Photodegradable, Photoadaptable Hydrogels via Radical-Mediated Disulfide Fragmentation Reaction.
Photodegradable, Photoadaptable Hydrogels via Radical-Mediated Disulfide Fragmentation Reaction.
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DOI：
10.1021/ma200202w
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发表时间：
2011-04-26
期刊：
影响因子：
5.5
通讯作者：
Anseth KS
中科院分区：
文献类型：
--
作者：
Fairbanks BD;Singh SP;Bowman CN;Anseth KS
已经采用了各种技术来赋予合成水凝胶生物响应性，用于递送治疗剂以及研究和操纵生物过程和组织发育。这样的技术和材料包括随着pH的变化而溶胀和去溶胀的凝胶、在生理温度下收缩的热敏性凝胶、以及在通过细胞分泌的酶进行肽分解时降解的肽交联水凝胶。在本文中，我们报告了一种独特的方法来光化学变形和降解二硫化物交联的水凝胶，减轻光衰减和低量子产率的挑战，允许在低光强度（10 mW/cm 2，365 nm）下在120 s内降解高达2 mm厚的水凝胶。通过氧化硫醇官能化的4臂聚（乙二醇）大分子形成水凝胶。然后将这些二硫化物交联的水凝胶在酰基次膦酸锂光引发剂溶液中溶胀。在暴露于光时，光生自由基引发多个断裂和二硫键交换反应，允许并促进光变形、光焊接和光降解。这种新的，但简单的，方法来产生光适应性水凝胶预示着细胞响应的机械和地形动态基板的研究，以及通过焊接的固体基板的新的结晶。本文描述的原理和技术不仅对水凝胶材料有影响，而且对更广泛的光适应性聚合物也有影响。
Various techniques have been adopted to impart a biological responsiveness to synthetic hydrogels for the delivery of therapeutic agents as well as the study and manipulation of biological processes and tissue development. Such techniques and materials include polyelectrolyte gels that swell and deswell with changes in pH, thermosensitive gels that contract at physiological temperatures, and peptide cross-linked hydrogels that degrade upon peptidolysis by cell-secreted enzymes. Herein we report a unique approach to photochemically deform and degrade disulfide cross-linked hydrogels, mitigating the challenges of light attenuation and low quantum yield, permitting the degradation of hydrogels up to 2 mm thick within 120 s at low light intensities (10 mW/cm2 at 365 nm). Hydrogels were formed by the oxidation of thiol-functionalized 4-armed poly(ethylene glycol) macromolecules. These disulfide cross-linked hydrogels were then swollen in a lithium acylphosphinate photoinitiator solution. Upon exposure to light, photogenerated radicals initiate multiple fragmentation and disulfide exchange reactions, permitting and promoting photodeformation, photowelding, and photodegradation. This novel, but simple, approach to generate photoadaptable hydrogels portends the study of cellular response to mechanically and topographically dynamic substrates as well as novel encapsulations by the welding of solid substrates. The principles and techniques described herein hold implications for more than hydrogel materials but also for photoadaptable polymers more generally.
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影响因子：
29.4
作者：
Kloxin, Christopher J.;Scott, Timothy F.;Bowman, Christopher N.
通讯作者：
Bowman, Christopher N.
影响因子：
56.9
作者：
Scott, TF;Schneider, AD;Bowman, CN
通讯作者：
Bowman, CN
DOI：
10.1073/pnas.0737381100
发表时间：
2003-04-29
影响因子：
11.1
作者：
Lutolf, MP;Lauer-Fields, JL;Hubbell, JA
通讯作者：
Hubbell, JA
影响因子：
16.6
作者：
Li, Chengming;Madsen, Jeppe;Lewis, Andrew L.
通讯作者：
Lewis, Andrew L.
影响因子：
16.6
作者：
Kim, Wookhyun;Thevenot, Julie;Chaikof, Elliot L.
通讯作者：
Chaikof, Elliot L.