Tuning Protein Hydrogel Mechanics through Modulation of Nanoscale Unfolding and Entanglement in Postgelation Relaxation.
Tuning Protein Hydrogel Mechanics through Modulation of Nanoscale Unfolding and Entanglement in Postgelation Relaxation.
复制标题
通过调节凝胶后弛豫过程中的纳米级解折叠和缠结来调控蛋白质水凝胶力学性能
DOI：
10.1021/acsnano.2c02369
复制
发表时间：
2022-07-26
期刊：
影响因子：
17.1
通讯作者：
Dougan, Lorna
中科院分区：
文献类型：
--
作者：
Hughes, Matt D. G.;Cussons, Sophie;Mahmoudi, Najet;Brockwell, David J.;Dougan, Lorna
关键词：
球状折叠蛋白质是多功能的纳米级构建块，由于其特定和明确的折叠结构，可以创建具有机械鲁棒性和固有生物功能的生物材料。在网络形成过程中调节蛋白质构建块的纳米级展开（原位蛋白质展开）提供了控制蛋白质网络结构和力学的有力机会。在这里，我们控制蛋白质展开过程中形成的水凝胶，从化学交联的麦芽糖结合蛋白质使用配体结合和添加共溶质来调节蛋白质的动力学和热力学稳定性。体剪切流变学表征了结合和未结合蛋白质水凝胶的储能模量，并揭示了网络刚性（表征为储能模量的增加）与蛋白质热力学稳定性之间的相关性。此外，网络松弛行为的分析确定了一个交叉，从展开为主的政权纠缠为主的政权。原位蛋白质解折叠和缠结的控制提供了一个重要的途径，微调蛋白质水凝胶的结构，力学和动态松弛。这种预测控制将有利于未来的智能生物材料的应用，需要响应和动态调制的机械性能和生物功能。
Globular folded proteins are versatile nanoscale building blocks to create biomaterials with mechanical robustness and inherent biological functionality due to their specific and well-defined folded structures. Modulating the nanoscale unfolding of protein building blocks during network formation (in situ protein unfolding) provides potent opportunities to control the protein network structure and mechanics. Here, we control protein unfolding during the formation of hydrogels constructed from chemically cross-linked maltose binding protein using ligand binding and the addition of cosolutes to modulate protein kinetic and thermodynamic stability. Bulk shear rheology characterizes the storage moduli of the bound and unbound protein hydrogels and reveals a correlation between network rigidity, characterized as an increase in the storage modulus, and protein thermodynamic stability. Furthermore, analysis of the network relaxation behavior identifies a crossover from an unfolding dominated regime to an entanglement dominated regime. Control of in situ protein unfolding and entanglement provides an important route to finely tune the architecture, mechanics, and dynamic relaxation of protein hydrogels. Such predictive control will be advantageous for future smart biomaterials for applications which require responsive and dynamic modulation of mechanical properties and biological function.
登录
查看更多内容
影响因子：
16.6
作者：
Bian Q;Fu L;Li H
通讯作者：
Li H
影响因子：
41.2
作者：
Chaudhuri O;Gu L;Klumpers D;Darnell M;Bencherif SA;Weaver JC;Huebsch N;Lee HP;Lippens E;Duda GN;Mooney DJ
通讯作者：
Mooney DJ
影响因子：
3.9
作者：
Duan, Tianyu;Bian, Qingyuan;Li, Hongbin
通讯作者：
Li, Hongbin
影响因子：
5.5
作者：
Hanson, Benjamin S.;Dougan, Lorna
通讯作者：
Dougan, Lorna
影响因子：
3.3
作者：
Das, Atanu;Mukhopadhyay, Chaitali
通讯作者：
Mukhopadhyay, Chaitali