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由最小构建块构成的反馈驱动的自主组装与拆卸循环。

Feedback driven autonomous cycles of assembly and disassembly from minimal building blocks.

作者信息

Reja Antara, Jha Sangam, Sreejan Ashley, Pal Sumit, Bal Subhajit, Gadgil Chetan, Das Dibyendu

机构信息

Department of Chemical Sciences and Centre for Advanced Functional Materials, Indian Institute of Science Education and Research (IISER) Kolkata, Mohanpur, 741246, India.

Chemical Engineering and Process Development, CSIR-National Chemical Laboratory, Pune, 411008, India.

出版信息

Nat Commun. 2024 Nov 18;15(1):9980. doi: 10.1038/s41467-024-54197-y.

Abstract

The construction of complex systems by simple chemicals that can display emergent network dynamics might contribute to our understanding of complex behavior from simple organic reactions. Here we design single amino acid/dipeptide-based systems that exhibit multiple periodic changes of (dis)assembly under non-equilibrium conditions in closed system, importantly in the absence of evolved biocatalysts. The two-component based building block exploits pH driven non-covalent assembly and time-delayed accelerated catalysis from self-assembled state to install orthogonal feedback loops with a single batch of reactants. Mathematical modelling of the reaction network establishes that the oscillations are transient for this network structure and helps to predict the relative contribution of the feedback loop to the ability of the system to exhibit such transient oscillation. Such autonomous systems with purely synthetic molecules are the starting point that can enable the design of active materials with emergent properties.

摘要

由能够展现出涌现网络动力学的简单化学物质构建复杂系统,这可能有助于我们从简单有机反应来理解复杂行为。在此,我们设计了基于单个氨基酸/二肽的系统,该系统在封闭体系的非平衡条件下呈现出多次(解)组装的周期性变化,重要的是,这一过程无需进化的生物催化剂。基于双组分的构建模块利用pH驱动的非共价组装以及从自组装状态开始的时间延迟加速催化,通过一批反应物建立正交反馈回路。反应网络的数学建模表明,对于这种网络结构,振荡是瞬态的,并且有助于预测反馈回路对系统展现此类瞬态振荡能力的相对贡献。这种具有纯合成分子的自主系统是能够设计具有涌现特性的活性材料的起点。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ed8a/11574191/b8ab200fa1c2/41467_2024_54197_Fig1_HTML.jpg

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