由生物钟蛋白控制的定时材料自组装
Timed material self-assembly controlled by circadian clock proteins
AI总结：
本研究利用生物钟蛋白KaiB和KaiC实现胶体的时间依赖性交联，使材料自组装具有可编程动力学，通过调控浓度实现材料结构的昼夜节律振荡或稳定，为合成材料引入生物计时器控制概念。
摘要：
活性生物分子为赋予材料自主调节能力提供了一个强大但很大程度上尚未开发的机会。由于这些系统能够稳健地调节化学反应发生的时间和地点，它们能够为合成材料带来复杂的、类似生命的行为。在这里，我们通过使用功能化的生物钟蛋白KaiB和KaiC来工程化胶体的时间依赖性交联，从而实现了这一设计壮举。由此产生的材料以可编程的动力学进行自组装，通过KaiB-KaiC复合物的分子组装，产生材料特性的宏观变化。我们表明，胶体交联严格依赖于KaiC的磷酸化状态，其动力学与KaiB-KaiC复合物的形成同步。我们的显微图像分析和计算模型表明，胶体超结构的稳定性敏感地依赖于每个胶体连接处的Kai复合物数量。与我们的模型预测一致，高浓度在稳健的自组装阶段后使材料稳定而不溶解，而低浓度则允许材料结构进行昼夜节律振荡。这项工作引入了利用生物计时器控制合成材料的概念；并且更广泛地说，为使用基于蛋白质的反应网络赋予合成系统类似生命的功能特性打开了大门。
英文摘要：
Active biological molecules present a powerful, yet largely untapped, opportunity to impart autonomous regulation to materials. Because these systems can function robustly to regulate when and where chemical reactions occur, they have the ability to bring complex, life-like behavior to synthetic materials. Here, we achieve this design feat by using functionalized circadian clock proteins, KaiB and KaiC, to engineer time-dependent crosslinking of colloids. The resulting material self-assembles with programmable kinetics, producing macroscopic changes in material properties, via molecular assembly of KaiB-KaiC complexes. We show that colloid crosslinking depends strictly on the phosphorylation state of KaiC, with kinetics that are synced with KaiB-KaiC complexing. Our microscopic image analyses and computational models indicate that the stability of colloidal super-structures depends sensitively on the number of Kai complexes per colloid connection. Consistent with our model predictions, a high concentration stabilizes the material against dissolution after a robust self-assembly phase, while a low concentration allows circadian oscillation of material structure. This work introduces the concept of harnessing biological timers to control synthetic materials; and, more generally, opens the door to using protein-based reaction networks to endow synthetic systems with life-like functional properties.
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