Synthetic Transient Crosslinks Program the Mechanics of Soft, Biopolymer-Based Materials.
Synthetic Transient Crosslinks Program the Mechanics of Soft, Biopolymer-Based Materials.
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DOI：
10.1002/adma.201706092
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发表时间：
2018-03
期刊：
影响因子：
--
通讯作者：
Smith DM
中科院分区：
文献类型：
--
作者：
Lorenz JS;Schnauß J;Glaser M;Sajfutdinow M;Schuldt C;Käs JA;Smith DM
肌动蛋白网络是一种自适应材料，能够实现活细胞的动态和静态功能。调整其潜在的结构和机械性能的一个核心因素是可逆连接的能力，即，瞬时交联，网络中的细丝。然而，天然交联剂在许多参数上有所不同。因此，由于其结构参数无法独立调节，系统地研究其尺寸和结合强度等基本特性的影响是不可行的。本文通过采用模块化策略从DNA和多肽中构建纯合成肌动蛋白交联剂，避免了这个问题。这些交联剂模拟了其天然对应物的直观和非规范机械特性。通过分离结合亲和力作为主要控制参数，表征了对肌动蛋白网络结构和动态行为的影响。由于出现的结构多态性，强交联剂和弱交联剂都产生了浓度依赖的三相行为。超过一定阈值，强结合导致非单调弹性脉冲，这是底层网络机械结构自毁的结果。模块化设计还促进了基于酶切的正交调节机制。该方法可用于指导进一步仿生元件的合理设计，以实现生物材料和细胞特性的可编程调制。
Actin networks are adaptive materials enabling dynamic and static functions of living cells. A central element for tuning their underlying structural and mechanical properties is the ability to reversibly connect, i.e., transiently crosslink, filaments within the networks. Natural crosslinkers, however, vary across many parameters. Therefore, systematically studying the impact of their fundamental properties like size and binding strength is unfeasible since their structural parameters cannot be independently tuned. Herein, this problem is circumvented by employing a modular strategy to construct purely synthetic actin crosslinkers from DNA and peptides. These crosslinkers mimic both intuitive and noncanonical mechanical properties of their natural counterparts. By isolating binding affinity as the primary control parameter, effects on structural and dynamic behaviors of actin networks are characterized. A concentration-dependent triphasic behavior arises from both strong and weak crosslinkers due to emergent structural polymorphism. Beyond a certain threshold, strong binding leads to a nonmonotonic elastic pulse, which is a consequence of self-destruction of the mechanical structure of the underlying network. The modular design also facilitates an orthogonal regulatory mechanism based on enzymatic cleaving. This approach can be used to guide the rational design of further biomimetic components for programmable modulation of the properties of biomaterials and cells.
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