Weak Polyelectrolytes as Nanoarchitectonic Design Tools for Functional Materials: A Review of Recent Achievements
Abstract
:1. Context
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- In the initial part, organic and hybrid thin films obtained from weak polyelectrolyte brushes and electrodeposited coatings are described, including those based on natural polyelectrolytes (e.g., chitosan, alginate, hyaluronic acid). The cohesion of such systems relies on covalent, hydrophobic and H-bonding interactions, most often leading to coatings containing one weak polyelectrolyte at a time. Basic synthesis approaches for these films are discussed as well as their applications, with an emphasis on their response to post-assembly pH changes in terms of swelling, adhesion, and cargo encapsulation and release.
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- The next two sections describe systems based on polyelectrolyte complexes, including those formed from the electrostatic complexation of weak polyanions and polycations [34]. Their assembly in aqueous media, without aggressive chemicals, allows for the use of more environmentally friendly routes to obtain surface coatings (films and layer-by-layer capsules), vectors, and functional gels. The resulting systems usually include several polyelectrolytes at the same time, and their cohesion is based on reversible interactions. The fundamentals of these films, gels, and colloids are discussed with respect to their response to pH and salt stimuli both during and after assembly. Emphasis is placed on recently proposed processing strategies to transform electrostatic complexes into gels and membranes. The applications of these systems are reviewed with a focus on nanovectors, and a subsection is devoted to systems that have been identified as relevant to pharmaceutical needs.
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- The final part addresses the growing significance of block copolymers (BCP) containing weak polyelectrolyte blocks for nanostructuring surfaces, colloids, and membranes. Accordingly, their directed self-assembly into microphase-separated films and their micellization behavior are discussed as a function of complexation, pH, and salt stimuli. Emerging applications, including sensors, nanolithography, and vectorization, are discussed.
2. Weak Polyelectrolytes Layers for Stimuli-Responsive Surfaces
2.1. Brushes of Weak Polyelectrolytes
2.2. Electrodeposited Weak Polyelectrolytes Films
Electrodeposition Principle | Polyelectrolyte Type and Typical Conditions (vs. Ag/AgCl) | Applications | Reference |
---|---|---|---|
Electrocoupling by click reaction | P AA or PAH grafted with alkyne and azide (−0.3 V, 0.6 mM CuSO4, H2O) | pH sensors, triggered release | [60,70] |
Controlled dimerization | Dimerization of alkylcarbazoles (+1.0 V/+1.2 V, acetonitrile) | Photovoltaics | [87] |
Electropolymerization | PANI (1.0 M HNO3 aqueous, 2 mA cm−2) PANI (0.5 M H2SO4 aqueous, CV −0.6 V/+1.5 V) Polycarbazoles (+1.3 V, aqueous or acetonitrile) Polydopamine (0.1 M phosphate buffer saline, CV −0.5 V/+0.5 V) | Capacitors, Capacitor sensors, Opto-electronic and electrochemical Sensors, biocoatings | [61,78] [76] [88] |
Electrochemically induced precipitation | Chitin (+1.2 V with Fe2+ ions) CHI (+1.5 V with Cu(s)) CHI (+1 to +3 V) Collagen (pH 3.5; 0.1 M H2O2, 8 mA/cm2) ALG (oxidation of oxides, 1.7–4.4 mA/cm2) PAH (+0.6 V, with MoO42−) | Drug release Sensor Drug delivery, biocoatings Biomaterials and actuators Wound treatment Implant coating | [89] [63] [90] [91] [69,71] [68] |
Electrochemical co-deposition | HA + Polydopamine (+1 V in PBS buffer) | Antifouling | [92] |
Complexation by pH-induced shift of PAH protonation | PAH/PAA (−0.5 V, 0.12 M H2O2) PAA/protected PAH and polyampholytes (H+ generation with 90 µA rate) | None reported | [65,66,67] |
3. Layer-by-Layer Films and Vectors from Weak Polyelectrolytes
3.1. Layer by Layer Films
3.2. Colloidal Systems Based on LbL Multilayers of Weak Polyelectrolytes
4. Gels and Vectors Based on Weak Polyelectrolytes Complexes
4.1. Gels Based on Weak Polyelectrolyte Complexes
4.2. Weak Polyelectrolyte Complexes for Pharmaceutical Vectorization
5. Block Copolymer Systems Based on Weak Polyelectrolytes
5.1. Directed Self-Assembly of BCPs for Nanopatterning
5.2. Colloidal Systems from Weak Polyelectrolytes BCP for Drug Delivery
5.3. Membranes from Weak Polyelectrolytes BCP for Filtration
BCP Polyelectrolyte | Chemical Structure | Applications | References |
---|---|---|---|
Poly(styrene)-b-poly(4-vinylpyridine) PS-b-P4VP | | Pattern transfer filtration colloids | [210,238] |
Poly(styrene)-b-poly(2-vinylpyridine) PS-b-P2VP | | Etch masks, drug delivery filtration | [213,215,216] |
Poly(styrene)-b-poly(acrylic acid) PS-b-PAA | | Ultra-filtration Drug delivery NP synthesis | [233,239] |
Poly(styrene)-b-poly(methacrylic acid) PS-b-PMAA | | Filtration Pattern transfer drug delivery | [240] |
Poly(ethylene oxide)-b-poly(2-vinylpyridine) PEO-b-P2VP | | Membranes | [241] |
Poly(ethylene glycol)-b-poly(2-(dimethylamino)ethyl methacrylate) PEG-b- PDMAEMA | | Drug delivery | [242] |
Poly(ethylene oxide)-b-poly(acrylic acid) PEO-b-PAA | | Drug delivery vehicle | [243] |
Poly(ethylene oxide)-b-poly(acrylic acid)-b-poly(styrene) PEO-b-PAA-b-PS | | Controlled drug delivery | [244] |
Poly(n-butyl acrylate)-b-poly(acrylic acid) PnBA-b-PAA | | Nanoreactors NP synthesis | [245] |
Poly(styrene)-b-poly(L-lysine) PS-b-PLL | | DNA carrier Encapsulation | [246] |
Poly(N-isopropylacrylamide)-b- poly(acrylic acid) PNIPAM-b-PAA | | Encapsulation Drug delivery | [247] |
6. Closing Remarks
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
Abbreviations
ALG | Alginic acid |
ATRP | Atom-Transfer-Radical-Polymerization |
BCP | Block copolymers |
CHI | Chitosan |
COPEC | Compacted complexes of Polyelectrolytes |
DNA | Deoxyribonucleic acid |
DIB | 1,4-diiodobutane |
HA | Hyaluronic acid |
LbL | Layer-by-Layer |
MeI | Methyl iodide |
NMP | Nitroxide-Mediated Polymerization |
NIPS | Non-solvent-induced phase separation |
P2VP | Poly(2-vinylpyridine) |
P4VP | Poly(4-vinylpyridine) |
PAA | Poly(acrylic acid) |
PAH | Poly(allylamine hydrochloride) |
PANI | Poly(aniline) |
PBS | Phosphate Buffer Saline |
PDADMAC | Poly(diallyldimethylammonium chloride) |
PDMA | Poly(N,N-dimethylacrylamide) |
PDMAEMA | Poly(2-(dimethylamino)ethyl methacrylate) |
PEG | Poly(ethylene glycol) |
PEG-b-PDMAEMA | Poly(ethylene glycol)-b-poly(2-(dimethylamino)ethyl methacrylate) |
PEI | Poly(ethyleneimine) |
PEO | Poly(ethylene oxide) |
PEO-b-P2VP | Poly(ethylene oxide)-b-poly(2-vinylpyridine) |
PEO-b-PAA | Poly(ethylene oxide)-b-poly(acrylic acid) |
PEO-b-PAA-b-PS | Poly(ethylene oxide)-b-poly(acrylic acid)-b-poly(styrene) |
PGA | Poly(glutamic acid) |
PLL | Poly(L-lysine) |
PMAA | Poly(methacrylic acid) |
PnBA | Poly(n-butyl acrylate) |
PnBA-b-PAA | Poly(n-butyl acrylate)-b-poly(acrylic acid) |
PNIPAM | Poly(N-isopropylacrylamide) |
PNIPAM-b-PAA | Poly(N-isopropylacrylamide)-b- poly(acrylic acid) |
PS-b-P2VP | Poly(styrene)-b-poly(2-vinylpyridine) |
PS-b-P4VP | Poly(styrene)-b-poly(4-vinylpyridine) |
PS-b-PAA | Poly(styrene)-b-poly(acrylic acid) |
PS-b-PLL | Poly(styrene)-b-poly(L-lysine) |
PS-b-PMAA | Poly(styrene)-b-poly(methacrylic acid) |
PSS | Poly(sodium 4-styrenesulfonate) |
RAFT | Reversible Addition-Fragmentation Chain Transfer |
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Type | Polyelectrolyte | First pKa/pKaH of Monomer | pKa/pKaH of Polymer * | Reference |
---|---|---|---|---|
Synthetic polyanions | Poly(acrylic acid) (PAA) Poly(methacrylic acid) (PMAA) | 4.2 4.7 | 4.5–6.6 up to 6.8 | [21,22] [21] |
Natural polyanions | Poly(glutamic acid) (PGA) Hyaluronic acid (HA) Alginic acid (ALG) | 2.1 ≈3.0 3.5–4.6 | 6.1 | [21] [23] [24] |
Synthetic polycations | Poly(allylamine hydrochloride) (PAH) Poly(aniline) (PANI) Poly(ethyleneimine) (PEI) Poly(2-vinylpyridine) (P2VP) Poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) Poly(L-lysine) (PLL) | 9.7 4.6 8.0 5–5.6 8.4 10.5 | 8.6 5.5 8.2–9.9 3.5–4.5 ≈7.5 10–10.5 | [25] [26] [27] [28,29] [20,30] [31,32] |
Natural polycations | Chitosan (CHI) | 7.5 | ~6.5 | [33] |
Target Application | Brushes Type | Reference |
---|---|---|
Reversible adhesion | PDMAEMA/PMAA | [51] |
poly(N,N-dimethylacrylamide)/PAA | [50] | |
Bio-adhesion | PMAA | [54] |
PAA | [55] | |
Cargo immobilization/release | PAA/PMAA | [48] |
PDMAEMA | [56] | |
PDMAEMA/PAA | [52] | |
Antifouling | P4VP | [57] |
PMAA | [58] |
Target Application | Multilayer Type | References |
---|---|---|
Cargo encapsulation and release | PAH/PAA | [95] |
PEI/PAA CHI/HA and PLL/PGA | [114] [115] | |
Tunable bio-interface | PAH/PAA CHI/PGA | [116] [117] |
Slippery liquid-infused porous surface | (PEI/PAH)/PAA PEI/Nafion | [106] [107] |
Methylmercaptan gas sensor Urea sensor | (PAH-Ag+)/PAA | [113] |
PEI/Urease/reduced graphene oxide | [118] | |
Ionic conductivity Ionic current rectification Ion selective ultrafiltration Micropollutant filtration Solvent resistant nanofiltration membrane | PDADMA/PAA PLL/PAA and PEI/PAA | [110] [109] |
CHI/Chondroitin sulfate PAH/PAA PAH/PAA | [111] [119] [120] |
Applications | Weak Polyelectrolyte Used | Chemical Structures | References |
---|---|---|---|
PAH | | Drug delivery, imaging | [140,141] |
PEI | | Drug delivery, gene delivery | [142,143] |
PMAA and PAA | | Drug delivery, cancer therapy | [128,134,144] |
Poly(N-isopropylacrylamide) (PNIPAM) | | Drug delivery | [144] |
Poly-L-Arginine | | Hyperthermia, imaging, drug delivery, gene silencing/editing | [145,146,147,148,149,150] |
PLL | | Hyperthermia, imaging | [139,151] |
Polyelectrolyte Complex | Processing | Target Applications | References |
---|---|---|---|
PAH/PAA | Compacted by ultracentrifugation | Catalysis support | [164] |
CHI/ALG | Compacted by ultracentrifugation | Biomaterials and biomedical applications | [162] |
β-Cyclodextrin-CHI/ALG | [163] | ||
poly[triethyl(4-vinylbenzyl)ammonium/ALG | [161] | ||
PAH/PMAA | Compacted by centrifugation | Sorption of transition metal ions Catalysis support | [158] [8] |
Poly(vinyl alcohol)/PAA | Injection | Adhesives | [159] |
CHI/ALG | Sedimentation | Tissue engineering | [160] |
PEI/PSS | Aqueous phase Separation | Filtration membranes | [165] |
PDADMAC/PAA | [13] | ||
PAH/PSS | [166] |
Polyelectrolyte | Chemical Structure | Applications | References |
---|---|---|---|
CHI | R = H or COCH3 | Oral drug delivery Mucosal delivery Gene delivery Cancer therapy Anti HVI therapy | [179] [187] [188] [189] [190] |
ALG | | Drug delivery Mucoadhesive | [191,192] |
Pectin | | Mucoadhesive, i.e., nasal inserts, ocular delivery Oral drug delivery | [193] [194] [195] |
Carrageenan | | Drug delivery Selective protein adsorption | [196] [197] |
HA | | Vectors for protein, peptide, and gene delivery | [198,199] |
Carboxymethyl starch | | Oral drug delivery Protein carrier | [200] [201] |
PGA | | Drug delivery Biomolecule carrier | [202] [203] |
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Sanchez-Ballester, N.M.; Sciortino, F.; Mir, S.H.; Rydzek, G. Weak Polyelectrolytes as Nanoarchitectonic Design Tools for Functional Materials: A Review of Recent Achievements. Molecules 2022, 27, 3263. https://doi.org/10.3390/molecules27103263
Sanchez-Ballester NM, Sciortino F, Mir SH, Rydzek G. Weak Polyelectrolytes as Nanoarchitectonic Design Tools for Functional Materials: A Review of Recent Achievements. Molecules. 2022; 27(10):3263. https://doi.org/10.3390/molecules27103263
Chicago/Turabian StyleSanchez-Ballester, Noelia M., Flavien Sciortino, Sajjad Husain Mir, and Gaulthier Rydzek. 2022. "Weak Polyelectrolytes as Nanoarchitectonic Design Tools for Functional Materials: A Review of Recent Achievements" Molecules 27, no. 10: 3263. https://doi.org/10.3390/molecules27103263