Modification of Spherical Polyelectrolyte Brushes by Layer-by-Layer Self-Assembly as Observed by Small Angle X-ray Scattering

Multilayer modified spherical polyelectrolyte brushes were prepared through alternate deposition of positively charged poly(allylamine hydrochloride) (PAH) and negatively charged poly-l-aspartic acid (PAsp) onto negatively charged spherical poly(acrylic acid) (PAA) brushes (SPBs) on a poly(styrene) core. The charge reversal determined by the zeta potential indicated the success of layer-by-layer (LBL) deposition. The change of the structure during the construction of multilayer modified SPBs was observed by small-angle X-ray scattering (SAXS). SAXS results indicated that some PAH chains were able to penetrate into the PAA brush for the PAA-PAH double-layer modified SPBs whereas part of the PAH moved towards the outer layer when the PAsp layer was loaded to form a PAA-PAH-PAsp triple-layer system. The multilayer modified SPBs were stable upon changing the pH (5 to 9) and ionic strength (1 to 100 mM). The triple-layer modified SPBs were more tolerated to high pH (even at 11) compared to the double-layer ones. SAXS is proved to be a powerful tool for studying the inner structure of multilayer modified SPBs, which can establish guidelines for the a range of potential applications of multilayer modified SPBs.

[1]  Xuhong Guo,et al.  Interactions among spherical poly(acrylic acid) brushes: Observation by rheology and small angle X‐ray scattering , 2016 .

[2]  B. Liu,et al.  Efficient blue organic light-emitting devices based on solution-processed starburst macromolecular electron injection layer , 2016 .

[3]  N. Zacharia,et al.  Functional polyelectrolyte multilayer assemblies for surfaces with controlled wetting behavior , 2015 .

[4]  P. Hartley,et al.  Controlling the Mesostructure Formation within the Shell of Novel Cubic/Hexagonal Phase Cetyltrimethylammonium Bromide-Poly(acrylamide-acrylic acid) Capsules for pH Stimulated Release. , 2015, ACS applied materials & interfaces.

[5]  V. Chiono,et al.  Layer-by-layer assembly for biomedical applications in the last decade , 2015, Nanotechnology.

[6]  Min Feng,et al.  Nanocarriers with tunable surface properties to unblock bottlenecks in systemic drug and gene delivery. , 2015, Journal of controlled release : official journal of the Controlled Release Society.

[7]  Jian-jun Wang,et al.  Preparation of Au/Ag multilayers via layer-by-layer self-assembly in spherical polyelectrolyte brushes and their catalytic activity , 2015, Chinese Journal of Polymer Science.

[8]  Bing Xia,et al.  Accounting for observed small angle X‐ray scattering profile in the protein–protein docking server cluspro , 2015, J. Comput. Chem..

[9]  Kentaro Yoshida,et al.  pH-Dependent Release of Insulin from Layer-by-Layer-Deposited Polyelectrolyte Microcapsules , 2015 .

[10]  Xuhong Guo,et al.  Tunable immobilization of protein in anionic spherical polyelectrolyte brushes as observed by small-angle X-ray scattering , 2015, Colloid and Polymer Science.

[11]  H. Amenitsch,et al.  Core–Shell Structure of Monodisperse Poly(ethylene glycol)-Grafted Iron Oxide Nanoparticles Studied by Small-Angle X-ray Scattering , 2015, Chemistry of materials : a publication of the American Chemical Society.

[12]  Tomás E. Benavidez,et al.  Protein adsorption onto nanomaterials for the development of biosensors and analytical devices: a review. , 2015, Analytica chimica acta.

[13]  K. Kubiak,et al.  Influence of supporting polyelectrolyte layers on the coverage and stability of silver nanoparticle coatings. , 2015, Journal of colloid and interface science.

[14]  Xuhong Guo,et al.  Distribution of magnetic nanoparticles in spherical polyelectrolyte brushes as observed by small-angle X-ray scattering , 2014 .

[15]  Z. Haidar,et al.  Layer-by-layer assembly of liposomal nanoparticles with PEGylated polyelectrolytes enhances systemic delivery of multiple anticancer drugs. , 2014, Acta biomaterialia.

[16]  D. Sebők,et al.  BSA/polyelectrolyte core-shell nanoparticles for controlled release of encapsulated ibuprofen. , 2014, Colloids and surfaces. B, Biointerfaces.

[17]  Meng-Xia Chen,et al.  Layer-by-layer assembly of chitosan stabilized multilayered liposomes for paclitaxel delivery. , 2014, Carbohydrate polymers.

[18]  G. Sukhorukov,et al.  Micropackaging via layer-by-layer assembly: microcapsules and microchamber arrays , 2014 .

[19]  Xuhong Guo,et al.  Protein immobilization and separation using anionic/cationic spherical polyelectrolyte brushes based on charge anisotropy , 2013 .

[20]  Si-wei Zhang,et al.  Fabrication and tribological properties of polyelectrolyte multilayers containing in situ gold and silver nanoparticles , 2013 .

[21]  Xuhong Guo,et al.  Spherical polyelectrolyte brushes: Ideal templates for preparing pH-sensitive core–shell and hollow silica nanoparticles , 2012 .

[22]  Kwangmeyung Kim,et al.  The tumor accumulation and therapeutic efficacy of doxorubicin carried in calcium phosphate-reinforced polymer nanoparticles. , 2012, Biomaterials.

[23]  Q. Gao,et al.  An amperometric glucose biosensor based on layer-by-layer GOx-SWCNT conjugate/redox polymer multilayer on a screen-printed carbon electrode , 2011 .

[24]  Jean Paul Remon,et al.  Polymeric multilayer capsules in drug delivery. , 2010, Angewandte Chemie.

[25]  M. Ballauff,et al.  Adsorption of beta-lactoglobulin on spherical polyelectrolyte brushes: direct proof of counterion release by isothermal titration calorimetry. , 2010, Journal of the American Chemical Society.

[26]  F. Caruso,et al.  Tuning the formation and degradation of layer-by-layer assembled polymer hydrogel microcapsules. , 2009, Langmuir : the ACS journal of surfaces and colloids.

[27]  Yan Lu,et al.  Well-Defined Crystalline TiO2 Nanoparticles Generated and Immobilized on a Colloidal Nanoreactor , 2009 .

[28]  Sanyog Jain,et al.  Polyelectrolyte coated multilayered liposomes (nanocapsules) for the treatment of Helicobacter pylori infection. , 2009, Molecular pharmaceutics.

[29]  R. Zbořil,et al.  Optically Active Spherical Polyelectrolyte Brushes with a Nanocrystalline Magnetic Core , 2008 .

[30]  M. Ballauff,et al.  Stable Bimetallic Gold–Platinum Nanoparticles Immobilized on Spherical Polyelectrolyte Brushes: Synthesis, Characterization, and Application for the Oxidation of Alcohols , 2008 .

[31]  T. Narayanan,et al.  Directed motion of proteins along tethered polyelectrolytes. , 2008, Physical review letters.

[32]  M. Ballauff,et al.  Adsorption of bovine hemoglobin onto spherical polyelectrolyte brushes monitored by small-angle X-ray scattering and Fourier transform infrared spectroscopy. , 2007, Biomacromolecules.

[33]  H. Möhwald,et al.  Microcapsules made of weak polyelectrolytes: templating and stimuli-responsive properties. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[34]  F. Caruso,et al.  Nanoporous Protein Particles Through Templating Mesoporous Silica Spheres , 2006 .

[35]  Yan Lu,et al.  Thermosensitive core-shell particles as carriers for ag nanoparticles: modulating the catalytic activity by a phase transition in networks. , 2006, Angewandte Chemie.

[36]  Changyou Gao,et al.  Stable microcapsules assembled stepwise from weak polyelectrolytes followed by thermal crosslinking , 2005 .

[37]  M. Ballauff,et al.  Interaction of proteins with spherical polyelectrolyte brushes in solution as studied by small-angle x-ray scattering. , 2004, Physical review. E, Statistical, nonlinear, and soft matter physics.

[38]  F. Caruso,et al.  Two-component, ultrathin microcapsules prepared by a core-mediated layer-by-layer approach , 2004 .

[39]  M. Ballauff,et al.  Cationic Spherical Polyelectrolyte Brushes as Nanoreactors for the Generation of Gold Particles , 2004 .

[40]  M. Ballauff,et al.  Adsorption of proteins on spherical polyelectrolyte brushes in aqueous solution , 2003 .

[41]  M. Ballauff.  Nanoscopic Polymer Particles with a Well-Defined Surface: Synthesis, Characterization, and Properties , 2003 .

[42]  M. Ballauff,et al.  Spherical polyelectrolyte brushes: comparison between annealed and quenched brushes. , 2001, Physical review. E, Statistical, nonlinear, and soft matter physics.

[43]  Peter Lindner,et al.  Small-angle x-ray and neutron scattering studies of the volume phase transition in thermosensitive core-shell colloids , 2001 .

[44]  U. Kaatze,et al.  Ultrasonic Spectrometry of Polystyrene Latex Suspensions. Scattering and Configurational Elasticity of Polymer Chains , 2001 .

[45]  T. Narayanan,et al.  Spatial Correlation of Spherical Polyelectrolyte Brushes in Salt-Free Solution As Observed by Small-Angle X-ray Scattering , 2000 .

[46]  T. Cosgrove,et al.  Novel microgel-particle colloids: the detailed characterisation of the layer structure and chain topology of silica:poly(NIPAM) core–shell particles , 2000 .

[47]  Xuhong Guo,et al.  Synthesis of Spherical Polyelectrolyte Brushes by Photoemulsion Polymerization , 1999 .

[48]  M. Ballauff,et al.  Observation of the volume transition in thermosensitive core-shell latex particles by small-angle X-ray scattering , 1998 .

[49]  Caruso,et al.  Nanoengineering of inorganic and hybrid hollow spheres by colloidal templating , 1998, Science.

[50]  Z. Madeja,et al.  Growth and motility of human skin fibroblasts on multilayer strong polyelectrolyte films. , 2016, Journal of colloid and interface science.

[51]  P. Gokul,et al.  Stimuli-responsive weak polyelectrolyte multilayer films: A thin film platform for self triggered multi-drug delivery. , 2016, Materials science & engineering. C, Materials for biological applications.

[52]  J. Weiss,et al.  Formation and stability of multiple-layered liposomes by layer-by-layer electrostatic deposition of biopolymers , 2013 .

[53]  M. Ballauff,et al.  The osmotic coefficient of spherical polyelectrolyte brushes in aqueous salt-free solution , 2002 .

[54]  M. Stamm,et al.  Dewetting of confined polymer films: an X-ray and neutron scattering study , 1999 .