Naturally Occurring Polyelectrolytes and Their Use for the Development of Complex-Based Mucoadhesive Drug Delivery Systems: An Overview
Abstract
:1. Introduction
2. Naturally Occurring Polyelectrolytes
2.1. Classification
- Depending on the ionizable groups:
- Polyanions
- Polycations
- Polyampholytes
- Annealed
- Quenched
- Betainic
- Depending on the dissociation ability:
- Strong
- Weak
- Depending on the charge location:
- Integral
- Pendant
- Depending on the composition:
- Homopolymers
- Heteropolymers or copolymers
- Depending on the origin:
- Natural (biopolymers or biopolyelectrolytes)
- Semisynthetic
- Synthetic
2.2. Biopolycations
Chitosan
2.3. Biopolyanions
2.3.1. Alginate
- Acid gelation: Alginic acid gels are obtained when the pH of the medium is lower than the constant of dissociation (or pKa) of the polymer. A rapid decrease in pH implies the precipitation of polymeric aggregates, while a progressive drop in pH leads to the formation of a continuous gel. Acid gels from alginate are stabilized by hydrogen bonding, with residues of ManA blocks playing a major role in the gelation process. Gel strength is known to be correlated with the content of GulA blocks in the alginate chain [41].
- Ionotropic gelation: Alginate can form ionic gels in the presence of multivalent cations, which are being widely explored for biomedical applications such as drug encapsulation and cell immobilization. Alginate affinity towards cations is directly dependent on the number of G-blocks present in the alginate structure, and increases in the order of Mn < Zn, Ni, Co < Fe < Ca < Sr < Ba < Cd < Cu < Pb. It should be noted that some of these cations are toxic, and cannot be considered for biomedical application; Pb, Cu, and Cd exhibit high toxicity. Calcium alginate gels, which are highly biocompatible, are the most commonly used for the development of biomedical devices. The gelation of alginate occurs through the binding of divalent cations and the GulA blocks by dimerization of GulA residues. Thus, Ca ions cause the two GulA blocks to bind on opposite sides, forming a diamond-shaped hole consisting of a hydrophilic cavity that binds the Ca ions to the oxygen atoms of the carboxylic groups. This tightly bound polymer conformation has been described as an egg-box-like structure, where each cation binds with four G residues in the egg-box formation to form a 3-D network. The binding of trivalent cations with alginate is generally enhanced compared to divalent cations, as they are able to interact with three carboxyl groups from different alginate biopolymers at the same time, forming a three-dimensional bonding structure that produces a more compact network [41].
- Non-conventional methods: Other methods worth highlighting are cation-free cryogelation, ionotropic cryogelation, non-solvent induced phase separation and carbon dioxide induced gelation, among others [43].
2.3.2. Pectin
2.3.3. Xanthan Gum
2.3.4. Gum Arabic
2.3.5. Carrageenan
2.3.6. Hyaluronic Acid
3. Polyelectrolyte Complexes
3.1. Polyelectrolyte Complex-Based System Production Methods
3.2. Properties of Biopolymer-Based PECs
- Electronic theory: electron transfer occurs upon contact between the polymer and the mucus surface due to different electronic charges in their structure. This leads to the adhesion of the surfaces through the formation of an electrical double layer at the interface.
- Adsorption theory: the polymer binds the mucus by weak chemical interactions, for instance Van der Waals forces or hydrogen bonds, or hydrophobic interactions.
- Wetting theory: this refers to the polymer’s ability to spontaneously spread over the mucus surface and develop adhesion.
- Diffusion theory: a process driven by concentration gradients and affected by the available molecular chain lengths and their mobilities. Sufficient depth of penetration creates a semi-permanent adhesive bond, and this depends on several parameters such as the nature of the mucoadhesive chains, the diffusion coefficient and the flexibility and motility of the polymer chains.
- Mechanical theory: according to this theory, a liquid adhesiveness is created with the presence of irregularities in the mucosal surface, as this increases the area of contact between the polymer and the mucosa.
- Contact stage: the first stage occurs when the biopolymer is wetted in the medium and swells after it is placed on the mucous membrane. This is governed by the wetting theory.
- Polymer chains and mucosal surface interpenetration: the polymer chains of the biopolymer and the mucosal layer become entangled by forming physical bonds. This occurs through the combination of the adsorption theory and electronic theory, and is favored by the mechanical theory.
- Creation of bonds between the chains or consolidation stage: the entangled polymer chains, bound by physical interaction, consolidate the adhesion by forming covalent bonds. This is governed by the combination of the diffusion theory, electronic theory and adsorption theory.
3.3. Polyelectrolyte Complexes for Medical Applications
3.3.1. Drug Delivery Systems
- Dissolution of the drug in the medium, followed by its entrapment in the precipitation of the complex.
- Absorption of a dissolved drug in the preformed PEC (especially with sponge-like PECs).
- Chemical binding of the drug to polyanions or polycations, and the subsequent formation and precipitation of the PEC.
- Use of the drug as a partner in the formation of the PEC. This requires the drug to possess at least one ionizable polar group.
3.3.2. Tissue Engineering
3.3.3. Other Applications
3.4. Advances in Biopolymer-Based Polyelectrolyte Complexes for Mucoadhesive Drug Delivery Systems
3.4.1. Ocular Drug Delivery Systems
3.4.2. Nasal Drug Delivery Systems
3.4.3. Buccal Drug Delivery Systems
3.4.4. Oral Drug Delivery Systems
3.4.5. Vaginal Drug Delivery Systems
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Polyanion | Polycation | Formulation | Drug | Reference |
---|---|---|---|---|
Salecan | Chitosan | Hydrogel | Vitamin C | Hu et al. [85] |
Carboxymethyl xanthan gum | N-trimethyl chitosan | Hydrogel | Ciprofloxacin | Hanna and Saad [111] |
Alginate Guar gum Xanthan gum | Chitosan | Tablet | Isosorbide nitrate | Syed et al. [112] |
Xanthan gum | Eudragit® E100 | Tablet | Diclofenac sodium | Moin et al. [113] |
Kappa, Iota and Lambda carrageenan | Chitosan | Tablet | Trimetazidine hydrochloride | Li et al. [114] |
Eudragit® S100 | Chitosan lactate Chitosan tartrate Chitosan citrate | Film | Tenofovir | Cazorla-Luna et al. [36] |
Pectin | Chitosan | Film | Theophylline anhydrous | Ghaffari et al. [115] |
Alginate | Chitosan | Microparticles | Vancomycin | Unagolla et al. [116] |
Alginate Eudragit® L100-55 | Oligochitosan | Microparticles | Naproxen | Čalija et al. [117] |
Pectin | Lactoferrin | Nanoparticles | Curcumin | Yan et al. [118] |
Poly(maleic acid-alt-ethylene) Poly(maleic acid-alt-octadecene) | Chitosan | Nanoparticles | Methotrexate | Ciro et al. [119] |
Alginate | Cationized gelatin | Nanoparticles | Curcumin | Sarika et al. [120] |
Pectin | Chitosan | Nanoparticles | Insulin | Maciel et al. [121] |
Alginate Xanthan gum Carbopol® | Chitosan | Freeze-dried inserts | Fluconazole | Darwesh et al. [122] |
Administration Route | Advantages of Using Mucoadhesive Drug Delivery Systems |
---|---|
Ocular |
|
Nasal |
|
Buccal |
|
Oral |
|
Vaginal |
|
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Cazorla-Luna, R.; Martín-Illana, A.; Notario-Pérez, F.; Ruiz-Caro, R.; Veiga, M.-D. Naturally Occurring Polyelectrolytes and Their Use for the Development of Complex-Based Mucoadhesive Drug Delivery Systems: An Overview. Polymers 2021, 13, 2241. https://doi.org/10.3390/polym13142241
Cazorla-Luna R, Martín-Illana A, Notario-Pérez F, Ruiz-Caro R, Veiga M-D. Naturally Occurring Polyelectrolytes and Their Use for the Development of Complex-Based Mucoadhesive Drug Delivery Systems: An Overview. Polymers. 2021; 13(14):2241. https://doi.org/10.3390/polym13142241
Chicago/Turabian StyleCazorla-Luna, Raúl, Araceli Martín-Illana, Fernando Notario-Pérez, Roberto Ruiz-Caro, and María-Dolores Veiga. 2021. "Naturally Occurring Polyelectrolytes and Their Use for the Development of Complex-Based Mucoadhesive Drug Delivery Systems: An Overview" Polymers 13, no. 14: 2241. https://doi.org/10.3390/polym13142241
APA StyleCazorla-Luna, R., Martín-Illana, A., Notario-Pérez, F., Ruiz-Caro, R., & Veiga, M. -D. (2021). Naturally Occurring Polyelectrolytes and Their Use for the Development of Complex-Based Mucoadhesive Drug Delivery Systems: An Overview. Polymers, 13(14), 2241. https://doi.org/10.3390/polym13142241