Sonocatalytic Degradation of p-Chlorophenol by Nanoscale Zero-valent Copper Activated Persulfate under Ultrasonic Irradiation in Aqueous Solutions

Document Type : Original Article

Authors

1 Department of Environmental Health Engineering, Hamadan University of Medical Sciences, Hamadan, Iran

2 Social Determinants of Health Research Center, Department of Environmental Health Engineering, Hamadan University of Medical Sciences, Hamadan, Iran

Abstract

In this study, nanoscale zero-valent copper (nZVC) as catalyst activated persulfate (PS) was used for the degradation of p-chlorophenol (p-CP) under ultrasonic (US) irradiation in aqueous solution. The effect of different operational parameters such as solution pH (3.5-10.5), PS concentration (1-7.5 mm/L), nZVC dosage (5-35 mg/L) and initial p-CP concentration (10-100 mg/L) were evaluated at different contact time. Results indicated that US/PS/nZVC system achieve higher efficiency in p-CP degradation than US/PS, US/nZVC and PS/nZVC systems. The optimal p-CP removal efficiency (98%) was achieved within 40 min with 5 mm/L PS and 30mg/L nanocatalyst at 25 mg/L initial p-CP concentration. It was also observed that the p-CP degradation rate depends on initial p-CP concentrations. To clarify the mineralization of p-CP, TOC and COD were analyzed at optimum conditions. COD and TOC removal rate obtained from the US/PS/nZVC system with contact time of 60 min were 61and 75%, respectively. Through the use of methanol (MA) and tert-butyl alcohol (TBA) as radical scavengers,  was identified as the main radical species that are generated during processes. The removal process of p-CP could be described by the pseudo-first-order kinetics. The apparent degradation rate constant (k) was 0.076 min-1 in US/PS/nZVC system at optimal conditions.

Keywords


 
1. Zhou, P., Zhang, J., Zhang, Y., Zhang, G., Li, W., Wei, C., Liang,
J., Liu, Y. and Shu, S., “Degradation of 2,4-dichlorophenol by
activating persulfate andperoxomonosulfate using micron or
nanoscale zero-valent copper”, Journal of Hazardous Materials,
Vol. 344, (2018),  1209-1219.  
2. Nguyen, A.T  and Juang, R.S., “Photocatalytic degradation of pchlorophenol
byhybrid H2O2 and TiO2
 in aqueous suspensions
under UV irradiation”, Journal of  Environmental Management,
Vol. 147, (2015),  271-277.  
3. Jamali, A., Vanraes, R., Hanselaer, P. and Van Gerven,  T., “A
batch LED reactor for the photocatalytic degradation of phenol”,
Chemical Engineering Journal, Vol. 71, (2013), 43-50.  
4. Seidmohammadi, A., Amiri, R., Faradmal, J., Lili, M. and Asgari,
Gh., “UVA-LED assisted persulfate/nZVI and hydrogen
peroxide/ nZVI for degrading 4-chlorophenol in aqueous
solutions”, Korean Journal of Chemical Engineering, Vol. 35,
(2018), 694-701.  
5. Van Aken, P., Van den Broeck, R., Degrève, J., Dewil, R., “The
effect of ozonation on the toxicity and biodegradability of 2,4dichlorophenol-containing
wastewater”,
Chemical Engineering
Journal, Vol. 280, (2015), 728-736.  
6. Swati, S. and Anurag, G., “Catalytic oxidative degradation of 4‐
chlorophenol: Effect of operating parameters and prediction of
intermediates/by‐products”, Environmental Progress and
Sustainable, Vol. 36, (2017), 1734-1742.  
7. Movahedyan, H., Mohammadi, A.S. and Assadi, A.,
“Comparison of different advanced oxidation processes
degrading p-chlorophenol in aqueous solution”. Iranian Journal
of Environmental Health Science Enginering, Vol. 6, (2009),
153-160. 
8. Dadban, Y., bahram kamarehie, B., Seyyed Alireza Mousavi,
SA., khoramabadi, Gh., Mohamadiyan, J. and Godini, H.,
"Aniline degradation using advanced oxidation process by
UV/peroxy disulfate from aqueous solution", International
Journal of Engineering, Transactions B: Applications, Vol. 30,
No. 5, (2017), 684-690. 
9. Behfar, R., Davarnejad, R. and Heydari, R., "Pharmaceutical
Wastewater Chemical Oxygen Demand Reduction: ElectroFenton,
UV-enhanced Electro-Fenton and Activated Sludge",
International Journal of Engineering, Transactions C:
Aspects, Vol. 32, No. 12, (2019), 1710-1715. 
10. Sun, J., Liu, X., Zhang, F., Zhou, J. and Li, J., “Insight into the
mechanism of adsorption of phenol and resorcinol on activated
carbons with different oxidation degrees”, Colloids and Surfaces
A: Physicochemical and Engineering Aspects, Vol. 563, (2019),
22-30.  
11. Titus, M.P., Molina, V.G. and Banos M.A., “Degradation of
chlorophenols by means advanced oxidation process: a general
review”, Applied Catalysis B: Environmental, Vol. 47, (2004),
219-226.  
12. Oputu, O., Chowdhury, M., Nyamayaro, K., Fatoki, O. and
Fester, V., “Catalytic activities of ultra-small β-FeOOH nanorods
in ozonation of 4-chlorophenol”, Journal of Environmental
Science.  Vol. 35, (2015), 83-90.  
13. Barzegar, G.; Jorfi, S.; Zarezade, V.; Khatebasreh, M. and
Ghanbari, F., “4-Chlorophenol degradation using
ultrasound/peroxymonosulfate/nanoscale zero valent iron:
Reusability, identification of degradation intermediates and
potential application for real wastewater”, Chemosphere, Vol.
201, (2018), 370-379. 
14. Seidmohammadi, A.; Asgari,  G. and Torabi,  L., “Removal of
metronidazole using ozone activated persulfate from aqua
solutions in presence of ultrasound”. Journal of Mazendradan
University of Medical Siences, Vol. 26, (2016), 160-169.  
15. Wang, C. and Liu, C., “Decontamination of alachlor herbicide
wastewater by a continuous dosing mode ultarsound/Fe2+/H2O2
process”, Journal of Environmental Science, Vol. 26, (2014),
1332-1339.  
16. Wang, S. and Zhou, N., “Removal of carmazepine from aqueous
solution using sono-activated persulfate process”, Ultrasound
Sonochemistry, Vol. 29, (2016), 156-162.   
17. Seidmohammadi, A.; Asgari, Gh.; Ghorbanian, Z. and Dargahi,
A., “The removal of cephalexin antibiotic in aqueous solutions by
ultrasonic waves/hydrogen peroxide/nickel oxide nanoparticles
(US/H2O2/NiO) hybrid process”, Separation and Science Technology, Vol. 55, (2020). 
18. Song, S., He, Z. and Chen, J., “US/O3 combination degradation of aniline in aqueous solution”, Ultrasound Sonochemistry, Vol. 14,
(2007), 84-88.  
19. Seid-Mohammadi, A., Asgari, G., Poormohammadi, A.,
Ahmadian, M. and Rezaeivahidian, H., “Removal of phenol at
high concentrations using UV/Persulfate from saline
wastewater”, Desalination and Water Treatment, Vol. 57,
(2016), 19988-19995.  
20. Weng, C.H., Ding, F., Lin, Y.T. and Liu, N., “Effective
decolorization of polyazo direct dye Sirius Red F3B using
persulfate activated with Fe aggregate”, Sepration and
Purification  Technology, Vol. 147, (2015), 147-155.  
21. Wei, X., Gao, N., Li, C., Deng, Y., Deng, S. and Li,  L. “ZeroValent iron activation of persulfate (PS) for oxidation of bentazon in water”. Chemical Engineering Journal, Vol. 285, (2016),
660-670.  
22. Monteagudo, J. M., El-taliawy, H., Durán, A., Caro, G. and
Bester, K., “Sono-activated persulfate oxidation of diclofenac:
Degradation, kinetics, pathway and contribution of the different
radicals involved”, Journal of Hazardous Materials, Vol. 357,
(2018), 457-465.  
23. Yuefei, J., Changxun, D., Deyang, K., Junhe, L. and Quansuo, Z.,
“Heat-activated persulfate oxidation of atrazine: Implications for
remediation of groundwater contaminated by herbicides”,
Chemical Engineering Journal,   Vol. 263, (2015), 45-54.  
24. Ghorbanian, Z.,  Asgari, Gh., Sammadi, MT. and Seidmohammadi,
A., “Removal of 2,4 dichlorophenol using microwave assisted
nanoscale zero-valent copper activated persulfate from aqueous
solutions: Mineralization, kinetics, and degradation pathways”, 
Journal of Molecular Liquids, Vol. 296, (2019), 111-120.
25. Gao, Y., Gao, N., Wang, W., Kang, S., Xu, J., Xiang, H. and Yin, 
D., “Ultrasound-assisted heterogeneous activation of persulfate
by nano zerovalent iron (nZVI) for the propranolol degradation in
water”, Ultrasound Sonochemistry, Vol. 49, (2018), 33–40.  
26. Chen, W. and Huang, C.P., “Mineralization of dinitrotoluenes in
aqueous solution by sono-activated persulfate enhanced with
electrolytes”, Ultrasound Sonochemistry, Vol. 51, (2019), 129133.

27. Liu, F., Yi, P., Wang, X., Gao, H. and Zhang, H., “Degradation
of Acid Orange 7 by an ultrasound/ZnO-GAC/persulfate Process.
Separation Science Technology, Vol. 194, (2018),  181-187.  
28. Drijvers, D., Van Langenhove, H. and Beckers, M.,
“Decomposition of phenol and trichloroethylene by the
ultrasound/H2O2/CuO process”, Water Research, Vol. 33,
(1999), 1187-1194.   
29. Zhang, Y., Zhang, Q., Dong, Z., Wu, L. and Hong, J.,
“Degradation of acetaminophen with ferrous/copperoxide
activate persulfate: Synergism of iron and copper”, Water
Research, Vol. 146, (2018), 232-243.  
30. APHA, AWWA, WEF. (2005). Standard methods for the
examination of water and wastewater. APHA. 31 Ed.,
Washington. DC.  
31. Wen, G., Wang, S.J., Ma. J., Huang, T.L., Liu, Z.Q., Zhao. L. and
Xu, J.L., “Oxidative degradation of organic pollutants in aqueous
solution using zero valent copper under aerobic atmosphere
condition”, Journal of Hazardous Materials, Vol. 275, (2014),
193-199.  
32. Zhang, Y.F., Fan, J.H., Yang, B., Huang, W.T. and Ma, L.M.,
“Copper-catalyzed activationof molecular oxygen for oxidative
destruction of acetaminophen: the mechanism and superoxide