Poly(allylamine)/tripolyphosphate coacervates enable high loading and multiple-month release of weakly amphiphilic anionic drugs: an <i>in vitro</i> study with ibuprofen

Silva, Udaka K. de; Brown, Jennifer; Lapitsky, Yakov

doi:10.1039/c8ra02588f

Cited by 23 publications

(28 citation statements)

References 51 publications

(123 reference statements)

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“…The moderate increase in swelling of the payload-free coacervates when placed in water was consistent with those previously reported for both PAH/TPP networks , and polyelectrolyte complex coacervates (prepared through the mixing of oppositely charged polymers). , Moreover, the increase in swelling with the coacervate loading was qualitatively similar to that seen in prior work upon the encapsulation of a nonbinding zwitterionic dye (Rhodamine B) . Because the LCs with the dye molecules were orders of magnitude lower than those used here, however, the swelling in that earlier work was much more modest (with the coacervate weights changing by just 10–30% when placed in deionized water or phosphate-buffered saline) .…”

Section: Resultssupporting

confidence: 89%

“…Recently, one of us hypothesized that highly sustained disinfection could be achieved using putty-like complex coacervates formed from aqueous mixtures of the cationic polymer, poly(allylamine hydrochloride) (PAH), and pentavalent anion, tripolyphosphate (TPP) (see Scheme a,b) . These coacervates can both adhere to diverse surfaces , and release small molecules over multiple months. , The long-term sustained release functionality of PAH/TPP coacervates likely reflects their high network densities and has, to date, been demonstrated using water-soluble (anionic and zwitterionic) dyes and the anti-inflammatory drug ibuprofen . Besides their adhesion and long-term release functionalities, PAH/TPP coacervates have shown promising cytocompatibilities with human cells, which suggests these materials to be relatively nontoxic .…”

Section: Introductionmentioning

confidence: 99%

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Highly Sustained Release of Bactericides from Complex Coacervates

Alam

Seo

Lapitsky

2020

ACS Appl. Bio Mater.

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Materials for preventing harmful bacterial contamination attract widespread interest in areas that include healthcare, home/personal care products, and crop protection. One approach to achieving this functionality is through the sustained release of antibacterial compounds. To this end, we show how putty-like complex coacervates, formed through the association of poly(allylamine hydrochloride) (PAH) with pentavalent tripolyphosphate (TPP) ions, can provide a sustained antibacterial effect by slowly releasing bactericides. Using triclosan (TC) as a model bactericide, we demonstrate that, through their dispersion in the parent PAH solution with nonionic surfactants, hydrophobic biocides can be efficiently and predictably encapsulated within PAH/TPP coacervates. Once encapsulated, the bactericide can be released over multiple months, and the release rates can be readily tuned by varying the bactericide and surfactant compositions used during encapsulation. Through this release, the PAH/TPP coacervates provide sustained bactericidal activity against model Gram-positive and Gram-negative bacteria (Staphylococcus aureus and Escherichia coli) grown under a nutrient-rich condition over at least two weeks. Thereafter, though some partial activity persists after one month, the release slows down and the bactericide-eluting coacervates lose their efficacy. Overall, we show that bactericide release from easy-to-prepare complex coacervates can provide a pathway to sustained disinfection.

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Section: Resultssupporting

confidence: 89%

Section: Introductionmentioning

confidence: 99%

Highly Sustained Release of Bactericides from Complex Coacervates

Alam

Seo

Lapitsky

2020

ACS Appl. Bio Mater.

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“…Previously, Lapitsky and coworkers observed this reduction in cross‐link density induced by salt effects in gel‐like coacervates prepared from the ionic self‐assembly of PAH with either pyrophosphate or tripolyphosphate . On the other hand, these gels showed a high capacity to encapsulate small molecules and release them over multiple‐month timescales . The slow release rate is possibly due to a higher cross‐link density generated by the use of ionic cross‐linkers with higher net charge as compared to single phosphate.…”

Section: Resultsmentioning

confidence: 96%

Layer‐by‐Layer Formation of Polyamine‐Salt Aggregate/Polyelectrolyte Multilayers. Loading and Controlled Release of Probe Molecules from Self‐Assembled Supramolecular Networks

Herrera

Agazzi

Cortez

et al. 2019

Macro Chemistry & Physics

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The use of soft materials as building blocks in layer‐by‐layer (LbL) assemblies represent a very appealing and useful approach to enhance the loading capacity of thin films. Here, the capacity of positively charged polyamine‐salt aggregates (PSAs) based on ionically crosslinked poly(allylamine hydrochloride) (PAH) with phosphate anions (Pi) is explored to act as building blocks in construction of multilayers by alternated deposition with poly(sodium 4‐styrenesulfonate). Hybrid thin films are successfully prepared by the LbL technique with a highly regular growth and a material deposition rate higher than the traditional full polyelectrolyte LbL. The loading of bromophenol blue (BPB) is evaluated by integration into PSAs followed by LbL deposition and monitored with UV–vis spectroscopy. Finally, the release of the dye molecules is carried out by exposing the film to different aqueous solutions. It is shown that a fully controlled release can be achieved by simply varying the media pH obtaining total BPB release over periods between minutes and months. The data obtained reveal that this new LbL construction strategy using ionically crosslinked PAH/Pi colloids allows to obtain nanoarchitectures with high loading capacity and remarkable properties for controlled release.

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“…To ensure that amino groups remain un‐ionized, experiments were conducted in a HEPES 2‐[4‐(2‐hydroxyethyl)piperazin‐1‐yl]ethanesulfonic acid buffer with pH 7.5 and 150 mmol L −1 of NaCl. Although poly(allylamine) is a weak cationic polymer with pK a ranging from 8.6 80 to 8.7, 81 its apparent pK a remained below pH under the experimental conditions (based on a rough estimate that 1 mmol L −1 of a monovalent salt in an aqueous solution induces reduction of pK a by 0.1) 80 . Details of the preparation of the microgel are provided in Appendix S1.…”

Section: Fitting Of Experimental Datamentioning

confidence: 99%

A model for equilibrium swelling of the upper critical solution temperature type thermoresponsive hydrogels

Drozdov

Christiansen

2021

Polymer International

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Thermoresponsive gels of the upper critical solution temperature (UCST) type shrink below their critical temperature and swell above it. Changes in water uptake by these gels are driven by thermally induced dissociation of hydrogen or ionic bonds between chains. A simple model is developed for the description of the equilibrium swelling of thermophilic gels with hydrogen bonds. To confirm its ability to describe observations, equilibrium swelling diagrams are fitted on poly(acrylamide‐acrylic acid) and poly(acrylamide‐acrylonitrile) macroscopic gels and microgels with various structures (copolymer gels, gels with interpenetrating networks, nanocomposite gels), as well as on biocompatible poly(N‐acryloyl‐glycinamide) and poly(allylurea‐co‐allylamine) gels. Numerical simulation reveals that material parameters evolve consistently with molar fractions of crosslinker, hydrophobic and hydrophilic comonomers in the feed, degree of ionization of functional groups, and concentration of nanofiller. It is shown that the model can also be applied to describe observations on thermophilic zwitterionic gels. © 2021 Society of Industrial Chemistry.

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Poly(allylamine)/tripolyphosphate coacervates enable high loading and multiple-month release of weakly amphiphilic anionic drugs: an in vitro study with ibuprofen

Abstract: Gel-like coacervates prepared through ionotropic gelation enable very high loading and multiple-month release of weakly amphiphilic small molecules. Conversely, strong amphiphile incorporation disrupts ionic crosslinking and strikingly alters the coacervate properties.

Cited by 23 publications

References 51 publications

Highly Sustained Release of Bactericides from Complex Coacervates

Highly Sustained Release of Bactericides from Complex Coacervates

Layer‐by‐Layer Formation of Polyamine‐Salt Aggregate/Polyelectrolyte Multilayers. Loading and Controlled Release of Probe Molecules from Self‐Assembled Supramolecular Networks

A model for equilibrium swelling of the upper critical solution temperature type thermoresponsive hydrogels

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