Development of Molecular Imprinted Polymers (MIPs) for the Selective Removal of Carbamazepine from Aqueous Solution
The occurrence and removal of trace organic
contaminants in the aquatic environment has become a focus of
environmental concern. For the selective removal of carbamazepine
from loaded waters molecularly imprinted polymers (MIPs) were
synthesized with carbamazepine as template. Parameters varied were
the type of monomer, crosslinker, and porogen, the ratio of starting
materials, and the synthesis temperature. Best results were obtained
with a template to crosslinker ratio of 1:20, toluene as porogen, and
methacrylic acid (MAA) as monomer. MIPs were then capable to
recover carbamazepine by 93% from a 10-5 M landfill leachate
solution containing also caffeine and salicylic acid. By comparison,
carbamazepine recoveries of 75% were achieved using a nonimprinted
polymer (NIP) synthesized under the same conditions, but
without template. In landfill leachate containing solutions
carbamazepine was adsorbed by 93-96% compared with an uptake of
73% by activated carbon. The best solvent for desorption was
acetonitrile, with which the amount of solvent necessary and dilution
with water was tested. Selected MIPs were tested for their reusability
and showed good results for at least five cycles. Adsorption
isotherms were prepared with carbamazepine solutions in the
concentration range of 0.01 M to 5*10-6 M. The heterogeneity index
showed a more homogenous binding site distribution.
[1] T. A. Ternes, "Occurrence of drugs in German sewage treatment plants
and rivers," Water Res., vol. 32, pp. 3245-3260, Nov. 1998.
[2] T. A. Ternes, M. Bonerz, T. J. Schmidt, 2001. "Determination of neutral
pharmaceuticals in wastewater and rivers by liquid chromatography-
electrospray tandem mass spectrometry," J. Chromatogr. A, vol. 938, pp.
175-185, Dec. 2001.
[3] T. A. Ternes, J. St├╝ber, N. Herrmann, D. McDowell, A. Ried, M.
Kampmann, B. Teiser, "Ozonation: A tool for removal of
pharmaceutical contrast media and musk fragrances from wastewater?,"
Water Res., vol. 37, pp. 1976-1982, Apr. 2003.
[4] H. Zhang, H. Yamada, S.-E. Kim, H.-S. Kim, H. Tsuno, "Removal of
endocrine disrupting chemicals by ozonation in sewage treatment,"
Water Sci. Technol., Vol. 54, pp. 123-132, 2006.
[5] C. Zwiener, F. H. Frimmel, "Oxidative treatment of pharmaceuticals in
water," Water Res., vol. 34, pp. 1881-1885, Apr. 2000.
[6] R. Andreozzi,V. Caprio, R. Marotta, A. Radovnikovic, "Ozonation and
H2O2/UV treatment of clofibric acid in water: A kinetic investigation," J.
Hazard. Mater., vol. 103, pp. 233-246, Oct. 2003.
[7] D. Vogna, R. Marotta, R. Andreozzi, A. Napolitano, M. d-Ischia,
"Kinetic and chemical assessment of the UV/H2O2 treatment of
antiepileptic drug carbamazepine" Chemosphere, vol. 54, pp. 497-505,
Jan. 2004.
[8] T. E. Doll, F. H. Frimmel, "Photocatalytic degradation of
carbamazepine, clofibric acid and iomeprol with P25 and Hombikat
UV100 in the presence of natural organic matter (NOM) and other
organic water constituents," Water Res., vol. 39, pp. 403-411, Jan.-Feb.
2005.
[9] S. Esplugas, D. M. Bila, L. G. T. Krause, M. Dezotti, "Ozonation and
advanced oxidation technologies to remove endocrine disrupting
chemicals (EDCs) and pharmaceuticals and personal care products
(PPCPs) in water effluents," J. Hazard. Mater., vol. 149, pp. 631-642,
Nov. 2007.
[10] B. R. Locke, M. Sato, P. Sunka, M. R. Hoffmann, J.-S. Chang,
"Electrohydraulic discharge and nonthermal plasma for water
treatment," Ind. Eng. Chem. Res., vol. 45, pp. 882-905, Feb. 2006.
[11] H. Krause, B. Schweiger, J. Schuhmacher, S. Scholl, U. Steinfeld,
"Degradation of the endocrine disrupting chemicals (EDCs)
carbamazepine, clofibric acid, and iopromide by corona discharge over
water," Chemosphere, vol. 75, pp. 163-168, Apr. 2009.
[12] Y. Zhang, J. Zheng, X. Qu, H. Chen, "Design of a novel non-equilibrium
plasma-based water treatment reactor," Chemosphere, vol. 70, pp. 1518-
1524, Feb. 2008.
[13] T. A. Ternes, M. Meisenheimer, D. McDowell, F. Sacher, H.-J. Brauch,
B. Haist-Gulde, G. Preuss, U. Wilme, N. Zulei-Seibert, "Removal of
Pharmaceuticals during Drinking Water Treatment," Environ. Sci. and
Technol., vol. 36, pp. 3855-3863, Sept. 2002.
[14] M. Le Noir, A.-S. Lepeuple, B. Guieysse, B. Mattiasson, "Selective
removal of 17¶Çêò-estradiol at trace concentration using a molecularly
imprinted polymer," Water Res., vol. 41, pp. 2825-2831, June 2007.
[15] A. J. Hall, M. Emgenbroich, B. Sellergren, "Imprinted polymers," in
Top. Curr. Chem., vol. 249, pp. 317-349, Springer-Verlag Berlin
Heidelberg, 2005.
[16] W. Sch├╝ssler, M. Sengl, "Arzneimittel in der Umwelt (Pharmaceuticals
in the environment)," Materialien Nr. 114, Bayerisches Landesamt f├╝r
Wasserwirtschaft, Germany, Aug. 2004.
[17] T. Heberer, "Occurrence, fate, and removal of pharmaceutical residues
in the aquatic environment: a review of recent research data," Toxicol.
Lett., vol. 131, pp. 5-17, May 2002.
[18] J. W. Metzger, ÔÇ×Drugs in municipal landfills and landfill leachate," In:
K├╝mmerer, K. (Ed.). Pharmaceuticals in the Environment: Sources,
Fate, Effects and Risks, Springer, Berlin, 2004, pp. 133-137.
[19] B. Ferrari, N. Paxéus, R. Lo Giudice, A. Pollio, J. Garrica,
"Ecotoxicological impact of pharmaceuticals found in treated
wastewaters: study of carbamazepine, clofibric acid, and diclofenac,"
Ecotoxicol. Environ. Saf., vol. 55, pp. 359-370, July 2003.
[20] P. M. Álvarez, F. J. Beltrán, V. Gómez-Serrano, J. Jaramillo, E. M.
Rodríguez, "Comparison between thermal and ozone regenerations of
spent activated carbon exhausted with phenol," Water Res., vol. 38, pp.
2155-2165, Apr. 2004.
[1] T. A. Ternes, "Occurrence of drugs in German sewage treatment plants
and rivers," Water Res., vol. 32, pp. 3245-3260, Nov. 1998.
[2] T. A. Ternes, M. Bonerz, T. J. Schmidt, 2001. "Determination of neutral
pharmaceuticals in wastewater and rivers by liquid chromatography-
electrospray tandem mass spectrometry," J. Chromatogr. A, vol. 938, pp.
175-185, Dec. 2001.
[3] T. A. Ternes, J. St├╝ber, N. Herrmann, D. McDowell, A. Ried, M.
Kampmann, B. Teiser, "Ozonation: A tool for removal of
pharmaceutical contrast media and musk fragrances from wastewater?,"
Water Res., vol. 37, pp. 1976-1982, Apr. 2003.
[4] H. Zhang, H. Yamada, S.-E. Kim, H.-S. Kim, H. Tsuno, "Removal of
endocrine disrupting chemicals by ozonation in sewage treatment,"
Water Sci. Technol., Vol. 54, pp. 123-132, 2006.
[5] C. Zwiener, F. H. Frimmel, "Oxidative treatment of pharmaceuticals in
water," Water Res., vol. 34, pp. 1881-1885, Apr. 2000.
[6] R. Andreozzi,V. Caprio, R. Marotta, A. Radovnikovic, "Ozonation and
H2O2/UV treatment of clofibric acid in water: A kinetic investigation," J.
Hazard. Mater., vol. 103, pp. 233-246, Oct. 2003.
[7] D. Vogna, R. Marotta, R. Andreozzi, A. Napolitano, M. d-Ischia,
"Kinetic and chemical assessment of the UV/H2O2 treatment of
antiepileptic drug carbamazepine" Chemosphere, vol. 54, pp. 497-505,
Jan. 2004.
[8] T. E. Doll, F. H. Frimmel, "Photocatalytic degradation of
carbamazepine, clofibric acid and iomeprol with P25 and Hombikat
UV100 in the presence of natural organic matter (NOM) and other
organic water constituents," Water Res., vol. 39, pp. 403-411, Jan.-Feb.
2005.
[9] S. Esplugas, D. M. Bila, L. G. T. Krause, M. Dezotti, "Ozonation and
advanced oxidation technologies to remove endocrine disrupting
chemicals (EDCs) and pharmaceuticals and personal care products
(PPCPs) in water effluents," J. Hazard. Mater., vol. 149, pp. 631-642,
Nov. 2007.
[10] B. R. Locke, M. Sato, P. Sunka, M. R. Hoffmann, J.-S. Chang,
"Electrohydraulic discharge and nonthermal plasma for water
treatment," Ind. Eng. Chem. Res., vol. 45, pp. 882-905, Feb. 2006.
[11] H. Krause, B. Schweiger, J. Schuhmacher, S. Scholl, U. Steinfeld,
"Degradation of the endocrine disrupting chemicals (EDCs)
carbamazepine, clofibric acid, and iopromide by corona discharge over
water," Chemosphere, vol. 75, pp. 163-168, Apr. 2009.
[12] Y. Zhang, J. Zheng, X. Qu, H. Chen, "Design of a novel non-equilibrium
plasma-based water treatment reactor," Chemosphere, vol. 70, pp. 1518-
1524, Feb. 2008.
[13] T. A. Ternes, M. Meisenheimer, D. McDowell, F. Sacher, H.-J. Brauch,
B. Haist-Gulde, G. Preuss, U. Wilme, N. Zulei-Seibert, "Removal of
Pharmaceuticals during Drinking Water Treatment," Environ. Sci. and
Technol., vol. 36, pp. 3855-3863, Sept. 2002.
[14] M. Le Noir, A.-S. Lepeuple, B. Guieysse, B. Mattiasson, "Selective
removal of 17¶Çêò-estradiol at trace concentration using a molecularly
imprinted polymer," Water Res., vol. 41, pp. 2825-2831, June 2007.
[15] A. J. Hall, M. Emgenbroich, B. Sellergren, "Imprinted polymers," in
Top. Curr. Chem., vol. 249, pp. 317-349, Springer-Verlag Berlin
Heidelberg, 2005.
[16] W. Sch├╝ssler, M. Sengl, "Arzneimittel in der Umwelt (Pharmaceuticals
in the environment)," Materialien Nr. 114, Bayerisches Landesamt f├╝r
Wasserwirtschaft, Germany, Aug. 2004.
[17] T. Heberer, "Occurrence, fate, and removal of pharmaceutical residues
in the aquatic environment: a review of recent research data," Toxicol.
Lett., vol. 131, pp. 5-17, May 2002.
[18] J. W. Metzger, ÔÇ×Drugs in municipal landfills and landfill leachate," In:
K├╝mmerer, K. (Ed.). Pharmaceuticals in the Environment: Sources,
Fate, Effects and Risks, Springer, Berlin, 2004, pp. 133-137.
[19] B. Ferrari, N. Paxéus, R. Lo Giudice, A. Pollio, J. Garrica,
"Ecotoxicological impact of pharmaceuticals found in treated
wastewaters: study of carbamazepine, clofibric acid, and diclofenac,"
Ecotoxicol. Environ. Saf., vol. 55, pp. 359-370, July 2003.
[20] P. M. Álvarez, F. J. Beltrán, V. Gómez-Serrano, J. Jaramillo, E. M.
Rodríguez, "Comparison between thermal and ozone regenerations of
spent activated carbon exhausted with phenol," Water Res., vol. 38, pp.
2155-2165, Apr. 2004.
@article{"International Journal of Medical, Medicine and Health Sciences:64377", author = "Bianca Schweiger and Lucile Bahnweg and Barbara Palm and Ute Steinfeld", title = "Development of Molecular Imprinted Polymers (MIPs) for the Selective Removal of Carbamazepine from Aqueous Solution", abstract = "The occurrence and removal of trace organic
contaminants in the aquatic environment has become a focus of
environmental concern. For the selective removal of carbamazepine
from loaded waters molecularly imprinted polymers (MIPs) were
synthesized with carbamazepine as template. Parameters varied were
the type of monomer, crosslinker, and porogen, the ratio of starting
materials, and the synthesis temperature. Best results were obtained
with a template to crosslinker ratio of 1:20, toluene as porogen, and
methacrylic acid (MAA) as monomer. MIPs were then capable to
recover carbamazepine by 93% from a 10-5 M landfill leachate
solution containing also caffeine and salicylic acid. By comparison,
carbamazepine recoveries of 75% were achieved using a nonimprinted
polymer (NIP) synthesized under the same conditions, but
without template. In landfill leachate containing solutions
carbamazepine was adsorbed by 93-96% compared with an uptake of
73% by activated carbon. The best solvent for desorption was
acetonitrile, with which the amount of solvent necessary and dilution
with water was tested. Selected MIPs were tested for their reusability
and showed good results for at least five cycles. Adsorption
isotherms were prepared with carbamazepine solutions in the
concentration range of 0.01 M to 5*10-6 M. The heterogeneity index
showed a more homogenous binding site distribution.", keywords = "Carbamazepine, landfill leachate, removal, reuse", volume = "3", number = "6", pages = "96-6", }