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Engineering >> 2019, Volume 5, Issue 5 doi: 10.1016/j.eng.2019.06.001

Green Synthesis of Magnetic Adsorbent Using Groundwater Treatment Sludge for Tetracycline Adsorption

a Science and Technology Innovation Center for Municipal Wastewater Treatment and Water Quality Protection, Northeast Normal University, Changchun 130117, China

b School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China

c Engineering Lab for Water Pollution Control and Resources Recovery, Northeast Normal University, Changchun 130117, China

d Guangdong Shouhui Lantian Engineering and Technology Corporation, Guangzhou 510075, China

Received: 2018-11-05 Revised: 2019-01-27 Accepted: 2019-03-07 Available online: 2019-06-22

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Abstract

Groundwater treatment sludge is an industrial waste that is massively produced from groundwater treatment plants. Conventional methods for treatment of this sludge, such as discharge into deep wells or the sea, or disposal at landfills, are not environmentally sustainable. Here, we demonstrate an alternative strategy to recycle the sludge by preparing a magnetic maghemite adsorbent via a one-step hydrothermal method with NaOH solution as the only solvent. With this method, the weakly magnetized sludge, which contained 33.2% iron (Fe) and other impurities (e.g., silicon (Si), aluminum (Al), and manganese (Mn)), was converted to magnetic adsorbent (MA) with the dissolution of Si/Al oxides (e.g., quartz and albite) into the liquid fraction. At a NaOH concentration of 2 mol·L1, approximately 18.1% of the ferrihydrite in the Fe oxides of the sludge was converted into 11.2% maghemite and 6.9% hematite after the hydrothermal treatment. MA2 (MA produced by a 2 mol·L1 NaOH concentration) exhibited a good magnetic response of 8.2 emu·g1 (1 emu = 103 A·m2), and a desirable surface site concentration of 0.75 mmol·g1. The synthesized MA2 was used to adsorb the cationic pollutant tetracycline (TC). The adsorption kinetics of TC onto MA2 fitted well with a pseudo-second-order model, and the adsorption isotherms complied well with the Langmuir model. The maximum adsorption capacity of MA2 for TC was 362.3 mg·g1, and the main mechanism for TC adsorption was cationic exchange. This study is the first to demonstrate the preparation of an MA from recycled sludge without a reductant and/or exogenous Fe source. The prepared adsorbent can be used as a low-cost adsorbent with high capacity for TC sorption in the treatment of TC-containing wastewater.

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References

[ 1 ] Dotremont C, Molenberghs B, Doyen W, Bielen P, Huysman K. The recovery of backwash water from sand filters by ultrafiltration. Desalination 1999;126 (1):87–94. link1

[ 2 ] Osman SBS, Iqbal F. Possible stabilization of sludge from groundwater treatment plant using electrokinetic method. Appl Mech Mater 2014;567 (419):110–5. link1

[ 3 ] Zhu S, Fang S, Huo M, Yu Y, Chen Y, Yang X, et al. A novel conversion of the groundwater treatment sludge to magnetic particles for the adsorption of methylene blue. J Hazard Mater 2015;292(113):173–9. link1

[ 4 ] Gibbons MK, Gagnon GA. Adsorption of arsenic from a Nova Scotia groundwater onto water treatment residual solids. Water Res 2010;44 (19):5740–9. link1

[ 5 ] Zhu S, Dong G, Yu Y, Yang J, Yang W, Fan W, et al. Hydrothermal synthesis of a magnetic adsorbent from wasted iron mud for effective removal of heavy metals from smelting wastewater. Environ Sci Pollut Res Int 2018;25 (23):22710–24. link1

[ 6 ] Liu J, Yu Y, Zhu S, Yang J, Song J, Fan W, et al. Synthesis and characterization of a magnetic adsorbent from negatively-valued iron mud for methylene blue adsorption. PLoS One 2018;13(2):e0191229. link1

[ 7 ] Ong DC, Pingul-Ong SMB, Kan CC, de Luna MDG. Removal of nickel ions from aqueous solutions by manganese dioxide derived from groundwater treatment sludge. J Clean Prod 2018;190:443–51. link1

[ 8 ] Ngatenah SNI, Kutty SRM, Isa MH. Optimization of heavy metal removal from aqueous solution using groundwater treatment plant sludge (GWTPS). In: Proceedings of the International Conference on Environment; 2010 Dec 13–15; Penang, Malaysia; 2010. p. 1–9.

[ 9 ] Yang H, Jing L, Zhang B. Recovery of iron from vanadium tailings with coalbased direct reduction followed by magnetic separation. J Hazard Mater 2011;185(2–3):1405–11. link1

[10] Costa RC, Moura FC, Oliveira PE, Magalhães F, Ardisson JD, Lago RM. Controlled reduction of red mud waste to produce active systems for environmental applications: heterogeneous Fenton reaction and reduction of Cr(VI). Chemosphere 2010;78(9):1116–20. link1

[11] Sushil S, Alabdulrahman AM, Balakrishnan M, Batra VS, Blackley RA, Clapp J, et al. Carbon deposition and phase transformations in red mud on exposure to methane. J Hazard Mater 2010;180(1–3):409–18. link1

[12] Mohammed MA, Shitu A, Ibrahim A. Removal of methylene blue using low cost adsorbent: a review. Res J Chem Sci 2014;4(1):91–102. link1

[13] Arabi M, Ghaedi M, Ostovan A. Water compatible molecularly imprinted nanoparticles as a restricted access material for extraction of hippuric acid, a biological indicator of toluene exposure, from human urine. Microchim Acta 2017;184(3):879–87. link1

[14] Rajendran S, Khan MM, Gracia F, Qin J, Gupta VK, Arumainathan S. Ce3+-ioninduced visible-light photocatalytic degradation and electrochemical activity of ZnO/CeO2 nanocomposite. Sci Rep 2016;6(1):31641. link1

[15] Saravanan R, Karthikeyan S, Gupta VK, Sekaran G, Narayanan V, Stephen A. Enhanced photocatalytic activity of ZnO/CuO nanocomposite for the degradation of textile dye on visible light illumination. Mater Sci Eng C 2013;33(1):91–8. link1

[16] Ghaedi M, Hajjati S, Mahmudi Z, Tyagi I, Agarwal S, Maity A, et al. Modeling of competitive ultrasonic assisted removal of the dyes—methylene blue and safranin-O using Fe3O4 nanoparticles. Chem Eng J 2015;268:28–37. link1

[17] Ostovan A, Ghaedi M, Arabi M. Fabrication of water-compatible superparamagnetic molecularly imprinted biopolymer for clean separation of baclofen from bio-fluid samples: a mild and green approach. Talanta 2018;179:760–8. link1

[18] Arabi M, Ghaedi M, Ostovan A. Development of a lower toxic approach based on green synthesis of water-compatible molecularly imprinted nanoparticles for the extraction of hydrochlorothiazide from human urine. ACS Sustain Chem Eng 2017;5(5):3775–85. link1

[19] Ostovan A, Ghaedi M, Arabi M, Yang Q, Li J, Chen L. Hydrophilic multitemplate molecularly imprinted biopolymers based on a green synthesis strategy for determination of B-family vitamins. ACS Appl Mater Interfaces 2018;10 (4):4140–50. link1

[20] Gupta VK, Atar N, Yola ML, Üstündag˘ Z, Uzun L. A novel magnetic Fe@Au core–shell nanoparticles anchored graphene oxide recyclable nanocatalyst for the reduction of nitrophenol compounds. Water Res 2014;48:210–7. link1

[21] Sandroni V, Smith CMM. Microwave digestion of sludge, soil and sediment samples for metal analysis by inductively coupled plasma–atomic emission spectrometry. Anal Chim Acta 2002;468(2):335–44. link1

[22] Duquette M, Hendershot W. Soil surface charge evaluation by back-titration: I. Theory and method development. Soil Sci Soc Am J 1993;57(5):1222–8. link1

[23] Barrón V, Torrent J, de Grave E. Hydromaghemite, an intermediate in the hydrothermal transformation of 2-line ferrihydrite into hematite. Am Mineral 2003;88(11–12):1679–88. link1

[24] Cornell RM. Effect of silicate species on the transformation of ferrihydrite into goethite and hematite in alkaline media. Clays Clay Miner 1987;35(1):21–8. link1

[25] Liu Q, Barrón V, Torrent J, Eeckhout SG, Deng C. Magnetism of intermediate hydromaghemite in the transformation of 2-line ferrihydrite into hematite and its paleoenvironmental implications. J Geophys Res 2008;113(B1): B01103. link1

[26] Sidhu PS. Transformation of trace element-substituted maghemite to hematite. Clays Clay Miner 1988;36(1):31–8. link1

[27] Zhao J, Huggins FE, Feng Z, Lu FL, Shah N, Huffman GP. Structure of a nanophase iron oxide catalyst. J Catal 1993;143(2):499–509. link1

[28] Jianmin Z. Ferrihydrite: surface structure and its effects on phase transformation. Clays Clay Miner 1994;42(6):737–46. link1

[29] Brinza L, Vu HP, Shaw S, Mosselmans JFW, Benning LG. Effect of Mo and V on the hydrothermal crystallization of hematite from ferrihydrite: an in situ energy dispersive X-ray diffraction and X-ray absorption spectroscopy study. Cryst Growth Des 2015;15(10):4768–80. link1

[30] Ostovan A, Ghaedi M, Arabi M, Asfaram A. Hollow porous molecularly imprinted polymer for highly selective clean-up followed by influential preconcentration of ultra-trace glibenclamide from bio-fluid. J Chromatogr A 2017;1520:65–74. link1

[31] Arabi M, Ghaedi M, Ostovan A. Development of dummy molecularly imprinted based on functionalized silica nanoparticles for determination of acrylamide in processed food by matrix solid phase dispersion. Food Chem 2016;210:78–84. link1

[32] Arabi M, Ghaedi M, Ostovan A. Synthesis and application of in-situ molecularly imprinted silica monolithic in pipette-tip solid-phase microextraction for the separation and determination of gallic acid in orange juice samples. J Chromatogr B Analyt Technol Biomed Life Sci 2017;1048:102–10. link1

[33] Militello MC, Gaarenstroom SW. Manganese dioxide (MnO2) by XPS. Surf Sci Spectra 2001;8(3):200–6. link1

[34] Saravanan R, Gupta VK, Narayanan V, Stephen A. Visible light degradation of textile effluent using novel catalyst ZnO/c-Mn2O3. J Taiwan Inst Chem E 2014;45(4):1910–7. link1

[35] Saravanan R, Khan MM, Gupta VK, Mosquera E, Gracia F, Narayanan V, et al. ZnO/Ag/Mn2O3 nanocomposite for visible light-induced industrial textile effluent degradation, uric acid and ascorbic acid sensing and antimicrobial activity. RSC Adv 2015;5(44):34645–51. link1

[36] Lan S, Wang X, Xiang Q, Yin H, Tan W, Qiu G, et al. Mechanisms of Mn(II) catalytic oxidation on ferrihydrite surfaces and the formation of manganese (oxyhydr)oxides. Geochim Cosmochim Acta 2017;211:79–96. link1

[37] Sajih M, Bryan ND, Livens FR, Vaughan DJ, Descostes M, Phrommavanh V, et al. Adsorption of radium and barium on goethite and ferrihydrite: a kinetic and surface complexation modelling study. Geochim Cosmochim Acta 2014;146:150–63. link1

[38] Kulshrestha P, Giese Jr RF, Aga DS. Investigating the molecular interactions of oxytetracycline in clay and organic matter: insights on factors affecting its mobility in soil. Environ Sci Technol 2004;38(15):4097–105. link1

[39] Saravanan R, Sacari E, Gracia F, Khan MM, Mosquera E, Gupta VK. Conducting PANI stimulated ZnO system for visible light photocatalytic degradation of coloured dyes. J Mol Liq 2016;221:1029–33. link1

[40] Ho YS, McKay G. Pseudo-second order model for sorption processes. Process Biochem 1999;34(5):451–65. link1

[41] Gupta VK, Saleh TA. Sorption of pollutants by porous carbon, carbon nanotubes and fullerene—an overview. Environ Sci Pollut Res Int 2013;20(5):2828–43. link1

[42] Gupta VK, Nayak A, Agarwal S, Tyagi I. Potential of activated carbon from waste rubber tire for the adsorption of phenolics: effect of pre-treatment conditions. J Colloid Interface Sci 2014;417:420–30. link1

[43] Mittal A, Mittal J, Malviya A, Gupta VK. Removal and recovery of chrysoidine Y from aqueous solutions by waste materials. J Colloid Interface Sci 2010;344 (2):497–507. link1

[44] Saleh TA, Gupta VK. Photo-catalyzed degradation of hazardous dye methyl orange by use of a composite catalyst consisting of multi-walled carbon nanotubes and titanium dioxide. J Colloid Interface Sci 2012;371(1):101–6. link1

[45] Yu B, Bai Y, Ming Z, Yang H, Chen L, Hu X, et al. Adsorption behaviors of tetracycline on magnetic graphene oxide sponge. Mater Chem Phys 2017;198:283–90. link1

[46] Liu Q, Zheng Y, Zhong L, Cheng X. Removal of tetracycline from aqueous solution by a Fe3O4 incorporated PAN electrospun nanofiber mat. J Environ Sci 2015;28:29–36. link1

[47] Zhou Q, Li Z, Shuang C, Li A, Zhang M, Wang M. Efficient removal of tetracycline by reusable magnetic microspheres with a high surface area. Chem Eng J 2012;210:350–6. link1

[48] Guan W, Wang X, Pan J, Lei J, Zhou Y, Lu C, et al. Synthesis of magnetic halloysite composites for the effective removal of tetracycline hydrochloride from aqueous solutions. Adsorpt Sci Technol 2012;30(7):579–91. link1

[49] Zhang M, Li A, Zhou Q, Shuang C, Zhou W, Wang M. Effect of pore size distribution on tetracycline adsorption using magnetic hypercrosslinked resins. Micropor Mesopor Mat 2014;184:105–11. link1

[50] Li B,Ma J, Zhou L, Qiu Y.Magneticmicrosphere to remove tetracycline from water: adsorption, H2O2 oxidation and regeneration. Chem Eng J 2017;330:191–201. link1

[51] Zhang B, Zhang H, Li X, Lei X, Li C, Yin D, et al. Synthesis of BSA/Fe3O4 magnetic composite microspheres for adsorption of antibiotics. Mater Sci Eng C 2013;33 (7):4401–8. link1

[52] Raeiatbina P, Açıkelb YS. Removal of tetracycline by magnetic chitosan nanoparticles from medical wastewaters. Desalination 2017;73:380–8. link1

[53] Yan X, Gan K, Tian B, Zhang J, Wang L, Lu D. Photo-fenton refreshable Fe3O4@HCS adsorbent for the elimination of tetracycline hydrochloride. Res Chem Intermed 2018;44(1):1–11. link1

[54] Khani H, Rofouei MK, Arab P, Gupta VK, Vafaei Z. Multi-walled carbon nanotubes-ionic liquid-carbon paste electrode as a super selectivity sensor: application to potentiometric monitoring of mercury ion(II). J Hazard Mater 2010;183(1–3):402–9. link1

[55] Gupta VK, Nayak A, Agarwal S. Bioadsorbents for remediation of heavy metals: current status and their future prospects. Environ Eng Res 2015;20(1):1–18. link1

[56] Gupta VK, Jain R, Nayak A, Agarwal S, Shrivastava M. Removal of the hazardous dye—tartrazine by photodegradation on titanium dioxide surface. Mat Sci Eng C Mater 2011;31(5):1062–7. link1

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