Novel coprecipitation–oxidation method for recovering iron from steel waste pickling liquor

Abstract

Coprecipitation–oxidation method was developed to recover the iron from wastewater.

Fe₃O₄ nanoparticles were well synthesized from steel waste pickling liquor.

Promoters greatly improved the properties of synthesized Fe₃O₄ nanoparticle.

Real-time control of the Fe²⁺/Fe³⁺ molar ratio was achieved by ORP monitoring.

Waste pickling liquors (WPLs) containing high concentrations of iron and acid are hazardous waste products from the steel pickling processes. A novel combined coprecipitation–oxidation method for iron recovery by Fe₃O₄ nanoparticle production from the WPLs was developed in this study. An oxidation–reduction potential monitoring method was developed for real-time control of the Fe²⁺/Fe³⁺ molar ratio. The key coprecipitation–oxidation parameters were determined using the orthogonal experimental design method. The use of promoters greatly improved the Fe₃O₄ nanoparticle crystallinity, size, magnetization, and dispersion. X-ray diffraction patterns showed that the produced Fe₃O₄ nanoparticles were single phase. The Fe₃O₄ nanoparticles were approximately spherical and slightly agglomerated. Vibrating sample magnetometry showed that the Fe₃O₄ nanoparticles produced from the WPLs had good magnetic properties, with a saturation magnetization of 80.206 emu·g⁻¹ and a remanence of 10.500 emu·g⁻¹. The results show that this novel coprecipitation–oxidation method has great potential for recycling iron in WPLs.

Graphical abstract

Keywords

Waste pickling liquor / Coprecipitation–oxidation / Fe₃O₄ nanoparticles / Oxidation–reduction potential / Promoter

References

[1] Konishi Y, Nomura T, Mizoe K. A new synthesis route from spent sulfuric acid pickling solution to ferrite nanoparticles. Hydrometallurgy, 2004, 74(1–2): 57–65

[2] Tang B, Yuan L, Shi T, Yu L, Zhu Y. Preparation of nano-sized magnetic particles from spent pickling liquors by ultrasonic-assisted chemical co-precipitation. Journal of Hazardous Materials, 2009, 163(2–3): 1173–1178

[3] Regel-Rosocka M. A review on methods of regeneration of spent pickling solutions from steel processing. Journal of Hazardous Materials, 2010, 177(1–3): 57–69

[4] Agrawal A, Sahu K K. An overview of the recovery of acid from spent acidic solutions from steel and electroplating industries. Journal of Hazardous Materials, 2009, 171(1–3): 61–75

[5] Loos R, Carvalho R, António D C, Comero S, Locoro G, Tavazzi S, Paracchini B, Ghiani M, Lettieri T, Blaha L, Jarosova B, Voorspoels S, Servaes K, Haglund P, Fick J, Lindberg R H, Schwesig D, Gawlik B M. EU-wide monitoring survey on emerging polar organic contaminants in wastewater treatment plant effluents. Water Research, 2013, 47(17): 6475–6487

[6] Guo H, Zhang T. Sinks of steel in China–addition to in-use stock, export and loss. Frontiers of Environmental Science & Engineering, 2016, 10(1): 141–149

[7] Tang B, Su W, Wang J, Fu F, Yu G, Zhang J. Minimizing the creation of spent pickling liquors in a pickling process with high-concentration hydrochloric acid solutions: mechanism and evaluation method. Journal of Environmental Management, 2012, 98: 147–154

[8] Devi A, Singhal A, Gupta R, Panzade P. A study on treatment methods of spent pickling liquor generated by pickling process of steel. Clean Technologies and Environmental Policy, 2014, 16(8): 1515–1527

[9] Narasimhan B R V, Kumar S, Sankara Narayanan T S. Synthesis of manganese zinc ferrite using ferrous pickle liquor and pyrolusite ore. Environmental Chemistry Letters, 2011, 9(2): 243–250

[10] Horák D, Babič M, Macková H, Beneš M J. Preparation and properties of magnetic nano- and microsized particles for biological and environmental separations. Journal of Separation Science, 2007, 30(11): 1751–1772

[11] Cai Y, Liang B, Fang Z, Xie Y, Tsang E P. Effect of humic acid and metal ions on the debromination of BDE209 by nZVM prepared from steel pickling waste liquor. Frontiers of Environmental Science & Engineering, 2015, 9(5): 879–887

[12] Gao J, Ran X, Shi C, Cheng H, Cheng T, Su Y. One-step solvothermal synthesis of highly water-soluble, negatively charged superparamagnetic Fe₃O₄ colloidal nanocrystal clusters. Nanoscale, 2013, 5(15): 7026–7033

[13] Ji L, Bai X, Zhou L, Shi H, Chen W, Hua Z. One-pot preparation of graphene oxide magnetic nanocomposites for the removal of tetrabromobisphenol A. Frontiers of Environmental Science & Engineering, 2013, 7(3): 442–450

[14] Mollahosseini A, Toghroli M, Kamankesh M. Zeolite/Fe₃O₄ as a new sorbent in magnetic solid-phase extraction followed by gas chromatography for determining phthalates in aqueous samples. Journal of Separation Science, 2015, 38(21): 3750–3757

[15] Klaine S J, Alvarez P J J, Batley G E, Fernandes T F, Handy R D, Lyon D Y, Mahendra S, McLaughlin M J, Lead J R. Nanomaterials in the environment: behavior, fate, bioavailability, and effects. Environmental Toxicology and Chemistry, 2008, 27(9): 1825–1851

[16] Horst M F, Lassalle V, Ferreira M L. Nanosized magnetite in low cost materials for remediation of water polluted with toxic metals, azo- and antraquinonic dyes. Frontiers of Environmental Science & Engineering, 2015, 9(5): 746–769

[17] Vayssières L, Chanéac C, Tronc E, Jolivet J P. Size tailoring of magnetite particles formed by aqueous precipitation: an example of thermodynamic stability of nanometric oxide particles. Journal of Colloid and Interface Science, 1998, 205(2): 205–212

[18] Deng J, He C, Peng Y, Wang J, Long X, Li P, Chan A. Magnetic and conductive Fe₃O₄-polyaniline nanoparticles with core-shell structure. Synthetic Metals, 2003, 139(2): 295–301

[19] Fan R, Chen X H, Gui Z, Liu L, Chen Z Y. A new simple hydrothermal preparation of nanocrystalline magnetite Fe₃O₄. Materials Research Bulletin, 2001, 36(3–4): 497–502

[20] Szczygieł I, Winiarska K, Bieńko A, Suracka K, Gaworska-Koniarek D. The effect of the sol–gel autocombustion synthesis conditions on the Mn–Zn ferrite magnetic properties. Journal of Alloys and Compounds, 2014, 604: 1–7

[21] Iwasaki T, Kosaka K, Yabuuchi T, Watano S, Yanagida T, Kawai T. Novel mechanochemical process for synthesis of magnetite nanoparticles using coprecipitation method. Advanced Powder Technology, 2009, 20(6): 521–528

[22] Murray C B, Kagan C R, Bawendi M G. Synthesis and characterization of monodisperse nanocrystals and close-packed nanocrystal assemblies. Annual Review of Materials Science, 2000, 30(1): 545–610

[23] Su L, Zhang J, Wang C, Zhang Y, Li Z, Song Y, Jin T, Ma Z. Identifying main factors of capacity fading in lithium ion cells using orthogonal design of experiments. Applied Energy, 2016, 163: 201–210

[24] Chen S, Wu B H, Fang J B, Liu Y L, Zhang H H, Fang L C, Guan L, Li S H. Analysis of flavonoids from lotus (Nelumbo nucifera) leaves using high performance liquid chromatography/photodiode array detector tandem electrospray ionization mass spectrometry and an extraction method optimized by orthogonal design. Journal of Chromatography. A, 2012, 1227: 145–153

[25] Cheng Y, Liao Z, Li R, Lu J, Wang K. Characterization of free radicals generated from the reaction of Fe³⁺/ Fe²⁺ with tert-butyl hydroperoxide and the effect of lanthanide ions. Applied Magnetic Resonance, 2000, 18(3): 407–417

[26] Gerber S, Gröger H, Ensling J, Gütlich P, Krautscheid H. (Pr₄N)₄[Ag₃Fe₂(ECN)₁₂]–anionic network structures with mutual interpenetration. Angewandte Chemie (International ed. in English), 2005, 44(47): 7787–7790

[27] Agnihotri S, Mukherji S, Mukherji S. Size-controlled silver nanoparticles synthesized over the range 5–100 nm using the same protocol and their antibacterial efficacy. RSC Advances, 2014, 4(8): 3974–3983

[28] Xing A, Zhang J, Bao Z, Mei Y, Gordin A S, Sandhage K H. A magnesiothermic reaction process for the scalable production of mesoporous silicon for rechargeable lithium batteries. Chemical communications (Cambridge, England), 2013, 49(60): 6743–6745

[29] Sun X, Zheng C, Zhang F, Yang Y, Wu G, Yu A, Guan N. Size-controlled synthesis of magnetite (Fe₃O₄) nanoparticles coated with glucose and gluconic acid from a single Fe(III) precursor by a sucrose bifunctional hydrothermal method. Journal of Physical Chemistry C, 2009, 113(36): 16002–16008

[30] Huang R, Fang Z, Fang X, Tsang E P. Ultrasonic Fenton-like catalytic degradation of bisphenol A by ferroferric oxide (Fe₃O₄) nanoparticles prepared from steel pickling waste liquor. Journal of Colloid and Interface Science, 2014, 436: 258–266

[31] Tang B, Yuan L, Shi T, Yu L, Zhu Y. Preparation of nano-sized magnetic particles from spent pickling liquors by ultrasonic-assisted chemical co-precipitation. Journal of Hazardous Materials, 2009, 163(2–3): 1173–1178

[32] Cumberland S A, Lead J R. Particle size distributions of silver nanoparticles at environmentally relevant conditions. Journal of Chromatography. A, 2009, 1216(52): 9099–9105

[33] Tejamaya M, Römer I, Merrifield R C, Lead J R. Stability of citrate, PVP, and PEG coated silver nanoparticles in ecotoxicology media. Environmental Science & Technology, 2012, 46(13): 7011–7017

[34] Chen D, Mei C Y, Yao L H, Jin H M, Qian G R, Xu Z P. Flash fixation of heavy metals from two industrial wastes into ferrite by microwave hydrothermal co-treatment. Journal of Hazardous Materials, 2011, 192(3): 1675–1682

[35] Mo Z, Zhang C, Guo R, Meng S, Zhang J. Synthesis of Fe₃O₄ nanoparticles using controlled ammonia vapor diffusion under ultrasonic irradiation. Industrial & Engineering Chemistry Research, 2011, 50(6): 3534–3539

Acknowledgments

This work is supported by the Tianjin Research Program of Application Foundation and Advanced Technology, Tianjin City, China (Key Project, No.15JCZDJC40400).The authors declare no financial/commercial conflicts of interest.

Electronic Supplementary Materialƒ

Supplementary material is available in the online version of this article at http://dx.doi.org/10.1007/s11783-017-0902-1 and is accessible for authorized users.

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2017 Higher Education Press and Springer-Verlag Berlin Heidelberg