Abstract
In this work, a UV-light assisted peroxymonosulfate (PMS) activation system was constructed with the composite catalyst of multi-walled carbon nanotubes (CNT) — titanium dioxide (TiO2). Under the UV light irradiation, the photoinduced electrons generated from TiO2 could be continuously transferred to CNT for the activation of PMS to improve the catalytic performance of organic pollutant degradation. Meanwhile, the separation of photoinduced electron-hole pairs could enhance the photocatalysis efficiency. The electron spin resonance spectroscopy (EPR) and quenching experiments confirmed the generation of sulfate radical (SO4•−), hydroxyl radical (•OH) and singlet oxygen (1O2) in the UV/PMS/20%CNT-TiO2 system. Almost 100% phenol degradation was observed within 20 min UV-light irradiation. The kinetic reaction rate constant of the UV/PMS/20%CNT-TiO2 system (0.18 min−1) was 23.7 times higher than that of the PMS/Co3O4 system (0.0076 min−1). This higher catalytic performance was ascribed to the introduction of photoinduced electrons, which could enhance the activation of PMS by the transfer of electrons in the UV/PMS/CNT-TiO2 system.
Article PDF
Similar content being viewed by others
Explore related subjects
Discover the latest articles, news and stories from top researchers in related subjects.Avoid common mistakes on your manuscript.
References
Anipsitakis G P, Dionysiou D D (2003). Degradation of organic contaminants in water with sulfate radicals generated by the conjunction of peroxymonosulfate with cobalt. Environmental Science & Technology, 37(20): 4790–4797
Anipsitakis G P, Dionysiou D D (2004). Radical generation by the interaction of transition metals with common oxidants. Environmental Science & Technology, 38(13): 3705–3712
Cao F, Guo Y, Zheng S F, Wu X, Jiang L, Bi R, Wan L, Maier J (2010). Symbiotic coaxial nanocables: Facile synthesis and an efficient and elegant morphological solution to the lithium storage problem. Chemistry of Materials, 22(5): 1908–1914
Chen Q, Ji F, Guo Q, Fan J, Xu X (2014). Combination of heterogeneous Fenton-like reaction and photocatalysis using Co-TiO2 nanocatalyst for activation of KHSO5 with visible light irradiation at ambient conditions. Journal of Environmental Sciences- China, 26(12): 2440–2450
Dikdim J M D, Gong Y, Noumi G B, Sieliechi J M, Zhao X, Ma N, Yang M, Tchatchueng J B (2019). Peroxymonosulfate improved photo-catalytic degradation of atrazine by activated carbon/graphitic carbon nitride composite under visible light irradiation. Chemosphere, 217: 833–842
Duan X, Ao Z, Zhou L, Sun H, Wang G, Wang S (2016). Occurrence of radical and nonradical pathways from carbocatalysts for aqueous and nonaqueous catalytic oxidation. Applied Catalysis B: Environmental, 188: 98–105
Duan X, Sun H, Kang J, Wang Y, Indrawirawan S, Wang S (2015a). Insights into heterogeneous catalysis of persulfate activation on dimensional-structured nanocarbons. ACS Catalysis, 5(8): 4629–4636
Duan X, Sun H, Wang Y, Kang J, Wang S (2015b). N-doping-induced nonradical reaction on single-walled carbon nanotubes for catalytic phenol oxidation. ACS Catalysis, 5(2): 553–559
Fujihara K, Izumi S, Ohno T, Matsumura M (2000). Time-resolved photoluminescence of particulate TiO2 photocatalysts suspended in aqueous solutions. Journal of Photochemistry and Photobiology A Chemistry, 132(1–2): 99–104
Gao Y, Zhu Y, Lyu L, Zeng Q, Xing X, Hu C (2018). Electronic structure modulation of graphitic carbon nitride by oxygen doping for enhanced catalytic degradation of organic pollutants through peroxymonosulfate activation. Environmental Science & Technology, 52(24): 14371–14380
Ghanbari F, Moradi M (2017). Application of peroxymonosulfate and its activation methods for degradation of environmental organic pollutants. Chemical Engineering Journal, 310: 41–62
Golshan M, Kakavandi B, Ahmadi M, Azizi M (2018). Photocatalytic activation of peroxymonosulfate by TiO2 anchored on cupper ferrite (TiO2@CuFe2O4) into 2,4-D degradation: Process feasibility, mechanism and pathway. Journal of Hazardous Materials, 359: 325–337
Guo X, Zhu Y, Han W, Fan X, Li Y, Zhang F, Zhang G, Peng W, Wang S (2019). Nitrogen-doped graphene quantum dots decorated graphite foam as ultra-high active free-standing electrode for electrochemical hydrogen evolution and phenol degradation. Chemical Engineering Science, 194(SI): 54–57
Guo Y, Zeng Z, Li Y, Huang Z, Cui Y (2018). In-situ sulfur-doped carbon as a metal-free catalyst for persulfate activated oxidation of aqueous organics. Catalysis Today, 307: 12–19
He Z, Mansfeld F (2009). Exploring the use of electrochemical impedance spectroscopy (EIS) in microbial fuel cell studies. Energy & Environmental Science, 2(2): 215–219
Hu L, Yang X, Dang S (2011). An easily recyclable Co/SBA-15 catalyst: Heterogeneous activation of peroxymonosulfate for the degradation of phenol in water. Applied Catalysis B: Environmental, 102(1–2): 19–26
Khan A, Liao Z, Liu Y, Jawad A, Ifthikar J, Chen Z (2017). Synergistic degradation of phenols using peroxymonosulfate activated by CuO-Co3O4@MnO2 nanocatalyst. Journal of Hazardous Materials, 329: 262–271
Lee H, Kim H I, Weon S, Choi W, Hwang Y S, Seo J, Lee C, Kim J H (2016). Activation of persulfates by graphitized nanodiamonds for removal of organic compounds. Environmental Science & Technology, 50(18): 10134–10142
Lee H, Lee H J, Jeong J, Lee J, Park N B, Lee C (2015). Activation of persulfates by carbon nanotubes: Oxidation of organic compounds by nonradical mechanism. Chemical Engineering Journal, 266: 28–33
Lei Y, Chen C S, Tu Y J, Huang Y H, Zhang H (2015). Heterogeneous degradation of organic pollutants by persulfate activated by CuO-Fe3O4: Mechanism, stability, and effects of pH and bicarbonate Ions. Environmental Science & Technology, 49(11): 6838–6845
Liang H, Sun H, Patel A, Shukla P, Zhu Z, Wang S (2012). Excellent performance of mesoporous Co3O4/MnO2 nanoparticles in heterogeneous activation of peroxymonosulfate for phenol degradation in aqueous solutions. Applied Catalysis B: Environmental, 127: 330–335
Lim J, Kwak D Y, Sieland F, Kim C, Bahnemann D W, Choi W (2018). Visible light-induced catalytic activation of peroxymonosulfate using heterogeneous surface complexes of amino acids on TiO2. Applied Catalysis B: Environmental, 225: 406–414
Lu S, Wang G, Chen S, Yu H, Ye F, Quan X (2018). Heterogeneous activation of peroxymonosulfate by LaCo1 xCuxO3 perovskites for degradation of organic pollutants. Journal of Hazardous Materials, 353: 401–409
Matafonova G, Batoev V (2018). Recent advances in application of UV light-emitting diodes for degrading organic pollutants in water through advanced oxidation processes: A review. Water Research, 132: 177–189
Ren Y, Lin L, Ma J, Yang J, Feng J, Fan Z (2015). Sulfate radicals induced from peroxymonosulfate by magnetic ferrospinel MFe2O4(M = Co, Cu, Mn, and Zn) as heterogeneous catalysts in the water. Applied Catalysis B: Environmental, 165: 572–578
Shukla P, Fatimah I, Wang S, Ang H M, Tadé M O (2010). Photocatalytic generation of sulphate and hydroxyl radicals using zinc oxide under low-power UV to oxidise phenolic contaminants in wastewater. Catalysis Today, 157(1–4): 410–414
Taha S M, Amer M E, Elmarsafy A M, Elkady M Y, Chovelon J M (2016). Degradation of boscalid by nitrogen-doped/undoped TiO2 and persulfate ions using different activation conditions and the identification of its main degradation products using LC/MS/MS. Chemical Engineering Journal, 288: 845–857
Verma S, Nakamura S, Sillanpää M (2016). Application of UV-C LED activated PMS for the degradation of anatoxin-a. Chemical Engineering Journal, 284: 122–129
Wang G, Chen S, Quan X, Yu H, Zhang Y (2017). Enhanced activation of peroxymonosulfate by nitrogen doped porous carbon for effective removal of organic pollutants. Carbon, 115: 730–739
Wang G, Nie X, Ji X, Quan X, Chen S, Wang H, Yu H, Guo X (2019). Enhanced heterogeneous activation of peroxymonosulfate by Co and N codoped porous carbon for degradation of organic pollutants: the synergism between Co and N. Environmental Science. Nano, 6(2): 399–410
Wang H, Liu S, Wang H, Jiang W (2010). Solar photocatalytic decomposition of two azo dyes on multi walled carbon nanotubes (MWCNTs)/TiO2 composites. Frontiers of Environmental Science & Engineering in China, 4(3): 311–320
Wang J, Wang S (2018). Activation of persulfate (PS) and peroxymonosulfate (PMS) and application for the degradation of emerging contaminants. Chemical Engineering Journal, 334: 1502–1517
Yang M Q, Zhang N, Xu Y J (2013). Synthesis of fullerene-, carbon nanotube-, and graphene-TiO2 nanocomposite photocatalysts for selective oxidation: A comparative study. ACS Applied Materials & Interfaces, 5(3): 1156–1164
Yang Q, Choi H, Chen Y, Dionysiou D D (2008). Heterogeneous activation of peroxymonosulfate by supported cobalt catalysts for the degradation of 2,4-dichlorophenol in water: The effect of support, cobalt precursor, and UV radiation. Applied Catalysis B: Environmental, 77(3–4): 300–307
Yao Y, Li G, Ciston S, Lueptow R M, Gray K A (2008). Photoreactive TiO2/carbon nanotube composites: Synthesis and reactivity. Environmental Science & Technology, 42(13): 4952–4957
Yu H, Quan X, Chen S, Zhao H (2007). TiO2-multiwalled carbon nanotube heterojunction arrays and their charge separation capability. Journal of Physical Chemistry, 111(35): 12987–12991
Yun E T, Lee J H, Kim J, Park H D, Lee J (2018). Identifying the nonradical mechanism in the peroxymonosulfate activation process: Singlet oxygenation versus mediated electron transfer. Environmental Science & Technology, 52(12): 7032–7042
Zhang A, He Y, Chen Y, Feng J, Huang N, Lian F (2018). Degradation of organic pollutants by Co3O4-mediated peroxymonosulfate oxidation: Roles of high-energy exposed TiO2 support. Chemical Engineering Journal, 334: 1430–1439
Zhang D, Qiu R, Song L, Eric B, Mo Y, Huang X (2009). Role of oxygen active species in the photocatalytic degradation of phenol using polymer sensitized TiO2 under visible light irradiation. Journal of Hazardous Materials, 163(2–3): 843–847
Zhang X, Feng M, Wang L, Qu R, Wang Z (2017). Catalytic degradation of 2-phenylbenzimidazole-5-sulfonic acid by peroxymonosulfate activated with nitrogen and sulfur co-doped CNTs-COOH loaded CuFe2O4. Chemical Engineering Journal, 307: 95–104
Zhang Y, Tang Z R, Fu X, Xu Y J (2010). TiO2-graphene nanocomposites for gas-phase photocatalytic degradation of volatile aromatic pollutant: Is TiO2-graphene truly different from other TiO2-carbon composite materials? ACS Nano, 4(12): 7303–7314
Zhang Y, Tang Z R, Fu X, Xu Y J (2011). Engineering the unique 2D mat of graphene to achieve graphene-TiO2 nanocomposite for photocatalytic selective transformation: what advantage does graphene have over its forebear carbon nanotube? ACS Nano, 5(9): 7426–7435
Zhao Q, Mao Q, Zhou Y, Wei J, Liu X, Yang J, Luo L, Zhang J, Chen H, Chen H, Tang L (2017). Metal-free carbon materials-catalyzed sulfate radical-based advanced oxidation processes: A review on heterogeneous catalysts and applications. Chemosphere, 189: 224–238
Zhou Y, Jiang J, Gao Y, Ma J, Pang S Y, Li J, Lu X T, Yuan L P (2015). Activation of peroxymonosulfate by benzoquinone: A novel nonradical oxidation process. Environmental Science & Technology, 49(21): 12941–12950
Zhou Y, Jiang J, Gao Y, Pang S Y, Yang Y, Ma J, Gu J, Li J, Wang Z, Wang L H, Yuan L P, Yang Y (2017). Activation of peroxymonosulfate by phenols: Important role of quinone intermediates and involvement of singlet oxygen. Water Research, 125: 209–218
Acknowledgements
This work was supported by National Natural Science Foundation of China (Grant No. 21590813), Department of Science and Technology of Dalian (No. 2018J11CY012), the Program of Introducing Talents of Discipline to Universities (No. B13012), and program for Changjiang Scholars and Innovative Research Team in University (No. IRT_13R05).
Author information
Authors and Affiliations
Corresponding author
Additional information
Highlights
• CNT-TiO2 composite is used to activate PMS under UV-light assistance.
• Superior performance is due to the enhanced electron-transfer ability of CNT.
• SO4•−, •OH and 1O2 play key roles in the degradation of organic pollutants.
Rights and permissions
About this article
Cite this article
Hao, X., Wang, G., Chen, S. et al. Enhanced activation of peroxymonosulfate by CNT-TiO2 under UV-light assistance for efficient degradation of organic pollutants. Front. Environ. Sci. Eng. 13, 77 (2019). https://doi.org/10.1007/s11783-019-1161-0
Received:
Revised:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11783-019-1161-0