Abstract
Carbonized rice husk (CRH) is a promising material to separate oil from water owing to its abundance, low-cost, and environmentally benign characteristics. However, CRH’s performance is somewhat limited by its similar surface charge to that of oil, leading to repulsive interactions. To improve the separation efficiency of CRH, CRH was modified via impregnation with a cationic biocompatible polymer, polyethlyenimine (PEI) to form PEI-CRH. The modified sample exhibits a remarkably higher (10–50 times) oil/water (O/W) separation efficiency than that of the unmodified one. Small PEI-CRH particles (about 64 μm) are found to adsorb oil droplets faster and larger quantities than bigger particles (about 113 and 288 μm). PEI-CRH exhibits higher separation efficiency at high temperatures owing to the destabilization of the emulsion. It is also found that the oil adsorption mechanism involves a chemical interaction between PEI-CRH and oil droplets. The addition of NaCl considerably improves the separation efficiency, while the addition of a cationic surfactant has the opposite effect. In acidic emulsions, PEI-CRH adsorbs more oil than in neutral or basic conditions owing to favorable attractive forces between oil droplets and the surface of PEI-CRH. PEI-CRH can be easily regenerated by washing with ethanol. These promising features of PEI-CRH indicate that PEI-CRH could be an efficient and low-cost adsorbent for the O/W separation applications.
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References
Abo-El Ela SI, Nawar SS (1980) Treatment of wastewater from an oil and soap factory via dissolved air flotation. Environ Int 4:47–52. doi:10.1016/0160-4120(80)90093-8
Ahmad AL, Sumathi S, Hameed BH (2005) Adsorption of residue oil from palm oil mill effluent using powder and flake chitosan: equilibrium and kinetic studies. Water Res 39:2483–2494. doi:10.1016/j.watres.2005.03.035
Almeida RM, Pantano CG (1990) Structural investigation of silica gel films by infrared spectroscopy. J Appl Phys 68:4225–4232. doi:10.1063/1.346213
Al-Shamrani AA, James A, Xiao H (2002a) Destabilisation of oil–water emulsions and separation by dissolved air flotation. Water Res 36:1503–1512. doi:10.1016/S0043-1354(01)00347-5
Al-Shamrani AA, James A, Xiao H (2002b) Separation of oil from water by dissolved air flotation. Colloids Surf A Physicochem Eng Asp 209:15–26. doi:10.1016/S0927-7757(02)00208-X
Alther G (2008) Cleaning wastewater: removing oil from water with organoclays. Filtr Sep 45:22–24. doi:10.1016/S0015-1882(08)70057-0
Angelova D, Uzunov I, Uzunova S, Gigova A, Minchev L (2011) Kinetics of oil and oil products adsorption by carbonized rice husks. Chem Eng J 172:306–311. doi:10.1016/j.cej.2011.05.114
Arnold L, Choudhury RB (1962) Ethanol extraction of soybean oil. J Am Oil Chem Soc 39:379–380. doi:10.1007/BF02631987
Bharathi KS, Ramesh ST (2013) Removal of dyes using agricultural waste as low-cost adsorbents: a review. Appl Water Sci 3:773–790. doi:10.1007/s13201-013-0117-y
Binks BP, Rodrigues JA (2005) Inversion of emulsions stabilized solely by ionizable nanoparticles. Angew Chem Int Ed 44:441–444. doi:10.1002/anie.200461846
Binks BP, Murakami R, Armes SP, Fujii S (2006) Effects of pH and salt concentration on oil-in-water emulsions stabilized solely by nanocomposite microgel particles. Langmuir 22:2050–2057. doi:10.1021/la053017+
Cañizares P, Martínez F, Jiménez C, Sáez C, Rodrigo MA (2008) Coagulation and electrocoagulation of oil-in-water emulsions. J Hazard Mater 151:44–51. doi:10.1016/j.jhazmat.2007.05.043
Carmona M, Khemis M, Leclerc J-P, Lapicque F (2006) A simple model to predict the removal of oil suspensions from water using the electrocoagulation technique. Chem Eng Sci 61:1237–1246. doi:10.1016/j.ces.2005.08.030
Chen C-M, Lu C-H, Chang C-H, Yang Y-M, Maa J-R (2000) Influence of pH on the stability of oil-in-water emulsions stabilized by a splittable surfactant. Colloids Surf A Physicochem Eng Asp 170:173–179. doi:10.1016/S0927-7757(00)00480-5
Costa TMH, Gallas MR, Benvenutti EV, da Jornada JAH (1997) Infrared and thermogravimetric study of high pressure consolidation in alkoxide silica gel powders. J Non-Cryst Solids 220:195–201. doi:10.1016/S0022-3093(97)00236-6
Demetriades K, Coupland JN, McClements DJ (1997) Physical properties of whey protein stabilized emulsions as related to pH and NaCl. J Food Sci 62:342–347. doi:10.1111/j.1365-2621.1997.tb03997.x
Djordjevic D, McClements DJ, Decker EA (2004) Oxidative stability of whey protein-stabilized oil-in-water emulsions at pH 3: potential ω-3 fatty acid delivery systems (Part B). J Food Sci 69:C356–C362. doi:10.1111/j.1365-2621.2004.tb10697.x
Enujiugha VN, Nwanna LC (2004) Aquatic oil pollution impact indicators. J Appl Sci Environ Manag 8:71–75
Frankel EN, Huang S-W, Aeschbach R, Prior E (1996) Antioxidant activity of a rosemary extract and its constituents, carnosic acid, carnosol, and rosmarinic acid, in bulk oil and oil-in-water emulsion. J Agric Food Chem 44:131–135. doi:10.1021/jf950374p
Freundlich HMF (1906) Über die adsorption in lösungen. Z Phys Chem 57:385–470
Hegazi HA (2013) Removal of heavy metals from wastewater using agricultural and industrial wastes as adsorbents. HBRC J 9:276–282. doi:10.1016/j.hbrcj.2013.08.004
Hilal N, Busca G, Hankins N, Mohammad AW (2004) The use of ultrafiltration and nanofiltration membranes in the treatment of metal-working fluids. Desalination 167:227–238. doi:10.1016/j.desal.2004.06.132
Ho YS, McKay G (1999) Pseudo-second order model for sorption processes. Process Biochem 34:451–465. doi:10.1016/S0032-9592(98)00112-5
Hsu S-T, Pan T-C (2007) Adsorption of paraquat using methacrylic acid-modified rice husk. Bioresour Technol 98:3617–3621. doi:10.1016/j.biortech.2006.11.060
Hu B, Scott K (2007) Influence of membrane material and corrugation and process conditions on emulsion microfiltration. J Membr Sci 294:30–39. doi:10.1016/j.memsci.2007.02.002
Huat BBK, Gue SS, Ali FH (2004) Tropical residual soils engineering. CRC Press, p 377–403
Ibrahim S, Wang S, Ang HM (2010) Removal of emulsified oil from oily wastewater using agricultural waste barley straw. Biochem Eng J 49:78–83. doi:10.1016/j.bej.2009.11.013
Ismagilov ZR et al (2009) Preparation of carbonized rice husk monoliths and modification of the porous structure by SiO2 leaching. Catal Today 147(Supplement: S58–S65) doi:10.1016/j.cattod.2009.07.043
Johnson RF, Manjreker TG, Halligan JE (1973) Removal of oil from water surfaces by sorption on unstructured fibers. Environ Sci Technol 7:439–443. doi:10.1021/es60077a003
Jones TJ, Neustadter EL, Whittingham KP (1978) Water-in-crude oil emulsion stability and emulsion destabilization by chemical demulsifiers. doi:10.2118/78-02-08
Klinkesorn U, Sophanodora P, Chinachoti P, McClements DJ (2004) Stability and rheology of corn oil-in-water emulsions containing maltodextrin. Food Res Int 37:851–859. doi:10.1016/j.foodres.2004.05.001
Kumagai S, Noguchi Y, Kurimoto Y, Takeda K (2007) Oil adsorbent produced by the carbonization of rice husks. Waste Manag 27:554–561. doi:10.1016/j.wasman.2006.04.006
Kumagal S, KAWA K, TAKEDA K (2006) Ammonia gas adsorption by carbonized rice husk. Int J Soc Mater Eng Resour 13:92–95
Lagergren S (1898) About the theory of so-called adsorption of soluble substances. Kungliga Svenska Vetenskapsakademiens Handlingar 24:1–39
Langmuir I (1916) The constitution and fundamental properties of solids and liquids. Part I. Solids. J Am Chem Soc 38:2221–2295. doi:10.1021/ja02268a002
Lee K (2002) Oil–particle interactions in aquatic environments: influence on the transport, fate, effect and remediation of oil spills. Spill Sci Technol Bull 8:3–8. doi:10.1016/S1353-2561(03)00006-9
Lin K-YA, Yang H, Petit C, Hsu F-K (2014) Removing oil droplets from water using a copper-based metal organic frameworks. Chem Eng J 249:293–301. doi:10.1016/j.cej.2014.03.107
Lobo A, Cambiella Á, Benito JM, Pazos C, Coca J (2006) Ultrafiltration of oil-in-water emulsions with ceramic membranes: influence of pH and crossflow velocity. J Membr Sci 278:328–334. doi:10.1016/j.memsci.2005.11.016
Luo P, Zhao Y, Zhang B, Liu J, Yang Y, Liu J (2010) Study on the adsorption of Neutral Red from aqueous solution onto halloysite nanotubes. Water Res 44:1489–1497. doi:10.1016/j.watres.2009.10.042
Maruyama H, Seki H, Satoh Y (2012) Removal kinetic model of oil droplet from o/w emulsion by adding methylated milk casein in flotation. Water Res 46:3094–3100
Moazed H, Viraraghavan T (2005a) Removal of oil from water by bentonite organoclay. Pract Peri Hazard Toxic Radioact Waste Manag 9:130–134. doi:10.1061/(ASCE)1090-025X(2005)9:2(130)
Moazed H, Viraraghavan T (2005b) Use of organo-clay/anthracite mixture in the separation of oil from oily waters. Energy Sources 27:101–112. doi:10.1080/00908310490448145
Nelson-Smith A (1968) The effects of oil pollution and emulsifier cleansing on shore life in South-West Britain. J Appl Ecol 5:97–107
Owlad M, Aroua MK, Wan Daud WMA (2010) Hexavalent chromium adsorption on impregnated palm shell activated carbon with polyethyleneimine. Bioresour Technol 101:5098–5103. doi:10.1016/j.biortech.2010.01.135
Paterson JW (1985) Industrial wastewater treatment technology. Butterworth Publishers
Patzek TW (2009) A first law thermodynamic analysis of biodiesel production from soybean. Bull Sci Technol Soc 29:194–204. doi:10.1177/0270467609334022
Pollard SJT, Fowler GD, Sollars CJ, Perry R (1992) Low-cost adsorbents for waste and wastewater treatment: a review. Sci Total Environ 116:31–52. doi:10.1016/0048-9697(92)90363-W
Quéméneur M, Marty Y (1994) Fatty acids and sterols in domestic wastewaters. Water Res 28:1217–1226. doi:10.1016/0043-1354(94)90210-0
Rajakovic V, Aleksic G, Radetic M, Rajakovic L (2007) Efficiency of oil removal from real wastewater with different sorbent materials. J Hazard Mater 143:494–499. doi:10.1016/j.jhazmat.2006.09.060
Rashed MN (2013) Adsorption technique for the removal of organic pollutants from water and wastewater. Org Pollutants Monit Risk Treat. doi:10.5772/54048
Rı́os G, Pazos C, Coca J (1998) Destabilization of cutting oil emulsions using inorganic salts as coagulants. Colloids Surf A Physicochem Eng Asp 138:383–389. doi:10.1016/S0927-7757(97)00083-6
Salam KK, Alade AO, Arinkoola AO, Opawale A (2013) Improving the demulsification process of heavy crude oil emulsion through blending with diluent. J Pet Eng 2013:6. doi:10.1155/2013/793101
Shinoda K, Saito H (1969) The stability of O/W type emulsions as functions of temperature and the HLB of emulsifiers: the emulsification by PIT-method. J Colloid Interface Sci 30:258–263. doi:10.1016/S0021-9797(69)80012-3
Sindhu M, Meera Sheriffa Begum KM, Sugashini S (2012) A comparative study of surface modification in carbonized rice husk by acid treatment. Desalin Water Treat 45:170–176. doi:10.1080/19443994.2012.692039
Stone-Masui J, Watillon A (1975) Characterization of surface charge on polystyrene latices. J Colloid Interface Sci 52:479–503. doi:10.1016/0021-9797(75)90273-8
Strassner JE (1968) J Pet Technol 243:303
Sud D, Mahajan G, Kaur MP (2008) Agricultural waste material as potential adsorbent for sequestering heavy metal ions from aqueous solutions—a review. Bioresour Technol 99:6017–6027. doi:10.1016/j.biortech.2007.11.064
Takamura A, Ishii F, Noro SI, Koishi M (1984) Physicopharmaceutical characteristics of an oil-in-water emulsion-type ointment containing diclofenac sodium. J Pharm Sci 73:676–681. doi:10.1002/jps.2600730521
Vlaev L, Petkov P, Dimitrov A, Genieva S (2011) Cleanup of water polluted with crude oil or diesel fuel using rice husks ash. J Taiwan Inst Chem Eng 42:957–964. doi:10.1016/j.jtice.2011.04.004
Wang D, Silbaugh T, Pfeffer R, Lin YS (2010) Removal of emulsified oil from water by inverse fluidization of hydrophobic aerogels. Powder Technol 203:298–309. doi:10.1016/j.powtec.2010.05.021
Wang H et al (2013a) Removal of oil droplets from contaminated water using magnetic carbon nanotubes. Water Res 47:4198–4205. doi:10.1016/j.watres.2013.02.056
Wang J, Chen H, Zhou H, Liu X, Qiao W, Long D, Ling L (2013b) Carbon dioxide capture using polyethylenimine-loaded mesoporous carbons. J Environ Sci 25:124–132. doi:10.1016/S1001-0742(12)60011-4
Wiese FK, Ryan PC (2003) The extent of chronic marine oil pollution in southeastern Newfoundland waters assessed through beached bird surveys 1984–1999. Mar Pollut Bull 46:1090–1101. doi:10.1016/S0025-326X(03)00250-9
Yang C-h (1998) Statistical mechanical study on the Freundlich isotherm equation. J Colloid Interface Sci 208:379–387. doi:10.1006/jcis.1998.5843
Yin C, Aroua M, Daud W (2008) Enhanced adsorption of metal ions onto polyethyleneimine-impregnated palm shell activated carbon: equilibrium studies. Water Air Soil Pollut 192:337–348. doi:10.1007/s11270-008-9660-9
Yudovin-Farber I, Beyth N, Weiss E, Domb A (2010) Antibacterial effect of composite resins containing quaternary ammonium polyethyleneimine nanoparticles. J Nanoparticle Res 12:591–603. doi:10.1007/s11051-009-9628-8
Zakaria Z, Mohd Ishak MA, Abdullah MF, Ismail K (2010) Thermal decomposition study of coals, rice husk, rice husk char and their blends during pyrolysis and combustion via thermogravimetric analysis international. J Chem Technol 2:78–87
Zhou Y-B, Tang X-Y, Hu X-M, Fritschi S, Lu J (2008) Emulsified oily wastewater treatment using a hybrid-modified resin and activated carbon system. Sep Purif Technol 63:400–406. doi:10.1016/j.seppur.2008.06.002
Zouboulis AI, Avranas A (2000) Treatment of oil-in-water emulsions by coagulation and dissolved-air flotation. Colloids Surf A Physicochem Eng Asp 172:153–161. doi:10.1016/S0927-7757(00)00561-6
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This work is supported by the Ministry of Science and Technology, Taiwan(103-2622-E-005-021-CC3).
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Lin, KY.A., Yang, H., Petit, C. et al. Removal of oil droplets from water using carbonized rice husk: enhancement by surface modification using polyethylenimine. Environ Sci Pollut Res 22, 8316–8328 (2015). https://doi.org/10.1007/s11356-014-3961-x
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DOI: https://doi.org/10.1007/s11356-014-3961-x