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Enzymatic Reaction-Coupled, Cooperative Supramolecular Polymerization
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2024-05-15 , DOI: 10.1021/jacs.4c03588
Angshuman Das 1 , Saikat Ghosh 1 , Ananya Mishra 1 , Arka Som 1 , Vijay Basavaraj Banakar 1 , Sarit S. Agasti 1 , Subi J. George 1
Affiliation  

Nature employs sophisticated mechanisms to precisely regulate self-assembly and functions within biological systems, exemplified by the formation of cytoskeletal filaments. Various enzymatic reactions and auxiliary proteins couple with the self-assembly process, meticulously regulating the length and functions of resulting macromolecular structures. In this context, we present a bioinspired, reaction-coupled approach for the controlled supramolecular polymerization in synthetic systems. To achieve this, we employ an enzymatic reaction that interfaces with the adenosine triphosphate (ATP)-templated supramolecular polymerization of naphthalene diimide monomers (NSG). Notably, the enzymatic production of ATP (template) plays a pivotal role in facilitating reaction-controlled, cooperative growth of the NSG monomers. This growth process, in turn, provides positive feedback to the enzymatic production of ATP, creating an ideal reaction-coupled assembly process. The success of this approach is further evident in the living-growth characteristic observed during seeding experiments, marking this method as the pioneering instance where reaction-coupled self-assembly precisely controls the growth kinetics and structural aspects of supramolecular polymers in a predictive manner, akin to biological systems.

中文翻译:


酶促反应偶联、协同超分子聚合



大自然采用复杂的机制来精确调节生物系统内的自组装和功能,细胞骨架丝的形成就是例证。各种酶促反应和辅助蛋白质与自组装过程相结合,精心调节所得大分子结构的长度和功能。在这种情况下,我们提出了一种受生物启发的反应耦合方法,用于合成系统中受控的超分子聚合。为了实现这一目标,我们采用了一种酶促反应,该反应与三磷酸腺苷 (ATP) 模板的萘二酰亚胺单体 (NSG) 超分子聚合反应相结合。值得注意的是,ATP(模板)的酶促生产在促进 NSG 单体的反应控制、协同生长方面发挥着关键作用。反过来,这个生长过程为 ATP 的酶促生产提供正反馈,从而创建理想的反应耦合组装过程。这种方法的成功在播种实验期间观察到的活体生长特征中得到进一步证明,这标志着该方法是反应耦合自组装以预测方式精确控制超分子聚合物的生长动力学和结构方面的开创性实例,类似于到生物系统。
更新日期:2024-05-15
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