Self-healing poly(acrylic acid) hydrogels fabricated by hydrogen bonding and Fe³⁺ ion cross-linking for cartilage tissue engineering

Abstract

Autonomous self-healing hydrogels were achieved through a dynamic combination of hydrogen bonding and ferric ion (Fe³⁺) migration. N,N′-methylenebis (acrylamide) (MBA), a cross-linking agent, was added in this study. Poly(acrylic acid) (PAA)/Fe³⁺ and PAA–MBA/Fe³⁺ hydrogels were prepared by introducing Fe³⁺ into the PAA hydrogel network. The ionic bonds were formed between Fe³⁺ ions and carboxyl groups. The microstructure, mechanical properties, and composition of hydrogels were characterized by field emission scanning electron microscopy and Fourier transform infrared spectroscopy. The experimental results showed that PAA/Fe³⁺ and PAA–MBA/Fe³⁺ hydrogels healed themselves without external stimuli. The PAA/Fe³⁺ hydrogel exhibited good mechanical properties, i.e., the tensile strength of 50 kPa, the breaking elongation of 750%, and the self-healing efficiency of 82%. Meanwhile, the PAA–MBA/Fe³⁺ hydrogel had a tensile strength of 120 kPa. These fabricated hydrogels are biocompatible, which may have promising applications in cartilage tissue engineering.

Graphical abstract

Keywords

poly(acrylic acid) / hydrogel / cartilage tissue / self-healing

References

[1] Francis Suh J K, Matthew H W T . Application of chitosan-based polysaccharide biomaterials in cartilage tissue engineering: a review.Biomaterials, 2000, 21(24): 2589–2598

[2] Martel-Pelletier J, Boileau C, Pelletier J P, . Cartilage in normal and osteoarthritis conditions.Best Practice & Research. Clinical Rheumatology, 2008, 22(2): 351–384

[3] Hunter W. Of the structure and disease of articulating cartilages. 1743. Clinical Orthopaedics and Related Research, 1995, (317): 3–6

[4] Buckwalter J A, Lane N E . Athletics and osteoarthritis.The American Journal of Sports Medicine, 1997, 25(6): 873–881

[5] Martin J A, Buckwalter J A . Roles of articular cartilage aging and chondrocyte senescence in the pathogenesis of osteoarthritis.The Iowa Orthopaedic Journal, 2001, 21: 1–7

[6] Martin J A, Buckwalter J A . Aging, articular cartilage chondrocyte senescence and osteoarthritis.Biogerontology, 2002, 3(5): 257–264

[7] de Windt T S, Vonk L A, Brittberg M, . Treatment and prevention of (early) osteoarthritis using articular cartilage repair ― fact or fiction? A systematic review.Cartilage, 2013, 4(3 Suppl): 5S–12S

[8] Chang C-H, Lin F-H, Kuo T-F, . Cartilage tissue engineering.Biomedical Engineering: Applications, Basis and Communications, 2005, 17(2): 61–71

[9] Solchaga L A, Goldberg V M, Caplan A I . Cartilage regeneration using principles of tissue engineering.Clinical Orthopaedics and Related Research, 2001, 391(Suppl): S161–S170

[10] Buckwalter J A, Mankin H J . Articular cartilage: degeneration and osteoarthritis, repair, regeneration, and transplantation.Instructional Course Lectures, 1998, 47: 487–504

[11] Widuchowski W, Widuchowski J, Trzaska T . Articular cartilage defects: study of 25,124 knee arthroscopies.Knee, 2007, 14(3): 177–182

[12] Athanasiou K A, Shah A R, Hernandez R J, . Basic science of articular cartilage repair.Clinics in Sports Medicine, 2001, 20(2): 223–247

[13] Hayes D W Jr, Brower R L, John K J . Articular cartilage.Anatomy, injury, and repair. Clinics in Podiatric Medicine and Surgery, 2001, 18(1): 35–53

[14] Hunziker E B . Articular cartilage repair: basic science and clinical progress.A review of the current status and prospects. Osteoarthritis and Cartilage, 2002, 10(6): 432–463

[15] Zheng Q, Ma Z, Gong S . Multi-stimuli-responsive self-healing metallo–supramolecular polymer nanocomposites.Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2016, 4(9): 3324–3334

[16] Song M M, Wang Y M, Liang X Y, . Functional materials with self-healing properties: a review.Soft Matter, 2019, 15(33): 6615–6625

[17] Beddoes C M, Whitehouse M R, Briscoe W H, . Hydrogels as a replacement material for damaged articular hyaline cartilage.Materials, 2016, 9(6): 443

[18] Li L, Yu F, Zheng L, . Natural hydrogels for cartilage regeneration: modification, preparation and application.Journal of Orthopaedic Translation, 2019, 17: 26–41

[19] Liu J, Qu S, Suo Z, . Functional hydrogel coatings.National Science Review, 2021, 8(2): nwaa254

[20] Calvert P . Hydrogels for soft machines.Advanced Materials, 2009, 21(7): 743–756

[21] Taylor D L, Panhuis M I H . Self-healing hydrogels.Advanced Materials, 2016, 28(41): 9060–9093

[22] Hillewaere X K D, Du Prez F E . Fifteen chemistries for autonomous external self-healing polymers and composites.Progress in Polymer Science, 2015, 49–50: 121–153

[23] Bakarich S E, Gorkin R, Panhuis M I H, . Three-dimensional printing fiber reinforced hydrogel composites.ACS Applied Materials & Interfaces, 2014, 6(18): 15998–16006

[24] Yu F, Cao X, Du J, . Multifunctional hydrogel with good structure integrity, self-healing, and tissue-adhesive property formed by combining die is alder click reaction and acylhydrazone bond.ACS Applied Materials & Interfaces, 2015, 7(43): 24023–24031

[25] Yang L, Wang Z, Fei G, . Polydopamine particles reinforced poly(vinyl alcohol) hydrogel with NIR light triggered shape memory and self-healing capability.Macromolecular Rapid Communications, 2017, 38(23): 1700421

[26] Yang W J, Tao X, Zhao T, . Antifouling and antibacterial hydrogel coatings with self-healing properties based on a dynamic disulfide exchange reaction.Polymer Chemistry, 2015, 6(39): 7027–7035

[27] Tie J, Liu H, Lv J, . Multi-responsive, self-healing and adhesive PVA based hydrogels induced by the ultrafast complexation of Fe³⁺ ions.Soft Matter, 2019, 15(37): 7404–7411

[28] Zhang H, Xia H, Zhao Y . Poly(vinyl alcohol) hydrogel can autonomously self-heal.ACS Macro Letters, 2012, 1(11): 1233–1236

[29] Okay O. In: Seiffert S, ed. Supramolecular Polymer Networks and Gels. Springer, 2015

[30] Deng Y, Huang M, Sun D, . Dual physically cross-linked κ-carrageenan-based double network hydrogels with superior self-healing performance for biomedical application.ACS Applied Materials & Interfaces, 2018, 10(43): 37544–37554

[31] Zhou H, Xu G, Li J, . Preparation and self-healing behaviors of poly(acrylic acid)/cerium ions double network hydrogels.Macromolecular Research, 2015, 23(12): 1098–1102

[32] Dalei G, Das S . Polyacrylic acid-based drug delivery systems: a comprehensive review on the state-of-art.Journal of Drug Delivery Science and Technology, 2022, 78: 103988

[33] Peng F, Li G, Liu X, . Redox-responsive gel–sol/sol–gel transition in poly(acrylic acid) aqueous solution containing Fe(III) ions switched by light.Journal of the American Chemical Society, 2008, 130(48): 16166–16167

[34] Anjum S, Gurave P, Badiger M V, . Design and development of trivalent aluminum ions induced self healing polyacrylic acid novel hydrogels.Polymer, 2017, 126: 196–205

[35] Gosset M, Berenbaum F, Thirion S, . Primary culture and phenotyping of murine chondrocytes.Nature Protocols, 2008, 3(8): 1253–1260

[36] Gumbiner B M . Cell adhesion: the molecular basis of tissue architecture and morphogenesis.Cell, 1996, 84(3): 345–357

[37] Parker K K, Brock A L, Brangwynne C, . Directional control of lamellipodia extension by constraining cell shape and orienting cell tractional forces.FASEB Journal, 2002, 16(10): 1195–1204

RIGHTS & PERMISSIONS

Higher Education Press