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박스-벤켄 설계법을 이용한 폐감귤박 활성탄에 의한 수용액 중의 항생제 Trimethoprim의 흡착 연구

Study on the Adsorption of Antibiotics Trimethoprim in Aqueous Solution by Activated Carbon Prepared from Waste Citrus Peel Using Box-Behnken Design

  • 이민규 (제주대학교 환경공학과) ;
  • 감상규 (부경대학교 화학공학과)
  • Lee, Min-Gyu (Department of Environmental Engineering, Jeju National University) ;
  • Kam, Sang-Kyu (Department of Chemical Engineering, Pukyong National University)
  • 투고 : 2018.04.05
  • 심사 : 2018.05.24
  • 발행 : 2018.08.01

초록

폐감귤박으로 제조한 활성탄(WCAC, waste citrus peel based activated carbon)에 의한 항생제 trimethoprim (TMP)의 흡착 특성을 조사하기 위해 반응표면법(RSM, response surface methodology)을 사용하여 TMP 흡착에 대한 운전인자들의 영향을 조사하였다. 농도($X_1$: 50-150 mg/L), pH ($X_2$: 4-10), 온도($X_3$: 293-323 K), 흡착제 투여량($X_4$: 0.05-0.15 g)의 4가지 입력 파라미터를 가진 4-요인 Box-Behnken 실험 설계에 따라 회분식 실험을 수행하고, 얻어진 실험 결과를 다중 회귀 분석으로 2차 다항식에 맞추고 통계적 방법을 사용하여 검토하였다. 독립 변수 및 변수들 간의 교호 작용의 유의성은 ANOVA 및 t-검정 통계기법으로 평가하였으며, 통계적 결과는 TMP 농도가 다른 요인들에 비하여 가장 많은 영향을 미치는 운전인자라는 것을 보여 주었다. 흡착공정은 유사 2차 속도식에 잘 부합하였으며, 등온흡착평형관계는 Langmuir 식이 Freundlich 식 보다 잘 부합하였다. Langmuir 등온식으로 부터 계산한 WCAC에 의한 TMP의 최대 흡착량은 293 K에서 144.9 mg/g이었다.

In order to investigate the adsorption characteristics of the antibiotics trimethoprim (TMP) by activated carbon (WCAC) prepared from waste citrus peel, the effects of operating parameters on the TMP adsorption were investigated by using a response surface methodology (RSM). Batch experiments were carried out according to a four-factor Box-Behnken experimental design with four input parameters : concentration ($X_1$: 50-150 mg/L), pH ($X_2$: 4-10), temperature ($X_3$: 293-323 K), adsorbent dose ($X_4$: 0.05-0.15 g). The experimental data were fitted to a second-order polynomial equation by the multiple regression analysis and examined using statistical methods. The significance of the independent variables and their interactions was assessed by ANOVA and t-test statistical techniques. Statistical results showed that concentration of TMP was the most effective parameter in comparison with others. The adsorption process can be well described by the pseudo-second order kinetic model. The experimental data of isotherm followed the Langmuir isotherm model. The maximum adsorption amount of TMP by WCAC calculated from the Langmuir isotherm model was 144.9 mg/g at 293 K.

키워드

참고문헌

  1. Jo, J. H., Lim, D. H. and Seo, G. T., "A Study on the Adsorption of Sulfonamide Antibiotics on Activated Carbon Using Density Functional Theory," J. Kor. Soc. Environ. Eng., 35(7), 457-463(2013). https://doi.org/10.4491/KSEE.2013.35.7.457
  2. Dominguez-Vargas, J. R., Carrillo-Perez, V., Gonzalez-Montero, T. and Cuerda-Correa, E. M., "Removal of Trimethoprim by a Low-Cost Adsorbent: Influence of Operation Conditions," Water Air Soil Pollut., 223, 4577-4588(2012). https://doi.org/10.1007/s11270-012-1219-0
  3. Pedrouzo, M., Borrull, F., Pocurull, E. and Marce, R. M., "Presence of Pharmaceuticals and Hormones in Waters from Sewage Treatment Plants," Water Air Soil Pollut., 217, 267-281(2011). https://doi.org/10.1007/s11270-010-0585-8
  4. Fukahori, S., Fujiwara, T., Ito, R. and Funamizu, N., "pH-Dependent Adsorption of Sulfa Drugs on High Silica Zeolite: Modeling and Kinetic Study," Desalination, 275, 237-242(2011). https://doi.org/10.1016/j.desal.2011.03.006
  5. Dardouri, S. and Sghaier, J., "Adsorptive Removal of Methylene Blue from Aqueous Solution using Different Agricultural Wastes as Adsorbents," Korean J. Chem. Eng., 34(4), 1037-1043(2017). https://doi.org/10.1007/s11814-017-0008-2
  6. Snyder, S., Westerhoff, P., Yoon, Y. and Sedlak, D. L., "Pharmaceuticals, Personal Care Products, and Endocrine Disruptors in Water: Implications for the Water Industry," Environ. Eng. Sci., 20, 449-469(2003). https://doi.org/10.1089/109287503768335931
  7. Ternes, T. A., Meisenheimer, M., McDowell, D., Sacher, F., Brauch, H.-J., Haist-Gulde, B., Preuss, G., Wilme, U. and Zulei-Seibert, N., "Removal of Pharmaceuticals During Drinking Water Treatment," Environ. Sci. Technol., 36(17), 3855-3863(2002). https://doi.org/10.1021/es015757k
  8. Putra, E. K., Pranowo, R., Sunarso, J., Indraswati, N. and Ismadji, S., "Performance of Activated Carbon and Bentonite for Adsorption of Amoxicillin from Wastewater: Mechanisms, Isotherms and Kinetics," Water Res., 43, 2419-2430(2009). https://doi.org/10.1016/j.watres.2009.02.039
  9. Chayid, M. A. and Ahmed, M. A., "Amoxicillin Adsorption on Microwave Prepared Activated Carbon from Arundo donax Linn: Isotherms, Kinetics, and Thermodynamics Studies," J. Environ. Chem. Eng., 3, 1592-1601(2015). https://doi.org/10.1016/j.jece.2015.05.021
  10. Mendez-Diaz, J. D., Prados-Joya, G., Rivera-Utrilla, J., Leyva-Ramos, R., Sanchez-Polo, M., Ferro-Garcia, M. A. and Medellin-Castillo, N. A., "Kinetic Study of the Adsorption of Nitroimidazole Antibiotics on Activated Carbons in Aqueous Phase," J. Colloid Interface Sci., 345, 481-490(2010). https://doi.org/10.1016/j.jcis.2010.01.089
  11. Ocampo-Perez, R., Orellana-Garcia, F., Sanchez-Polo, M., Rivera-Utrilla, J., Velo-Gala, I., Lopez-Ramon, M. V. and Alvarez-Merino, M. A., "Nitroimidazoles Adsorption on Activated Carbon Cloth from Aqueous Solution," J. Colloid Interface Sci., 401, 116-124(2013). https://doi.org/10.1016/j.jcis.2013.03.038
  12. Cahskan, E. and Gokturka, S., "Adsorption Characteristics of Sulfamethoxazole and Metronidazole on Activated Carbon," Sep. Sci. Technol., 45(2), 244-255(2010). https://doi.org/10.1080/01496390903409419
  13. Aksu, Z. and Tunc,, O., "Application of Biosorption for Penicillin G Removal: Comparison with Activated Carbon," Process Biochem., 40, 831-847(2005). https://doi.org/10.1016/j.procbio.2004.02.014
  14. Crisafully, R., Milhome, M. A. L., Cavalcante, R. M., Silveira, E. R., Keukeleire, D. De and Nascimento, R. F., "Removal of Some Polycyclic Aromatic Hydrocarbons from Petrochemical Wastewater Using Low-Cost Adsorbents of Natural Origin," Bioresour. Technol., 99(10), 4515-4519(2008). https://doi.org/10.1016/j.biortech.2007.08.041
  15. Xu, X., Cao, X. and Zhao, L., "Comparison of Rice Husk-and Dairy Manure-Derived Biochars for Simultaneously Removing Heavy Metals from Aqueous Solutions: Role of Mineral Components in Biochars," Chemosphere, 92(8), 955-961(2013). https://doi.org/10.1016/j.chemosphere.2013.03.009
  16. Baccar, R., Sarra, M., Bouzid, J., Feki, M. and Blanquez, P., "Removal of Pharmaceutical Compounds by Activated Carbon Prepared from Agricultural By-Product," Chem. Eng. J., 211-212, 310-317(2012). https://doi.org/10.1016/j.cej.2012.09.099
  17. Flores-Cano, J. V., Sanchez-Polo, M., Messoud, J., Ocampo-Perez, R. and Rivera-Utrilla, J., "Overall Adsorption Rate of Metronidazole, Dimetridazole and Diatrizoate on Activated Carbons Prepared from Coffee Residues and Almond Shells," J. Environ. Manage., 169, 116-125(2016). https://doi.org/10.1016/j.jenvman.2015.12.001
  18. Wan, S., Hua, Z., Sun, L., Bai, X. and Liang, L., "Biosorption of Nitroimidazole Antibiotics onto Chemically Modified Porous Biochar Prepared by Experimental Design: Kinetics, Thermodynamics, and Equilibrium Analysis," Process Safety Environ. Protection, 104, 422-435(2016). https://doi.org/10.1016/j.psep.2016.10.001
  19. Kam, S. K., Kang, K. H. and Lee, M. G., "Characterisitics of Activated Carbon Prepared from Waste Citrus Peel by KOH Activation," Appl. Chem. Eng., 28(6), 649-654(2017). https://doi.org/10.14478/ACE.2017.1073
  20. Lee, C. H., Kam, S. K. and Lee, M. G., "Adsorption Characteristics Analysis of 2,4-Dichlorophenol in Aqueous Solution with Activated Carbon Prepared from Waste Citrus Peel Using Response Surface Modeling Approach," Korean Chem. Eng. Res., 55(5), 723-730(2017). https://doi.org/10.9713/KCER.2017.55.5.723
  21. Kam, S. K. and Lee, M. G., "Response Surface Modeling for the Adsorption of Dye Eosin Y by Activated Carbon Prepared from Waste Citrus Peel," Appl. Chem. Eng., 29(3), 270-277(2018). https://doi.org/10.14478/ACE.2017.1130
  22. Alam, Z., Muyibi, S. A. and Toramae, J., "Statistical Optimization of Adsorption Processes for Removal of 2,4-Dichlorophenol by Activated Carbon Derived from Oil Palm Empty Fruit Bunches," J. Environ. Sci., 19, 674-677(2007). https://doi.org/10.1016/S1001-0742(07)60113-2
  23. Saadat, S. and Karimi-Jashni, A., "Optimization of Pb(II) Adsorption onto Modified Walnut Shells Using Factorial Design and Simplex Methodologies," Chem. Eng. J., 173, 743-749(2011). https://doi.org/10.1016/j.cej.2011.08.042
  24. Kim, D. S. and Park, Y. S., "Disinfection of E. coli Using Electro-UV Complex Process: Disinfection Characteristics and Optimization by the Design of Experiment Based on the Box-Behnken Technique," J. Environ. Sci. Int., 19(7), 889-900(2010). https://doi.org/10.5322/JES.2010.19.7.889
  25. Park, H. E. and Row, K. H., "Optimization of Synthesis Condition of Monolithic Sorbent Using Rsponse Surface Methodology," Appl. Chem. Eng., 24(3), 299-304(2013).
  26. Lee, S. E., Kim, J. K., Han, S. K., Chae, J. S., Lee, K. D. and Koo, K. K., "Optimization of a Crystallization Process by Response Surface Methodology," Appl. Chem. Eng., 26(6), 730-736(2015). https://doi.org/10.14478/ace.2015.1109
  27. Kam, S. K., Hyun, S. S. and Lee, M. G., "Removal of Divalent Heavy Metal Ions by Na-P1 Synthesized from Jeju Scoria," J. Environ. Sci. Intern., 20(10), 1337-1345(2011). https://doi.org/10.5322/JES.2011.20.10.1337
  28. Lagergren, S., "About the Theory of So-Called Adsorption of Soluble Substances," Kunglia Svenska Vetenskapsa-kademiens Handlingar, 24, 1-39(1898).
  29. Ho, Y. S. and McKay, G., "The Kinetics of Sorption of Basic Dyes from Aqueous Solution by Sphagnum Moss Peat," Can. J. Chem. Eng., 76, 822-827(1998). https://doi.org/10.1002/cjce.5450760419
  30. Langmuir, I., "The Adsorption of Gases on Plane Surface of Glass, Mica and Platinum," J. Am. Chem. Soc., 40, 1361-1403(1918). https://doi.org/10.1021/ja02242a004
  31. Freundlich, H. M. F., "Over the Adsorption in Solution," J. Phys. Chem., 57, 385-470(1906).
  32. Kim, S. H., Shon, H. K. and Ngo, H. H., "Adsorption Characteristics of Antibiotics Trimethoprim on Powdered and Granular Activated Carbon," J. Ind. Eng. Chem., 16, 344-349(2010). https://doi.org/10.1016/j.jiec.2009.09.061