Abstract
Polyelectrolyte complexes formed with polysaccharides have generated much interest among researchers because of their excellent performances and mild process. In this work, using calcium alginate/sodium cellulose sulfate [CA/NaCS] as template, [CA/NaCS–CHC] n microcapsules with one, two and three outer layers were self-assembled with NaCS and chitosan hydrochloride (CHC). PEC layer assembly on the [CA/NaCS] cores was achieved, which could be observed from the FITC-labeled [CA/NaCS–CHC] n microcapsules. The first and second PEC layer assemblies were available to help slow the drug loss, and the [CA/NaCS–CHC]2 microcapsules had a maximum drug-loading and encapsulation efficiency of 38.14 ± 4.04 and 64.72 ± 6.86%, respectively. Ritger-Peppas model analysis showed the drug release occurred under the mechanism of Fickian diffusion for the [CA/NaCS] cores, anomalous (non-Fickian) transport for the [CA/NaCS–CHC]1 and [CA/NaCS–CHC]2 microcapsules and case-II transport for the [CA/NaCS–CHC]3 microcapsules. The prepared microcapsules could be used as vehicles for sustained drug release.
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References
And STD, Schlenoff JB (1999) Factors controlling the growth of polyelectrolyte multilayers. Macromolecules 219:U532
Araya-Hermosilla E, Muñoz D, Orellana S, Yáñez A, Olea AF, Oyarzun-Ampuero F, Moreno-Villoslada I (2014) Immobilization of rhodamine 6G in calcium alginate microcapsules based on aromatic–aromatic interactions with poly(sodium 4-styrenesulfonate). React Funct Polym 81:14–21
Arnon H, Granit R, Porat R, Poverenov E (2015) Development of polysaccharides-based edible coatings for citrus fruits: a layer-by-layer approach. Food Chem 166:465–472
Bertr P, Jonas A, Laschewsky A, Legras R (2000) Ultrathin polymer coatings by complexation of polyelectrolytes at interfaces: Suitable materials, structure and properties. Macromol Rapid Commun 21:319–348
Borges J, Mano JF (2014) Molecular interactions driving the layer-by-layer assembly of multilayers. Chem Rev 114:8883–8942
Chambin O, Dupuis G, Champion D, Voilley A, Pourcelot Y (2006) Colon-specific drug delivery: influence of solution reticulation properties upon pectin beads performance. Int J Pharm 321:86–93
Cheng HC, Chang CY, Hsieh FI, Yeh JJ, Chien MY, Pan RN, Deng MC, Liu DZ (2011) Effects of tremella–alginate–liposome encapsulation on oral delivery of inactivated H5N3 vaccine. J Microencapsul 28:55–61
Choi D, Hong J (2014) Layer-by-layer assembly of multilayer films for controlled drug release. Arch Pharm Res 37:79–87
Chou H, Chiu S, Hu T (2015) LbL assembly of albumin on nitric oxide-releasing silica nanoparticles using suramin, a polyanion drug, as an inter layer linker. Biomacromolecules 16:2288–2295
Dam HH, Caruso F (2013) Formation and degradation of layer-by-layer-assembled polyelectrolyte polyrotaxane capsules. Langmuir 29:7203–7208
Das S, Ng KY, Ho PC (2010) Formulation and optimization of zinc-pectinate beads for the controlled delivery of resveratrol. AAPS PharmSciTech 11:729–742
De Villiers MM, Otto DP, Strydom SJ, Lvov YM (2011) Introduction to nanocoatings produced by layer-by-layer (LbL) self-assembly. Adv Drug Deliv Rev 63:701–715
Decher G (1997) Fuzzy nanoassemblies: toward layered polymeric multicomposites. Science 277:1232–1237
Deepthi S, Sundaram MN, Kadavan JD, Jayakumar R (2016) Layered chitosan-collagen hydrogel/aligned PLLA nanofiber construct for flexor tendon regeneration. Carbohydr Polym 153:492–500
Deshmukh PK, Ramani KP, Singh SS, Tekade AR, Chatap VK, Patil GB, Bari SB (2013) Stimuli-sensitive layer-by-layer (LbL) self-assembly systems: targeting and biosensory applications. J Control Release 166:294–306
Fang L, Wang P, Wen X, Guo X, Luo L, Yu J, Guo X (2017) Layer-by-layer self-assembly of gold nanoparticles/thiols beta-cyclodextrin coating as the stationary phase for enhanced chiral differentiation in open tubular capillary electrochromatography. Talanta 167:158–165
Gunbas ID, Sezer UA, Iz SG, Gurhan ID, Hasirci N (2012) Semi-IPN chitosan/PEG microspheres and films for biomedical applications: characterization and sustained release optimization. Ind Eng Chem Res 51:11946–11954
Han U, Seo Y, Hong J (2016) Effect of pH on the structure and drug release profiles of layer-by-layer assembled films containing polyelectrolyte, micelles, and graphene oxide. Sci Rep 6:1–10
Lacerda L, Parize AL, Favere V, Laranjeira M, Stulzer HK (2014) Development and evaluation of pH-sensitive sodium alginate/chitosan microparticles containing the antituberculosis drug rifampicin. Mater Sci Eng C Mater 39:161–167
Li W, Li XY, Chen Y, Li XX, Deng HB, Wang T, Huang R, Fan G (2013) Poly(vinyl alcohol)/sodium alginate/layered silicate based nanofibrous mats for bacterial inhibition. Carbohydr Polym 92:2232–2238
Li X, Hu D, Cao L, Yang C (2015) Sensitivity of coalescence separation of oil-water emulsions using stainless steel felt enabled by LBL self-assembly and CVD. RSC Adv 5:71345–71354
Liu WL, Liu JH, Liu W, Li T, Liu CM (2013) Improved physical and in vitro digestion stability of a polyelectrolyte delivery system based on layer-by-layer self-assembly alginate–chitosan-coated nanoliposomes. J Agric Food Chem 61:4133–4144
Liu MX, Zheng HJ, Chen J, Li SL, Huang JF, Zhou CR (2016) Chitosan-chitin nanocrystal composite scaffolds for tissue engineering. Carbohydr Polym 152:832–840
Luo Y, Wang Q (2014) Recent development of chitosan-based polyelectrolyte complexes with natural polysaccharides for drug delivery. Int J Biol Macromol 64:353–367
Mazeau K, Rinaudo M (2012) Comparative properties of hyaluronan and chitosan in aqueous environment. Polym Sci Ser C 54:96–107
Michel M, Vautier D, Voegel JC, Schaaf P, Ball V (2004) Layer by layer self-assembled polyelectrolyte multilayers with embedded phospholipid vesicles. Langmuir 20:4835–4839
Mohanta V, Madras G, Patil S (2013) Albumin-mediated incorporation of water-insoluble therapeutics in layer-by-layer assembled thin films and microcapsules. J Mater Chem B 1:4819–4827
Moussa SH, Tayel AA, Al-Turki AI (2013) Evaluation of fungal chitosan as a biocontrol and antibacterial agent using fluorescence-labeling. Int J Biol Macromol 54:204–208
Mura C, Nacher A, Merino V, Merino-Sanjuan M, Manconi M, Loy G, Fadda AM, Diez-Sales O (2012) Design, characterization and in vitro evaluation of 5-aminosalicylic acid loaded N-succinyl-chitosan microparticles for colon specific delivery. Colloid Surf B 94:199–205
Peng XH, Zhang L (2005) Surface fabrication of hollow microspheres from N-methylated chitosan cross-linked with gultaraldehyde. Langmuir 21:1091–1095
Qin S, Zhang A, Cheng S, Rong L, Zhang X (2017) Drug self-delivery systems for cancer therapy. Biomaterials 112:234–247
Rajitha P, Gopinath D, Biswas R, Sabitha M, Jayakumar R (2016) Chitosan nanoparticles in drug therapy of infectious and inflammatory diseases. Expert Opin Drug Deliv 13:1177–1194
Ramos J, Stahl S, Richter RP, Moya SE (2010) Water content and buildup of poly(diallyldimethylammonium chloride)/poly(sodium 4-styrenesulfonate) and poly(allylamine hydrochloride)/poly(sodium 4-styrenesulfonate) polyelectrolyte multilayers studied by an in situ combination of a quartz crystal microbalance with dissipation monitoring and spectroscopic ellipsometry. Macromolecules 43:9063–9070
Ran JB, Xie LJ, Sun GL, Hu JX, Chen S, Jiang P, Shen XY, Tong H (2016) A facile method for the preparation of chitosan-based scaffolds with anisotropic pores for tissue engineering applications. Carbohydr Polym 152:615–623
Ritger PL, Peppas NA (1987) A simple equation for description of solute release I. Fickian and non-Fickian release from non-swellable devices in the form of slabs, spheres, cylinders or discs. J Control Release 5:37–42
Sato K, Takahashi S, Anzai J (2012) Layer-by-layer thin films and microcapsules for biosensors and controlled release. Anal Sci 28:929–938
Schönhoff M (2003) Layered polyelectrolyte complexes: physics of formation and molecular properties. J Phys Condens Matter 15:R1781–R1808
Shen L, Cui X, Yu G, Li F, Li L, Feng S, Lin H, Chen J (2017) Thermodynamic assessment of adsorptive fouling with the membranes modified via layer-by-layer self-assembly technique. J Colloid Interface Sci 494:194–203
Song Y, Zhang DM, Lv Y, Guo X, Lou RY, Wang SJ, Wang XL, Yu WT, Ma XJ (2016) Microfabrication of a tunable collagen/alginate–chitosan hydrogel membrane for controlling cell-cell interactions. Carbohydr Polym 153:652–662
Starr BJ, Tarabara VV, Herrera-Robledo M, Zhou M, Roualdes S, Ayral A (2016) Coating porous membranes with a photocatalyst: comparison of LbL self-assembly and plasma-enhanced CVD techniques. J Membr Sci 514:340–349
Stiegler P, Sereinigg M, Haimel G, Zeugswetter F, Dupre G, Iberer F, Witter K, Stadlbauer-Koellner V (2014) Biocompatibility of sodium cellulose sulfate (SCS) microencapsulated porcine islet cells in five beagle dogs. Am J Transpl 143:419
Terada T, Tagami M, Ohtsubo T, Iwao Y, Noguchi S, Itai S (2016) Sustained-release microsphere formulation containing an agrochemical by polyurethane polymerization during an agitation granulation process. Int J Pharm 509:328–337
Tian C, Zhang C, Wu H, Song Y, Shi J, Wang X, Song X, Yang C, Jiang Z (2014) Merging of covalent cross-linking and biomimetic mineralization into an LBL self-assembly process for the construction of robust organic-inorganic hybrid microcapsules. J Mater Chem B 2:4346–4355
Wang MJ, Xie YL, Zheng QD, Yao SJ (2009) A novel, potential microflora-activated carrier for a colon-specific drug delivery system and its characteristics. Ind Eng Chem Res 48:5276–5284
Wang P, Zhang AX, Jin Y, Zhang Q, Zhang LY, Peng Y, Du SH (2014) Molecularly imprinted layer-coated hollow polysaccharide microcapsules toward gate-controlled release of water-soluble drugs. RSC Adv 4:26063–26073
Wischke C, Borchert HH (2006) Fluorescein isothiocyanate labelled bovine serum albumin (FITC-BSA) as a model protein drug: opportunities and drawbacks. Pharmazie 61:770–774
Wood KC, Boedicker JQ, Lynn DM, Hammond PT (2005) Tunable drug release from hydrolytically degradable layer-by-layer thin films. Langmuir 21:1603–1609
Wu QX, Yao SJ (2013) Novel NaCS-CS-PPS microcapsules as a potential enzyme-triggered release carrier for highly-loading 5-ASA. Colloid Surf B. 109:147–153
Wu QX, Zhang QL, Lin DQ, Yao SJ (2013) Characterization of novel lactoferrin loaded capsules prepared with polyelectrolyte complexes. Int J Pharm 455:124–131
Wu QX, Li MZ, Yao SJ (2014a) Performances of NaCS–WSC protein drug microcapsules with different degree of substitution of NaCS using sodium polyphosphate as cross-linking agent. Cellulose 21:1897–1908
Wu QX, Lin DQ, Yao SJ (2014b) Design of chitosan and its water soluble derivatives-based drug carriers with polyelectrolyte complexes. Mar Drugs 12:6236–6253
Wu H, Guo LX, Zhang JL, Miao SL, He CY, Wang B, Wu YQ, Chen ZM (2016a) Polyelectrolyte-free layer by layer self-assembled multilayer films of cationic phthalocyanine cobalt(II) and carbon nanotube for the efficient detection of 4-nitrophenol. Sens Actuator B Chem 230:359–366
Wu QX, Lin DQ, Yao SJ (2016b) Fabrication and formation studies on single-walled CA/NaCS–WSC microcapsules. Mater Sci Eng C Mater 59:909–915
Wu QX, Xu X, Wang ZL, Yao SJ, Tong WY, Chen Y (2016c) Effect of the cross-linking agent on performances of NaCS-CS/WSC microcapsules. Colloid Surf B 147:416–421
Wu QX, Xu X, Xie Q, Tong WY, Chen Y (2016d) Evaluation of chitosan hydrochloride-alginate as enteric micro-probiotic-carrier with dual protective barriers. Int J Biol Macromol 93:665–671
Yao SJ (2000) An improved process for the preparation of sodium cellulose sulphate. Chem Eng J 78:199–204
Yilmaz MD (2016) Layer-by-layer hyaluronic acid/chitosan polyelectrolyte coated mesoporous silica nanoparticles as pH-responsive nanocontainers for optical bleaching of cellulose fabrics. Carbohydr Polym 146:174–180
Yuan W, Ji J, Fu J, Shen J (2008) A facile method to construct hybrid multilayered films as a strong and multifunctional antibacterial coating. J Biomed Mater Res B 85:556–563
Zakharova LY, Ibragimova AR, Vasilieva EA, Mirgorodskaya AB, Yackevich EI, Nizameev IR, Kadirov MK, Zuev YF, Konovalov AI (2012) Polyelectrolyte capsules with tunable shell behavior fabricated by the simple layer-by-layer technique for the control of the release and reactivity of small guests. J Phys Chem C 116:18865–18872
Zhang QL, Wu QX, Lin DQ, Yao SJ (2013) Effect and mechanism of sodium chloride on the formation of chitosan–cellulose sulfate–tripolyphosphate crosslinked beads. Soft Matter 9:10354–10363
Zhao JM, Wang XP, Kuang YS, Zhang YF, Shi XW, Liu XY, Deng HB (2014) Multilayer composite beads constructed via layer-by-layer self-assembly for lysozyme controlled release. RSC Adv 4:24369–24376
Zheng GS, Liu XD, Wang XL, Chen L, Xie HG, Wang F, Zheng HZ, Yu WT, Ma XJ (2014) Improving stability and biocompatibility of alginate/chitosan microcapsule by fabricating bi-functional membrane. Macromol Biosci 14:655–666
Zhou GC, Lu Y, Zhang H, Chen Y, Yu Y, Gao J, Sun DX, Zhang GQ, Zou H, Zhong YQ (2013) A novel pulsed drug-delivery system: polyelectrolyte layer-by-layer coating of chitosan–alginate microgels. Int J Nanomed 8:877–887
Zhu LY, Yan XQ, Zhang HM, Yao SJ, Jiang L (2015) Novel double-walled microspheres based on chitosan, sodium cellulose sulfate and sodium tripolyphosphate: preparation, characterization and in vitro release study. Korean J Chem Eng 32:369–372
Acknowledgments
This work was supported by the National Natural Science Foundation of China (21606002), Natural Science Foundation of Anhui Province (CN) (1708085QC64), Postdoctoral Science Foundation of China (2017M611998), Doctoral Research Start-up Fund of Anhui University (J01001319) and Undergraduate Research Training Programs for Innovation (KYXL2017036, 201710357034, 201710357268).
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Wu, QX., Wang, DD., Su, T. et al. Self-assembly of polyelectrolyte complexes microcapsules with natural polysaccharides for sustained drug release. Cellulose 24, 4949–4962 (2017). https://doi.org/10.1007/s10570-017-1454-z
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DOI: https://doi.org/10.1007/s10570-017-1454-z