Abstract
Recent work regarding the Layer by Layer (LbL) engineering of poly(lactide-co-glycolide) nanoparticles (PLGA NPs) is reviewed here. The LbL engineering of PLGA NPs is applied as a means of generating advanced drug delivery devices with tailored recognition, protection, cargo and release properties. LbL in combination with covalent chemistry is used to attach PEG and folic acid to control cell uptake and direct it towards cancer cells. LbL coatings composed of chitosan and alginate show low protein interactions and can be used as an alternative to Pegylation. The assembly on top of LbL coatings of lipid layers composed of variable percentages of 1,2-dioleoyl-sn-glycero-3-choline (DOPC) and 1,2-dioleoyl-sn-glycero-3-phospho-l-serine (DOPS) increases NP uptake and directs the NPs towards the endoplasmic reticulum. The antibody anti-TNF-α is encapsulated forming a complex with alginate that is assembled LbL on top of PLGA NPs. The antibody is released in cell culture following first order kinetics. The release kinetics of encapsulated molecules inside PLGA NPs are studied when the PLGA NPs are coated via LbL with different polyelectrolytes. The intracellular release of encapsulated Doxorubicin is studied in the HepG2 cell line by means of Fluorescence Lifetime Imaging.
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References
Hans ML, Lowman AM. Biodegradable nanoparticles for drug delivery and targeting. Curr Opin Solid State Mater Sci, 2002, 6: 319–327
Langer R. New methods of drug delivery. Science, 1990, 249: 1527–1533
Uhrich KE, Cannizzaro SM, Langer RS, Shakesheff KM. Polymeric systems for controlled drug release. Chem Rev, 1999, 99: 3181–3198
Ishihara T, Mizushima T. Techniques for efficient entrapment of pharmaceuticals in biodegradable solid micro/nanoparticles. Exp Opin Drug Deliv, 2010, 7: 565–575
Patil YB, Swaminathan SK, Sadhukha T, Ma L, Panyam J. The use of nanoparticle-mediated targeted gene silencing and drug delivery to overcome tumor drug resistance. Biomaterials, 2010, 31: 358–365
Yuan XD, Rathinavelu A, Hao JS, Narasimhan M, He M, Heitlage V, Tam L, Viqar S, Salehi M, Li L. siRNA drug delivery by biodegradable polymeric nanoparticles. J Nanosci Nanotech, 2006, 6: 2821–2828
Hirsjärvi S, Peltonen L, Hirvonen J. Layer-by-layer polyelectrolyte coating of low molecular weight poly(lactic acid) nanoparticles. Colloids Surf B, 2006, 49: 93–99
Yang Y, Yueh-Hen Hsu P. The effect of poly(d,l-lactide-co-glycolide) microparticles with polyelectrolyte self-assembled multilayer surfaces on the cross-presentation of exogenous antigens. Biomaterials, 2008, 29: 2516–2526
Yu D, Zhang Y, Zhou X, Mao Z, Gao C. Influence of surface coating of PLGA particles on the internalization and functions of human endothelial cells. Biomacromolcules, 2012, 13: 3272–3282
Cohen H, Gao J, Fishbein I, Kousaev V, Sosnowski S, Slomkowski S, Golomb G. Levy RJ. Sustained delivery and expression of DNA encapsulated in polymeric nanoparticles. Gene Therapy, 2000, 7: 1896–1905
Allémann E, Leroux JC, Gurny R, Doelker E. In vitro extended-release properties of drug-loaded poly(dl-lactic acid) nanoparticles produced by a salting-out procedure. Pharm Res, 1993, 10: 1732–1737
Zambaux MF, Bonneaux F, Gref R, Maincent P, Dellacherie E, Alonso MJ, Labrude P, Vigneron C. Influence of experimental parameters on the characteristics of poly(lactic acid) nanoparticles prepared by a double emulsion method. J Controlled Release, 1998, 50: 31–40
Crotts G, Sah H, Park TG. Adsorption determines in-vitro protein release rate from biodegradable microspheres: Quantitative analysis of surface area during degradation. J Controlled Release, 1997, 47: 101–111
Panyam J, Labhasetwar V. Biodegradable nanoparticles for drug and gene delivery to cells and tissue. Adv Drug Deliv Rev, 2003, 55: 329–347
Scholes PD, Coombes AGA, Illum L, Davis SS, Vert M, Davies MC. The preparation of sub-200 nm poly(lactide-co-glycolide) microspheres for site-specific drug delivery. J Controlled Release, 1993, 25: 145–153
Weiss B, Schneider M, Muys L, Taetz S, Neumann D, Schaefer UF, Lehr CM. Coupling of biotin-(poly(ethylene glycol))amine to poly(d,l-lactide-co-glycolide) nanoparticles for versatile surface modification. Bioconjugate Chem, 2007, 18: 1087–1094
Mundargi RC, Babu VR, Rangaswamy V, Patel P, Aminabhavi TM. Nano/micro technologies for delivering macromolecular Ttherapeutics using poly(d,l-lactide-co-glycolide) and its derivatives. J Controlled Release, 2008, 125: 193–209
Bala I, Hariharan S, Kumar MNVR. PLGA nanoparticles in drug delivery: The state of the art. Crit Rev Ther Drug, 2004, 21: 387–422
Yang YY, Chia HH, Chung TS. Effect of preparation temperature on the characteristics and release profiles of PLGA microspheres containing protein fabricated by double-emulsion solvent extraction/evaporation method. J Controlled Release, 2000, 69: 81–96
Hornig S, Heinze T, Becer CR, Schubert US. Synthetic polymeric nanoparticles by nanoprecipitation. J Mater Chem, 2009, 19: 3838–3840
Bilati U, Allémann E, Doelker E. Development of a nanoprecipitation method intended for the entrapment of hydrophilic drugs into nanoparticles. Eur J Pharm Sci, 2005, 24: 67–75
Jensen DMK, Cun D, Maltesen MJ, Frokjaer S, Nielsen HM, Foged C. Spray drying of siRNA-containing PLGA nanoparticles intended for inhalation. J Controlled Release, 2010, 142: 138–145
Fessi H, Piusieux F, Devissaguet JP, Ammoury N, Benita S. Nanocapsule formation by interfacial polymer deposition following solvent displacement. Int J Pharm, 1989, 55: R1–R4
O’Donnell PB, McGinity JW. Preparation of microspheres by the solvent evaporation technique. Adv Drug Deliv Rev, 1997, 28: 25–42
Zambaux MF, Bonneaux F, Gref R, Dellacherie E, Vigneron C. Preparation and characterization of protein c-loaded PLA nanoparticles. J Controlled Release, 1999, 60: 179–188
Doiron AL, Homan KA, Emelianov S, Brannon-Peppas L. Poly(lactic-co-glycolic) acid as a carrier for imaging contrast agents. Pharm Res, 2009, 26: 674–682
Decher G, Hong JD, Schmitt J. Buildup of ultrathin multilayer films by a self-assembly process: III. Consecutively alternating adsorption of anionic and cationic polyelectrolytes on charged surfaces. Thin Solid Films, 1992, 210–211: 831–835
Decher G. Fuzzy nanoassemblies: toward layered polymeric multicomposites. Science, 1997, 277: 1232–1237
Sukhorukov GB, Donath E, Lichtenfeld H, Knippel E, Knippel M, Budde A Möhwald H. Layer-by-layer self assembly of polyelectrolytes on colloidal particles. Colloid Surf A-Physicochem Eng Asp, 1998, 137: 253–266
Dubas ST, Schlenoff JB. Factors controlling the growth of polyelectrolyte multilayers. Macromolecules, 1999, 32: 8153–8160
Donath E, Sukhorukov GB, Caruso F, Davis SA, Möhwald H. Novel hollow polymer shells by colloid-templated assembly of polyelectrolytes. Angew Chem Int Edi, 1998, 37: 2202–2205
Donath E, Moya S, Neu B, Sukhorukov GB, Georgieva R, Voigt A, Baumler H, Kiesewetter H, Mohwald H. Hollow polymer shells from biological templates: fabrication and potential applications. Chem-A Euro J, 2002, 8: 5481–5485
Wang B, Zhang Y, Mao Z, Gao C. Cellular uptake of covalent poly(allylamine hydrochloride) microcapsules and its influences on cell functions. Macromol biosci, 2012, 12: 1534–45
Kiryukhin MV, Gorelik SR, Man SM, Subramanian GS, Antipina MN, Low HY, Sukhorukov GB. Individually addressable patterned multilayer microchambers for site-specific release-on-demand. Macromol rapid commun, 2013, 34: 87–93
Zhou J, Romero G, Rojas E, Moya S, Ma L, Gao C. Folic acid modified poly(lactide-co-glycolide) nanoparticles, layer-by-layer surface engineered for targeted delivery. Macromol Chem Phys, 2010, 211: 404–411
Zhou J, Ma L, Gao C, Shen J, Moya S. Polyelectrolyte coated PLGA nanoparticles: templation and release behavior. Macromol Biosci, 2009, 9: 326–335
Zhou J, Romero G, Rojas E, Ma L, Moya S, Gao C. Layer by layer chitosan/alginate coatings on poly(lactide-co-glycolide) nanoparticles for antifouling protection and folic acid binding to achieve selective cell targeting. J colloid interf sci, 2010, 345: 241–247
Romero G, Sanz DJ, Qiu Y, Yu D Mao Z, Gao C, Moya S. E. Lipid layer engineering of poly(lactide-co-glycolide) nanoparticles to control their uptake and intracellular co-localisation. J Mater Chem B, 2013, 1: 2252–2259
Moya S, Donath E, Sukhorukov GB, Auch M, Baumler H, Lichtenfeld H, Mohwald H. Lipid coating on polyelectrolyte surface modified colloidal particles and polyelectrolyte capsules. Macromolecules, 2000, 33: 4538–4544
Fischlechner M, Zaulig M, Meyer S, Estrela-Lopis I, Cuéllar L, Irigoyen J, Pescador P, Brumen M, Messner P, Moya S. Lipid layers on polyelectrolyte multilayer supports. Soft Matter, 2008, 4: 2245–2258
Romero G, Zhou J, Rojas E, Franco A, Sanchez Espinal C, González Fernández A, Gao C, Donath E, Moya S, Estrela-Lopis I. Surface engineered poly(lactide-co-glycolide) nanoparticles for intracellular delivery: Uptake and cytotoxicity-A confocal raman microscopic study. Biomacromolecules, 2010, 11: 2993–2999
Kempeni J. Preliminary results of early clinical trials with the fully human anti-TNF monoclonal antibody. Ann Rheum Dis, 1999, 58(suppl I): 70–73
Zhou J, Moya S, Ma L, Gao C, Shen J. Polyelectrolyte coated PLGA nanoparticles: templation and release behavior. Macromol biosci, 2009, 9: 326–35
Siepmann J, Faisant N, Akiki J, Richard J, Benoit JP. Effect of the size of biodegradable microparticles on drug release: Experiment and theory. J Controlled Release, 2004, 96: 123–134
Aso Y, Yoshioka S, Li Wan Po A, Terao T. Effect of temperature on mechanisms of drug release and matrix degradation of poly (d,l-lactide) microspheres. J Controlled Release, 1994, 31: 33–39
Dai X, Yue Z, Eccleston ME, Swartling J, Slater NKH, Kaminski CF. Fluorescence intensity and lifetime imaging of free and micellar-encapsulated doxorubicin in living cells. Nanomed nanotech bio med, 2008, 4: 49–56
Romero G, Qiu Y, Murray RA, Moya S. Study of intracellular delivery of doxorubicin from poly(lactide-co-glycolide) nanoparticles by means of fluorescence lifetime imaging and confocal raman microscopy. Macromol biosci, 2013, 13: 234–241
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Recommended by Prof. GAO Changyou (Zhejiang University)
MOYA Sergio E. (left) studied chemistry at the National University of the South, Argentina and received his Ph.D. in Physical Chemistry from the University of Potsdam, Germany, working at the Max Planck Institute of Colloids and Interfaces. After post doctoral stages at the College de France, Paris, and at the University of Cambridge, UK, he worked for a year and a half at CIQA, Mexico as an independent researcher. After that he joined the Cooperative Centre of Biomaterials in San Sebastian, Spain, as a research group leader. He is also a visiting professor at Zhejiang University, China. His research interests focus on physical chemistry at the nanoscale, soft matter nanotechnology, polyelectrolytes, nanomedicine and nanotoxicology. He is the author of around 75 articles in material science, chemistry, and polymer science.
ROMERO Gabriela (right) received her B.S. in Chemical Engineering from the Autonomous University of San Luis Potosí, Mexico, in 2007. She joined the group of Dr. MOYA at CIC biomaGUNE in 2008 and under her supervision she received a Masters degree in Advanced Materials Engineering from the University of the Basque Country, Spain, in 2009. In the same group she carried out her doctorate studies and she received her Ph.D. degree in Applied Chemistry and Polymer Science from the University of the Basque Country, Spain, in 2012. In October 2012 she joined the group of Dr. Brad Berron as a postdoctoral research associate from the University of Colorado and the University of Kentucky in the USA.
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Romero, G., Murray, R.A., Qiu, Y. et al. Layer by layer surface engineering of poly (lactide-co-glycolide) nanoparticles: A versatile tool for nanoparticle engineering for targeted drug delivery. Sci. China Chem. 56, 1029–1039 (2013). https://doi.org/10.1007/s11426-013-4891-z
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DOI: https://doi.org/10.1007/s11426-013-4891-z