全氟和多氟烷基化合物(PFASs)广泛应用于化工、半导体、消防、工业制造等领域。由于其残留物可进入环境并在大范围内扩散,且C—F键具有高键能(485kJ/mol),导致PFASs在环境中难以降解,成为一类典型的持久性有机污染物。因此,PFASs的环境去除面临着巨大挑战。近年来,光化学降解作为一种新兴的PFASs降解技术,因反应条件温和与降解效率高等优势而备受关注。该技术通过光激发光催化剂产生活性自由基,进而实现PFASs分子的高效分解。其高度选择性和能量效率使其成为替代传统化学方法的有力选择。系统评述了PFASs光化学降解领域的最新研究进展,深入探讨了相关反应机制,并展望了未来发展方向与面临的挑战,旨在为研究人员设计高效PFASs光化学降解体系提供理论指导。
Perfluoroalkyl and polyfluoroalkyl substances (PFASs) are widely used in fields such as chemical engineering,semiconductors,firefighting,and industrial manufacturing.Because their residues can enter the environment and diffuse over a large area,and the C—F bond has a high bond energy of 485 kJ·mol-1,PFASs are difficult to degrade in the environment,making them a typical persistent organic pollutant.Therefore,the environmental removal of PFASs faces significant challenges.In recent years,photochemical degradation,as an emerging PFASs degradation technology,has attracted much attention due to its advantages of mild reaction conditions and high degradation efficiency.This technology generates active free radicals through photoexcited photocatalysts,thereby achieving efficient decomposition of PFASs molecules.Its high selectivity and energy efficiency make it a powerful alternative to traditional chemical methods.This article systematically reviewed the latest research progress in the field of photocatalytic degradation of PFASs,explored the relevant reaction mechanisms in depth,and looked forward to future development directions and challenges,providing theoretical guidance for researchers to design efficient PFASs photocatalytic degradation systems.
[1] Leung S C E,Shukla P,Chen D,et al.Emerging technologies for PFOS/PFOA degradation and removal:a review[J].Science of the Total Environment,2022,827:153669.
[2] Death C,Bell C,Champness D,et al.Per- and polyfluoroalkyl substances (PFASS) in livestock and game species:a review[J].Science of the Total Environment,2021,774:144795.
[3] Fair P A,Wolf B,White N D,et al.Perfluoroalkyl substances (PFASs) in edible fish species from Charleston Harbor and tributaries,South Carolina,United States:exposure and risk assessment[J].Environmental Research,2019,171:266-277.
[4] Wang S,Yang Q,Chen F,et al.Photocatalytic degradation of perfluorooctanoic acid and perfluorooctane sulfonate in water:a critical review[J].Chemical Engineering Journal,2017,328:927-942.
[5] Chen J,Zhang P Y,Liu J.Photodegradation of perfluorooctanoic acid by 185 nm vacuum ultraviolet light[J].Journal of Environmental Sciences,2007,19(4):387-390.
[6] Giri R R,Ozaki H,Okada T,et al.Factors influencing UV photodecomposition of perfluorooctanoic acid in water[J].Chemical Engineering Journal,2012,180:197-203.
[7] Liu D,Xiu Z,Liu F,et al.Perfluorooctanoic acid degradation in the presence of Fe(Ⅲ) under natural sunlight[J].Journal of Hazardous Materials,2013,262:456-463.
[8] Tang H,Xiang Q,Lei M,et al.Efficient degradation of perfluorooctanoic acid by UV-Fenton process[J].Chemical Engineering Journal,2012,184:156-162.
[9] Cheng J H,Liang X Y,Yang S W,et al.Photochemical defluorination of aqueous perfluorooctanoic acid (PFOA) by VUV/Fe3+ system[J].Chemical Engineering Journal,2014,239:242-249.
[10] Ohno M,Ito M,Ohkura R,et al.Photochemical decomposition of perfluorooctanoic acid mediated by iron in strongly acidic conditions[J].Journal of Hazardous Materials,2014,268:150-155.
[11] Yang S W,Sun J,Hu Y Y,et al.Effect of vacuum ultraviolet on ultrasonic defluorination of aqueous perfluorooctanesulfonate[J].Chemical Engineering Journal,2013,234:106-114.
[12] Liang X,Cheng J,Yang C,et al.Factors influencing aqueous perfluorooctanoic acid (PFOA) photodecomposition by VUV irradiation in the presence of ferric ions[J].Chemical Engineering Journal,2016,298:291-299.
[13] Qian L,Georgi A,Gonzalez-olmos R,et al.Degradation of perfluorooctanoic acid adsorbed on Fe-zeolites with molecular oxygen as oxidant under UV-A irradiation[J].Applied Catalysis B:Environmental,2020,278:119283.
[14] Lutze H V,Brekenfeld J,Naumov S,et al.Degradation of perfluorinated compounds by sulfate radicals-new mechanistic aspects and economical considerations[J].Water Research,2018,129:509-519.
[15] Qian Y,Guo X,Zhang Y,et al.Perfluorooctanoic acid degradation using UV-persulfate process:modeling of the degradation and chlorate formation[J].Environmental Science & Technology,2016,50(2):772-781.
[16] Qu Y,Zhang C,Li F,et al.Photo-reductive defluorination of perfluorooctanoic acid in water[J].Water Research,2010,44(9):2939-2347.
[17] Tenorio R,Liu J,Xiao X,et al.Destruction of per- and polyfluoroalkyl substances (PFASs) in aqueous film-forming foam (AFFF) with UV-Sulfite photoreductive treatment[J].Environmental Science & Technology,2020,54(11):6957-6967.
[18] Li Z,Zhang P,Shao T,et al.In2O3 nanoporous nanosphere:a highly efficient photocatalyst for decomposition of perfluorooctanoic acid[J].Applied Catalysis B:Environmental,2012,125:350-357.
[19] Nzeribe B N,Crimi M,Mededovic Thagard S,et al.Physico-chemical processes for the treatment of per- and polyfluoroalkyl substances (PFASS):a review[J].Critical Reviews in Environmental Science and Technology,2019,49(10):866-915.
[20] Chen M J,Lo S L,Lee Y C,et al.Photocatalytic decomposition of perfluorooctanoic acid by transition-metal modified titanium dioxide[J].Journal of Hazardous Materials,2015,288:168-175.
[21] Park H,Vecitis C D,Cheng J,et al.Reductive defluorination of aqueous perfluorinated alkyl surfactants:effects of ionic headgroup and chain length[J].The Journal of Physical Chemistry A,2009,113(4):690-696.
[22] 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.
[23] Park H,Vecitis C D,Cheng J,et al.Reductive degradation of perfluoroalkyl compounds with aquated electrons generated from iodide photolysis at 254 nm[J].Photochemical & Photobiological Sciences,2011,10(12):1945-1953.
[24] Qu Y,Zhang C J,Chen P,et al.Effect of initial solution pH on photo-induced reductive decomposition of perfluorooctanoic acid[J].Chemosphere,2014,107:218-223.
[25] Giri R R,Ozaki H,Guo X,et al.Oxidative-reductive photodecomposition of perfluorooctanoic acid in water[J].International Journal of Environmental Science and Technology,2014,11(5):1277-1284.
[26] 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.
[27] Jiao H,Zhang C,Yang M,et al.Photoreductive defluorination of trifluoroacetic acid (TFA) in the aqueous phase by hydrated electrons[J].Chemical Engineering Journal,2022,430:132724.
[28] Cao H,Zhang W,Wang C,et al.Photodegradation of F-53B in aqueous solutions through an UV/Iodide system[J].Chemosphere,2022,292:133436.
[29] Yu K,Li X,Chen L,et al.Mechanism and efficiency of contaminant reduction by hydrated electron in the sulfite/iodide/UV process[J].Water Research,2018,129:357-364.
[30] Chen Z,Li C,Gao J,et al.Efficient reductive destruction of perfluoroalkyl substances under self-assembled micelle confinement[J].Environmental Science & Technology,2020,54(8):5178-5185.
[31] Chen Z,Teng Y,Mi N,et al.Highly efficient hydrated electron utilization and reductive destruction of perfluoroalkyl substances induced by intermolecular interaction[J].Environmental Science & Technology,2021,55(6):3996-4006.
[32] Chen Z,Dong R,Wang X,et al.Efficient decomposition of perfluoroalkyl substances by low concentration indole:new insights into the molecular mechanisms[J].Environmental Science & Technology,2024,58(7):3530-3539.
[33] Tian H,Gu C.Effects of different factors on photodefluorination of perfluorinated compounds by hydrated electrons in organo-montmorillonite system[J].Chemosphere,2018,191:280-287.
[34] Chen Z,Tian H,Li H,et al.Application of surfactant modified montmorillonite with different conformation for photo-treatment of perfluorooctanoic acid by hydrated electrons[J].Chemosphere,2019,235:1180-1188.
[35] Chen Z,Mi N,Li C,et al.Effects of different variables on photodestruction of perfluorooctanoic acid in self-assembled micelle system[J].Science of The Total Environment,2020,742:140438.
[36] Deng Y,Liang Z,Lu X,et al.The degradation mechanisms of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) by different chemical methods:a critical review[J].Chemosphere,2021,283:131168.
[37] Rao U,Su Y,Khor C M,et al.Structural dependence of reductive defluorination of linear PFASS compounds in a UV/electrochemical system[J].Environmental Science & Technology,2020,54(17):10668-10677.
[38] Yamamoto Y I,Suzuki T.Ultrafast dynamics of water radiolysis:hydrated electron formation,solvation,recombination,and scavenging[J].The Journal of Physical Chemistry Letters,2020,11(14):5510-5516.
[39] Bentel M J,Yu Y,Xu L,et al.Defluorination of per- and polyfluoroalkyl substances (PFASs) with hydrated electrons:structural dependence and implications to PFASS remediation and management[J].Environmental Science & Technology,2019,53(7):3718-3728.
[40] Wang X,Wang P,Liu X,et al.Enhanced degradation of PFOA in water by dielectric barrier discharge plasma in a coaxial cylindrical structure with the assistance of peroxymonosulfate[J].Chemical Engineering Journal,2020,389:124381.
[41] Li T,Wang C,Wang T,et al.Highly efficient photocatalytic degradation toward perfluorooctanoic acid by bromine doped BiOI with high exposure of (001) facet[J].Applied Catalysis B:Environmental,2020,268:118442.
[42] Liu X,Wei W,Xu J,et al.Photochemical decomposition of perfluorochemicals in contaminated water[J].Water Research,2020,186:116311.
[43] Yang J S,Lai W W P,Panchangam S C,et al.Photoelectrochemical degradation of perfluorooctanoic acid (PFOA) with GOP25/FTO anodes:intermediates and reaction pathways[J].Journal of Hazardous Materials,2020,391:122247.
[44] Trojanowicz M,Bartosiewicz I,Bojanowska-czajkaa,et al.Application of ionizing radiation in decomposition of perfluorooctane sulfonate (PFOS) in aqueous solutions[J].Chemical Engineering Journal,2020,379:122303.
[45] Khan M Y,So S,Da Silva G.Decomposition kinetics of perfluorinated sulfonic acids[J].Chemosphere,2020,238:124615.
[46] 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.
[47] Gu P,Zhang C,Sun Z,et al.Enhanced photoreductive degradation of perfluorooctanesulfonate by UV irradiation in the presence of ethylenediaminetetraacetic acid[J].Chemical Engineering Journal,2020,379:122338.
[48] 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.
[49] Cui J,Gao P,Deng Y.Destruction of per- and polyfluoroalkyl substances (PFASS) with advanced reduction processes (ARPs):a critical review[J].Environmental Science & Technology,2020,54(7):3752-3766.
基金资助
江苏省双创团队项目[(2018)2017号]