Current Advances in the Development of Hydrogel-Based Wound Dressings for Diabetic Foot Ulcer Treatment
Abstract
:1. Introduction
2. Normal Wound Healing
3. Diabetic Foot Ulcers (DFUs)
4. Hydrogel Wound Dressings for DFU Treatment
4.1. Natural DFU Hydrogel Dressings
4.1.1. Collagen and Gelatin Hydrogels
4.1.2. Chitosan Hydrogels
4.1.3. Alginate Hydrogels
Ref. | Year | Polymer Source and Material | Additional Functional Component (s) | Synthesis Method | Diabetic Model | Therapeutic Effect |
---|---|---|---|---|---|---|
[59] | 2022 | Sodium alginate (2% w/v) hydrogel | Deferoxamine (560 μg/mL) and copper nanoparticles (200 μg/mL) | Ionic crosslinking with 0.1M CaCl2 | STZ-induced male C57BL/6 mice | Enhanced antimicrobial effect as well as angiogenesis by upregulation of HIF-1α and VEGF. Reduced inflammatory response. |
[60] | 2021 | Sodium alginate/pectin (5% w/w) composite hydrogel | Simvastatin (20 mg/mL) | Combined solvent-casting and ionic crosslinking with 0.5% w/v CaCl2 | STZ-induced male Wistar rats | Accelerated wound closure due to the presence of SIM, which promoted re-epithelialization, fibroblast proliferation and collagen production. |
[61] | 2021 | Silk nanofiber (1 wt%) hydrogel | Deferoxamine (60 μM and 120 μM) | Concentration-dilution-thermal incubation method | STZ-induced male Sprague−Dawley rats | Enhanced collagen deposition and wound healing rates: 80% on day 14, and 100% on day 21. Improved angiogenic and inflammatory responses. |
[57] | 2020 | Sodium alginate (2–5% w/v) hydrogel | Polydeoxyribonucleotide (100 μg/mL) | Ionic crosslinking with CaCO3 | Male C57BLKS/J-db/db mice | Improved re-epithelialization and granulation tissue formation. Increased collagen production and angiogenesis. |
[62] | 2019 | Sodium alginate (1.5% w/w) hydrogel | Edaravone-loaded Eudragit nanoparticles | Ionic crosslinking with 0.5% w/w CaCl2 | STZ-induced male C57BL/6 mice | Downregulation of reactive oxygen species favored accelerated wound healing. |
[43] | 2019 | Gelatin (4% w/v)/hyaluronic acid (0.1% w/v) composite hydrogel | Thrombomodulin (9 and 15 μg) | Chemical crosslinking (0.05% EDC) | STZ-induced male C57BL/6JNarl mice | Enhanced granulation tissue formation, re-epithelialization, collagen deposition, and angiogenesis. |
[46] | 2018 | Chitosan (6% w/v) hydrogel | D-(+) raffinose pentahydrate (290 mM) | Physical crosslinking in alkaline solution (8% w/v KOH) | STZ-induced female Wistar rats | Increased bactericidal effect and accelerated wound healing. |
[52] | 2017 | Chitosan (2 wt. %) hydrogel | L-glutamic acid (0.25–1.0%) | Physical crosslinking in alkaline solution (1M NaOH) | STZ-induced male Wistar rats | Enhanced re-epithelialization, collagen deposition, and neovascularization. |
[39] | 2016 | Chitosan/starch hydrogel | Chitosan silver nanoparticles (5 ppm Ag in 6.9 mg/mL chitosan) | Reductive alkylation crosslinking | Alloxan-induced male albino rats | Significantly improved wound healing rate. Increased bactericidal response. |
[39] | 2016 | Collagen/alginate (50/50 w/w) hydrogel | Curcumin (1 wt.%) -loaded chitosan nanoparticles | Chemical crosslinking (EDC) | STZ-induced male Wistar rats | Reduced inflammation. Enhanced cell adhesion and proliferation. Accelerated wound closure. |
[63] | 2016 | Gelatin/hydroxyphenyl propionic acid hydrogel (5 wt%) | Interleukin-8 (IL-8, 0.5 μg/mL) or macrophage inflammatory protein-3α (MIP-3α, 1 μg/mL) | Horseradish peroxidase (HRP)-catalyzed cross-linking | STZ-induced male ICR mice | Increased cell infiltration, re-epithelialization, neovascularization, and collagen deposition. |
4.2. Synthetic and Semi-Synthetic DFU Hydrogel Dressings
4.2.1. Polyethylene Glycol (PEG)-Based Systems
Ref. | Year | Polymer Source and Material | Additional Functional Component(s) | Synthesis Method | Diabetic Model | Therapeutic Effect |
---|---|---|---|---|---|---|
[69] | 2022 | Methacrylate gelatin (GelMA)/PEGDA microneedle patch | Tazarotene (1 mg/10 mL) and exosomes (100 µg/mL) from human umbilical vein endothelial cells (HUVECs) | Photopolymerization with lithium acylphosphinate salt (LAP 0.05%, g/mL) | STZ-induced male C57BL mice | Accelerated collagen deposition, epithelial regeneration, and angiogenesis. |
[70] | 2022 | PLGA-PEG-PLGA thermosensitive hydrogel | Copper-based MOFs containing curcumin and metformin hydrochloride | Thermal gelation | STZ-induced male BALB/c mice | Significant reduction of oxidative stress; enhanced cell migration, neovascularization, and collagen formation. |
[71] | 2022 | Injectable hydrogel prepared from 4,5-imidazoledicarboxylic acid, zinc nitrate hexahydrate, deferoxamine mesylate and glucose oxidase (GOX) | Deferoxamine mesylate (DFO, 8.3 µg/mL) | Phase- transfer-mediated programmed GOX loading | STZ-induced female BALB/c mice | Release of zinc ions and DFO resulted in enhanced antibacterial and angiogenic effect. Significant induction of re-epithelialization and collagen deposition. |
[72] | 2022 | PDLLA-PEG-PDLLA (25% w/v) thermosensitive hydrogel | Prussian blue nanoparticles (PBNPs, 333.3 µg/mL and 666.6 µg/mL) | Thermal gelation | STZ-induced C57BL/6J mice | Decreased reactive oxygen species (ROS) production as well as IL-6 and TNF-α levels. PBNPs dose-dependent accelerated wound closure. |
[73] | 2022 | pH/glucose dual responsive hydrogel prepared from dihydrocaffeic acid and L-Arginine co-grafting chitosan, phenylboronic acid and benzaldehyde difunctional polyethylene glycol-co-poly(glycerol sebacic acid) and polydopamine-coated graphene oxide (GO) | Metformin (2 mg/mL) | Double dynamic bond of a Schiff-base and phenylboronate ester | STZ-induced Sprague−Dawley rats | Antibacterial properties, tissue adhesion, hemostasis. Decreased inflammatory response. Increased wound closure ratio, re-epithelialization, and regeneration of blood vessels. |
[74] | 2022 | Supramolecular guanosine-quadruplex hydrogel | Hemin (0.36–0.54 mg) and GOX (0.125–0.5 mg) | Self-assembled gelation | STZ-induced male BABL/c mice | Significantly faster antibacterial effect, relative to commercial antibiotic. Decreased glucose concentration in the wound. |
[75] | 2022 | Chitosan/polyvinyl acetate heterogeneous hydrogel | Human epidermal growth factor (EGF)-loaded nanoparticles, polyhexamethylene biguanide, and perfluorocarbon emulsions | Freeze-thaw cycling | STZ-induced Sprague-Dawley rats | High antibacterial and anti-inflammatory effect. Enhanced collagen production and wound closure efficiency, relative to commercial dressings. |
[76] | 2022 | Double-layered GelMA-PLL hydrogel | Vascular endothelial growth factor (VEGF)-mimetic peptide | Photopolymerization with lithium acylphosphinate salt (LAP) | STZ-induced Sprague-Dawley rats | Enhanced antibacterial and wound-healing effect. Improved collagen deposition, angiogenesis, and re-vascularization. |
[77] | 2022 | Oxidized alginate / platelet-rich plasma (PRP) fibrin hydrogel | Ionic crosslinking with 1.22 M CaSO4·2H2O | Male db/db (BKS.Cg-m+/+Leprdb/J) mice | Accelerated wound maturation and closure. | |
[78] | 2022 | PTFE/PU patch | Calcium-alginate hydrogel microparticles (MPs) containing Chlorella vulgaris and Bacillus licheniformis | MP encapsulation in porous PTFE membrane (inner lining) and a transparent PU film (back lining) | STZ-induced mice | Enhanced wound healing effect: 50% wound closure by day 3, and full wound closure on day 12. |
[79] | 2021 | GelMA (10% w/v) hydrogel | Bioactive glass particles loaded with cerium (1% w/v) | Photopolymerization with LAP (0.1% w/v) | STZ-induced Sprague-Dawley rats | Wound closure of almost 95% on day 21. |
[80] | 2021 | Cecropin-modified hyaluronic acid/ oxidized dextran / PRP composite hydrogel | Schiff base reaction | Male db/db mice | Accelerated healing of infected wounds. Shortened inflammatory stage. Increased mature collagen content. | |
[81] | 2021 | Pluronic F-127 (20%) hydrogel | Ag nanocubes with virus-like mesoporous silica containing gentamicin | Thermal gelation | STZ-induced Kunming mice | Bacterial infected wounds were fully healed by day 20, with enhanced collagen production. |
[82] | 2021 | Carboxymethyl chitosan/poly(dextran-g-4-formylbenzoic acid) hydrogel | Peptide-modified PAN nanofibers | Schiff base reaction | Diabetic ICR mice | Enhanced antibacterial and angiogenic effect. Reduced inflammatory response. Wound closure > 96% at day 14. |
[83] | 2021 | Hydroxyl propyl methyl cellulose (2% w/w) hydrogel | Lipid nanoparticles loaded with Valsartan (1% w/w) | Thermal gelation | STZ-induced male Sprague-Dawley rats | Enhanced healing response mediated through COX-2, NF-κB, NO, TGF-β, MMPs and VEGF pathways. |
[84] | 2021 | Polyacrylamide/gelatin/ε-polylysine composite hydrogel | Free-radical polymerization | STZ-induced male Sprague-Dawley rats | Increased granulation tissue formation, collagen deposition, and angiogenesis. Enhanced antibacterial effect. | |
[85] | 2021 | Conductive hydrogel made from acrylamide-co-polymerized ionic liquid (VAPimBF4) and konjac glucomannan | Chemical crosslinking (EDC/NHS chemistry) | STZ-induced male Kunming mice | Highest wound healing rate when coupled with electrical stimulation. Increased antibacterial effect, Col-1 production, and new vessel growth. | |
[86] | 2021 | N-carboxyethyl chitosan/adipic acid dihydrazide pH responsive hydrogel | Insulin (0.67 U/mL) | Crosslinking by hyaluronic acid-aldehyde (imine and acylhydrazone bonds) | STZ-induced male Sprague-Dawley rats | Significant reduction of glucose levels in the wound. Decreased inflammation phase. Increased granulation tissue formation, collagen deposition, and re-epithelialization. |
[87] | 2021 | Quaternized chitosan/oxidized hyaluronic acid self-healing hydrogel | α-lipoic acid-loaded MOFs | Schiff base reaction | STZ-induced male Sprague-Dawley rats | Increased collagen deposition, cell proliferation and neovascularization. Accelerated wound healing. |
[88] | 2021 | Chitosan/polyvinyl acetate hydrogel | Chitosan nanoparticles loaded with human epidermal growth factor (EGF, 60 µg/mL) and Ag+ ions | Freeze-thaw cycling | STZ-induced Sprague-Dawley rats | Remarkable antibacterial effect. Enhanced tissue maturation and wound closure: 40% on day 3, and 97% on day 14. |
[89] | 2021 | Pluronic F-127 (20% w/v) hydrogel | Sodium ascorbyl phosphate (400 μM) and Wharton’s jelly mesenchymal stem cells (WJMSC) | Thermal gelation | STZ-induced male Sprague-Dawley rats | Shortened inflammatory response. Improved dermis regeneration, neovascularization, and collagen deposition. |
[90] | 2020 | Supramolecular hydrogel based on ferrocene, hyaluronic acid, β-cyclodextrin, and rhein | Intermolecular π−π interactions and hydrogen bonds | STZ-induced C57 mice | Anti-inflammatory properties of rhein facilitated transition from the inflammatory phase into the proliferation phase, thus, favoring normal wound healing. | |
[91] | 2020 | Pluronic F-127 hydrogel | Exosomes derived from human umbilical cord MSCs (300 μg/mL) | Thermal gelation | STZ-induced male Sprague-Dawley rats | Increased vascularization of wound granulation tissue, shortening wound healing time. Improved epithelial regeneration. |
[92] | 2020 | 4-carboxybenzaldehyde-PEG/glycol chitosan/silk fibroin/PRP self-healing hydrogel | Schiff base reaction + crosslinking with 10% calcium gluconate | STZ-induced Sprague-Dawley rats | Enhanced angiogenesis, re-epithelialization, nerve repair, and wound healing rate. | |
[93] | 2020 | Chitosan/polyurethane hydrogel membrane | Bone marrow mononuclear cells (1 × 106) injected into the edge of the wound prior to hydrogel application | Chemical crosslinking (urea/urethane bonds) | STZ-induced female Wistar rats | Hemostatic and anti-inflammatory effect. Wound closure > 90% after 14 days. |
[94] | 2020 | Stimuli-responsive supramolecular hydrogel made from polyvinyl alcohol/N-carboxyethyl chitosan/agarose/Ag nanowires | Hydrogen bonding | STZ-induced male Sprague-Dawley rats | Bactericidal effect. Promoted angiogenesis and collagen deposition. Accelerated wound healing rate. | |
[95] | 2020 | Poly(N-isopropyl-acrylamide)/poly(γ-glutamic acid) hydrogel (20 mg/mL total concentration) | Superoxide dismutase (2 mg/mL) | Thermal gelation | STZ-induced male Sprague-Dawley rats | Reduced inflammation. Enhanced collagen production and epidermal formation. |
[96] | 2020 | N-carboxyethyl chitosan (7.5% w/v)/adipic acid dihydrazide (7.5% w/v)/hyaluronic acid-aldehyde (5% w/v) composite hydrogel | Encapsulated bone marrow mesenchymal stem cells (2 × 105) | Crosslinking by hyaluronic acid-aldehyde (imine and acylhydrazone bonds) | STZ-induced male Sprague-Dawley rats | Inhibited chronic inflammation. Enhanced formation of granulation tissue, cell proliferation and neovascularization. |
[97] | 2020 | γ-polyglutamic acid (0.5 g/mL) hydrogel | Human cell-free fat extract (5 mg/mL) | Chemical crosslinking (EDC/NHS chemistry) | Male BKS-Leprem2Cd479/Nju mice | Improved cell proliferation, collagen deposition and continuous epidermal formation. Significant angiogenesis. |
[98] | 2020 | Silk fibroin-polyvinyl pyrrolidone hydrogel | L-carnosine and curcumin | Mixing/vortex shearing (physical crosslinking) | STZ-induced BALB/c mice | Significant antibacterial and anti-inflammatory effect. Enhanced wound healing. |
[99] | 2020 | [2-(methacryloloxy)ethyl]dimethyl-(3-sulfopropyl) ammonium hydroxide (SBMA)/2-Hydroxyethyl methacrylate (HEMA) and 3-[[2-(Methacryloyloxy)ethyl] dimethylammonio] propionate (CBMA)/HEMA zwitterionic cryogels | miRNA146a-conjugated cerium oxide nanoparticles | Free-radical polymerization with 13.6 mg/mL ammonium persulfate | Db/Db female mice | Full wound healing on day 14. Downregulation of inflammatory markers. Increased Col1a2 expression. |
[100] | 2020 | Polyvinyl alcohol (8% w/v)/sodium alginate (1% w/v) hydrogel | Green tea polyphenol nanoparticles | Ionic crosslinking (CaCl2, 100 μg/mL) and hydrogen bonding | STZ-induced female Sprague-Dawley rats | Increased granulation tissue formation and collage deposition. Accelerated wound healing. |
[101] | 2019 | Chitosan/PEG hydrogel | Ag nanoparticles | Chemical crosslinking with glutaraldehyde | Alloxan-induced rabbits | Increased bactericidal effect. Accelerated re-epithelialization and collagen deposition. Full wound closure on day 14. |
[102] | 2018 | A5G81-modified poly(polyethylene glycol cocitric acid-co-N-isopropylacrylamide) hydrogel | Thermal gelation | B6.BKS(D)-Leprdb/J mice | Enhanced re-epithelialization and granulation tissue formation. Faster wound closure than that achieved with commercial dressings. | |
[103] | 2018 | Hyperbranched PEG/thiolated hyaluronic acid injectable hydrogel | Encapsulated adipose-derived stem cells (2.5 × 106 cell/mL) | thiol-ene click reaction | STZ-induced male Sprague-Dawley rats | Reduced inflammatory response. Increased angiogenesis and re-epithelialization. |
[104] | 2017 | Polymethyl methacrylate/Polyvinyl alcohol hydrogel particles | Collagen, Ag nanowires, and chitosan | UV photocrosslinking (Irgacure 184) | STZ-induced male Wistar ratsSTZ-induced Landrace pigs | Enhanced collagen production and epidermal cell migration. Reduced inflammatory response. |
[105] | 2017 | Phenylboronic-modified chitosan (1.2 wt%)/poly(vinyl alcohol) (0.6 wt%)/benzaldehyde-capped PEG (0.6 wt%) hydrogel | Insulin (0.3 wt%) and L929 fibroblasts (1.2 × 106 cells/mL) | Schiff base reaction | STZ-induced Sprague-Dawley rats | Improved control of glucose levels in wound. Increased neovascularization and collagen deposition. Enhanced wound closure rate. |
[106] | 2016 | Sodium carboxymethylcellulose/propylene glycol hydrogel | Blechnum orientale extract (2–4% wt) | Hydrogen bonding | STZ-induced male Sprague-Dawley rats | Significant bactericidal and antioxidative effect. Enhanced re-epithelialization, fibroblast proliferation, collagen synthesis, and angiogenesis. |
[107] | 2016 | Gelatin methacrylate (15% w/v) hydrogel | Desferrioxamine (1% w/v) | UV photocrosslinking with Irgacure 2959 (0.5% w/v) | STZ-induced male Sprague-Dawley rats | Accelerated neovascularization, granulation tissue remodeling, and wound closure. |
4.2.2. Polyvinyl Alcohol (PVA)-Based Systems
4.2.3. Gelatin-Based Systems
4.2.4. Chitosan-Based Systems
4.2.5. Plasma-Based Systems
5. Conclusions
Author Contributions
Funding
Conflicts of Interest
References
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Güiza-Argüello, V.R.; Solarte-David, V.A.; Pinzón-Mora, A.V.; Ávila-Quiroga, J.E.; Becerra-Bayona, S.M. Current Advances in the Development of Hydrogel-Based Wound Dressings for Diabetic Foot Ulcer Treatment. Polymers 2022, 14, 2764. https://doi.org/10.3390/polym14142764
Güiza-Argüello VR, Solarte-David VA, Pinzón-Mora AV, Ávila-Quiroga JE, Becerra-Bayona SM. Current Advances in the Development of Hydrogel-Based Wound Dressings for Diabetic Foot Ulcer Treatment. Polymers. 2022; 14(14):2764. https://doi.org/10.3390/polym14142764
Chicago/Turabian StyleGüiza-Argüello, Viviana R., Víctor A. Solarte-David, Angie V. Pinzón-Mora, Jhair E. Ávila-Quiroga, and Silvia M. Becerra-Bayona. 2022. "Current Advances in the Development of Hydrogel-Based Wound Dressings for Diabetic Foot Ulcer Treatment" Polymers 14, no. 14: 2764. https://doi.org/10.3390/polym14142764