Preparation of collagen-polysaccharide composite hydrogels and research progress in biomedical applications_Journal of Biomedical Engineering

Authors：

XU Meihong ¹ ,  JIAO Enxiang ^1,2,3 , SUN Ziru ¹ , YUAN Kunshan ² , FENG Xiangyi ¹ , LIU Yuanbiao ^1,2 , GUO Kai ^1,2 , LI Kun ^1,2 ,  ZHANG Haijun ^1,2,3 , ZHANG Xuehai ¹

1. College of Materials Science and Engineering, Shandong University of Technology, Zibo, Shandong 255000, P. R. China;
2. National Local Joint Engineering Laboratory of Biomedical Material Modification Technology, Dezhou, Shandong 253000, P. R. China;
3. School of Medicine, Tongji University, Shanghai 200000, P. R. China;

Corresponding author：

JIAO Enxiang, Email: jiaoex@sdut.edu.cn

Keywords：

Collagen; Polysaccharide; Hydrogels; Biomedicine

DOI：

10.7507/1001-5515.202407008

Video：

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Collagen contains abundant cell binding motifs, which are conducive to adhesion, migration, and differentiation, maintain cell vitality and promote cell proliferation. However, pure collagen hydrogel has some shortcomings such as poor mechanical properties, poor thermal stability and fast degradation. Numerous studies have shown that the properties of collagen can be improved by combining it with natural polysaccharides such as alginate, chitosan, hyaluronic acid and cellulose. In this paper, the research status and biological application fields of four kinds of composite hydrogels, including collagen-alginate composite hydrogels, collagen-chitosan hydrogels, collagen-hyaluronic acid hydrogels and collagen-cellulose hydrogels, were summarized. The common preparation methods of four kinds of composite hydrogels were introduced, and the future development direction of collagen-based composite hydrogels was prospected.

Citation： XU Meihong, JIAO Enxiang, SUN Ziru, YUAN Kunshan, FENG Xiangyi, LIU Yuanbiao, GUO Kai, LI Kun, ZHANG Haijun, ZHANG Xuehai. Preparation of collagen-polysaccharide composite hydrogels and research progress in biomedical applications. Journal of Biomedical Engineering, 2024, 41(6): 1286-1292. doi: 10.7507/1001-5515.202407008 Copy

1.	Wang L, Hou W, Zhang Q, et al. Hierarchical self-Assembly of injectable alginate supramolecular nanofibril hydrogels for hemostasis in vivo. Adv Fiber Mater, 2024, 6(2): 489-500.
2.	Li H, Zhu X, Wang M, et al. Drug sustained release from degradable drug-loaded in-situ hydrogels in the posterior eye: A mechanistic model and analytical method. J Biomech, 2022, 136: 111052.
3.	Sun L, Xu Y, Han Y, et al. Collagen-based hydrogels for cartilage regeneration. Orthop Surg, 2023, 15(12): 3026-3045.
4.	Islam H B M Z, Krishna S B N, Imran A B. Enhancing the mechanical properties of hydrogels with vinyl-functionalized nanocrystalline cellulose as a green crosslinker. Nanotechnology, 2023, 34(50). DOI: 10.1088/1361-6528/acf93b.
5.	Okoro P D, Frayssinet A, De Oliveira S, et al. Combining biomimetic collagen/hyaluronan hydrogels with discogenic growth factors promotes mesenchymal stroma cell differentiation into nucleus pulposus like cells. Biomater Sci, 2023, 11(24): 7768-7783.
6.	Sardroud H A, Chen X B, Eames B F. Reinforcement of hydrogels with a 3D-printed polycaprolactone (PCL) structure enhances cell numbers and cartilage ECM production under compression. J Funct, 2023, 14(6): 313.
7.	El Soury M, García-García O D, Tarulli I, et al. Chitosan conduits enriched with fibrin-collagen hydrogel with or without adipose-derived mesenchymal stem cells for the repair of 15-mm-long sciatic nerve defect. Neural Regen Res, 2023, 18(6): 1378-1385.
8.	Ghazagh P, Frounchi M. Hydroxyapatite/alginate/polyvinyl alcohol/agar composite double-network hydrogels as injectable drug delivery microspheres. Chem Pap, 2024, 78(5): 2967-2976.
9.	Houben S, Pitet L M. Ionic crosslinking strategies for poly(acrylamide)/alginate hybrid hydrogels. React Funct Polym, 2023, 191: 105676.
10.	Tomic S L J, Radic M M B, Vukovic J S, et al. Alginate-based hydrogels and scaffolds for biomedical applications. Mar Drugs, 2023, 21(3): 177.
11.	Zdiri K, Cayla A, Elamri A, et al. Alginate-based bio-composites and their potential applications. JFB, 2022, 13(3): 117.
12.	Nakada M, Ishida H, Uchiyama H, et al. Disaggregation and fibrillation during sol-gel transition of alginate hydrogels. Int J Biol Macromol, 2024, 269(Pt 2): 131890.
13.	Gorshkova M Y, Vanchugova L V, Volkova I F, et al. Novel mucoadhesive carriers based on alginate-acrylamide hydrogels for drug delivery. Mendeleev Commun, 2022, 32(2): 189-191.
14.	Ahmad F, Mushtaq B, Ahmad S, et al. A novel composite of hemp fiber and alginate hydrogel for wound dressings. J Polym Environ, 2023, 31(6): 2294-2305.
15.	Kavand A, Noverraz F, Gerber-Lemaire S. Recent advances in alginate-based hydrogels for cell transplantation applications. Pharmaceutics, 2024, 16(4): 469.
16.	Krishna D V, Sankar M R. Extrusion based bioprinting of alginate based multicomponent hydrogels for tissue regeneration applications: State of the art. Mater Today Commun, 2023, 35: 105696.
17.	Hu X, Zhang Z, Wu H, et al. Progress in the application of 3D-printed sodium alginate-based hydrogel scaffolds in bone tissue repair. Mat Sci Eng C-Mater, 2023, 152: 213501.
18.	Ledo A M, Vining K H, Alonso M J, et al. Extracellular matrix mechanics regulate transfection and SOX9-directed differentiation of mesenchymal stem cells. Acta Biomater, 2020, 110: 153-163.
19.	Wang M, Yang Y, Han L, et al. Effect of three-dimensional ECM stiffness on cancer cell migration through regulating cell volume homeostasis. Biochem Bioph Res Co, 2020, 528(3): 459-465.
20.	Zheng H, Tian W, Yan H, et al. Rotary culture promotes the proliferation of MCF-7 cells encapsulated in three-dimensional collagen–alginate hydrogels via activation of the ERK1/2-MAPK pathway. Biomed Mater, 2012, 7(1): 015003.
21.	Mei E, Li S, Song J, et al. Self-assembling collagen/alginate hybrid hydrogels for combinatorial photothermal and immuno tumor therapy. Colloid Surface A, 2019, 577: 570-575.
22.	Sakai S, Yamamoto S, Hirami R, et al. Enzymatically gellable chitosan inks with enhanced printability by chitosan nanofibers for 3D printing of wound dressings. Eur Polym, 2024, 210: 112960.
23.	Kankariya Y, Chatterjee B. Biomedical application of chitosan and chitosan derivatives: a comprehensive review. Curr Pharm Design, 2023, 29(17): 1311-1325.
24.	Tang W, Wang J, Hou H, et al. Review: Application of chitosan and its derivatives in medical materials. Int J Biol Macromol, 2023, 240: 124398.
25.	Yang J Y, Chen Y, Zhao L, et al. Constructions and properties of physically cross-linked hydrogels based on natural polymers. Polym Rev, 2023, 63(3): 574-612.
26.	Guillén-Carvajal K, Valdez-Salas B, Beltrán-Partida E, et al. Chitosan, gelatin, and collagen hydrogels for bone regeneration. Polymers, 2023, 15(13): 2762.
27.	Sánchez-Cid P, Jiménez-Rosado M, Rubio-Valle J F, et al. Biocompatible and thermoresistant hydrogels based on collagen and chitosan. Polymers, 2022, 14(2): 272.
28.	Deepthi S, Nivedhitha Sundaram M, Deepti Kadavan J, et al. Layered chitosan-collagen hydrogel/aligned PLLA nanofiber construct for flexor tendon regeneration. Carbohydr Polym, 2016, 153: 492-500.
29.	Sparks H D, Sigaeva T, Tarraf S, et al. Biomechanics of wound healing in an equine limb model: effect of location and treatment with a peptide-modified collagen–chitosan hydrogel. ACS Biomater Sci, 2020, 7(1): 265-278.
30.	Salva E, Akdag A E, Alan S, et al. Evaluation of the effect of honey-containing chitosan/hyaluronic acid hydrogels on wound healing. Gels, 2023, 9(11): 856.
31.	Zhong S, Lu C, Liu H-Y, et al. Electrical and immune stimulation-based hydrogels synergistically realize scarless wound healing via amplifying endogenous electrophysiological function and promoting macrophage phenotype-switching. Chem Eng J, 2024, 491: 152048.
32.	O’Shea D G, Hodgkinson T, Curtin C M, et al. An injectable and 3D printable pro-chondrogenic hyaluronic acid and collagen type II composite hydrogel for the repair of articular cartilage defects. Biofabrication, 2024, 16(1): 015007.
33.	Shopperly L K, Spinnen J, Krüger J P, et al. Blends of gelatin and hyaluronic acid stratified by stereolithographic bioprinting approximate cartilaginous matrix gradients. J Biomed Mater Res B Appl Biomater, 2022, 110(10): 2310-2322.
34.	Yamamoto T, Randriantsilefisoa R, Sprecher C M, et al. Fabrication of collagen-hyaluronic acid cryogels by directional freezing mimicking cartilage arcade-like structure. Biomolecules, 2022, 12(12): 1809.
35.	Yuan T, He L, Yang J, et al. Conjugated icariin promotes tissue-engineered cartilage formation in hyaluronic acid/collagen hydrogel. Process Biochem, 2015, 50(12): 2242-2250.
36.	Rodler A, Samanta A, Goh W-J, et al. Engineering and characterization of a hydrogel mimicking subcutaneous interstitial space. Eur Polym, 2024, 205: 112739.
37.	Jia Y, Zhang X, Yang W, et al. A pH-responsive hyaluronic acid hydrogel for regulating the inflammation and remodeling of the ECM in diabetic wounds. J Mater Chem, 2022, 10(15): 2875-2888.
38.	Li Y, Dong X, Yao L, et al. Preparation and characterization of nanocomposite hydrogels based on self-assembling collagen and cellulose nanocrystals. Polymers, 2023, 15(5): 1308.
39.	Tudoroiu E-E, Kaya M G A, Titorencu I, et al. Design and evaluation of new wound dressings based on collagen-cellulose derivatives. Mater Design, 2023, 236(3): 112469.
40.	张霞, 周浩, 杨宇红, 等. 氧化纤维素增强胶原水凝胶. 高等学校化学学报 2015, 36(10): 2040-2046.
41.	Lohrasbi S, Mirzaei E, Karimizade A, et al. Collagen/cellulose nanofiber hydrogel scaffold: physical, mechanical and cell biocompatibility properties. Cellulose, 2019, 27(2): 927-940.
42.	Kutová A, Svorcík V. Bacterial nanocellulose and its medical usage. Chem Listy, 2022, 116(5): 308-315.
43.	Moraes P R F D S, Saska S, Barud H, et al. Bacterial cellulose/collagen hydrogel for wound healing. Mater Res, 2016, 19(1): 106-116.

1. Wang L, Hou W, Zhang Q, et al. Hierarchical self-Assembly of injectable alginate supramolecular nanofibril hydrogels for hemostasis in vivo. Adv Fiber Mater, 2024, 6(2): 489-500.
2. Li H, Zhu X, Wang M, et al. Drug sustained release from degradable drug-loaded in-situ hydrogels in the posterior eye: A mechanistic model and analytical method. J Biomech, 2022, 136: 111052.
3. Sun L, Xu Y, Han Y, et al. Collagen-based hydrogels for cartilage regeneration. Orthop Surg, 2023, 15(12): 3026-3045.
4. Islam H B M Z, Krishna S B N, Imran A B. Enhancing the mechanical properties of hydrogels with vinyl-functionalized nanocrystalline cellulose as a green crosslinker. Nanotechnology, 2023, 34(50). DOI: 10.1088/1361-6528/acf93b.
5. Okoro P D, Frayssinet A, De Oliveira S, et al. Combining biomimetic collagen/hyaluronan hydrogels with discogenic growth factors promotes mesenchymal stroma cell differentiation into nucleus pulposus like cells. Biomater Sci, 2023, 11(24): 7768-7783.
6. Sardroud H A, Chen X B, Eames B F. Reinforcement of hydrogels with a 3D-printed polycaprolactone (PCL) structure enhances cell numbers and cartilage ECM production under compression. J Funct, 2023, 14(6): 313.
7. El Soury M, García-García O D, Tarulli I, et al. Chitosan conduits enriched with fibrin-collagen hydrogel with or without adipose-derived mesenchymal stem cells for the repair of 15-mm-long sciatic nerve defect. Neural Regen Res, 2023, 18(6): 1378-1385.
8. Ghazagh P, Frounchi M. Hydroxyapatite/alginate/polyvinyl alcohol/agar composite double-network hydrogels as injectable drug delivery microspheres. Chem Pap, 2024, 78(5): 2967-2976.
9. Houben S, Pitet L M. Ionic crosslinking strategies for poly(acrylamide)/alginate hybrid hydrogels. React Funct Polym, 2023, 191: 105676.
10. Tomic S L J, Radic M M B, Vukovic J S, et al. Alginate-based hydrogels and scaffolds for biomedical applications. Mar Drugs, 2023, 21(3): 177.
11. Zdiri K, Cayla A, Elamri A, et al. Alginate-based bio-composites and their potential applications. JFB, 2022, 13(3): 117.
12. Nakada M, Ishida H, Uchiyama H, et al. Disaggregation and fibrillation during sol-gel transition of alginate hydrogels. Int J Biol Macromol, 2024, 269(Pt 2): 131890.
13. Gorshkova M Y, Vanchugova L V, Volkova I F, et al. Novel mucoadhesive carriers based on alginate-acrylamide hydrogels for drug delivery. Mendeleev Commun, 2022, 32(2): 189-191.
14. Ahmad F, Mushtaq B, Ahmad S, et al. A novel composite of hemp fiber and alginate hydrogel for wound dressings. J Polym Environ, 2023, 31(6): 2294-2305.
15. Kavand A, Noverraz F, Gerber-Lemaire S. Recent advances in alginate-based hydrogels for cell transplantation applications. Pharmaceutics, 2024, 16(4): 469.
16. Krishna D V, Sankar M R. Extrusion based bioprinting of alginate based multicomponent hydrogels for tissue regeneration applications: State of the art. Mater Today Commun, 2023, 35: 105696.
17. Hu X, Zhang Z, Wu H, et al. Progress in the application of 3D-printed sodium alginate-based hydrogel scaffolds in bone tissue repair. Mat Sci Eng C-Mater, 2023, 152: 213501.
18. Ledo A M, Vining K H, Alonso M J, et al. Extracellular matrix mechanics regulate transfection and SOX9-directed differentiation of mesenchymal stem cells. Acta Biomater, 2020, 110: 153-163.
19. Wang M, Yang Y, Han L, et al. Effect of three-dimensional ECM stiffness on cancer cell migration through regulating cell volume homeostasis. Biochem Bioph Res Co, 2020, 528(3): 459-465.
20. Zheng H, Tian W, Yan H, et al. Rotary culture promotes the proliferation of MCF-7 cells encapsulated in three-dimensional collagen–alginate hydrogels via activation of the ERK1/2-MAPK pathway. Biomed Mater, 2012, 7(1): 015003.
21. Mei E, Li S, Song J, et al. Self-assembling collagen/alginate hybrid hydrogels for combinatorial photothermal and immuno tumor therapy. Colloid Surface A, 2019, 577: 570-575.
22. Sakai S, Yamamoto S, Hirami R, et al. Enzymatically gellable chitosan inks with enhanced printability by chitosan nanofibers for 3D printing of wound dressings. Eur Polym, 2024, 210: 112960.
23. Kankariya Y, Chatterjee B. Biomedical application of chitosan and chitosan derivatives: a comprehensive review. Curr Pharm Design, 2023, 29(17): 1311-1325.
24. Tang W, Wang J, Hou H, et al. Review: Application of chitosan and its derivatives in medical materials. Int J Biol Macromol, 2023, 240: 124398.
25. Yang J Y, Chen Y, Zhao L, et al. Constructions and properties of physically cross-linked hydrogels based on natural polymers. Polym Rev, 2023, 63(3): 574-612.
26. Guillén-Carvajal K, Valdez-Salas B, Beltrán-Partida E, et al. Chitosan, gelatin, and collagen hydrogels for bone regeneration. Polymers, 2023, 15(13): 2762.
27. Sánchez-Cid P, Jiménez-Rosado M, Rubio-Valle J F, et al. Biocompatible and thermoresistant hydrogels based on collagen and chitosan. Polymers, 2022, 14(2): 272.
28. Deepthi S, Nivedhitha Sundaram M, Deepti Kadavan J, et al. Layered chitosan-collagen hydrogel/aligned PLLA nanofiber construct for flexor tendon regeneration. Carbohydr Polym, 2016, 153: 492-500.
29. Sparks H D, Sigaeva T, Tarraf S, et al. Biomechanics of wound healing in an equine limb model: effect of location and treatment with a peptide-modified collagen–chitosan hydrogel. ACS Biomater Sci, 2020, 7(1): 265-278.
30. Salva E, Akdag A E, Alan S, et al. Evaluation of the effect of honey-containing chitosan/hyaluronic acid hydrogels on wound healing. Gels, 2023, 9(11): 856.
31. Zhong S, Lu C, Liu H-Y, et al. Electrical and immune stimulation-based hydrogels synergistically realize scarless wound healing via amplifying endogenous electrophysiological function and promoting macrophage phenotype-switching. Chem Eng J, 2024, 491: 152048.
32. O’Shea D G, Hodgkinson T, Curtin C M, et al. An injectable and 3D printable pro-chondrogenic hyaluronic acid and collagen type II composite hydrogel for the repair of articular cartilage defects. Biofabrication, 2024, 16(1): 015007.
33. Shopperly L K, Spinnen J, Krüger J P, et al. Blends of gelatin and hyaluronic acid stratified by stereolithographic bioprinting approximate cartilaginous matrix gradients. J Biomed Mater Res B Appl Biomater, 2022, 110(10): 2310-2322.
34. Yamamoto T, Randriantsilefisoa R, Sprecher C M, et al. Fabrication of collagen-hyaluronic acid cryogels by directional freezing mimicking cartilage arcade-like structure. Biomolecules, 2022, 12(12): 1809.
35. Yuan T, He L, Yang J, et al. Conjugated icariin promotes tissue-engineered cartilage formation in hyaluronic acid/collagen hydrogel. Process Biochem, 2015, 50(12): 2242-2250.
36. Rodler A, Samanta A, Goh W-J, et al. Engineering and characterization of a hydrogel mimicking subcutaneous interstitial space. Eur Polym, 2024, 205: 112739.
37. Jia Y, Zhang X, Yang W, et al. A pH-responsive hyaluronic acid hydrogel for regulating the inflammation and remodeling of the ECM in diabetic wounds. J Mater Chem, 2022, 10(15): 2875-2888.
38. Li Y, Dong X, Yao L, et al. Preparation and characterization of nanocomposite hydrogels based on self-assembling collagen and cellulose nanocrystals. Polymers, 2023, 15(5): 1308.
39. Tudoroiu E-E, Kaya M G A, Titorencu I, et al. Design and evaluation of new wound dressings based on collagen-cellulose derivatives. Mater Design, 2023, 236(3): 112469.
40. 张霞, 周浩, 杨宇红, 等. 氧化纤维素增强胶原水凝胶. 高等学校化学学报 2015, 36(10): 2040-2046.
41. Lohrasbi S, Mirzaei E, Karimizade A, et al. Collagen/cellulose nanofiber hydrogel scaffold: physical, mechanical and cell biocompatibility properties. Cellulose, 2019, 27(2): 927-940.
42. Kutová A, Svorcík V. Bacterial nanocellulose and its medical usage. Chem Listy, 2022, 116(5): 308-315.
43. Moraes P R F D S, Saska S, Barud H, et al. Bacterial cellulose/collagen hydrogel for wound healing. Mater Res, 2016, 19(1): 106-116.

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