Photoinduced Dithiolane Crosslinking for Multiresponsive Dynamic Hydrogels,Advanced Materials

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Photoinduced Dithiolane Crosslinking for Multiresponsive Dynamic Hydrogels
Advanced Materials ( IF 27.4 ) Pub Date : 2023-01-30 , DOI: 10.1002/adma.202211209
Benjamin R Nelson _{1,

2} , Bruce E Kirkpatrick _{1,

2,

3} , Connor E Miksch _{1,

2} , Matthew D Davidson _{1,

2} , Nathaniel P Skillin _{1,

2,

3} , Grace K Hach _{1,

2} , Alex Khang _{1,

2} , Sydney N Hummel ₁ , Benjamin D Fairbanks ₁ , Jason A Burdick _{1,

2} , Christopher N Bowman _{1,

4} , Kristi S Anseth _{1,

2,

4}

Affiliation

While many hydrogels are elastic networks crosslinked by covalent bonds, viscoelastic hydrogels with adaptable crosslinks are increasingly being developed to better recapitulate time and position-dependent processes found in many tissues. In this work, 1,2-dithiolanes are presented as dynamic covalent photocrosslinkers of hydrogels, resulting in disulfide bonds throughout the hydrogel that respond to multiple stimuli. Using lipoic acid as a model dithiolane, disulfide crosslinks are formed under physiological conditions, enabling cell encapsulation via an initiator-free light-induced dithiolane ring-opening photopolymerization. The resulting hydrogels allow for multiple photoinduced dynamic responses including stress relaxation, stiffening, softening, and network functionalization using a single chemistry, which can be supplemented by permanent reaction with alkenes to further control network properties and connectivity using irreversible thioether crosslinks. Moreover, complementary photochemical approaches are used to achieve rapid and complete sample degradation via radical scission and post-gelation network stiffening when irradiated in the presence of reactive gel precursor. The results herein demonstrate the versatility of this material chemistry to study and direct 2D and 3D cell-material interactions. This work highlights dithiolane-based hydrogel photocrosslinking as a robust method for generating adaptable hydrogels with a range of biologically relevant mechanical and chemical properties that are varied on demand.

中文翻译：

用于多响应动态水凝胶的光诱导二硫环交联

虽然许多水凝胶是通过共价键交联的弹性网络，但具有适应联的粘弹性水凝胶正在越来越多地被开发出来，以更好地概括许多组织中发现的时间和位置依赖性过程。在这项工作中，1,2-二硫代烷被呈现为水凝胶的动态共价光交联剂，导致整个水凝胶中产生响应多种刺激的二硫键。使用硫辛酸作为模型二硫代烷，在生理条件下形成二硫键交联，通过无引发剂的光诱导二硫代烷开环光聚合实现细胞包封。所得水凝胶允许使用单一化学成分进行多种光诱导动态响应，包括应力松弛、硬化、软化和网络功能化，这可以通过与烯烃的永久反应来补充，以使用不可逆的硫醚交联进一步控制网络特性和连接性。此外，在反应性凝胶前体存在下照射时，使用互补光化学方法通过自由基切割和凝胶后网络硬化实现快速和完全的样品降解。本文的结果证明了这种材料化学在研究和指导 2D 和 3D 细胞-材料相互作用方面的多功能性。这项工作强调了基于二硫环的水凝胶光交联是一种强大的方法，可用于生成适应性强的水凝胶，这些水凝胶具有一系列生物相关的机械和化学性质，可根据需求变化。

更新日期：2023-01-30

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