High-gravity intensified iron-carbon micro-electrolysis for degradation of dinitrotoluene

doi:10.1007/s11705-022-2204-9

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (11) : 1595-1605 https://doi.org/10.1007/s11705-022-2204-9

RESEARCH ARTICLE

High-gravity intensified iron-carbon micro-electrolysis for degradation of dinitrotoluene

Jiaxin Jing, Weizhou Jiao(

), Zhixing Li, Kechang Gao, Jingwen Zhang, Gaomiao Ren, Youzhi Liu

Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering, North University of China, Taiyuan 030051, China

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Abstract

The application of iron–carbon (Fe–C) micro-electrolysis to wastewater treatment is limited by the passivation potential of the Fe–C packing. In order to address this problem, high-gravity intensified Fe–C micro-electrolysis was proposed in this study for degradation of dinitrotoluene wastewater in a rotating packed bed (RPB) using commercial Fe–C particles as the packing. The effects of reaction time, high-gravity factor, liquid flow rate and initial solution pH were investigated. The degradation intermediates were determined by gas chromatography-mass spectrometry, and the possible degradation pathways of nitro compounds by Fe–C micro-electrolysis in RPB were also proposed. It is found that under optimal conditions, the removal rate of nitro compounds reaches 68.4% at 100 min. The removal rate is maintained at approximately 68% after 4 cycles in RPB, but it is decreased substantially from 57.9% to 36.8% in a stirred tank reactor. This is because RPB can increase the specific surface area and the renewal of the liquid–solid interface, and as a result the degradation efficiency of Fe–C micro-electrolysis is improved and the active sites on the Fe–C surface can be regenerated for continuous use. In conclusion, high-gravity intensified Fe–C micro-electrolysis can weaken the passivation of Fe–C particles and extend their service life.

Keywords high-gravity technology rotating packed bed Fe–C micro-electrolysis dinitrotoluene wastewater active sites

Corresponding Author(s): Weizhou Jiao

Online First Date: 01 November 2022 Issue Date: 13 December 2022

Cite this article:

Jiaxin Jing,Weizhou Jiao,Zhixing Li, et al. High-gravity intensified iron-carbon micro-electrolysis for degradation of dinitrotoluene[J]. Front. Chem. Sci. Eng., 2022, 16(11): 1595-1605.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2204-9
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I11/1595

Fig.1 Schematic view of high-gravity intensified Fe–C micro-electrolysis: 1) reservoir; 2) centrifugal pump; 3) valve; 4) flow meter; 5) RPB; 6) frequency conversion motor.

Tab.1 Characteristic parameters of RPB

Fig.2 Variations of (a) pH and (b) removal rate of nitro compounds and total iron concentration in the wastewater with reaction time (pH = 1.1, Q = 80 L?h^?1, β = 104).

Fig.3 Effects of operating parameters on the removal rate of nitro compounds and the total iron concentration in the solution: (a, b) high-gravity factor (Q = 80 L?h^?1, pH = 1.1), (c, d) liquid flow rate (β = 46.22, pH = 1.1), and (e, f) initial solution pH (β = 46.22, Q = 80 L?h^?1).

Fig.4 Comparison between RPB and STR in single and cycling experiments (pH = 1.1, t = 100 min; for RPB: β = 46.22, Q = 80 L?h^?1; for STR: r = 200 r?min^?1).

Fig.5 SEM images and EDX spectra of Fe–C packing: (a) fresh Fe–C packing; Fe–C packing used for four cycles in (b) STR and (c) RPB.

Tab.2 Compositions of dinitrotoluene wastewater

Fig.6 Gas chromatogram of dinitrotoluene wastewater.

Fig.7 High-gravity intensified Fe–C micro-electrolysis for degradation of nitrobenzene by ultraviolet–visible spectroscopy (pH = 1.1, t = 100 min, β = 46.22, Q = 80 L?h^?1).

Tab.3 Intermediates by GC–MS

Fig.8 GC–MS analysis of high-gravity intensified Fe–C micro-electrolysis for degradation of nitrobenzene.

Fig.9 Degradation mechanism of nitrobenzene by Fe–C micro-electrolysis.

Fig.10 Changes in the concentration of nitrobenzene and aniline (pH = 1.1, t = 60 min, β = 46.22, Q = 80 L?h^–1).

1	N GuoY P Li. Reaction mechanism and influence factors of treating dinitrotoluene wastewater by wet air oxidation. Chinese Journal of Explosives and Propellants, 2010, 33(3): 25‒29 (In Chinese)
2	M A Fierke, E J Olson, P Buhlmann, A Stein. Receptor-based detection of 2,4-dinitrotoluene using modified three-dimensionally ordered macroporous carbon electrodes. ACS Applied Materials & Interfaces, 2012, 4(9): 4731–4739 https://doi.org/10.1021/am301108a
3	J D Rodgers, N J Bunce. Treatment methods for the remediation of nitroaromatic explosives. Water Research, 2001, 35(9): 2101–2111 https://doi.org/10.1016/S0043-1354(00)00505-4
4	W S Chen, W C Chiang, K M Wei. Recovery of nitrotoluenes from wastewater by solvent extraction enhanced with salting-out effect. Journal of Hazardous Materials, 2007, 147(1–2): 197–204 https://doi.org/10.1016/j.jhazmat.2006.12.066
5	C Rajagopal, J C Kapoor. Development of adsorptive removal process for treatment of explosives contaminated wastewater using activated carbon. Journal of Hazardous Materials, 2001, 87(1–3): 73–98 https://doi.org/10.1016/S0304-3894(01)00179-0
6	F L Li, C Chen, Y D Wang, W P Li, G L Zhou, H Q Zhang, J Zhang, J T Wang. Activated carbon-hybridized and amine-modified polyacrylonitrile nanofibers toward ultrahigh and recyclable metal ion and dye adsorption from wastewater. Frontiers of Chemical Science and Engineering, 2021, 15(4): 984–997 https://doi.org/10.1007/s11705-020-2000-3
7	V O Abramov, O V Abramov, A E Gekhman, V M Kuznetsov, G J Price. Ultrasonic intensification of ozone and electrochemical destruction of 1,3-dinitrobenzene and 2,4-dinitrotoluene. Ultrasonics Sonochemistry, 2006, 13(4): 303–307 https://doi.org/10.1016/j.ultsonch.2005.04.007
8	W S Chen, S Z Lin. Destruction of nitrotoluenes in wastewater by electro-Fenton oxidation. Journal of Hazardous Materials, 2009, 168(2–3): 1562–1568 https://doi.org/10.1016/j.jhazmat.2009.03.048
9	W Z Jiao, S J Shao, P Z Yang, K C Gao, Y Z Liu. Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced by high gravity technology. Frontiers of Chemical Science and Engineering, 2021, 15(5): 1197–1205 https://doi.org/10.1007/s11705-020-1998-6
10	Y J SongS Q ZhongY J LiK DongY Luo G W ChuH K ZouB C Sun. Study on the catalytic degradation of sodium lignosulfonate to aromatic aldehydes over nano-CuO: process optimization and reaction kinetics. Chinese Journal of Chemical Engineering, 2022, in press
11	J Paca, M Halecky, J Barta, R Bajpai. Aerobic biodegradation of 2,4-dinitrotoluene and 2,6-dinitrotoluene: performance characteristics and biofilm composition changes in continuous packed-bed bioreactors. Journal of Hazardous Materials, 2009, 163(2–3): 848–854 https://doi.org/10.1016/j.jhazmat.2008.07.037
12	H J Christopher, G D Boardman, D L Freedman. Aerobic biological treatment of 2,4-dinitrotoluene in munitions plant wastewater. Water Research, 2000, 34(5): 1595–1603 https://doi.org/10.1016/S0043-1354(99)00308-5
13	H S Parham, S Saeed. Simultaneous removal of nitrobenzene, 1,3-dinitrobenzene and 2,4-dichloronitrobenzene from water samples using anthracite as a potential adsorbent. Journal of Environmental Chemical Engineering, 2013, 1(4): 1117–1123 https://doi.org/10.1016/j.jece.2013.08.028
14	M Arowo, Z M Zhao, G J Li, G W Chu, B C Sun, L Shao. Ozonation of o-phenylenediamine in the presence of hydrogen peroxide by high-gravity technology. Chinese Journal of Chemical Engineering, 2018, 26(3): 601–607 https://doi.org/10.1016/j.cjche.2017.05.021
15	E Chamarro, A Marco, S Esplugas. Use of Fenton reagent to improve organic chemical biodegradability. Water Research, 2001, 35(4): 1047–1051 https://doi.org/10.1016/S0043-1354(00)00342-0
16	G M S El Shafei, F Z Yehia, O I H Dimitry, A M Badawi, G Eshaq. Ultrasonic assisted-Fenton-like degradation of nitrobenzene at neutral pH using nanosized oxides of Fe and Cu. Ultrasonics Sonochemistry, 2014, 21(4): 1358–1365 https://doi.org/10.1016/j.ultsonch.2013.12.019
17	M V Bagal, P R Gogate. Wastewater treatment using hybrid treatment schemes based on cavitation and Fenton chemistry: a review. Ultrasonics Sonochemistry, 2014, 21(1): 1–14 https://doi.org/10.1016/j.ultsonch.2013.07.009
18	A Agrawal, P Tratnyek. Reduction of nitro aromatic compounds by zero-valent iron metal. Environmental Science & Technology, 1995, 30(1): 153–160 https://doi.org/10.1021/es950211h
19	S Yang, Z Liang, H Yu, Y Wang, Y Chen. Chemical oxygen demand removal efficiency and limited factors study of aminosilicone polymers in a water emulsion by iron-carbon micro-electrolysis. Water Environment Research, 2014, 86(2): 156–162 https://doi.org/10.2175/106143013X13596524516509
20	B Lai, Y X Zhou, P Yang, J H Yang, J L Wang. Degradation of 3,3′-iminobis-propanenitrile in aqueous solution by Fe0/GAC micro-electrolysis system. Chemosphere, 2013, 90(4): 1470–1477 https://doi.org/10.1016/j.chemosphere.2012.09.040
21	H D Zhao, T N Nie, H X Zhao, Y Liu, J Zhang, Q Ye, H Xu, S H Shu. Enhancement of Fe–C micro-electrolysis in water by magnetic field: mechanism, influential factors and application effectiveness. Journal of Hazardous Materials, 2020, 410: 124643 https://doi.org/10.1016/j.jhazmat.2020.124643
22	H N Liu, G T Li, J H Qu, H J Liu. Degradation of azo dye acid orange 7 in water by Fe0/granular activated carbon system in the presence of ultrasound. Journal of Hazardous Materials, 2007, 144(1‒2): 180–186 https://doi.org/10.1016/j.jhazmat.2006.10.009
23	H Zhou, P Lv, Y Shen, J Wang, J Fan. Identification of degradation products of ionic liquids in an ultrasound assisted zero-valent iron activated carbon micro-electrolysis system and their degradation mechanism. Water Research, 2013, 47(10): 3514–3522 https://doi.org/10.1016/j.watres.2013.03.057
24	H M Hung, M R Hoffmann. Kinetics and mechanism of the enhanced reductive degradation of CCl4 by elemental iron in the presence of ultrasound. Environmental Science & Technology, 1998, 32(19): 3011–3016 https://doi.org/10.1021/es980273i
25	W H Zhang, D Wang, J X Wang, Y Pu, J F Chen. High-gravity-assisted emulsification for continuous preparation of waterborne polyurethane nanodispersion with high solids content. Frontiers of Chemical Science and Engineering, 2020, 14(6): 1087–1099 https://doi.org/10.1007/s11705-019-1895-z
26	W Z Jiao, S Luo, Z He, Y Z Liu. Applications of high gravity technologies for wastewater treatment: a review. Chemical Engineering Journal, 2017, 313: 912–927 https://doi.org/10.1016/j.cej.2016.10.125
27	L Fang, Q Sun, Y H Duan, J Zhai, D Wang, J X Wang. Preparation of transparent BaSO4 nanodispersions by high-gravity reactive precipitation combined with surface modification for transparent X-ray shielding nanocomposite films. Frontiers of Chemical Science and Engineering, 2021, 15(4): 902–912 https://doi.org/10.1007/s11705-020-1985-y
28	C C Lin, W T Liu. Ozone oxidation in a rotating packed bed. Journal of Chemical Technology and Biotechnology (Oxford, Oxfordshire), 2003, 78(2–3): 138–141 https://doi.org/10.1002/jctb.708
29	H H Cheng, C S Tan. Removal of CO2 from indoor air by alkanolamine in a rotating packed bed. Separation and Purification Technology, 2011, 82: 156–166 https://doi.org/10.1016/j.seppur.2011.09.004
30	X Y Wei, S J Shao, X Ding, W Z Jiao, Y Z Liu. Degradation of phenol with heterogeneous catalytic ozonation enhanced by high gravity technology. Journal of Cleaner Production, 2020, 248: 119179 https://doi.org/10.1016/j.jclepro.2019.119179
31	W L LiuW Z JiaoY Z LiuJ GaoQ Su J LiL Guo C C Xu. Treatment of dinitrotoluene production wastewater by iron-carbon micro-electrolysis method. Chinese Journal of Explosives and Propellants, 2014, 37(3): 33–38 (In Chinese)
32	D Meyer, R D Prien, O Dellwig, D P Connelly, D E Schulz-Bull. In situ determination of iron (II) in the anoxic zone of the central Baltic Sea using ferene as spectrophotometric reagent. Marine Chemistry, 2012, 130: 21–27 https://doi.org/10.1016/j.marchem.2011.12.002
33	H M Hung, M R Hoffmann. Kinetics and mechanism of the enhanced reductive degradation of nitrobenzene by elemental iron in the presence of ultrasound. Environmental Science & Technology, 2000, 32(19): 3011–3016 https://doi.org/10.1021/es980273i
34	P Y Li, X Y Wei, S J Shao, W Q Gao, J X Jing, W Z Jiao, Y Z Liu. Degradation of nitrobenzene in wastewater by O3/FeOOH in a rotating packed bed. Chemical Engineering and Processing, 2020, 153: 107981 https://doi.org/10.1016/j.cep.2020.107981
35	S Shao, D Lei, Y Song, L Liang, Y Liu, W Jiao. Cu–MnOx/γ-Al2O3 catalyzed ozonation of nitrobenzene in a high-gravity rotating packed bed. Industrial & Engineering Chemistry Research, 2012, 60(5): 2123–2135 https://doi.org/10.1021/acs.iecr.0c05751
36	M Panda, A Bhowal, S Datta. Removal of hexavalent chromium by biosorption process in rotating packed bed. Environmental Science & Technology, 2011, 45(19): 8460–8466 https://doi.org/10.1021/es2015346
37	G Chen, X Zhu, R Chen, Q Liao, D D Ye, H Feng, J Liu, M Liu. Gas–liquid–solid monolithic microreactor with Pd nanocatalyst coated on polydopamine modified nickel foam for nitrobenzene hydrogenation. Chemical Engineering Journal, 2018, 334: 1897–1904 https://doi.org/10.1016/j.cej.2017.11.126
38	W Z Jiao, Z R Feng, Y Z Liu. Treatment of nitrobenzene-containing wastewater by iron–carbon micro-electrolysis. Journal of Nanoparticle Research, 2016, 66: 1150–1155
39	Y Mu, H Q Yu, J C Zheng, S J Zhang, G P Sheng. Reductive degradation of nitrobenzene in aqueous solution by zero-valent iron. Chemosphere, 2004, 54(7): 789–794 https://doi.org/10.1016/j.chemosphere.2003.10.023
40	H Lee, B H Kim, Y K Park, S J Kim, S C Jung. Application of recycled zero-valent iron nanoparticle to the treatment of wastewater containing nitrobenzene. Journal of Nanomaterials, 2015, 16: 363–341 https://doi.org/10.1155/2015/392537
41	Z Q Cai, J Fu, P H Du, X Zhao, X D Hao, W Liu, D Y Zhao. Reduction of nitrobenzene in aqueous and soil phases using carboxymethyl cellulose stabilized zero-valent iron nanoparticles. Chemical Engineering Journal, 2018, 332: 227–236 https://doi.org/10.1016/j.cej.2017.09.066

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