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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2021, Vol. 15 Issue (5) : 85    https://doi.org/10.1007/s11783-020-1379-x
RESEARCH ARTICLE
UV-LED/P25-based photocatalysis for effective degradation of isothiazolone biocide
Xinzheng Li1, Zhiming Li1, Zhihui Xing1, Zhimin Song1, Bei Ye2, Zhengming Wang3(), Qianyuan Wu1()
1. Key Laboratory of Microorganism Application and Risk Control of Shenzhen, Guangdong Provincial Engineering Research Center for Urban Water Recycling and Environmental Safety, International Graduate School at Shenzhen, Tsinghua University, Shenzhen 518055, China
2. China Shenzhen Environmental Science and New Energy Technology Engineering Laboratory, Tsinghua-Berkeley Shenzhen Institute, Shenzhen 518055, China
3. Environmental Management Research Institute, National Institute of Advanced Industrial Science and Technology, 16-1 Onogawa, Tsukuba, Ibaraki, 305-8569, Japan
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Abstract

• UV-LED with shorter wavelength was beneficial for photocatalytic degradation.

• SRNOM dramatically inhibit the degradation.

• ·OH acts as the active radical in photocatalytic degradation.

• Degradation mainly undergoes oxidation, hydrolysis and chain growth reactions.

In this work, LED-based photocatalysis using mixed rutile and anatase phase TiO2 (P25) as the photocatalyst could effectively remove 5-chloro-2-methyl-4-isothiazolin-3-one (CMIT) and methylisothiazolone (MIT) simultaneously, with removal efficiencies above 80% within 20 min. The photocatalytic degradation of both CMIT and MIT could be modeled using a pseudo-first-order rate equation. The photocatalytic degradation rates of CMIT and MIT under LED280 illumination were higher than under LED310 or LED360 illumination. At concentrations below 100 mg/L, the degradation rate of CMIT and MIT under LED illumination significantly increased with increasing catalyst dosage. Additionally, the effects of the chloride ion concentration, alkalinity and dissolved organic matter on the photocatalytic degradation reaction were also investigated. The ·OH free radicals were determined to play the primary role in the photocatalytic degradation reaction, with a degradation contribution of >95%. The photocatalytic degradation of CMIT and MIT mainly occurred via oxidation, hydrolysis, and chain growth reactions. Finally, the possible photocatalytic degradation pathways of CMIT and MIT over LED/P25 are proposed.

Keywords Degradation      Photocatalytic      LED      CMIT      P25     
Corresponding Author(s): Zhengming Wang,Qianyuan Wu   
Issue Date: 17 December 2020
 Cite this article:   
Xinzheng Li,Zhiming Li,Zhihui Xing, et al. UV-LED/P25-based photocatalysis for effective degradation of isothiazolone biocide[J]. Front. Environ. Sci. Eng., 2021, 15(5): 85.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1379-x
https://academic.hep.com.cn/fese/EN/Y2021/V15/I5/85
Fig.1  Degradation of (a, c) CMIT and (b, d) MIT by photolysis (LED alone) and UV-LED photocatalysis over P25. Initial CMIT and MIT concentration were 1 mg/L and 0.33 mg/L respectively, P25 dosage= 200 mg/L, and pH= 7.
Fig.2  Light dose-based first-order kinetics rate constant of CMIT (a) and MIT (b) in photocatalytic degradation over P25 of different dosage under illuminations of LED280, LED310, and LED360. Initial CMIT and MIT concentration were 1 mg/L and 0.33 mg/L respectively, and pH= 7.
Fig.3  Light dose-based first-order kinetics rate constant of CMIT (a) and MIT (b) over P25 at different pH values. Initial CMIT and MIT concentration were 1 mg/L and 0.33 mg/L respectively, P25 dosage= 50 mg/L, and pH= 7.
Fig.4  Light dose-based first-order kinetics rate constant of CMIT (a) and MIT (b) in photocatalytic degradation over P25 under illuminations of LED280, LED310, and LED360 at different chloride ion concentrations. Initial CMIT and MIT concentration were 1 mg/L and 0.33 mg/L respectively, P25 dosage= 50 mg/L, and pH= 7.
Fig.5  Light dose-based first-order kinetics rate constant of CMIT (a) and MIT (b) in photocatalytic degradation over P25 under illuminations of LED280, LED310, and LED360 at different alkalinity, initial CMIT and MIT concentration were 1 mg/L and 0.33 mg/L respectively, P25 dosage= 50 mg/L, and pH= 7.
Fig.6  Light dose-based first-order kinetics rate constant of CMIT (a) and MIT (b) in photocatalytic degradation over P25 under illuminations of LED280, LED310, and LED360 at different NOM concentrations. Initial CMIT and MIT concentration were 1 mg/L and 0.33 mg/L respectively, P25 dosage= 50 mg/L, and pH= 7.
pH a (%) CMIT a (%) MIT
LED280 LED310 LED360 LED280 LED310 LED360
5 87.4 100 100 82.5 100 100
7 95.4 98.9 98.9 93.9 97.9 98.3
9 98.6 99.2 97.7 96.4 98.5 96.9
Tab.1  Inhibition ratio (a) of tBA toward photodegradation of CMIT and MIT at different pH values
No. Experimental m/z Molecular Formula Theorical
m/z
Proposed Structure
P 114 114.0913 C6H12NO+ 114.0913
P 136 136.0723 C6H11NONa+ 136.0733
P 198 197.9639 C4H5NO4S(35Cl)- 197.9633
P 200 199.9616 C4H5NO4S(37Cl)- 199.9604
Tab.2  Possible intermediate structures during photodegradation of CMIT as identified by LC-QTOF-MS
No. Experimental m/z Molecular Formula Theorical
m/z
Proposed Strcuture
P 114 114.0913 C6H12NO+ 114.0913
P 136 136.0723 C6H11NONa+ 136.0733
P 164 164.0006 C4H6NO4S- 164.0012
Tab.3  Possible intermediate structures during photodegradation of MIT as identified by LC-QTOF-MS
Fig.7  The change in MASS response intensity of degraded species during photocatalysis of CMIT (a,b,c) and MIT (d,e,f) under illuminations of LED280 (a, d), LED310 (b, e), and LED360 (c, f).
Fig.8  Possible degradation pathways of CMIT (a) and MIT (b) during the UV-LED/P25 photocatalysis.
1 G V Buxton, C L Greenstock, W P Helman, A B Ross (1988). Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (·OH/·O−) in aqueous solution. Journal of Physical and Chemical Reference Data, 17(2): 513
https://doi.org/10.1063/1.555805
2 L Chen, W Zhang, R Ye, C Hu, Q Wang, F Seemann, D W T Au, B Zhou, J P Giesy, P Y Qian (2016). Chronic exposure of marine medaka (Oryzias melastigma) to 4,5-dichloro-2-noctyl-4-isothiazolin-3-one (DCOIT) reveals its mechanism of action in endocrine disruption via the hypothalamus-pituitary- gonadal-liver (HPGL) axis. Environmental Science & Technology, 50(8): 4492–4501
https://doi.org/10.1021/acs.est.6b01137
3 Y Chen, J S Ye, C S Li, P L Zhou, J Liu, H Ou (2018). Degradation of 1H-benzotriazole by UV/H2O2 UV/TiO and2: Kinetics, mechanisms, products and toxicology. Environmental Science and Pollution Research International, 4: 1282–1295
4 P J Collier, A Ramsey, R D Waigh, K T Douglas, P Austin, P Gilbert (1990). Chemical reactivity of some isothiazolone biocides. Journal of Applied Bacteriology, 69(4): 578–584
https://doi.org/10.1111/j.1365-2672.1990.tb01551.x
5 X V Van Doorslaer, K Demeestere, P M Heynderickx, M Caussyn, H Van Langenhove, F Devlieghere, A Vermeulen, J Dewulf (2013). Heterogeneous photocatalysis of moxifloxacin: Identification of degradation products and determination of residual antibacterial activity. Applied Catalysis B: Environmental, 138-139: 333–341
https://doi.org/10.1016/j.apcatb.2013.03.011
6 E S Elmolla, M Chaudhuri (2010). Photocatalytic degradation of amoxicillin, ampicillin and cloxacillin antibiotics in aqueous solution using UV/TiO2 and UV/H2O2/TiO2 photocatalysis. Desalination, 252(1–3): 46–52
https://doi.org/10.1016/j.desal.2009.11.003
7 J Fang, Y Fu, C Shang (2014). The roles of reactive species in micropollutant degradation in the UV/free chlorine system. Environmental Science & Technology, 48(3): 1859–1868
https://doi.org/10.1021/es4036094
8 W Han, Y Chen, L Wang, X Sun, J Li (2011). Mechanism and kinetics of electrochemical degradation of isothiazolinones using Ti/SnO2-Sb/PbO2 anode. Desalination, 276(1–3): 82–88
https://doi.org/10.1016/j.desal.2011.03.027
9 K He, J Huang, C F Lagenaur, E Aizenman (2006). Methylisothiazolinone, a neurotoxic biocide, disrupts the association of SRC family tyrosine kinases with focal adhesion kinase in developing cortical neurons. Journal of Pharmacology and Experimental Therapeutics, 317(3): 1320–1329
https://doi.org/10.1124/jpet.106.103044
10 L Ismail, C Ferronato, L Fine, F Jaber, J M Chovelon (2018). Effect of water constituents on the degradation of sulfaclozine in the three systems: UV/TiO2, UV/K2S2O8, and UV/TiO2/K2S2O8. Environmental Science and Pollution Research International, 25(3): 2651–2663
https://doi.org/10.1007/s11356-017-0629-3
11 A Li, Q Y Wu, G P Tian, H Y Hu (2016). Effective degradation of methylisothiazolone biocide using ozone: Kinetics, mechanisms, and decreases in toxicity. Journal of Environmental Management, 183: 1064–1071
https://doi.org/10.1016/j.jenvman.2016.08.057
12 J Li, X Dong, G Zhang, W Cui, W Cen, S C Wu , Dong F Lee, (2019). Probing ring-opening pathways for efficient photocatalytic toluene decomposition. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 7(7): 3366–3374
https://doi.org/10.1039/C8TA11627J
13 Y Liu, X He, X Duan, Y Fu, D D Dionysiou (2015). Photochemical degradation of oxytetracycline: Influence of pH and role of carbonate radical. Chemical Engineering Journal, 276: 113–121
https://doi.org/10.1016/j.cej.2015.04.048
14 W Mao, L X Zhang, T Y Wang, Y C Bai, Y T Guan (2021). Fabrication of highly efficient Bi2WO6/CuS composite for visible-light photocatalytic removal of organic pollutants and Cr(VI) from wastewater. Frontiers of Environmental Science and Engineering, 15, 52
15 C Minero, P Pellizzari, V Maurino, E Pelizzetti, D Vione (2008). Enhancement of dye sonochemical degradation by some inorganic anions present in natural waters. Applied Catalysis B: Environmental, 77(3–4): 308–316
https://doi.org/10.1016/j.apcatb.2007.08.001
16 A Piscopo, D Robert, J V Weber (2001). Influence of pH and chloride anion on the photocatalytic degradation of organic compounds. Applied Catalysis B: Environmental, 35(2): 117–124
https://doi.org/10.1016/S0926-3373(01)00244-2
17 C Richard, F Bosquet, F J Pilichowski (1997). Photocatalytic transformation of aromatic compounds in aqueous zinc oxide suspensions: effect of substrate concentration on the distribution of products. Journal of Photochemistry and Photobiology A Chemistry, 108(1): 45–49
https://doi.org/10.1016/S1010-6030(96)04431-0
18 V A Sakkas, I K Konstantinou, T A Albanis (2002). Aquatic phototransformation study of the antifouling agent Sea-Nine 211: Identification of byproducts and the reaction pathway by gas chromatography-mass spectroscopy. Journal of Chromatography. A, 959(1–2): 215–227
https://doi.org/10.1016/S0021-9673(02)00430-2
19 T Sultan, J Cho (2016). Optimization of a UV/H2O2 AOP system using scavenger radicals and response surface methodology. Chemical Engineering Communications, 203(8): 1093–1104
https://doi.org/10.1080/00986445.2015.1124097
20 K Suttiponparnit, J K Jiang, M Sahu, S Suvachittanont, T Charinpanitkul, P Biswas (2011). Role of surface Area, primary particle size, and crystal phase on titanium dioxide nanoparticle dispersion properties. Nanoscale Research Letters, 6: 27–35
21 K H Wang, Y H Hsieh, M Y Chou, C Y Chang (1999). Photocatalytic degradation of 2-chloro and 2-nitrophenol by titanium dioxide suspensions in aqueous solution. Applied Catalysis B: Environmental, 21(1): 1–8
https://doi.org/10.1016/S0926-3373(98)00116-7
22 K H Wang, Y H Hsieh, C H Wu, C Y Chang (2000). The pH and anion effects on the heterogeneous photocatalytic degradation of o-methylbenzoic acid in TiO2 aqueous suspension. Chemosphere, 40(4): 389–394
https://doi.org/10.1016/S0045-6535(99)00252-0
23 W L Wang, Q Y Wu, Z M Wang, H Y Hu, N Negishi, M Torimura (2015). Photocatalytic degradation of the antiviral drug Tamiflu by UV-A/TiO2: Kinetics and mechanisms. Chemosphere, 131: 41–47
https://doi.org/10.1016/j.chemosphere.2015.02.032
24 Z M Wang, T Hirotsu, H Wu, H Kanoh (2018). Advantaging synergy photocatalysis with carbon as a counterpart player of titania. Chemical Record (New York, N.Y.), 18: 1–15
25 Q Y Wu, J Wang, Z W Wang, Y L Xu, Z H Xing, X Y Zhang, Y T Guan, G F Liao, X Z Li (2020). High-loaded single Cu atoms decorated on N-doped graphene for boosting Fenton-like catalysis under neutral pH. Journal of Material Chemistry A, 8:13685–13693
26 B Ye, Z Chen, X Z Li, J N Liu, Q Y Wu, C Yang, H Y Hu, R H Wang (2019). Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of bromide-containing water. Frontiers of Environmental Science and Engineering, 13(6): 86–94
27 K Zhang, J Wang, W J Jiang, W Q Yao, H P Yang, Y F Zhu (2018). Self-assembled perylene diimide based supramolecular heterojunction with Bi2WO6 for efficient visible-light-driven photocatalysis. Applied Catalysis B: Environmental, 232: 175–181
https://doi.org/10.1016/j.apcatb.2018.03.059
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