Removal of clofibric acid from aqueous solution by polyethylenimine-modified chitosan beads
Yao NIE, Shubo DENG, Bin WANG, Jun HUANG, Gang YU
Removal of clofibric acid from aqueous solution by polyethylenimine-modified chitosan beads
Polyethylenimine (PEI)-modified chitosan was prepared and used to remove clofibric acid (CA) from aqueous solution. PEI was chemically grafted on the porous chitosan through a crosslinking reaction, and the effects of PEI concentration and reaction time in the preparation on the adsorption of clofibric acid were optimized. Scanning electron microscopy (SEM) showed that PEI macromolecules were uniformly grafted on the porous chitosan, and the analysis of pore size distribution indicated that more mesopores were formed due to the crosslinking of PEI molecules in the macropores of chitosan. The PEI-modified chitosan had fast adsorption for CA within the initial 5 h, while this adsorbent exhibited an adsorption capacity of 349 mg·g−1 for CA at pH 5.0 according to the Langmuir fitting, higher than 213 mg·g−1 on the porous chitosan. The CA adsorption on the PEI-modified chitosan was pH-dependent, and the maximum adsorption was achieved at pH 4.0. Based on the surface charge analysis and comparison of different pharmaceuticals adsorption, electrostatic interaction dominated the sorption of CA on the PEI-modified chitosan. The PEI-modified chitosan has a potential application for the removal of some anionic micropollutants from water or wastewater.
clofibric acid / PEI-modified chitosan / adsorption capacity / adsorption mechanism / electrostatic interaction
[1] |
Fatta-Kassinos D, Meric S, Nikolaou A. Pharmaceutical residues in environmental waters and wastewater: current state of knowledge and future research. Analytical and Bioanalytical Chemistry, 2011, 399(1): 251–275
CrossRef
Pubmed
Google scholar
|
[2] |
Li W Z, Sui Q, Lu S G, Qiu Z F, Lin K F. Identification and ecotoxicity assessment of intermediates generated during the degradation of clofibric acid by advanced oxidation processes. Frontiers of Environmental Science & Engineering, 2012, 6(4): 445–454
CrossRef
Pubmed
Google scholar
|
[3] |
Tixier C, Singer H P, Oellers S, Müller S R. Occurrence and fate of carbamazepine, clofibric acid, diclofenac, ibuprofen, ketoprofen, and naproxen in surface waters. Environmental Science and Technology, 2003, 37(6): 1061–1068 doi:10.1021/es025834r
Pubmed
|
[4] |
Boyd G R, Reemtsma H, Grimm D A, Mitra S. Pharmaceuticals and personal care products (PPCPs) in surface and treated waters of Louisiana, USA and Ontario, Canada. The Science of the Total Environment, 2003, 311(1–3): 135–149
CrossRef
Pubmed
Google scholar
|
[5] |
Xu W H, Zhang G, Zou S C, Li X D, Liu Y C. Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using high-performance liquid chromatography-electrospray ionization tandem mass spectrometry. Environmental Pollution, 2007, 145(3): 672–679
CrossRef
Pubmed
Google scholar
|
[6] |
Kasprzyk-Hordern B, Dinsdale R M, Guwy A J. The effect of signal suppression and mobile phase composition on the simultaneous analysis of multiple classes of acidic/neutral pharmaceuticals and personal care products in surface water by solid-phase extraction and ultra performance liquid chromatography-negative electrospray tandem mass spectrometry. Talanta, 2008, 74(5): 1299–1312
CrossRef
Pubmed
Google scholar
|
[7] |
Jones O A H, Voulvoulis N, Lester J N. Aquatic environmental assessment of the top 25 English prescription pharmaceuticals. Water Research, 2002, 36(20): 5013–5022
CrossRef
Pubmed
Google scholar
|
[8] |
Weigel S, Kuhlmann J, Hühnerfuss H. Drugs and personal care products as ubiquitous pollutants: occurrence and distribution of clofibric acid, caffeine and DEET in the North Sea. The Science of the Total Environment, 2002, 295(1–3): 131–141
CrossRef
Pubmed
Google scholar
|
[9] |
Thomas K V, Hilton M J. The occurrence of selected human pharmaceutical compounds in UK estuaries. Marine Pollution Bulletin, 2004, 49(5–6): 436–444
CrossRef
Pubmed
Google scholar
|
[10] |
Barnes K K, Kolpin D W, Furlong E T, Zaugg S D, Meyer M T, Barber L B. A national reconnaissance of pharmaceuticals and other organic wastewater contaminants in the United States−I) groundwater. The Science of the Total Environment, 2008, 402(2–3): 192–200
CrossRef
Pubmed
Google scholar
|
[11] |
Gagné F, Blaise C, André C. Occurrence of pharmaceutical products in a municipal effluent and toxicity to rainbow trout (Oncorhynchus mykiss) hepatocytes. Ecotoxicology and Environmental Safety, 2006, 64(3): 329–336PMID:15923035
CrossRef
Google scholar
|
[12] |
Nassef M, Matsumoto S, Seki M, Khalil F, Kang I J, Shimasaki Y, Oshima Y, Honjo T. Acute effects of triclosan, diclofenac and carbamazepine on feeding performance of Japanese medaka fish (Oryzias latipes). Chemosphere, 2010, 80(9): 1095–1100
CrossRef
Pubmed
Google scholar
|
[13] |
Pfluger P, Dietrich D R. Effects on pharmaceuticals in the environment–an overview and principle considerations. In: Kummerer K, ed. Pharmaceuticals in the Environment. Heidelberg: Springer, 2011, 11–17
|
[14] |
Khetan S K, Collins T J. Human pharmaceuticals in the aquatic environment: a challenge to Green Chemistry. Chemical Reviews, 2007, 107(6): 2319–2364
CrossRef
Pubmed
Google scholar
|
[15] |
Heberer T. Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. Toxicology Letters, 2002, 131(1–2): 5–17
CrossRef
Pubmed
Google scholar
|
[16] |
Ternes T A. Occurrence of drugs in German sewage treatment plants and rivers. Water Research, 1998, 32(11): 3245–3260
CrossRef
Google scholar
|
[17] |
Nunes B, Gaio A R, Carvalho F, Guilhermino L. Behaviour and biomarkers of oxidative stress in Gambusia holbrooki after acute exposure to widely used pharmaceuticals and a detergent. Ecotoxicology and Environmental Safety, 2008, 71(2): 341– 354
CrossRef
Pubmed
Google scholar
|
[18] |
Heberer T. Tracking persistent pharmaceutical residues from municipal sewage to drinking water. Journal of Hazardous Materials, 2002, 266(3–4): 175–189
|
[19] |
Matamoros V, García J, Bayona J M. Organic micropollutant removal in a full-scale surface flow constructed wetland fed with secondary effluent. Water Research, 2008, 42(3): 653–660
CrossRef
Pubmed
Google scholar
|
[20] |
Mestre A S, Pinto M L, Pires J, Nogueira J M F, Carvalho A P. Effect of solution pH on the removal of clofibric acid by cork-based activated carbon. Carbon, 2010, 48(4): 92–980
CrossRef
Google scholar
|
[21] |
Simazaki D, Fujiwara J, Manabe S, Matsuda M, Asami M, Kunikane S. Removal of selected pharmaceuticals by chlorination, coagulation-sedimentation and powdered activated carbon treatment. Water Science and Technology, 2008, 58(5): 1129–1135
CrossRef
Pubmed
Google scholar
|
[22] |
Hasan Z, Jeon J, Jhung S H. Adsorptive removal of naproxen and clofibric acid from water using metal-organic frameworks. Journal of Hazardous Materials, 2012, 209–210(30): 151–157
CrossRef
Pubmed
Google scholar
|
[23] |
Bui T X, Choi H. Adsorptive removal of selected pharmaceuticals by mesoporous silica SBA-15. Journal of Hazardous Materials, 2009, 168(2–3): 602–608
CrossRef
Pubmed
Google scholar
|
[24] |
Wei H R, Deng S B, Huang Q, Nie Y, Wang B, Huang J, Yu G. Regenerable granular carbon nano tubes/ alumina hybrid adsorbents for diclofenac sodium and carbamazepine removal from aqueous solution. Water Research, 2013, 47(12): 4139–4147
CrossRef
Pubmed
Google scholar
|
[25] |
Chatterjee S, Lee D S, Lee M W, Woo S H. Enhanced adsorption of congo red from aqueous solutions by chitosan hydrogel beads impregnated with cetyl trimethyl ammonium bromide. Bioresource Technology, 2009, 100(11): 2803–2809
CrossRef
Pubmed
Google scholar
|
[26] |
Navarro R R, Sumi K, Fujii N, Matsumura M. Mercury removal from wastewater using porous cellulose carrier modified with polyethyleneimine. Water Research, 1996, 30(10): 2488–2494
CrossRef
Google scholar
|
[27] |
Deng S, Ting Y P. Polyethylenimine-modified fungal biomass as a high-capacity adsorbent for chromium anion removal. Environmental Science and Technology, 2005, 39(21): 8490–8496
CrossRef
Pubmed
Google scholar
|
[28] |
Deng S, Ma R, Yu Q, Huang J, Yu G. Enhanced removal of pentachlorophenol and 2,4-D from aqueous solution by an aminated biosorbent. Journal of Hazardous Materials, 2009, 165(1–3): 408–414
CrossRef
Pubmed
Google scholar
|
[29] |
United States National Library of Medicine (USNLM). Toxicology Data Network.
|
[30] |
Nebot C, Gibb S W, Boyd K G. Quantification of human pharmaceuticals in water samples by high performance liquid chromatography-tandem mass spectrometry. Analytica Chimica Acta, 2007, 598(1): 87–94
CrossRef
Pubmed
Google scholar
|
[31] |
Yamamoto E, Sakaguchi T, Kajima T, Mano N, Asakawa N. Novel methylcellulose-immobilized cation-exchange precolumn for on-line enrichment of cationic drugs in plasma. Journal of Chromatography. B, Analytical Technologies in the Biomedical and Life Sciences, 2004, 807(2): 327–334
CrossRef
Pubmed
Google scholar
|
[32] |
Yu Q, Deng S B, Yu G. Selective removal of perfluorooctane sulfonate from aqueous solution using chitosan-based molecularly imprinted polymer adsorbents. Water Research, 2008, 42(12): 3089–3097
CrossRef
Pubmed
Google scholar
|
[33] |
Zhang Q Y, Deng S B, Yu G, Huang J. Removal of perfluorooctane sulfonate from aqueous solution by crosslinked chitosan beads: sorption kinetics and uptake mechanism. Bioresource Technology, 2011, 102(3): 2265–2271
CrossRef
Pubmed
Google scholar
|
[34] |
Gao Y H, Deshusses M A. Adsorption of clofibric acid and ketoprofen onto powdered activated carbon: effect of natural organic matter. Environmental Technology, 2011, 33(15–16): 1719–1727
CrossRef
Pubmed
Google scholar
|
[35] |
Lindqvist N, Tuhkanen T, Kronberg L. Occurrence of acidic pharmaceuticals in raw and treated sewages and in receiving waters. Water Research, 2005, 39(11): 2219–2228
CrossRef
Pubmed
Google scholar
|
/
〈 | 〉 |