluorinated substances:A review[J]. Chemosphere, 2019,220:866-882.
[7] Trojanowicz M, Bojanowska-Czajka A, Bartosiewicz I, et al. Advanced oxidation/reduction processes treatment for aqueous perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS)-A review of recent advances[J]. Chemical Engineering Journal, 2018, 336:170-199.
[8] Ross I, Mcdonough J, Miles J, et al. A review of emerging technologies for remediation of PFASs[J]. Remediation Journal, 2018,28(2):101-126.
[9] Zhang Y, Zhi Y, Liu J, et al. Sorption of perfluoroalkyl acids to fresh and aged nanoscale zerovalent iron particles[J]. Environmental Science & Technology, 2018,52(11):6300-6308.
[10] Xiao X, Ulrich B A, Chen B, et al. Sorption of poly-and perfluoroalkyl substances (PFASs) relevant to aqueous film-forming foam (AFFF)-impacted groundwater by biochars and activated carbon[J]. Environmental Science & Technology, 2017,51(11):6342-6351.
[11] Wang J, Wang L, Xu C, et al. Perfluorooctane sulfonate and perfluorobutane sulfonate removal from water by nanofiltration membrane:The roles of solute concentration, ionic strength, and macromolecular organic foulants[J]. Chemical Engineering Journal, 2018,332:787-797.
[12] Chetverikov S P, Sharipov D A, Korshunova T Y, et al. Degradation of perfluorooctanyl sulfonate by strain Pseudomonas plecoglossicida 2.4-D[J]. Applied Biochemistry and Microbiology, 2017,53(5):533-538.
[13] Huang S, Jaffé P R. Defluorination of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) by Acidimicrobium sp. strain A6[J]. Environmental Science & Technology, 2019,53(19):11410-11419.
[14] Ochoa-Herrera V, Sierra-Alvarez R, Somogyi A, et al. Reductive defluorination of perfluorooctane sulfonate[J]. Environmental Science & Technology, 2008,42(9):3260-3264.
[15] Park S, de Perre C, Lee L S. Alternate reductants with VB12to transform C8and C6perfluoroalkyl sulfonates:Limitations and insights into isomer-specific transformation rates, products and pathways[J]. Environmental Science & Technology, 2017,51(23):13869-13877.
[16] 李飞,陈轶丹,杨志敏,等. 8:2氟调聚醇(8:2FTOH)厌氧生物降解特性[J]. 中国环境科学, 2016,36(11):3295-3303. Li F, Chen Y D, Yang Z M, et al. Anaerobic biodegradation of 8:2fluorotelomer alcohol (8:2FTOH)[J]. China Environmental Science, 2016,36(11):3295-3303
[17] Assaf-Anld N, Hayes K F, M V T. Reductive dechlorination of carbon tetrachloride by cobalamin(Ⅱ) in the presence of dithiothreitol:Mechanistic study, effect of redox potential and pH[J]. Environmental Science & Technology, 1994,28(2):246-252.
[18] Costentin C, Robert M, Savéant J. Does catalysis of reductive dechlorination of tetra-and trichloroethylenes by vitamin B12and corrinoid-based dehalogenases follow an electron transfer mechanism?[J]. Journal of American Chemical Society, 2005,127(35):12154-12155.
[19] Lochhead A G, Thexton R H. Vitamin B12as a growth factor for soil bacteria[J]. Nature, 1951,167(4260):1034.
[20] Liu J, Van Hoomissen D J, Liu T, et al. Reductive defluorination of branched per-and polyfluoroalkyl substances with cobalt complex catalysts[J]. Environmental Science & Technology Letters, 2018, 5(5):289-294.
[21] Lee Y, Chen Y, Chen M, et al. Reductive defluorination of perfluorooctanoic acid by titanium(Ⅲ) citrate with vitamin B12and copper nanoparticles[J]. Journal of Hazardous Materials, 2017,340:336-343.
[22] Arvaniti O S, Hwang Y, Andersen H R, et al. Reductive degradation of perfluorinated compounds in water using Mg-aminoclay coated nanoscale zero valent iron[J]. Chemical Engineering Journal, 2015, 262:133-139.
[23] Liu Y, Ptacek C J, Baldwin R J, et al. Application of zero-valent iron coupled with biochar for removal of perfluoroalkyl carboxylic and sulfonic acids from water under ambient environmental conditions[J]. Science of The Total Environment, 2020,719:137372.
[24] Li F, Zhang C, Qu Y, et al. Method development for analysis of short-and long-chain perfluorinated acids in solid matrices[J]. International Journal of Environmental Analytical Chemistry, 2011,91(12):1117-1134.
[25] Li F, Fang X, Zhou Z, et al. Adsorption of perfluorinated acids onto soils:Kinetics, isotherms, and influences of soil properties[J]. Science of The Total Environment, 2019,649:504-514.
[26] Li F, Su Q, Zhou Z, et al. Anaerobic biodegradation of 8:2fluorotelomer alcohol in anaerobic activated sludge:Metabolic products and pathways[J]. Chemosphere, 2018,200:124-132.
[27] Torres F J, Ochoa-Herrera V, Blowers P, et al. Ab initio study of the structural, electronic, and thermodynamic properties of linear perfluorooctane sulfonate (PFOS) and its branched isomers[J]. Chemosphere, 2009,76(8):1143-1149.
[28] Blotevogel J, Giraud R J, Borch T. Reductive defluorination of perfluorooctanoic acid by zero-valent iron and zinc:A DFT-based kinetic model[J]. Chemical Engineering Journal, 2018,335:248-254.
[29] Park S, Zenobio J E, Lee L S. Perfluorooctane sulfonate (PFOS) removal with Pd0/nFe0nanoparticles:Adsorption or aqueous Fe-complexation, not transformation?[J]. Journal of Hazardous Materials, 2018,342:20-28.
[30] Singh R K, Fernando S, Baygi S F, et al. Breakdown products from perfluorinated alkyl substances (PFAS) degradation in a plasma-based water treatment process[J]. Environmental Science & Technology, 2019,53(5):2731-2738.
[31] Sun Z, Zhang C, Xing L, et al. UV/nitrilotriacetic acid process as a novel strategy for efficient photoreductive degradation of perfluorooctanesulfonate[J]. Environmental Science & Technology, 2018,52(5):2953-2962.
[32] Sun Z, Zhang C, Chen P, et al. Impact of humic acid on the photoreductive degradation of perfluorooctane sulfonate (PFOS) by UV/iodide process[J]. Water Research, 2017,127:50-58.
[33] Kim T, Yu S, Choi Y, et al. Profiling the decomposition products of perfluorooctane sulfonate (PFOS) irradiated using an electron beam[J]. Science of The Total Environment, 2018,631-632:1295-1303.
[34] Kim T, Lee S, Kim H Y, et al. Decomposition of perfluorooctane sulfonate (PFOS) using a hybrid process with electron beam and chemical oxidants[J]. Chemical Engineering Journal, 2019,361:1363-1370.
[35] Gu Y, Liu T, Wang H, et al. Hydrated electron based decomposition of perfluorooctane sulfonate (PFOS) in the VUV/sulfite system[J]. Science of The Total Environment, 2017,607-608:541-548.
[36] Gu Y, Dong W, Luo C, et al. Efficient reductive decomposition of perfluorooctanesulfonate in a high photon flux UV/sulfite system[J]. Environmental Science & Technology, 2016,50(19):10554-10561.
[37] Sun M, Zhou H, Xu B, et al. Distribution of perfluorinated compounds in drinking water treatment plant and reductive degradation by UV/SO32- process[J]. Environmental Science and Pollution Research, 2018,25(8):7443-7453.
[38] Jin L, Zhang P. Photochemical decomposition of perfluorooctane sulfonate (PFOS) in an anoxic alkaline solution by 185nm vacuum ultraviolet[J]. Chemical Engineering Journal, 2015,280:241-247.
[39] Yamamoto T, Noma Y, Sakai S, et al. Photodegradation of perfluorooctane sulfonate by UV irradiation in water and alkaline 2-propanol[J]. Environmental Science & Technology, 2007,41(16):5660-5665.
国家自然科学基金（51878300,51108197,51878301）；福建省自然科学基金（2017J01096）；泉州市科技计划项目（2018C084R）；厦门市科技重大专项（3502Z20191012）；华侨大学中青年教师科研提升资助计划（ZQN-YX602）；华侨大学研究生科研创新基金资助项目
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