Enhanced activation of peroxymonosulfate by CNT-TiO<sub>2</sub> under UV-light assistance for efficient degradation of organic pollutants

doi:10.1007/s11783-019-1161-0

Front. Environ. Sci. Eng.

2019, Vol. 13

Issue (5) : 77 https://doi.org/10.1007/s11783-019-1161-0

RESEARCH ARTICLE

Enhanced activation of peroxymonosulfate by CNT-TiO₂ under UV-light assistance for efficient degradation of organic pollutants

Xuemin Hao¹, Guanlong Wang², Shuo Chen¹(

), Hongtao Yu¹, Xie Quan¹

¹. Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
². School of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian 116034, China

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Abstract

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.

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.

Keywords Peroxymonosulfate activation Carbon nanotubes TiO₂ Water treatment

Corresponding Author(s): Shuo Chen

Issue Date: 27 September 2019

Cite this article:

Xuemin Hao,Guanlong Wang,Shuo Chen, et al. Enhanced activation of peroxymonosulfate by CNT-TiO₂ under UV-light assistance for efficient degradation of organic pollutants[J]. Front. Environ. Sci. Eng., 2019, 13(5): 77.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-019-1161-0
https://academic.hep.com.cn/fese/EN/Y2019/V13/I5/77

Fig.1 The scheme of the reaction device.

Fig.2 The surface morphology images of CNT (a), TiO₂ (b) and 20% CNT-TiO₂ composite catalysts (c) with its details (d).

Tab.1 Specific surface properties and pore volume of TiO₂, CNT and composites

Fig.3 The pore distribution of the catalysts which based on their nitrogen desorption curves.

Fig.4 The UV-Vis spectra (a) and the X-ray diffraction pattern (b) of the TiO₂, CNT and CNT-TiO₂ composites of different CNT content.

Fig.5 The phenol removal (a) and kinetic rates of phenol degradation (b) in various reaction systems. ([phenol] = 10 mg/L, [catalyst] = 0.5 g/L, the molar ratio of phenol/PMS= 1:16, initial pH= 6.98, t = 30°C).

Fig.6 The phenol removal in the UV, PMS, UV/TiO₂ and PMS/CNT systems. ([phenol] = 10 mg/L, [catalyst] = 0.5 g/L, the molar ratio of phenol/PMS= 1:16, initial pH= 6.98, t = 30°C).

Fig.7 Degradation of different pollutants by UV/PMS/20%CNT-TiO₂ system. ([pollutant] = 10 mg/L, [catalyst] = 0.5 g/L, the molar ratio of pollutant/PMS= 1:16, initial pH= 6.98, t = 30°C).

Fig.8 The effect of different doping amounts of CNT in composite (a), initial pH (b), composite dosage (c) and the molar ratio of phenol/PMS (d) in UV/PMS/composite system ([phenol] = 10 mg/L, the doping amount of CNT= 5%–20%, [catalyst] = 0.1–0.7 g/L, the molar ratio of phenol/PMS= 1:4–1:32, initial pH= 3.19–9.13, t = 30°C).

Fig.9 Phenol degradation by the UV/PMS/20%CNT-TiO₂ system in the presence of TBA, MeOH and L-histidine. ([phenol] = 10 mg/L, [catalyst] = 0.5 g/L, the molar ratio of phenol/PMS= 1:16, the molar ratio of MeOH/PMS= TBA/PMS= 500, [L-histidine] = 0.1 mmol/L, initial pH= 6.98, t = 30°C).

Fig.10 The EPR spectra for SO₄•⁻, •OH and ¹O₂ in the various systems. ([catalyst] = 0.5 g/L, the molar ratio of phenol/PMS= 1:16, [DMPO] = 50 mmol/L, [TMP] = 50 mmol/L, t = 25°C).

Fig.11 The PL spectra of TiO₂, CNT and 20%CNT-TiO₂ composite.

Fig.12 Electrochemical impedance spectroscopy Nynquist plots of 20%CNT-TiO₂ /UV, 20%CNT-TiO₂/PMS and UV/PMS/20%CNT-TiO₂ reaction system. (Scan rate: 5 mV/s, frequency range 0.1–1.0 × 10⁶ Hz, [Na₂SO₄] = 0.01 mol/L, [PMS] = 0.087 mmol/L).

Fig.13 A hypothetical reaction mechanism diagram of the UV/PMS/20%CNT-TiO₂ system.

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