Box-Behnken Experimental Design for Optimization of Naproxen Adsorption on Activated Carbon Modified Chitosan-Polyvinyl Alcohol Biocomposite

Öz

In this paper, Box-Behnken experimental design was used to examine the effect of naproxen adsorption using activated carbon modified chitosan-polyvinyl alcohol biocomposite (KTS-PVA/AC) on operational parameters. Using the Box-Behnken experimental design, the adsorption process was optimized for low cost and maximum efficiency, the factors affecting the process were determined, and the interactions between these factors were evaluated. Experimental studies contain the naproxen removal in % using KTS-PVA/AC biocomposite depending on the amount of adsorbent, pH, and residence time. According to the results obtained from the regression analysis, the lack of fit value for the quadratic model was insignificant, the corrected R2 (0.9978) and estimated R2 (0.9871) values were high, these two R2 values were reasonably close to each other, and the quadratic model was selected to be suitable model. In addition, the parameter coefficients of adsorbent amount, pH, and residence time were calculated as positive in the regression equation. Based on the calculated parameter coefficients, residence time was determined to be most effective independent variable for naproxen adsorption compared to other parameters. Also, ANOVA analysis of variance was carried out to determine the optimum process parameters for the highest naproxen removal and to evaluate the effects of process parameters on adsorption. The highest naproxen removal in % was determined by the three-variable experimental design, 100 mg KTS-PVA/AC amount, 7.95 pH and 433.56 min residence time were found to be 99.57% under optimal experimental conditions. These results showed that the synthesized adsorbent was very effective on naproxen removal.

Anahtar Kelimeler

• Box-Behnken
• Naproxen
• Chitosan
• Polyvinyl alcohol
• Activated carbon

Aktif Karbon ile Modifiye Edilmiş Kitosan-Polivinil Alkol Biyokompoziti Üzerine Naproksen Adsorpsiyonunun Optimizasyonu için Box-Behnken Deneysel Tasarımı

Öz

Bu çalışmada, aktif karbon ile modifiye edilmiş kitosan-polivinil alkol biyokompoziti (KTS-PVA/AC) ile naproksen adsorpsiyonunun operayonel parametreleri üzerindeki etkisini incelemek amacıyla Box-Behnken deneysel tasarımı kullanılmıştır. Box-Behnken deneysel tasarımı ile adsorpsiyon sürecinin düşük maliyet ve maksimum verimlilikle optimize edilmesi, sürece etki eden faktörlerin belirlenmesi ve bu faktörler arasındaki etkileşimlerin değerlendirilmesi gerçekleştirilmiştir. Deneysel çalışmalar; adsorban miktarına, pH’a ve kalma zamanına bağlı olarak KTS-PVA/AC biyokompoziti ile naproksen giderim yüzdesini içermektedir. Regresyon analizinden elde edilen sonuçlara göre kuadratik model için lack of fit değerinin önemsiz olması, düzeltilmiş R2 (0,9978) ve tahmini R2 (0,9871) değerlerinin yüksek olması ve aynı zamanda bu iki R2 değerinin makul ölçüde birbirine yakın olması, kuadratik modeli en uygun model yapmaktadır. Ayrıca regresyon denkleminde adsorban miktarı, pH ve kalma zamanına ait parametre kaysayıları pozitif olarak hesaplanmıştır. Hesaplanan parametre katsayılarına dayanarak kalma zamanı diğer parametrelere kıyasla naproksen adsorpsiyonunda en etkili bağımsız değişken olarak tespit edilmiştir. Ayrıca, ANOVA varyans analizi en yüksek naproksen yüzde giderimi için optimum proses parametrelerinin belirlenmesi ve proses parametrelerinin adsorpsiyon üzerine etkisinin değerlendirilmesi amacıyla yapılmıştır. Üç değişkenli deneysel tasarımla tahmin edilen en yüksek naproksen yüzde giderimi, 100 mg KTS-PVA/AC miktarı, 7,95 pH ve 433,56 dk kalma zamanı optimum deney koşullarında % 99,57 olarak bulunmuştur. Bu sonuçlar sentezlenen adsorbanın naproksen giderimi üzerinde çok etkili olduğunu göstermektedir.

Anahtar Kelimeler

• Box-Behnken
• Naproksen
• Kitosan
• Polivinil alkol
• Aktif karbon

Kaynakça

1. Akay, P., Omay, D. (2014). Synthesis and characterization of chitosan & amino acid superabsorbent hydrogels. International Polymer Processing, 29(2), 287-294.
2. Boumya, W., Khnıifira, M., Machrouhi, A., Abdennouri, M., Achak, M., Qourzal, S., Tounsadi, H., Barka, N. (2021). Box–Behnken design for understanding of adsorption behaviors of cationic and anionic dyes by activated carbon. Desalination Water Treatment, 212, 204–211.
3. Boyd, G.R., Zhang, S.,. Grimm, D.A,. (2005). Naproxen removal from water by chlorination and biofilm processes. Water Research, 39(4), 668–676.
4. Boyda, G.R., Reemtsmaa, H., Grımmb, D.S., Mitrac, S. (2003). Pharma¬ceuticals and personal care products (PPCPs) in surface and treated waters of Louisiana, USA and Ontario, Canada. Science of the Total Environment, 311(1-3), 135–149.
5. Busar, H.R., Poiger, T., Muller, M.D. (1998). Occurrence and fate of the pharmaceutical drug diclofenac in surface waters: rapid photo degradation in a lake, Environmental Science and Technology, 32(22), 3449– 3556.
6. Büyükada, M. (2020). Hindi işleme tesisi atık sularından ozonlama ile renk, KOİ ve bulanıklık giderimi: Box-Behnken yaklaşımı ve Monte Carlo simülasyonu. Pamukkale Üniversitesi Mühendislik Bilimleri Dergisi, 26(7), 1282-1290.
7. Esplugas, S., Bila, D.M., Gustavo, L., Krause, T., Dezotti, M. (2007). Ozo¬nation and advanced oxidation technologies to remove endo¬crine disrupting chemicals (edcs) and pharmaceuticals and personal care products (Ppcps) in water effluents. Journal of Hazardous Materials, 149(3), 631–642.
8. Geng, Y., Ding, M., Chen, H., Li, H.F., Lin, J.M. (2012). Preparation of hydrophilic carbon-functionalized magnetic micro spheres coated with chitosan and application in solid-phase extraction of bisphenol a in aqueous samples. Talanta, 89, 189–194 .

9. Hasan, Z., Jeon, J., Jhung, S.H. (2012). Adsorptive removal of naproxen and clofibric acid from water using metal–organic frame¬Works. Journal of Hazardous Materials, 209–210, 151–157.
10. Ince, M., Kaplan Ince, O. (2017). Box-Behnken design approach for optimizing removal of opper from wastewater using a novel and green adsorbent, Atomic Spectroscopy, 38(6). 200-207.
11. Joss, A., Zabczynski, S., Gobel, A., Hoffmannc, B., Loffler, D., Mcardell, C.S., Ternes, T.A., Thomsen, A., Siegrist, H. (2006). Biological deg¬radation of pharmaceuticals in municipal wastewater treat¬ment: proposing a classification scheme. Water Research, 40(8), 1686–1696.
12. LIAO, H., QI, R., SHEN, M., CAO, X., GUO, R., ZHANG, Y., SHİ, X. (2011). Improved cellular response on multi walled carbon nano tube-incorporated electro spun polyvinyl alcohol/chitosan nano fibrous scaffolds. Colloids Surf. B: Biointerfaces, 84(2), 528–535. Ngah, W.S.W., Teong, L.C., Hanafıah, M.A. (2011). Adsorption of dyes and heavy metal ions by chitosan composites: a review. Carbohydrate Polymers, 83(4), 1446–1456.
13. Nguyen, N.T., Liu, J.H. (2014). A green method for in situ synthe¬sis of poly(vinyl alcohol)/chitosan hydrogel thin films with entrapped silver nano particles. Journal of the Taiwan Insttitute of Chemical Engineers, 45(5), 2827–2833.
14. Pandele, A.M., Ionia M., Crica, L., Dinescu, S., Costache, M., Iovu, H. (2014). Synthesis, characterization, and in-vitro studies of graphene oxide/chitosan–polyvinyl alcohol films. Carbohydrate Polymers, 102, 813–820 .
15. Quıre, M., Khamis, M., Malek, F., Nir, S., Abbadi, B., Scrano, L. (2013). Stability and removal of naproxen and its metabolite by advanced membrane wastewater treatment plant and micelle– clay complex. Clean- Soil Air Water, 42(5), 594-600.
16. Roberts, G.A.F. (1992). Chitin chemistry, Hong Kong: the Macmillan Press Ltd.
17. Saloglu, D., Ozcan, N. (2018). Activated carbon embedded chitosan/polyvinyl alcohol biocomposites for adsorption of nonsteroidal anti-inflammatory drug - naproxen from wastewater. Desalination Water Treatment, 107, 1–13.
18. Bilgin Simsek, E., Saloglu, D., Ozcan, N., Novak, I., Berek, D. (2017). Carbon fiber embedded chitosan/pva composites for decontamination of endocrine disruptor bisphenol-a from water. Journal of the Taiwan Insttitute of Chemical Engineers, 70, 291–301.
19. Subedi, B., Du, B., Chambliss, C.K., Koschorreck, J., Rudel H.,, Quack, M., Brooks, B.W., Usenko, S. (2012). Occurrence of pharmaceuticals and personal care products in German fish tissue: A national study. Environmental Science and Technology, 46(16), 9047–9054.
20. Ternes, T.A. (1998). Occurrence of drugs in German sewage treatment plants and rivers. Water Research, 32(11), 3245–3260. Xu, J., Wang, L., Zhu, Y. (2012). Decontamination of bisphenol a from aqueous solution by graphene adsorption. Langmuir, 28(22), 8418–8425.
21. Yudin, V.E., Dobrovolskaya, I.P., Neelova, I.M., Dres¬vyanına, E.N., Popryadukhın P.V., Ivan’kova, E.M. (2014). Wet spinning of fibers made of chitosan and chitin nanofibrils. Carbohydrate Polymers, 108, 176–182.