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A“T.E.S.T.”hydrogel bioadhesive assisted by corneal cross-linking for in situ sutureless corneal repair

Bioactive Materials 2023年第7期25卷 333-346页

作者： Meiyan Li Ruoyan Wei Chang Liu Haowei Fang Weiming Yang Yunzhe Wang Yiyong Xian Kunxi Zhang Yong He Xingtao Zhou Department of Ophthalmology EYE&ENT Hospital of Fudan University ShanghaiChina NHC Key Laboratory of Myopia(Fudan University) ShanghaiChina State Key Laboratory of Fluid Power and Mechatronic Systems School of Mechanical EngineeringZhejiang UniversityHangzhouChina Shanghai Research Center of Ophthalmology and Optometry ShanghaiChina Department of Ophthalmology Children’s Hospital of Fudan UniversityNational Children’s Medical CenterShanghaiChina Department of Polymer Materials School of Materials Science and EngineeringShanghai UniversityShanghaiChina

Corneal transplantation is an effective clinical treatment for corneal diseases,which,however,is limited by donor corneas.It is of great clinical value to develop bioadhesive corneal patches with functions of“Transparency”and“Epithelium&Stroma generation”,as well as“Suturelessness”and“toughness”.To simultaneously meet the“T.E.S.T.”requirements,a light-curable hydrogel is designed based on methacryloylated gelatin(GelMA),Pluronic F127 diacrylate(F127DA)&Aldehyded Pluronic F127(AF127)co-assembled bi-functional micelles and collagen type I(COL I),combined with clinically applied corneal cross-linking(CXL)technology for repairing damaged cornea.The patch formed after 5 min of ultraviolet irradiation possesses transparent,highly tough,and strongly bio-adhesive performance.Multiple cross-linking makes the patch withstand deformation near 600%and exhibit a burst pressure larger than 400 mmHg,significantly higher than normal intraocular pressure(10-21 mmHg).Besides,the slower degradation than GelMA-F127DA&AF127 hydrogel without COL I makes hydrogel patch stable on stromal beds in vivo,supporting the regrowth of corneal epithelium and stroma.The hydrogel patch can replace deep corneal stromal defects and well bio-integrate into the corneal tissue in rabbit models within 4 weeks,showing great potential in surgeries for keratoconus and other corneal diseases by combining with CXL.

关键词： tough hydrogel Bioadhesives Corneal patch CXL Sutureless repair

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Molecular design of an ultra-strong tissue adhesive hydrogel with tunable multifunctionality

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Bioactive Materials 2023年第11期29卷 214-229页

作者： Yuting Zheng Avijit Baidya Nasim Annabi Department of Chemical and Biomolecular Engineering University of Californi1Los AngelesLos AngelesCA90095United States Department of Bioengineering University of Californi1Los AngelesLos AngelesCA90095United States

Designing adhesive hydrogels with optimal properties for the treatment of injured tissues is challenging due to the tradeoff between material stiffness and toughness while maintaining adherence to wet tissue surfaces. In most cases, bioadhesives with improved mechanical strength often lack an appropriate elastic compliance, hindering their application for sealing soft, elastic, and dynamic tissues. Here, we present a novel strategy for engineering tissue adhesives in which molecular building blocks are manipulated to allow for precise control and optimization of the various aforementioned properties without any tradeoffs. To introduce tunable mechanical properties and robust tissue adhesion, the hydrogel network presents different modes of covalent and noncovalent interactions using N-hydroxysuccinimide ester (NHS) conjugated alginate (Alg-NHS), poly (ethylene glycol) diacrylate (PEGDA), tannic acid (TA), and Fe^(3+) ions. Through combining and tuning different molecular interactions and a variety of crosslinking mechanisms, we were able to design an extremely elastic (924%) and tough (4697 kJ/m3) multifunctional hydrogel that could quickly adhere to wet tissue surfaces within 5 s of gentle pressing and deform to support physiological tissue function over time under wet conditions. While Alg-NHS provides covalent bonding with the tissue surfaces, the catechol moieties of TA molecules synergistically adopt a mussel-inspired adhesive mechanism to establish robust adherence to the wet tissue. The strong adhesion of the engineered bioadhesive patch is showcased by its application to rabbit conjunctiva and porcine cornea. Meanwhile, the engineered bioadhesive demonstrated painless detachable characteristics and in vitro biocompatibility. Additionally, due to the molecular interactions between TA and Fe3+, antioxidant and antibacterial properties required to support the wound healing pathways were also highlighted. Overall, by tuning various molecular interactions, we were able to develop a single-hydrogel platform wit

关键词： Molecular engineering tough hydrogel Bioadhesive Multifunctionality

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蚕丝蛋白凝胶的结构与性能

蚕丝蛋白凝胶的结构与性能

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中国化学会2017全国高分子学术论文报告会

作者：苏帝翰姚萌邵正中聚合物分子工程国家重点实验室复旦大学先进材料实验室和高分子科学系

众所周知,溶液中的丝蛋白能够形成以β-折叠为主的物理交联点（区域）而产生凝胶网络,这是个热力学控制的过程。但由于力学性能较差,普通的再生蚕丝蛋白凝胶材料在若干应用上受到了较大的限制。我们在实践中发现,若采用适当的方法控制β... 详细信息

众所周知,溶液中的丝蛋白能够形成以β-折叠为主的物理交联点（区域）而产生凝胶网络,这是个热力学控制的过程。但由于力学性能较差,普通的再生蚕丝蛋白凝胶材料在若干应用上受到了较大的限制。我们在实践中发现,若采用适当的方法控制β-折叠区域的尺寸和均匀性,就能够在很大的程度上提高丝蛋白凝胶的力学性能。例如,辣根过氧化物酶能对桑蚕丝蛋白水溶液实施先期预（化学）交联,以形成交联不充分但丝蛋白分子链受限的"第一"交联网络;然后将由此酶化学交联的丝蛋白凝胶浸泡于能促进丝蛋白分子链构象发生β-折叠转变的乙醇溶液中,又可形成物理交联为主的"第二"网络,由此得到一类透明性好、模量高、韧性强且具有生物相容性的桑蚕丝蛋白水凝胶。另一方面,当将蚕丝蛋白的凝胶体系变化为恰当的离子液体（β-折叠的良溶剂）/水（β-折叠的非溶剂）后,所得到的丝蛋白凝胶不仅有着出色的力学性能,而且还具备了"不干"的特性

关键词： regenerated silk fibroin restricted network double networks,nanofibrils tough hydrogel

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