Synthesis and characterization of layered double hydroxide nanostructures and their application in the removal of Fe>sup>2+ and Ca2+ ions from oil wells
Four new metal-aluminum layered double hydroxides (LDHs): Mg-Al(OH)2PO4 1, Mg-Al(OH)2PO4PF6 2, Ca-Al(OH)2SO4, 3 and Ca-Al(OH)2PO4PF6 4, were prepared by co-precipitation method followed by mild hydrothermal processing at 60 o C. Mg2+ and Ca2+ in solution with Al3+ was titrated with NaOH over 3-5 h to yield Mg-Al and Ca-Al layered double hydroxides, respectively, incorporating PO43-, PO43-PF6- and SO42- anions in the inter-lamellar spaces. The isolated compounds were characterized with the help of XRD, IR, SEM/EDAX and their ability to remove scale forming ions from aqueous system was studied with the help of Atomic Absorption Spectroscopy (AAS). The SEM micrographs of Mg-O-Al-OH and Ca-O-Al-OH layers intercalated with PO43- and / or [PO4PF6 ]4- anions are similar consisting of uniform nano- spheres with average size of 100 nm, while the M-O-Al-OH layer of compound 3, intercalated with SO42- anions consists of hexagonal nano-plate crystals. In the infrared spectra, the characteristic absorption band for water molecules was observed in all the compounds. The XRD pattern showed that d012 and d104 peaks of M-Al-PO4 LDHs corresponding to interplanar spacing of 3.4804 and 2.5504 Å respectively, shifted to higher 2θ values for M-Al-PO4PF6 system, which indicates a decrease in the interlamellar spacing as PF6 - was incorporated along with PO43- anion. The XRD pattern for Ca-Al-SO4 LDHs was quite different, showing the presence of low angle peaks at 2θ = 11.68 and 14.72o. The results of the column adsorption studies showed that there was a significant removal of Ca2+ by all the compounds under investigation with efficiency of 84 -99 %. Whereas compounds 1 and 2 removes Fe2+ effectively with efficiency of 98.73 and 99.77 %, respectively, compounds 3 and 4 were shown to have little or no effect.
Keywords: Layered double hydroxides, nanospheres, nanoplates, adsorption, nanostructures
Ephraim E. Khansi, Chinyere A. Anyama, Ayi A. Ayi, Jude C. Onwuka. Synthesis and characterization of layered double hydroxide nanostructures and their application in the removal of Fe>sup>2+ and Ca2+ ions from oil wells. Acta Scientiae et Intellectus, 2(5)2016, 34-45.
- D. Shen, P. Zhang, A.T. Kan, G. Fu, J. Farrell, M.B. Tomson (2008), Control Placement of Scale Inhibitors in the Formation with Stable Ca-DTPMP Nanoparticle Suspension and its Transport Porous Media. Proceedings of SPE 114063, 1-20.
- M.B. Tonson, A.T. Kan. and J.E. Oddo (1994) Acid/ Base and Metal Complex Solution Chemistry of the polyphosphonate DTPMP versus temperature and ionic strength. Langmuir, 10(5), 1442-1449.
- M. Nergaard, C. Grimholt (2010) An Introduction to Scaling causes, problems and solutions. http://iptibm1.ipt.ntnu.no/~jsg/ undervisning/naturgass/oppgaver/Oppgaver2010/10Nergaard.pdf retrieved on May 21, 2016.
- O.F Joel, C.A. Amajouoyi, C.U. Nwokoye (2010) Characterization of Formation Water Constituents and the Eﬀect of Fresh Water Dilution from Land Rig Location of the Niger Delta, Nigeria. J Appl Sci Environ Manage. 14(2), 37–41.
- G.V. Chilingar, R. Mourhatch, G. D. Al-Qahtani (2008) Fundamentals of Corrosion and Scaling - For Petroleum and Environmental Engineers. Gulf Publishing Company.
- Sandengen K. Hydrates and Glycols.http://www.ipt.ntnu.no/~jsg/ undervisning/naturgass/lysark/LysarkSandengen2010.pdf; November 2010.
- F.L. Siega, E.B. Herras and B.C. Buñing (2005), Calcite Scale Inhibition: The Case of Mahanagdong Wells in Leyte Geothermal Production Field, Philippines Proceedings World Geothermal Congress, 1-6.
- B. Zumreoglu-Karan, A.N. Ay (2012) Layered double hydroxides – multifunctional nanomaterials Chemical Papers, 66 (1) 1–10
- Y. Kuang, L. Zhao, S. Zhang, F. Zhang, M. Dong, and S. Xu (2010) “Morphologies, preparations and applications of layered double hydroxide micro-/nanostructures,” Materials, 3(12), 5220–5235.
- Y. Lin, Q. Fang, and B. Chen (2014) “Perchlorate uptake and molecular mechanisms by magnesium/aluminum carbonate layered double hydroxides and the calcined layered double hydroxides,” Chemical Engineering Journal, 237, 38–46.
- F. Cavani, F. Trifiròa, A. Vaccaria (1991) Hydrotalcite-type anionic clays: Preparation, properties and applications. Catal. Today, 11, 173-301.
- V. Rives (2001) Layered Double Hydroxides: Present and Future; Nova Science Publishers: New York, NY, USA.
- I. Khan, D. O’Hare, (2002) Intercalation chemistry of layered double hydroxides: Recent developments and applications. J. Mater. Chem. 12, 3191-3198.
- P.J. Sideris, U.G. Nielsen, Z. Gan, C.P. Grey (2008) Mg/Al ordering in layered double hydroxides revealed by multinuclear NMR spectroscopy. Science, 321, 113-117.
- D. Scarpellini, C. Leonardi, A. Mattoccia, L. Di Giamberardino, P.G. Medaglia, G. Mantini, F. Gatta, E. Giovine, V. Foglietti, C. Falconi, A. Orsini, and R. Pizzoferrato (2015) Solution-Grown Zn/Al Layered Double Hydroxide Nanoplatelets onto Al Thin Films: Fine Control of Position and Lateral Thickness Journal of Nanomaterials, Vol. 2015, 1-8.
- M. Yang, E. Tuckley, J-C. Buffet and D. O’Hare (2016), Rapid efficient phase pure synthesis of Ca2AlNO3 layered double hydroxide. J. Mater. Chem. A, 4, 500-504.
- M. Everaert, R. Warrinnier, S. Baken, J-P. Gustafsson, D. De Vos, and E. Smolders (2016), Phosphate-Exchanged Mg–Al Layered Double Hydroxides: A New Slow Release Phosphate Fertilizer. ACS Sustainable Chem. Eng., 2016, 4 (8), pp 4280–4287
- W. Bao, J. Wang, Q. Wang, D. O’Hare and Y. Wan (2016), Layered Double Hydroxide Nano transporter for Molecule Delivery to Intact Plant Cells. Sci. Rep. 6, 26738; doi: 10.1038/srep26738
- D. Shan, S. Cosnier, and C. Mousty (2004) “HRP/[Zn-Cr-ABTS] redox clay-based biosensor: design and optimization for cyanide detection,” Biosensors and Bioelectronics, vol. 20, 390–396.
- Orsini, F. Gatta, C. Leonardi (2012) “CMOS compatible, low power, high-sensitivity Zn/Al layered double hydroxides humidity micro-sensor,” in Sensors: Proceedings of the First National Conference on Sensors, Rome.
- G.B. Douglas (2014), Contaminant removal from acidic mine pit water via in situ hydrotalcite formation. /Applied Geochemistry 42, 27–37; F. Baldini, A. D’Amico, C. Di Natale (2014). vol. 162 of Lecture Notes in Electrical Engineering, pp. 493–497, Springer, NewYork, NY, USA; G. B. Douglas, L. A. Wendling, R. Pleysier, M. G. Trefry (2010), Hydrotalcite Formation for Contaminant Removal from Ranger Mine Process Water. Mine Water Environ 1-8, DOI 10.1007/s10230-010-0106-4.
- Y. Lin, Q. Fang, and B. Chen (2014) “Perchlorate uptake and molecular mechanisms by magnesium/aluminum carbonate layered double hydroxides and the calcined layered double hydroxides,” Chemical Engineering Journal, vol. 237, 38–46.
- R. Yang, Y. Gao, J. Wang, and Q. Wang (2014) “Layered double hydroxide (LDH) derived catalysts for simultaneous catalytic removal of soot and NOx Dalton Transactions, vol. 43, 10317.
- A. Forano, T. Hibino, F. Lereoux, and C. Taviot-Gu´eho (2006) “Layered double hydroxide,” in Handbook of Clay Science, F. Bergaya, B. Theng, and G. Lagaly, Eds., pp. 1021–1095.
- Q. Wang and D. O’Hare (2012) “Recent advances in the synthesis and application of layered double hydroxide (LDH) nanosheets,” Chemical Reviews, vol. 112, no. 7, pp. 4124–4155.
- X. Guo, F. Zhang, D.G. Evans, and X. Duan, (2010) “Layered double hydroxide films: synthesis, properties and applications,” Chemical Communications, vol. 46, no. 29, pp. 5197–5210.
- T. Kameda, M. Saito and Y. Umetsu (2006) Preparation and Characterisation of Mg–Al Layered Double Hydroxides Intercalated with 2-Naphthalene Sulphonate and 2,6-Naphthalene Disulphonate, Materials Transactions, Vol. 47, No. 3, 923-930.
- S. Miyata (1975), The Syntheses of Hydrotalcite-Like Compounds and Their Structures and Physico- Chemical Properties I: The Systems Mg2+-Al3+-NO3−, Mg2+-Al3+-Cl−, Mg2+-Al3+-ClO4−, Ni2+-Al3+-Cl− and Zn2+-Al3+-Cl−, Clays and Clay Minerals, 23, 369-375.
- S. Miyata (1983), Anion-exchange properties of hydrotalcite-like compounds, Clays and Clay Minerals, 31, 305-311.
- S. Miyata (1980), Physico-chemical properties of synthetic hydrotalcites in relation to composition, Clays and Clay Minerals, 28, 50-56.
- J.B. Parsa, M. Abbasi (2007), Decolorization of synthetic and real wastewater by indirect electrochemical oxidation process, Acta Chimica Slovenica, 54, 792-796.
- M.C. Alexandrica, M. Silion, D. Hritcu, M.I. Popa (2015), layered double hydroxides as adsorbents for anionic dye removal from aqueous solutions Environmental Engineering and Management Journal 2015, Vol.14, No. 2, 381-388.
- R.L. Goswamee, P. Sengupta, K.G. Bhattacharyya, D.K. Dutta (1988), Adsorption of Cr (VI) in layered double hydroxides, Applied Clay Science, 13, 21-34.
- J. Inacio, C. Taviot-Gueho, C. Forano, J.P. Besse (2001), Adsorption of MCPA pesticide by MgAl-layered double hydroxides, Applied Clay Science, 18, 255- 264.
- T. Toraishi, S. Nagasaki, S. Tanaka (2002), Adsorption behavior of IO3- by CO32- and NO3- hydrotalcite, Applied Clay Science, 22, 17-23.
- D. Kovačević, a, B. N. Džakula, D. Hasenay, I. Nemet, S. Rončević, I. Dékány, and D. Petridise (2013), Adsorption of Arsenic on MgAl Layered Double Hydroxide Croat. Chem. Acta 86 (3), 273–279.