基于动态可逆共价键制备的自愈合水凝胶,因动态共价键能自发断裂与形成,且具有良好的生物相容性、无毒性等优点,从而成为自愈合水凝胶领域的研究热点。综述了国内外动态可逆共价键自愈合水凝胶的制备方法,及其在药物运输、伤口敷料、组织工程和生物传感器方面的应用研究进展。针对基于动态可逆共价键的自愈合水凝胶机械性能较弱、自愈合条件严格等缺点,提出了未来研究发展方向:设计具有多个动态可逆共价键的水凝胶、在温和条件下自愈合的水凝胶等,并对其在生物医学、智能材料等方面的应用前景做出了展望。
Self-healing hydrogels prepared based on dynamic reversible covalent bonds have become a research hotspot in the field of self-healing hydrogels because dynamic covalent bonds can spontaneously break and form,along with advantages like good biocompatibility and non-toxicity.In this paper,the preparation methods of dynamic reversible covalent self-healing hydrogels at home and abroad and their application research progress in drug transportation,wound dressing,tissue engineering and biosensor were reviewed.Aiming at the disadvantages of self-healing hydrogel based on dynamic reversible covalent bonds,such as weak mechanical properties and strict self-healing conditions,the future research directions were put forward:designing hydrogels with multiple dynamic reversible covalent bonds,self-healing hydrogels under mild conditions,etc.,and their application prospects in biomedicine,intelligent materials,etc.were also discussed.
[1] Perera M M,Ayres N.Dynamic covalent bonds in self-healing,shape memory,and controllable stiffness hydrogels[J].Polymer Chemistry,2020,11(8):1410-1423.
[2] Liu Y,Liu J,Yang H,et al.Dynamic covalent bond-based hydrogels with superior compressive strength,exceptional slice-resistance and self-healing properties[J].Soft Matter,2018,14(39):7950-7953.
[3] 刘瑞雪,陈纪超,李迎博.基于动态共价键和非共价键相互作用的自愈合水凝胶研究进展[J].轻工学报,2021,36(6):110-124.
[4] Cheng K C,Huang C F,Wei Y,et al.Novel chitosan-cellulose nanofiber self-healing hydrogels to correlate self-healing properties of hydrogels with neural regeneration effects[J].NPG Asia Materials,2019,11(1):25.
[5] Hauck S,Zager P,Halfter N,et al.Collagen/hyaluronan based hydrogels releasing sulfated hyaluronan improve dermal wound healing in diabetic mice via reducing inflammatory macrophage activity[J].Bioactive Materials,2021,6(12):4342-4359.
[6] Ye J,Fu S,Zhou S,et al.Advances in hydrogels based on dynamic covalent bonding and prospects for its biomedical application[J].European Polymer Journal,2020,139:110024.
[7] Jiao Y,Lu Y,Lu K Y,et al.Highly stretchable and self-healing cellulose nanofiber-mediated conductive hydrogel towards strain sensing application[J].Journal of Colloid and Interface Science,2021,597:171-181.
[8] Luo J H,Shi X S,Li L M,et al.An injectable and self-healing hydrogel with controlled release of curcumin to repair spinal cord injury[J].Bioactive Materials,2021,6(12):4816-4829.
[9] Hirayama C,Machida K,Noi K,et al.Distinct roles and actions of protein disulfide isomerase family enzymes in catalysis of nascent-chain disulfide bond formation[J].iScience,2021,24(4):102296-102296.
[10] Chen B,Zhou K,Xie Y,et al.Glutathione-mediated formation of disulfide bonds modulates the properties of myofibrillar protein gels at different temperatures[J].Food Chemistry,2021,364:130356-130356.
[11] Juho L,Phornwalan N,Arin K,et al.Malleable and recyclable thermoset network with reversible β-hydroxyl esters and disulfide bonds[J].Journal of Applied Polymer Science,2022,140(4):e53369.
[12] Luisa C,Paola B,Grazia M,et al.EAK hydrogels cross-linked by disulfide bonds:cys number and position are matched to performances[J].ACS Biomaterials Science & Engineering,2019,6(2):1154-1164.
[13] Ozay H,Iigin P,Ozay O.Novel hydrogels based on crosslinked chitosan with formyl-phosphazene using Schiff-base reaction[J].International Journal of Polymeric Materials and Polymeric Biomaterials,2021,70(4):246-255.
[14] Liao S S,Tang L Y,Qu J Q.Schiff-base-functionalized polymeric hydrogel with high stretchability and multifunction[J].Polymers for Advanced Technologies,2021,32(4):1844-1852.
[15] Jia L,Jun L,Fan Y,et al.In situ forming hydrogel of natural polysaccharides through Schiff base reaction for soft tissue adhesive and hemostasis[J].International Journal of Biological Macromolecules,2020,147:653-666.
[16] Jun P X,Yi L,Shan H.Hydrogels based on Schiff base linkages for biomedical applications[J].Molecules,2019,24(16):3005-3005.
[17] Guo R,Su Q,Zhang J,et al.Facile access to multisensitive and self-healing hydrogels with reversible and dynamic boronic ester and disulfide linkages[J].Biomacromolecules,2017,18(4):1356-1364.
[18] Zhao X,Pei D,Yang Y,et al.Green tea derivative driven smart hydrogels with desired functions for chronic diabetic wound treatment[J].Advanced Functional Materials,2021,31(18):2009442.
[19] Cai B,Luo Y,Guo Q,et al.A glucose-sensitive block glycopolymer hydrogel based on dynamic boronic ester bonds for insulin delivery[J].Carbohydrate Research,2017,445:32-39.
[20] Che Y,Zschoche S,Obst F,et al.Double-crosslinked reversible redox-responsive hydrogels based on disulfide-thiol interchange[J].Journal of Polymer Science Part A:Polymer Chemistry,2019,57(24):2590-2601.
[21] Chen M H,Ren X R,Dong L M,et al.Preparation of dynamic covalently crosslinking keratin hydrogels based on thiol/disulfide bonds exchange strategy[J].International Journal of Biological Macromolecules,2021,182:1259-1267.
[22] Joyner K,Song D,Hawkins R F,et al.A rational approach to form disulfide linked mucin hydrogels[J].Soft matter,2019,15(47):9632-9639.
[23] Fu B,Wang X,Chen Z,et al.Improved myocardial performance in infarcted rat heart by injection of disulfide-cross-linked chitosan hydrogels loaded with basic fibroblast growth factor[J].Journal of Materials Chemistry B,2022,2022,10(4):656-665.
[24] Su H,Zheng R,Jiang L,et al.Dextran hydrogels via disulfide-containing Schiff base formation:synthesis,stimuli-sensitive degradation and release behaviors[J].Carbohydrate Polymers,2021,265:118085.
[25] Liu S,Kang M,Li K,et al.Polysaccharide-templated preparation of mechanically-tough,conductive and self-healing hydrogels[J].Chemical Engineering Journal,2018,334:2222-2230.
[26] Grover G N,Braden R L,Christman Karen L.Oxime cross-linked injectable hydrogels for catheter delivery[J].Advanced Materials (Deerfield Beach,Fla.),2013,25(21):2937-42.
[27] 刘薇.高强度可自愈合双网络水凝胶的制备与性能研究[D].湘潭:湘潭大学,2020.
[28] Wang H,Zhu D,Paul A,et al.Covalently adaptable elastin-like protein-hyaluronic acid (ELP-HA) hybrid hydrogels with secondary thermoresponsive crosslinking for injectable stem cell delivery[J].Advanced Functional Materials,2017,27(28):1605609.
[29] Deng G,Li F,Yu H,et al.Dynamic hydrogels with an environmental adaptive self-healing ability and dual responsive sol-gel transitions[J].ACS Macro Letters,2012,1(2):275-279.
[30] Yang H S,Cho S,Eom Y,et al.Preparation of self-healable and spinnable hydrogel by dynamic boronate ester bond from hyperbranched polyglycerol and boronic acid-containing polymer[J].Macromolecular Research,2021,29(2):140-148.
[31] Lee S Y,Yang M,Seo J H,et al.Serially pH-modulated hydrogels based on boronate ester and polydopamine linkages for local cancer therapy[J].ACS Applied Materials & Interfaces,2021,13(2):2189-2203.
[32] An H,Bo Y,Chen D,et al.Cellulose-based self-healing hydrogel through boronic ester bonds with excellent biocompatibility and conductivity[J].RSC Advances,2020,10(19):11300-11310.
[33] 张丹.硼酸酯键交联的纤维素基自愈合水凝胶的制备与性能研究[D].南京:南京大学,2019.
[34] Ji F,Li J,Zhang G,et al.Alkaline monomer for mechanical enhanced and self-healing hydrogels based on dynamic borate ester bonds[J].Polymer,2019,184:121882.
[35] Wang M,Mo B,Chen B,et al.Self-healing quadruple-shape memory hydrogel based on imine,coordination,and borate bonds with tunable mechanical properties[J].Colloid and Polymer Science,2020,298(3):285-291.
[36] Agubata C O,Mbaoji C C,Nzekwe I T,et al.Biohydrogel based on dynamic covalent bonds for wound healing applications[J].Applied Sciences,2021,11(15):6945.
[37] Cao F,Ma G,Mei L,et al.Development of disulfide bond crosslinked antimicrobial peptide hydrogel[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2021,626:127026.
[38] Zhao X,Wu H,Guo B,et al.Antibacterial anti-oxidant electroactive injectable hydrogel as self-healing wound dressing with hemostasis and adhesiveness for cutaneous wound healing[J].Biomaterials,2017,122:34-47.
[39] Cao Y,Yao Y,Li Y,et al.Tunable keratin hydrogel based on disulfide shuffling strategy for drug delivery and tissue engineering[J].Journal of Colloid and Interface Science,2019,544:121-129.
[40] 杨越.二硫键交联的层层自组装微胶囊和水凝胶的制备及其药物控释应用[D].南昌:南昌大学,2018.
[41] 张永旺.近红外光响应的可注射水凝胶的制备及光控释药研究[D].北京:北京化工大学,2019.
[42] Tseng T C,Tao L,Hsieh F Y,et al.An injectable,self-healing hydrogel to repair the central nervous system[J].Advanced Materials,2015,27(23):3518-3524.
[43] Hsieh F Y,Tao L,Wei Y,et al.A novel biodegradable self-healing hydrogel to induce blood capillary formation[J].Npg Asia Materials,2017,9(3):e363.
[44] Dong R,Zhao X,Guo B,et al.Self-healing conductive injectable hydrogels with antibacterial activity as cell delivery carrier for cardiac cell therapy[J].ACS Applied Materials & Interfaces,2016,8(27):17138-17150.
[45] Choi Y,Park K,Choi H,et al.Self-healing,stretchable,biocompatible,and conductive alginate hydrogels through dynamic covalent bonds for implantable electronics[J].Polymers,2021,13(7):1133-1133.
[46] Han L,Lu X,Wang M,et al.A mussel-inspired conductive,self-adhesive,and self-healable tough hydrogel as cell stimulators and implantable bioelectronics[J].Small,2017,13(2):1601916.
[47] Wang X,Li Q,Guan Y,et al.Glucose oxidase-incorporated hydrogel thin film for fast optical glucose detecting under physiological conditions[J].Materials Today Chemistry,2016,1:7-14.
[48] 邱艺娟,林佳伟,秦济锐,等.双重动态共价键交联纳米纤维素导电水凝胶及其柔性传感器[J].化工进展,2022,41(8):4406-4416.
基金资助
上海市自然科学基金项目面上项目(21ZR1426200);国家自然科学基金(51703123)
PDF
