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

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.

Graphical abstract

Keywords

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

References

[1] GuoNLiY P. 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] Fierke M A, Olson E J, Buhlmann P, Stein A. Receptor-based detection of 2,4-dinitrotoluene using modified three-dimensionally ordered macroporous carbon electrodes. ACS Applied Materials & Interfaces, 2012, 4(9): 4731–4739

[3] Rodgers J D, Bunce N J. Treatment methods for the remediation of nitroaromatic explosives. Water Research, 2001, 35(9): 2101–2111

[4] Chen W S, Chiang W C, Wei K M. Recovery of nitrotoluenes from wastewater by solvent extraction enhanced with salting-out effect. Journal of Hazardous Materials, 2007, 147(1–2): 197–204

[5] Rajagopal C, Kapoor J C. Development of adsorptive removal process for treatment of explosives contaminated wastewater using activated carbon. Journal of Hazardous Materials, 2001, 87(1–3): 73–98

[6] Li F L, Chen C, Wang Y D, Li W P, Zhou G L, Zhang H Q, Zhang J, Wang J T. 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

[7] Abramov V O, Abramov O V, Gekhman A E, Kuznetsov V M, Price G J. Ultrasonic intensification of ozone and electrochemical destruction of 1,3-dinitrobenzene and 2,4-dinitrotoluene. Ultrasonics Sonochemistry, 2006, 13(4): 303–307

[8] Chen W S, Lin S Z. Destruction of nitrotoluenes in wastewater by electro-Fenton oxidation. Journal of Hazardous Materials, 2009, 168(2–3): 1562–1568

[9] Jiao W Z, Shao S J, Yang P Z, Gao K C, Liu Y Z. 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

[10] SongY JZhong S QLiY JDongKLuoY ChuG WZou H KSunB C. 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] Paca J, Halecky M, Barta J, Bajpai R. 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

[12] Christopher H J, Boardman G D, Freedman D L. Aerobic biological treatment of 2,4-dinitrotoluene in munitions plant wastewater. Water Research, 2000, 34(5): 1595–1603

[13] Parham H S, Saeed S. 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

[14] Arowo M, Zhao Z M, Li G J, Chu G W, Sun B C, Shao L. Ozonation of o-phenylenediamine in the presence of hydrogen peroxide by high-gravity technology. Chinese Journal of Chemical Engineering, 2018, 26(3): 601–607

[15] Chamarro E, Marco A, Esplugas S. Use of Fenton reagent to improve organic chemical biodegradability. Water Research, 2001, 35(4): 1047–1051

[16] El Shafei G M S, Yehia F Z, Dimitry O I 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(4): 1358–1365

[17] Bagal M V, Gogate P R. Wastewater treatment using hybrid treatment schemes based on cavitation and Fenton chemistry: a review. Ultrasonics Sonochemistry, 2014, 21(1): 1–14

[18] Agrawal A, Tratnyek P. Reduction of nitro aromatic compounds by zero-valent iron metal. Environmental Science & Technology, 1995, 30(1): 153–160

[19] Yang S, Liang Z, Yu H, Wang Y, Chen Y. 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

[20] Lai B, Zhou Y X, Yang P, Yang J H, Wang J L. Degradation of 3,3′-iminobis-propanenitrile in aqueous solution by Fe⁰/GAC micro-electrolysis system. Chemosphere, 2013, 90(4): 1470–1477

[21] Zhao H D, Nie T N, Zhao H X, Liu Y, Zhang J, Ye Q, Xu H, Shu S H. Enhancement of Fe–C micro-electrolysis in water by magnetic field: mechanism, influential factors and application effectiveness. Journal of Hazardous Materials, 2020, 410: 124643

[22] Liu H N, Li G T, Qu J H, Liu H J. 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

[23] Zhou H, Lv P, Shen Y, Wang J, Fan J. 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

[24] Hung H M, Hoffmann M R. 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

[25] Zhang W H, Wang D, Wang J X, Pu Y, Chen J F. 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

[26] 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

[27] Fang L, Sun Q, Duan Y H, Zhai J, Wang D, Wang J X. 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

[28] Lin C C, Liu W T. Ozone oxidation in a rotating packed bed. Journal of Chemical Technology and Biotechnology (Oxford, Oxfordshire), 2003, 78(2–3): 138–141

[29] Cheng H H, Tan C S. Removal of CO₂ from indoor air by alkanolamine in a rotating packed bed. Separation and Purification Technology, 2011, 82: 156–166

[30] Wei X Y, Shao S J, Ding X, Jiao W Z, Liu Y Z. Degradation of phenol with heterogeneous catalytic ozonation enhanced by high gravity technology. Journal of Cleaner Production, 2020, 248: 119179

[31] LiuW LJiao W ZLiuY ZGaoJSuQ LiJGuoL XuC C. 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] Meyer D, Prien R D, Dellwig O, Connelly D P, Schulz-Bull D E. 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

[33] Hung H M, Hoffmann M R. 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

[34] Li P Y, Wei X Y, Shao S J, Gao W Q, Jing J X, Jiao W Z, Liu Y Z. Degradation of nitrobenzene in wastewater by O₃/FeOOH in a rotating packed bed. Chemical Engineering and Processing, 2020, 153: 107981

[35] Shao S, Lei D, Song Y, Liang L, Liu Y, Jiao W. Cu–MnO_x/γ-Al₂O₃ catalyzed ozonation of nitrobenzene in a high-gravity rotating packed bed. Industrial & Engineering Chemistry Research, 2012, 60(5): 2123–2135

[36] Panda M, Bhowal A, Datta S. Removal of hexavalent chromium by biosorption process in rotating packed bed. Environmental Science & Technology, 2011, 45(19): 8460–8466

[37] Chen G, Zhu X, Chen R, Liao Q, Ye D D, Feng H, Liu J, Liu M. Gas–liquid–solid monolithic microreactor with Pd nanocatalyst coated on polydopamine modified nickel foam for nitrobenzene hydrogenation. Chemical Engineering Journal, 2018, 334: 1897–1904

[38] Jiao W Z, Feng Z R, Liu Y Z. Treatment of nitrobenzene-containing wastewater by iron–carbon micro-electrolysis. Journal of Nanoparticle Research, 2016, 66: 1150–1155

[39] Mu Y, Yu H Q, Zheng J C, Zhang S J, Sheng G P. Reductive degradation of nitrobenzene in aqueous solution by zero-valent iron. Chemosphere, 2004, 54(7): 789–794

[40] Lee H, Kim B H, Park Y K, Kim S J, Jung S C. Application of recycled zero-valent iron nanoparticle to the treatment of wastewater containing nitrobenzene. Journal of Nanomaterials, 2015, 16: 363–341

[41] Cai Z Q, Fu J, Du P H, Zhao X, Hao X D, Liu W, Zhao D Y. Reduction of nitrobenzene in aqueous and soil phases using carboxymethyl cellulose stabilized zero-valent iron nanoparticles. Chemical Engineering Journal, 2018, 332: 227–236

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