Abstract
A synergistic system of dielectric barrier discharge (DBD) combined with La/Ce-TiO2 was developed to investigate the decomposition performance of the environmentally persistent perfluorooctanoic acid (PFOA). The La/Ce-TiO2 was modified by sol–gel method and characterized by XRD, SEM, and energy dispersive X-ray. The effects of PFOA concentration, applied voltage, initial pH, liquid conductivity, and additives on the removal rate of PFOA were explored. The results showed that the La/Ce-TiO2 exhibited excellent catalytic effects on PFOA degradation in DBD system. When the applied voltage, PFOA concentration, pH value, and solution volume were 75 V, 100 mg/L, 3.63, and 1000 mL, respectively, the removal efficiency of PFOA was up to 97.5% by adding La4Ce1-TiO2 in DBD. The corresponding defluorination ratio, TOC removal, and decomposition yield were 62.2%, 57.3%, and 37 g/kWh, respectively. Furthermore, five main intermediates including CF3(CF2)6H, CF3(CF2)5COOH, CF3(CF2)5COH, CF3(CF2)4COOH, and CF3CF2CF3 were identified with LC–MS, and the degradation pathways of PFOA were proposed. The degradation mechanisms revealed that hydroxyl radicals play a significant role in the degradation of PFOA in the synergistic system.
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11356-017-9246-4/MediaObjects/11356_2017_9246_Fig1_HTML.gif)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11356-017-9246-4/MediaObjects/11356_2017_9246_Fig2_HTML.gif)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11356-017-9246-4/MediaObjects/11356_2017_9246_Fig3_HTML.gif)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11356-017-9246-4/MediaObjects/11356_2017_9246_Fig4_HTML.gif)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11356-017-9246-4/MediaObjects/11356_2017_9246_Fig5_HTML.gif)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11356-017-9246-4/MediaObjects/11356_2017_9246_Fig6_HTML.gif)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11356-017-9246-4/MediaObjects/11356_2017_9246_Fig7_HTML.gif)
Similar content being viewed by others
References
Abdel Aal A, Barakat MA, Mohamed RM (2008) Electrophoreted Zn–TiO2–ZnO nanocomposite coating films for photocatalytic degradation of 2-chlorophenol. Appl Surf Sci 254:4577–4583. doi:10.1016/j.apsusc.2008.01.049
Baroch P, Saito N, Takai O (2008) Special type of plasma dielectric barrier discharge reactor for direct ozonization of water and degradation of organic pollution. J Phys D Appl Phys 41:085207. doi:10.1088/0022-3727/41/8/085207
Cao GX, Li YG, Zhang QH, Wang HZ (2010b) Synthesis and characterization of La2O3/TiO2-xFx and the visible light photocatalytic oxidation of 4-chlorophenol. J Hazard Mater 178:440–449. doi:10.1016/j.jhazmat.2010.01.101
Cao MH, Wang BB, Yu HS, Wang LL, Yuan SH, Chen J (2010a) Photochemical decomposition of perfluorooctanoic acid in aqueous periodate with VUV and UV light irradiation. J Hazard Mater 179:1143–1146. doi:10.1016/j.jhazmat.2010.02.030
Chen MJ, Lo SL, Lee YC, Huang CC (2015b) Photocatalytic decomposition of perfluorooctanoic acid by transition-metal modified titanium dioxide. J Hazard Mater 288:168–175. doi:10.1016/j.jhazmat.2015.02.004
Chen MJ, Lo SL, Lee YC, Kuo J, Wu CH (2016) Decomposition of perfluorooctanoic acid by ultraviolet light irradiation with Pb-modified titanium dioxide. J Hazard Mater 303:111–118. doi:10.1016/j.jhazmat.2015.10.011
Chen XH, Bian WJ, Song XH, Liu DQ, Zhang J (2013) Degradation of 4-chlorophenol in a dielectric barrier discharge system. Sep Purif Technol 120:102–109. doi:10.1016/j.seppur.2013.09.029
Chen Y, Sun L, Yu ZB, Wang L, Xiang GL, Wan SG (2015a) Synergistic degradation performance and mechanism of 17β-estradiol by dielectric barrier discharge non-thermal plasma combined with Pt–TiO2. Sep Purif Technol 152:46–54. doi:10.1016/j.seppur.2015.07.061
Doong RA, Chen CH, Maithreepala RA, Chang SM (2001) The influence of pH and cadmium sulfide on the photocatalytic degradation of 2-chlorophenol in titanium dioxide suspensions. Water Res 35:2873–2880. doi:10.1016/S0043-1354(00)00580-7
Du CM, Yan JH, Cheron BG (2007) Degradation of 4-chlorophenol using a gas–liquid gliding arc discharge plasma reactor. Plasma Chem Plasma Process 27:635–646. doi:10.1007/s11090-007-9092-0
Elsellami L, Lachheb H, Houas A (2015) Synthesis, characterization and photocatalytic activity of Li-, Cd-, and La-doped TiO2. Mater Sci Semicond Process 36:103–114. doi:10.1016/j.mssp.2015.03.032
Feng JW, Zheng Z, Sun YB, Luan JF, Wang Z, Wang LH, Feng JF (2008) Degradation of diuron in aqueous solution by dielectric barrier discharge. J Hazard Mater 154:1081–1089. doi:10.1016/j.jhazmat.2007.11.013
Grymonpré DR, Sharma AK, Finney WC, Locke BR (2001) The role of Fenton’s reaction in aqueous phase pulsed streamer corona reactors. Chem Eng J 82:189–207. doi:10.1016/S1385-8947(00)00345-4
Hao XL, Zhou MH, Lei le C (2007) Non-thermal plasma-induced photocatalytic degradation of 4-chlorophenol in water. J Hazard Mater 141:475–482. doi:10.1016/j.jhazmat.2006.07.012
He D, Sun Y, Xin L, Feng J (2014) Aqueous tetracycline degradation by non-thermal plasma combined with nano-TiO2. Chem Eng J 258:18–25. doi:10.1016/j.cej.2014.07.089
Hori H, Hayakawa E, Einaga H, Kutsuna S, Koike K, Ibusuki T et al (2004) Decomposition of environmentally persistent perfluorooctanoic acid in water by photochemical approaches. Environ Sci Technol 38:6118–6124. doi:10.1021/es049719n
Hori H, Yamamoto A, Hayakawa E, Taniyasu S, Yamashita N, Kutsuna S et al (2005) Efficient decomposition of environmentally persistent perfluorocarboxylic acids by use of persulfate as a photochemical oxidant. Environ Sci Technol 39:2383–2388. doi:10.1021/es0484754
Hu YM, Bai YH, Li XJ, Chen JR (2013) Application of dielectric barrier discharge plasma for degradation and pathways of dimethoate in aqueous solution. Sep Purif Technol 120:191–197. doi:10.1016/j.seppur.2013.10.005
Huang JY, Wang X, Pan ZQ, Li XK, Ling Y, Li LS (2016) Efficient degradation of perfluorooctanoic acid (PFOA) by photocatalytic ozonation. Chem Eng J 296:329–334. doi:10.1016/j.cej.2016.03.116
Lee YC, Chen MJ, Huang CP, Kuo J, Lo SL (2016) Efficient sonochemical degradation of perfluorooctanoic acid using periodate. Ultrason Sonochem 31:499–505. doi:10.1016/j.ultsonch.2016.01.030
Li L, Zhai ZH, Liu JG, Hu JX (2015b) Estimating industrial and domestic environmental releases of perfluorooctanoic acid and its salts in China from 2004 to 2012. Chemosphere 129:100–109. doi:10.1016/j.chemosphere.2014.11.049
Li SP, Ma XL, Jiang YY, Cao XH (2014) Acetamiprid removal in wastewater by the low-temperature plasma using dielectric barrier discharge. Ecotoxicol Environ Saf 106:146–153. doi:10.1016/j.ecoenv.2014.04.034
Li SP, Ma XL, Liu LJ, Cao XH (2015a) Degradation of 2,4-dichlorophenol in wastewater by low temperature plasma coupled with TiO2 photocatalysis. RSC Adv 5:1902–1909. doi:10.1039/c4ra10797g
Li SP, Xu YJ, Wang XP, Guo YB, Mu QL (2016b) Catalytic degradation of 4-chlorophenol with La/TiO2 in a dielectric barrier discharge system. RSC Adv 6:28994–29002. doi:10.1039/c6ra02807a
Li X, Wang T, Qu G, Liang D, Hu S (2016a) Enhanced degradation of azo dye in wastewater by pulsed discharge plasma coupled with MWCNTs-TiO2/gamma-Al2O3 composite photocatalyst. J Environ Manag 172:186–192. doi:10.1016/j.jenvman.2016.02.040
Lin JC, Hu CY, Lo SL (2016) Effect of surfactants on the degradation of perfluorooctanoic acid (PFOA) by ultrasonic (US) treatment. Ultrason Sonochem 28:130–135. doi:10.1016/j.ultsonch.2015.07.007
Liu DD, Wu ZS, Tian F, Ye BC, Tong YB (2016) Synthesis of N and La co-doped TiO2/AC photocatalyst by microwave irradiation for the photocatalytic degradation of naphthalene. J Alloys Compd 676:489–498. doi:10.1016/j.jallcom.2016.03.124
Magureanu M, Piroi D, Mandache NB, David V, Medvedovici A, Parvulescu VI (2010) Degradation of pharmaceutical compound pentoxifylline in water by non-thermal plasma treatment. Water Res 44:3445–3453. doi:10.1016/j.watres.2010.03.020
Nguyen AT, Juang RS (2015) Photocatalytic degradation of p-chlorophenol by hybrid H(2)O(2) and TiO(2) in aqueous suspensions under UV irradiation. J Environ Manag 147:271–277. doi:10.1016/j.jenvman.2014.08.023
Nguyen HH, Kim K-S (2015) Combination of plasmas and catalytic reactions for CO2 reforming of CH4 by dielectric barrier discharge process. Catal Today 256:88–95. doi:10.1016/j.cattod.2015.04.034
Niu JF, Lin H, Gong C, Sun XM (2013) Theoretical and experimental insights into the electrochemical mineralization mechanism of perfluorooctanoic acid. Environ Sci Technol 47:14341–14349. doi:10.1021/es402987t
Oleyaei SA, Almasi H, Ghanbarzadeh B, Moayedi AA (2016) Synergistic reinforcing effect of TiO2 and montmorillonite on potato starch nanocomposite films: thermal, mechanical and barrier properties. Carbohydr Polym 152:253–262. doi:10.1016/j.carbpol.2016.07.040
Park S, Lee LS, Medina VF, Zull A, Waisner S (2016) Heat-activated persulfate oxidation of PFOA, 6:2 fluorotelomer sulfonate, and PFOS under conditions suitable for in-situ groundwater remediation. Chemosphere 145:376–383. doi:10.1016/j.chemosphere.2015.11.097
Pozan GS, Kambur A (2014) Significant enhancement of photocatalytic activity over bifunctional ZnO-TiO(2) catalysts for 4-chlorophenol degradation. Chemosphere 105:152–159. doi:10.1016/j.chemosphere.2014.01.022
Sansotera M, Persico F, Rizzi V, Panzeri W, Pirola C, Bianchi CL et al (2015) The effect of oxygen in the photocatalytic oxidation pathways of perfluorooctanoic acid. J Fluor Chem 179:159–168. doi:10.1016/j.jfluchem.2015.06.019
Silva AMT, Silva CG, Dražić G, Faria JL (2009) Ce-doped TiO2 for photocatalytic degradation of chlorophenol. Catal Today 144:13–18. doi:10.1016/j.cattod.2009.02.022
Sun B, Sato M, Clements JS (1997) Optical study of active species produced by a pulsed streamer corona discharge in water. J Electrost 39:189–202. doi:10.1016/S0304-3886(97)00002-8
Tian AJ, Wu YB, Mao K (2017) Enhanced performance of surface modified TiO2 nanotubes for the decomposition of perfluorooctanoic acid. 1802:020029. doi: 10.1063/1.4971911
Venkatachalam N, Palanichamy M, Murugesan V (2007) Sol–gel preparation and characterization of alkaline earth metal doped nano TiO2: Efficient photocatalytic degradation of 4-chlorophenol. J Mol Catal A Chem 273:177–185. doi:10.1016/j.molcata.2007.03.077
Wang J, Sun YB, Feng JW, Xin L, Ma JZ (2016a) Degradation of triclocarban in water by dielectric barrier discharge plasma combined with TiO2/activated carbon fibers: effect of operating parameters and byproducts identification. Chem Eng J 300:36–46. doi:10.1016/j.cej.2016.04.041
Wang J, Sun YB, Jiang H, Feng JW (2016b) Removal of caffeine from water by combining dielectric barrier discharge (DBD) plasma with goethite. J Saudi Chem Soc. doi:10.1016/j.jscs.2016.08.002
Xu HM, Cooper WJ, Jung J, Song WH (2011) Photosensitized degradation of amoxicillin in natural organic matter isolate solutions. Water Res 45:632–638. doi:10.1016/j.watres.2010.08.024
Zhang GY, Sun YB, Zhang CX, Yu ZQ (2017b) Decomposition of acetaminophen in water by a gas phase dielectric barrier discharge plasma combined with TiO2-rGO nanocomposite: mechanism and degradation pathway. J Hazard Mater 323:719–729. doi:10.1016/j.jhazmat.2016.10.008
Zhang JB, Zheng Z, Zhang YN, Feng JW, Li JH (2008) Low-temperature plasma-induced degradation of aqueous 2,4-dinitrophenol. J Hazard Mater 154:506–512. doi:10.1016/j.jhazmat.2007.10.053
Zhang WJ, Liu YX, Pei XB, Chen XJ (2017a) Effects of indium doping on properties of xIn-0.1%Gd-TiO2 photocatalyst synthesized by sol-gel method. J Phys Chem Solids 104:45–51. doi:10.1016/j.jpcs.2016.12.031
Zhang YF, Beesoon S, Zhu LY, Martin JW (2013) Isomers of perfluorooctanesulfonate and perfluorooctanoate and total perfluoroalkyl acids in human serum from two cities in North China. Environ Int 53:9–17. doi:10.1016/j.envint.2012.12.007
Zhu D, Jiang L, Liu RL, Chen P, Lang L, Feng JW et al (2014) Wire-cylinder dielectric barrier discharge induced degradation of aqueous atrazine. Chemosphere 117:506–514. doi:10.1016/j.chemosphere.2014.09.031
Acknowledgements
This research was supported by the Technological Progress Plan of Shandong, Grant no. 2011GGE27048, China. The authors are grateful to the anonymous reviewers for their reading of the manuscript and for their suggestions and critical comments.
Author information
Authors and Affiliations
Corresponding author
Additional information
Responsible editor: Vítor Pais Vilar
Electronic supplementary material
ESM 1
(DOCX 780 kb)
Rights and permissions
About this article
Cite this article
Li, S., Wang, X., Liu, L. et al. Enhanced degradation of perfluorooctanoic acid using dielectric barrier discharge with La/Ce-doped TiO2 . Environ Sci Pollut Res 24, 15794–15803 (2017). https://doi.org/10.1007/s11356-017-9246-4
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-017-9246-4