Research Article
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Monitoring the Effect of Molecular Weight and Blend Ratio of Polyelectrolytes on the Development of Multilayer Films and Their Use in Drug Adsorption/Desorption Applications by QCM-D Technique

Year 2024, Volume: 10 Issue: 1, 190 - 206, 15.03.2024
https://doi.org/10.28979/jarnas.1407665

Abstract

In this study, the preparation of multilayered functional films with controllable thickness composition and morphology using the Layer-by-Layer (LbL) technique from weak and strong polyelectrolyte couples and the use of dairy in the release of different structured drugs have been studied. Besides, following the growth of self-assembled pure/blend LbL thin films at the nanogram level, intraction with the model drug LbL film surfaces in drug loading and release characterizations and viscoelastic changes of films intructed with drugs have been successfully investigated. Moreover, UV-Vis and QCM-D analyses have been performed to follow the growth of LbL functional thin films and to find polyelectrolyte ratios in film structure. In addition, scanning electron microscopy (SEM) and contact angle measurements have been carried out to investigate the controllable surface of LbL pure/blend structured thin films depending on the use of biodegradable and synthetic polyelectrolyte couples, blend ratio, and LbL deposition conditions. Subsequently, drug loading and release stabilities for the ibuprofen sodium drug have been performed using QCM-D and UV-Visible at neutral (pH: 6.8) acidic (pH: 2) and basic (pH: 11) PBS solutions. In addition to offering an innovative, economic, and practical approach, new drug release platforms with (i) surfaces of controllable morphology and composition, (ii) adjustable loading and release properties for model drugs, and (iii) sustuinable drug release in wide range of pH: 2-11, have been developed. The obtained results show that LbL functional films must have different properties considering the surface properties of the film, the pH of the media, the interaction between drug and film for drugs, and their applications. In this respect, the preparation of functional films with controllable proporties using the LbL technique and their use in drug release applications exhibit quite promising results.

Supporting Institution

TÜBİTAK

Project Number

112M290

Thanks

Tüm yazarlar, 112M290 numaralı proje kapsamında Türkiye Bilimsel ve Teknolojik Araştırma Kurumu'nun (TÜBİTAK) finansal desteğine teşekkür etmektedir.

References

  • S. Bhusari, J. Kim, K. Polizzi, S. Sankaran, A. del Campo, Encapsulation of bacteria in bilayer Pluronic thin film hydrogels: A safe format for engineered living materials, Biomaterials Advances 145 (2023) 213240 8 pages.
  • A. Qasem, M. S. Mostafa, H. A. Yakout, M. Mahmoud, E. R. Shaaban, Determination of optical bandgap energy and optical characteristics of Cd30Se50S20 thin film at various thicknesses, Optics and Laser Technology 148 (2022) 107770 13 pages.
  • H. Yılmaz, M. Özkan, Micropollutant removal capacity and stability of aquaporin incorporated biomimetic thin-film composite membranes, Biotechnology Reports 35 (2022) e00745 12 pages.
  • G. Decher, Fuzzy nanoassemblies: Toward layered polymeric multicomposites, Science 277 (5330) (1997) 1232–1237.
  • A. E. Barberio, S. G. Smith, I. S. Pires, S. Iyer, F. Reinhardt, M. B. Melo, H. Suh, R. A. Weinberg, D. J. Irvine, P. T. Hammond, Layer-by-layer interleukin-12 nanoparticles drive a safe and effective response in ovarian tumors, Bioengineering and Translational Medicine 8 (2) (2023) e10453 12 pages.
  • J. Pickering, N. G. Lamson, M. H. Marand, W. Hwang, J. P. Straehla, P. T. Hammond, Layer-by-layer polymer functionalization improves nanoparticle penetration and glioblastoma targeting in the brain, ACS Nano 17 (2023) 24154−24169.
  • J. P. Straehla, C. Hajal, H. C. Safford, G. S. Offeddu, N. Boehnke, T. G. Dacoba, J. Wyckoff, R. D. Kamm, P. T. Hammond, B. Harley, S. Mitragotri, R. Satchi-Fainaro, A predictive microfluidic model of human glioblastoma to assess trafficking of blood-brain barrier-penetrant nanoparticles, Proceedings of the National Academy of Sciences (PNAS) 119 (23) (2022) e2118697119 12 pages.
  • D. Yilmaz-Aykut, O. Yolacan, H. Deligoz, A comparative QCM-D study for various drug sorption behaviors and chemical degradation of chitosan/PAA LbL multilayered films, Journal of Polymer Research 30 (8) (2023) Article Number 307 16 pages.
  • D. Yilmaz-Aykut, H. Deligöz, Examining layer-by-layer assembly of polyelectrolyte-drug interactions using quartz crystal microbalance with dissipation, Polymer Engineering and Science 63 (11) (2023) 3625–3638.
  • J. Hong, B. S. Kim, K. Char, P. T. Hammond, Inherent charge-shifting polyelectrolyte multilayer blends: A facile route for tunable protein release from surfaces, Biomacromolecules 12 (8) (2011) 2975–2981.
  • S. Amorim, I. Pashkuleva, C. A. Reis, R. L. Reis, R. A. Pires, Tunable layer-by-layer films containing hyaluronic acid and their interactions with CD44, Journal of Materials Chemistry B 8 (17) (2020) 3880–3885.
  • R. Lu, B. Zhao, L. Yang, S. Zheng, X. Zan, N. Li, Role of driving force on engineering layer-by-layer protein/polyphenol coating with flexible structures and properties, ACS Applied Materials and Interfaces 15 (16) (2023) 20551–20562.
  • J. T. O’Neal, E. Y. Dai, Y. Zhang, K. B. Clark, K. G. Wilcox, I. M. George, N. E. Ramasamy, D. Enriquez, P. Batys, M. Sammalkorpi, J. L. Lutkenhaus, QCM-D investigation of swelling behavior of layer-by-layer thin films upon exposure to monovalent ions, Langmuir 34 (3) (2018) 999–1009.
  • Z. Dong, C. Liang, J. Zhao, Quartz crystal microbalance with dissipation (QCM-D) as a way to study adsorption and adsorbed layer characteristics of hemicelluloses and other macromolecules on thin cellulose films: A review, BioResources 18 (2) (2023) 1–19.
  • X. Huang, Q. Chen, W. Pan, Y. Yao, Advances in the mass sensitivity distribution of quartz crystal microbalances: A review, Sensors 22 (14) (2022) 5112 20 pages.
  • H. Deligöz, B. Tieke, QCM-D study of layer-by-layer assembly of polyelectrolyte blend films and their drug loading-release behavior, Colloids and Surfaces A: Physicochemical and Engineering Aspects 441 (2014) 725–736.
  • Szilagyi, G. Trefalt, A. Tiraferri, P. Maroni, M. Borkovec, Polyelectrolyte adsorption, interparticle forces, and colloidal aggregation, Soft Matter 10 (15) (2014) 2479–2502.
  • E. Konyalı, H. Y. Cengiz, A. Müftüler, H. Deligöz, Monitoring the salt stability and solvent swelling behavior of PAH-based polyelectrolyte multilayers by quartz crystal microbalance with dissipation, Polymer Engineering and Science 63 (10) (2023) 3328–3342.
  • M. Anwar, F. Pervaiz, H. Shoukat, S. Noreen, K. Shabbir, A. Majeed, S. Ijaz, Formulation and evaluation of interpenetrating network of xanthan gum and polyvinylpyrrolidone as a hydrophilic matrix for controlled drug delivery system, Polymer Bulletin 78 (1) (2021) 59–80.
  • Y. Jang, B. Akgun, H. Kim, S. Satija, K. Char, Controlled release from model blend multilayer films containing mixtures of strong and weak polyelectrolytes, Macromolecules 45 (8) (2012) 3542–3549.
  • A. Ghiorghita, F. Bucatariu, E. S. Dragan, Influence of cross-linking in loading/release applications of polyelectrolyte multilayer assemblies. A review, Materials Science and Engineering C 105 (2019) 110050 20 pages.
  • H. Zhang, L. Yu, L. Han, X. Liu, S. Ruan, J. Hu, Fast modulation of surface amphiphobicity/amphiphilicity via bidirectional substitution between perfluorinated surfactants and polyanions throughout pre-assembled polyelectrolyte multilayers, Langmuir 35 (52) (2019) 17122–17131.
  • H. Y. Cengiz, E. Konyali, A. Müftüler, H. Deligöz, Investigating the effect of weak polyelectrolytes on the chemical stability and swelling recovery of multilayered coatings, Progress in Organic Coatings 183 (2023) 107775 10 pages.
  • C. Li, J. Zhang, J. Han, B. Yao, A numerical solution to the effects of surface roughness on water–coal contact angle, Scientific Reports 11 (1) (2021) Article Number 459 12 pages.
  • A. Quinn, E. Tjipto, A. Yu, T. R. Gengenbach, F. Caruso, Polyelectrolyte blend multilayer films: Surface morphology, wettability, and protein adsorption characteristics, Langmuir 23 (9) (2007) 4944–4949.
  • W. Zhang, Q. Zhao, J. Yuan, Poröse polyelektrolyte: Zusammenspiel zwischen Poren und Ladung für neue funktionen, Angewandte Chemie 130 (23) (2018) 6868–6889.

Polielektrolitlerin Molekül Ağırlığı ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi

Year 2024, Volume: 10 Issue: 1, 190 - 206, 15.03.2024
https://doi.org/10.28979/jarnas.1407665

Abstract

Bu çalışmada, harman zayıf ve kuvvetli polielektrolit çiftlerinin kullanımı ile tabakalı kaplama, layer-by-layer (LbL), yöntemi ile çok tabakalı fonksiyonel ince filmlerin kontrol edilebilir kalınlıkta, kompozisyonda, morfolojide hazırlanması ve ilaç salımında kullanımları araştırılmıştır. Kuartz Kristal Mikrobalans-Dissipasyon (QCM-D) tekniği ile kendi kendine bir araya gelen saf/harman yapılı LbL ince filmlerin gelişimlerinin nanogram seviyesinde takibi, ilaç yükleme/salım karakterizasyonu, model ilaç ile LbL film yüzeyi arası etkileşimler ve filmlerin ilaçla etkileşimde viskoelastik değişimleri başarıyla incelenmiştir. Ayrıca, hazırlanan çok tabakalı harman fonksiyonel ince filmlerin gelişiminin takibi için UV ve QCM-D analizi gerçekleştirilerek harman film yapısındaki polielektrolit oranları tespit edilmiştir. Ek olarak, LbL saf/harman yapılı ince filmlerin kontrol edilebilir yüzey ve topografik özelliklerinin kullanılan biyobozunur ve sentetik polielektrolit çiftlerine, harman oranına ve LbL kaplama koşullarına bağlı olarak değişimlerinin incelenmesi amacıyla taramalı elektron mikroskopu (SEM) analizleri ve yüzey temas açısı çalışmaları gerçekleştirilmiştir. Hazırlanan LbL saf/harman yapılı fonksiyonel filmlerde ibuprofen sodyum ilacı için yükleme ve salım çalışmaları QCM-D tekniği ve UV-Vis analizleriyle nötral (pH:6,8), asidik (pH:2) ve bazik (pH:11) fosfat tampon çözeltisinde (PBS) gerçekleştirilmiştir. Çalışmada, ilaç salım sistemleri için yenilikçi, ekonomik ve pratik bir yaklaşımın sunulmasının yanı sıra; LbL kaplama koşullarına bağlı olarak (i) morfolojisi ve kompozisyonu kontrol edilebilen, (ii) ilaç yükleme ve salım özellikleri ayarlanabilen ve geniş bir pH (pH:2-11) aralığında ilaç salımı yapabilen sistemler geliştirilmiştir. Elde edilen sonuçlar, ilaç uygulamaları için LbL fonksiyonel filmlerin yapısına, yüzey özelliklerine, ortamın pH’ına ve ilaç-film arası etkileşimine bağlı olarak farklılıklar taşıması gerektiğini göstermiştir. LbL tekniğiyle fonksiyonel filmlerin kontrol edilebilen özelliklerde hazırlanması ve ilaç salım uygulamalarında kullanılması oldukça ümit verici sonuçlar vermiştir.

Supporting Institution

TÜBİTAK

Project Number

112M290

References

  • S. Bhusari, J. Kim, K. Polizzi, S. Sankaran, A. del Campo, Encapsulation of bacteria in bilayer Pluronic thin film hydrogels: A safe format for engineered living materials, Biomaterials Advances 145 (2023) 213240 8 pages.
  • A. Qasem, M. S. Mostafa, H. A. Yakout, M. Mahmoud, E. R. Shaaban, Determination of optical bandgap energy and optical characteristics of Cd30Se50S20 thin film at various thicknesses, Optics and Laser Technology 148 (2022) 107770 13 pages.
  • H. Yılmaz, M. Özkan, Micropollutant removal capacity and stability of aquaporin incorporated biomimetic thin-film composite membranes, Biotechnology Reports 35 (2022) e00745 12 pages.
  • G. Decher, Fuzzy nanoassemblies: Toward layered polymeric multicomposites, Science 277 (5330) (1997) 1232–1237.
  • A. E. Barberio, S. G. Smith, I. S. Pires, S. Iyer, F. Reinhardt, M. B. Melo, H. Suh, R. A. Weinberg, D. J. Irvine, P. T. Hammond, Layer-by-layer interleukin-12 nanoparticles drive a safe and effective response in ovarian tumors, Bioengineering and Translational Medicine 8 (2) (2023) e10453 12 pages.
  • J. Pickering, N. G. Lamson, M. H. Marand, W. Hwang, J. P. Straehla, P. T. Hammond, Layer-by-layer polymer functionalization improves nanoparticle penetration and glioblastoma targeting in the brain, ACS Nano 17 (2023) 24154−24169.
  • J. P. Straehla, C. Hajal, H. C. Safford, G. S. Offeddu, N. Boehnke, T. G. Dacoba, J. Wyckoff, R. D. Kamm, P. T. Hammond, B. Harley, S. Mitragotri, R. Satchi-Fainaro, A predictive microfluidic model of human glioblastoma to assess trafficking of blood-brain barrier-penetrant nanoparticles, Proceedings of the National Academy of Sciences (PNAS) 119 (23) (2022) e2118697119 12 pages.
  • D. Yilmaz-Aykut, O. Yolacan, H. Deligoz, A comparative QCM-D study for various drug sorption behaviors and chemical degradation of chitosan/PAA LbL multilayered films, Journal of Polymer Research 30 (8) (2023) Article Number 307 16 pages.
  • D. Yilmaz-Aykut, H. Deligöz, Examining layer-by-layer assembly of polyelectrolyte-drug interactions using quartz crystal microbalance with dissipation, Polymer Engineering and Science 63 (11) (2023) 3625–3638.
  • J. Hong, B. S. Kim, K. Char, P. T. Hammond, Inherent charge-shifting polyelectrolyte multilayer blends: A facile route for tunable protein release from surfaces, Biomacromolecules 12 (8) (2011) 2975–2981.
  • S. Amorim, I. Pashkuleva, C. A. Reis, R. L. Reis, R. A. Pires, Tunable layer-by-layer films containing hyaluronic acid and their interactions with CD44, Journal of Materials Chemistry B 8 (17) (2020) 3880–3885.
  • R. Lu, B. Zhao, L. Yang, S. Zheng, X. Zan, N. Li, Role of driving force on engineering layer-by-layer protein/polyphenol coating with flexible structures and properties, ACS Applied Materials and Interfaces 15 (16) (2023) 20551–20562.
  • J. T. O’Neal, E. Y. Dai, Y. Zhang, K. B. Clark, K. G. Wilcox, I. M. George, N. E. Ramasamy, D. Enriquez, P. Batys, M. Sammalkorpi, J. L. Lutkenhaus, QCM-D investigation of swelling behavior of layer-by-layer thin films upon exposure to monovalent ions, Langmuir 34 (3) (2018) 999–1009.
  • Z. Dong, C. Liang, J. Zhao, Quartz crystal microbalance with dissipation (QCM-D) as a way to study adsorption and adsorbed layer characteristics of hemicelluloses and other macromolecules on thin cellulose films: A review, BioResources 18 (2) (2023) 1–19.
  • X. Huang, Q. Chen, W. Pan, Y. Yao, Advances in the mass sensitivity distribution of quartz crystal microbalances: A review, Sensors 22 (14) (2022) 5112 20 pages.
  • H. Deligöz, B. Tieke, QCM-D study of layer-by-layer assembly of polyelectrolyte blend films and their drug loading-release behavior, Colloids and Surfaces A: Physicochemical and Engineering Aspects 441 (2014) 725–736.
  • Szilagyi, G. Trefalt, A. Tiraferri, P. Maroni, M. Borkovec, Polyelectrolyte adsorption, interparticle forces, and colloidal aggregation, Soft Matter 10 (15) (2014) 2479–2502.
  • E. Konyalı, H. Y. Cengiz, A. Müftüler, H. Deligöz, Monitoring the salt stability and solvent swelling behavior of PAH-based polyelectrolyte multilayers by quartz crystal microbalance with dissipation, Polymer Engineering and Science 63 (10) (2023) 3328–3342.
  • M. Anwar, F. Pervaiz, H. Shoukat, S. Noreen, K. Shabbir, A. Majeed, S. Ijaz, Formulation and evaluation of interpenetrating network of xanthan gum and polyvinylpyrrolidone as a hydrophilic matrix for controlled drug delivery system, Polymer Bulletin 78 (1) (2021) 59–80.
  • Y. Jang, B. Akgun, H. Kim, S. Satija, K. Char, Controlled release from model blend multilayer films containing mixtures of strong and weak polyelectrolytes, Macromolecules 45 (8) (2012) 3542–3549.
  • A. Ghiorghita, F. Bucatariu, E. S. Dragan, Influence of cross-linking in loading/release applications of polyelectrolyte multilayer assemblies. A review, Materials Science and Engineering C 105 (2019) 110050 20 pages.
  • H. Zhang, L. Yu, L. Han, X. Liu, S. Ruan, J. Hu, Fast modulation of surface amphiphobicity/amphiphilicity via bidirectional substitution between perfluorinated surfactants and polyanions throughout pre-assembled polyelectrolyte multilayers, Langmuir 35 (52) (2019) 17122–17131.
  • H. Y. Cengiz, E. Konyali, A. Müftüler, H. Deligöz, Investigating the effect of weak polyelectrolytes on the chemical stability and swelling recovery of multilayered coatings, Progress in Organic Coatings 183 (2023) 107775 10 pages.
  • C. Li, J. Zhang, J. Han, B. Yao, A numerical solution to the effects of surface roughness on water–coal contact angle, Scientific Reports 11 (1) (2021) Article Number 459 12 pages.
  • A. Quinn, E. Tjipto, A. Yu, T. R. Gengenbach, F. Caruso, Polyelectrolyte blend multilayer films: Surface morphology, wettability, and protein adsorption characteristics, Langmuir 23 (9) (2007) 4944–4949.
  • W. Zhang, Q. Zhao, J. Yuan, Poröse polyelektrolyte: Zusammenspiel zwischen Poren und Ladung für neue funktionen, Angewandte Chemie 130 (23) (2018) 6868–6889.
There are 26 citations in total.

Details

Primary Language Turkish
Subjects Polymer Science and Technologies
Journal Section Research Article
Authors

Dilara Yılmaz Aykut 0000-0002-2287-2585

Öznur Yolaçan 0000-0001-6931-7979

Hüseyin Deligöz 0000-0002-0915-2911

Project Number 112M290
Early Pub Date March 15, 2024
Publication Date March 15, 2024
Submission Date December 20, 2023
Acceptance Date January 20, 2024
Published in Issue Year 2024 Volume: 10 Issue: 1

Cite

APA Yılmaz Aykut, D., Yolaçan, Ö., & Deligöz, H. (2024). Polielektrolitlerin Molekül Ağırlığı ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi. Journal of Advanced Research in Natural and Applied Sciences, 10(1), 190-206. https://doi.org/10.28979/jarnas.1407665
AMA Yılmaz Aykut D, Yolaçan Ö, Deligöz H. Polielektrolitlerin Molekül Ağırlığı ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi. JARNAS. March 2024;10(1):190-206. doi:10.28979/jarnas.1407665
Chicago Yılmaz Aykut, Dilara, Öznur Yolaçan, and Hüseyin Deligöz. “Polielektrolitlerin Molekül Ağırlığı Ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin Ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi”. Journal of Advanced Research in Natural and Applied Sciences 10, no. 1 (March 2024): 190-206. https://doi.org/10.28979/jarnas.1407665.
EndNote Yılmaz Aykut D, Yolaçan Ö, Deligöz H (March 1, 2024) Polielektrolitlerin Molekül Ağırlığı ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi. Journal of Advanced Research in Natural and Applied Sciences 10 1 190–206.
IEEE D. Yılmaz Aykut, Ö. Yolaçan, and H. Deligöz, “Polielektrolitlerin Molekül Ağırlığı ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi”, JARNAS, vol. 10, no. 1, pp. 190–206, 2024, doi: 10.28979/jarnas.1407665.
ISNAD Yılmaz Aykut, Dilara et al. “Polielektrolitlerin Molekül Ağırlığı Ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin Ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi”. Journal of Advanced Research in Natural and Applied Sciences 10/1 (March 2024), 190-206. https://doi.org/10.28979/jarnas.1407665.
JAMA Yılmaz Aykut D, Yolaçan Ö, Deligöz H. Polielektrolitlerin Molekül Ağırlığı ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi. JARNAS. 2024;10:190–206.
MLA Yılmaz Aykut, Dilara et al. “Polielektrolitlerin Molekül Ağırlığı Ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin Ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi”. Journal of Advanced Research in Natural and Applied Sciences, vol. 10, no. 1, 2024, pp. 190-06, doi:10.28979/jarnas.1407665.
Vancouver Yılmaz Aykut D, Yolaçan Ö, Deligöz H. Polielektrolitlerin Molekül Ağırlığı ve Harman Oranının Çok Tabakalı Filmlerin Gelişimine Etkisinin ve İlaç Adsorpsiyon/Desorpsiyon Uygulamalarında Kullanımlarının QCM-D Tekniğiyle Takibi. JARNAS. 2024;10(1):190-206.


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