RESEARCH ARTICLE

Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced by high gravity technology

  • Weizhou Jiao ,
  • Shengjuan Shao ,
  • Peizhen Yang ,
  • Kechang Gao ,
  • Youzhi Liu
Expand
  • Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering, National Demonstration Center for Experimental Comprehensive Chemical Engineering Education, North University of China, Taiyuan 030051, China

Received date: 03 May 2020

Accepted date: 25 Jul 2020

Published date: 15 Oct 2021

Copyright

2021 Higher Education Press

Abstract

This study investigated the indirect oxidation of nitrobenzene (NB) by hydroxyl radicals (·OH) in a rotating packed bed (RPB) using competitive kinetics method with p-nitrochlorobenzene as a reference compound. The rate constants of NB with ·OH are calculated to be between (1.465±0.113) × 109 L/(mol·s) and (2.497±0.192) × 109 L/(mol·s). The experimental data are fitted by the modified Arrhenius equation, where the activation energy is 4877.74 J/mol, the order of NB concentration, rotation speed, and initial pH is 0.2425, 0.1400 and 0.0167, respectively. The ozonation process of NB could be enhanced by RPB, which is especially effective for highly concentrated NB-containing wastewater under alkaline conditions. The high gravity technology can accelerate ozone mass transfer and self-decomposition of ozone to produce more ·OH, resulting in an increase in the indirect oxidation rate of NB by ·OH and consequently effective degradation of NB in wastewater.

Cite this article

Weizhou Jiao , Shengjuan Shao , Peizhen Yang , Kechang Gao , Youzhi Liu . Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced by high gravity technology[J]. Frontiers of Chemical Science and Engineering, 2021 , 15(5) : 1197 -1205 . DOI: 10.1007/s11705-020-1998-6

Acknowledgements

This work was supported by the Specialized Research Fund for Sanjin Scholars Program of Shanxi Province (No. 201707), Key Research & Development Plan of Shanxi Province (No. 201903D321059), Shanxi Scholarship Council of China (No. HGKY2019071), and Transformation and Cultivation Projects of Scientific and Technological Achievements of Higher Education Institutions for Shanxi Province (No. 2020CG040).
1
Liu H T, Sui M H, Yuan B J, Wang J Y, Lv Y N. Efficient degradation of nitrobenzene by Cu-Co-Fe-LDH catalyzed peroxymonosulfate to produce hydroxyl radicals. Chemical Engineering Journal, 2019, 357: 140–149

2
Palmisano G, Loddo V, Augugliaro V, Palmisano L, Yurdakal S. Photocatalytic oxidation of nitrobenzene and phenylamine: pathways and kinetics. AIChE Journal. American Institute of Chemical Engineers, 2010, 53: 961–968

3
Jiao W Z, Yang P Z, Gao W Q, Qiao J J, Liu Y Z. Apparent kinetics of the ozone oxidation of nitrobenzene in aqueous solution enhanced by high gravity technology. Chemical Engineering and Processing-Process Intensification, 2019, 146: 107690

4
Jiao W Z, Qin Y J, Luo S, He Z, Feng Z R, Liu Y Z. Simultaneous formation of nanoscale zero-valent iron and degradation of nitrobenzene in wastewater in an impinging stream-rotating packed bed reactor. Chemical Engineering Journal, 2017, 321: 564–571

5
Duan H T, Liu Y, Yin X H, Bai J F, Qi J. Degradation of nitrobenzene by Fenton-like reaction in a H2O2/schwertmannite system. Chemical Engineering Journal, 2016, 283: 873–879

6
Yang P Z, Luo S, Liu Y Z, Jiao W Z. Degradation of nitrobenzene wastewater in an acidic environment by Ti(IV)/H2O2/O3 in a rotating packed bed. Environmental Science and Pollution Research International, 2018, 25: 25060–25070

7
Elshafei G M S, Yehia F Z, Dimitry O H, Badawi A M, Eshaq G. Ultrasonic assisted-Fenton-like degradation of nitrobenzene at neutral pH using nanosized oxides of Fe and Cu. Ultrasonics Sonochemistry, 2014, 21: 1358–1365

8
Wu J, Su T M, Jiang Y X, Xie X L, Qin Z Z, Ji H B. Catalytic ozonation of cinnamaldehyde to benzaldehyde over CaO: experiments and intrinsic kinetics. AIChE Journal. American Institute of Chemical Engineers, 2017, 63: 4403–4417

9
Martins R C, Cardoso M, Dantas R F, Sans C, Esplugas S, Quinta-Ferreira R M. Catalytic studies for the abatement of emerging contaminants by ozonation. Journal of Chemical Technology and Biotechnology (Oxford, Oxfordshire), 2015, 90: 1611–1618

10
Huber M M, Canonica S, Park G Y, Von Gunten U. Oxidation of pharmaceuticals during ozonation and advanced oxidation processes. Environmental Science & Technology, 2013, 37: 1016–1024

11
Sun X M, Wu C Y, Zhou Y X, Han W. Using DOM fraction method to investigate the mechanism of catalytic ozonation for real wastewater. Chemical Engineering Journal, 2019, 369: 100–108

12
Chiang Y P, Liang Y Y, Chang C N, Chao A C. Differentiating ozone direct and indirect reactions on decomposition of humic substances. Chemosphere, 2006, 65: 2395–2400

13
Beltrán F J, Encinar J M, Alonso M A. Nitroaromatic hydrocarbon ozonation in water. 1. Single ozonation. Industrial & Engineering Chemistry Research, 1998, 37: 25–31

14
Hoigné J, Bader H. Rate constants of reactions of ozone with organic and inorganic compounds in water—I: non-dissociating organic compounds. Water Research, 1983, 17(2): 173–183

15
Jiao W Z, Luo S, He Z, Liu Y Z. Applications of high gravity technologies for wastewater treatment: a review. Chemical Engineering Journal, 2017, 313: 912–927

16
Burns J R, Ramshaw C. Process intensification: visual study of liquid maldistribution in rotating packed beds. Chemical Engineering Science, 1996, 51: 1347–1352

17
Chen Y H, Chang C Y, Su W L, Chiu C Y, Yu Y H, Chiang P C, Chang C F, Shie J L, Chiou C S. Chiang S I M. Ozonation of CI Reactive Black 5 using rotating packed bed and stirred tank reactor. Journal of Chemical Technology and Biotechnology, 2015, 80: 68–75

18
Chiang C Y, Chen Y S, Liang M S, Lin F Y, Tai C Y D, Liu H S. Absorption of ethanol into water and glycerol/water solution in a rotating packed bed. Journal of the Taiwan Institute of Chemical Engineers, 2009, 40: 418–423

19
Luo Y, Chu G W, Zhou H K, Zhao Z Q, Dudukovic M P, Chen J F. Gas-liquid effective interfacial area in a rotating packed bed. Industrial & Engineering Chemistry Research, 2012, 51: 16320–16352

20
Zeng Z Q, Zhou H K, Li X, Arowo M, Sun B C, Chen J F, Chu G W, Shao L. Degradation of phenol by ozone in the presence of Fenton reagent in a rotating packed bed. Chemical Engineering Journal, 2013, 229: 404–411

21
Jiao W Z, Liu Y Z, Liu W L, Li J, Shao F, Wang C R. Degradation of nitrobenzene-containing wastewater with O3 and H2O2 by high gravity technology. China Petroleum Processing and Petrochemical Technology, 2013, 15(1): 85–94

22
Guo L, Jiao W Z, Liu Y Z, Xu C C, Liu W L, Li J. Treatment of nitrobenzene-containing wastewater using different combined processes with ozone. Chinese Journal Energetic Materials, 2014, 22(5): 702–708

23
Yang P Z, Luo S, Liu H Y, Jiao W Z, Liu Y Z. Aqueous ozone decomposition kinetics in a rotating packed bed. Journal of the Taiwan Institute of Chemical Engineers, 2019, 96: 11–17

24
Jung Y, Hong E, Kwon M, Kang J W. A kinetic study of ozone decay and bromine formation in saltwater ozonation: effect of O3 dose, salinity, pH, and temperature. Chemical Engineering Journal, 2017, 312: 30–38

25
Chu W, Ma C W. Quantitative prediction of direct and indirect dye ozonation kinetics. Water Research, 2000, 34: 3153–3160

26
Zhao Y, Yu G, Chen S Y, Zhang S Y, Wang B, Huang J, Deng S B, Wang Y J. Ozonation of antidepressant fluoxetine and its metabolite product norfluoxetine: kinetics, intermediates and toxicity. Chemical Engineering Journal, 2017, 316: 951–963

27
Chen W R, Wu C, Elovitz M S, Linden K G, Suffet I H. Reactions of thiocarbamate, triazine and urea herbicides, RDX and benzenes on EPA Contaminant Candidate List with ozone and with hydroxyl radicals. Water Research, 2008, 42(1-2): 137–144

28
Hoigné J. Inter-calibration of ·OH radical sources and water quality parameters. Water Science and Technology, 1997, 35: 1–8

29
Leitner N K V, Roshani B. Kinetic of benzotriazole oxidation by ozone and hydroxyl radical. Water Research, 2010, 44(6): 2058–2066

30
El Najjar N H, Touffet A, Deborde M, Journel R, Leitner N K V. Levofloxacin oxidation by ozone and hydroxyl radicals: kinetic study, transformation products and toxicity. Chemosphere, 2013, 93(4): 604–611

31
Wang Z Y, Shao Y S, Gao N Y, An A. Degradation kinetic of dibutyl phthalate (DBP) by sulfate radical-and hydroxyl radical-based advanced oxidation process in UV/persulfate system. Separation and Purification Technology, 2018, 195: 92–100

32
Shen J M, Chen Z L, Xu Z Z, Li X Y, Xu B B, Qi F. Kinetics and mechanism of degradation of p-chloronitrobenzene in water by ozonation. Journal of Hazardous Materials, 2008, 152: 1325–1331

33
Li B Z, Xu X, Zhu L. Ozonation of chloronitrobenzenes in aqueous solution: kinetics and mechanism. Journal of Chemical Technology and Biotechnology, 2009, 84: 167–175

34
Wang F, Wang Y, Ji M. Mechanisms and kinetics models for ultrasonic waste activated sludge disintegration. Journal of Hazardous Materials, 2005, 123: 145–150

35
Ko C H, Guan C Y, Lu P J, Chern J M. Ozonation of guaiacol solution in a rotating packed bed. Chemical Engineering Journal, 2011, 171: 1045–1052

36
Zeng Z Q, Zou H K, Li X, Sun B C, Chen J F, Shao L. Ozonation of phenol with O3/Fe(II) in acidic environment in a rotating packed bed. Industrial & Engineering Chemistry Research, 2012, 51: 10509–10516

37
Zhao W R, Wu Z B, Wang D H. Ozone direct oxidation kinetics of cationic red X-GRL in aqueous solution. Journal of Hazardous Materials, 2006, 137(3): 1859–1865

38
Zhao W R, Liu F F, Yang Y, Tan M, Zhao D Y. Ozonation of cationic red X-GRL in aqueous solution: kinetics and modeling. Journal of Hazardous Materials, 2004, 57: 1189–1199

39
Matthews R W, Sangster D F. Measurement by benzoate radiolytic decarboxylation of relative rate constants for hydroxyl radical reactions. Journal of Physical Chemistry, 1965, 69(6): 1938–1946

40
Chen Y H, Chang C Y, Su W L, Chen C C, Chiu C Y, Yu Y H, Chiang P C, Chiang S I M. Modeling ozone contacting process in a rotating packed bed. Industrial & Engineering Chemistry Research, 2004, 43(1): 228–236

41
Hoigné J, Bader H. The role of hydroxyl radical reactions in ozonation processes in aqueous solutions. Water Research, 1976, 10(5): 377–386

Outlines

/