IF 3.1 Q2 CHEMISTRY, MULTIDISCIPLINARY ChemSystemsChem Pub Date : 2024-08-21 DOI:10.1002/syst.202400056
Iris B. A. Smokers, Brent S. Visser, Dr. Wojciech P. Lipiński, Dr. Karina K. Nakashima, Dr. Evan Spruijt
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摘要

相分离隔室可以定位(生物)化学反应并影响其动力学。人们认为,无论是在以生物分子凝聚物形式存在的现存生命中,还是在以凝聚原胞形式存在的生命起源中,它们都扮演着重要的角色。然而,实验测试凝聚态对不同反应的影响既具有挑战性又耗费时间。因此,我们使用一个数值模型来探索相分离液滴对不同化学反应体系的动力学和结果的影响,其中我们改变了凝聚态液滴的体积和反应物的分配。我们发现,在给定的反应物分配条件下,双分子反应的速率有一个最佳的稀释/凝聚相体积比。此外,共蒸物还能加速聚合和自我复制反应,从而形成更长的聚合物。最后,我们还发现,在单相体系中不会出现持续振荡的浓度条件下,凝聚态有机物可以 "拯救 "振荡的反应网络。我们的研究结果表明,共渗物可以引导多种反应的结果,并对产率、反应途径选择、产物长度和新兴功能等基本方面产生影响。这可能会对生命起源、合成细胞以及生物凝聚物的命运和功能产生深远影响。
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Phase-Separated Droplets Can Direct the Kinetics of Chemical Reactions Including Polymerization, Self-Replication and Oscillating Networks

Phase-separated compartments can localize (bio)chemical reactions and influence their kinetics. They are believed to play an important role both in extant life in the form of biomolecular condensates and at the origins of life as coacervate protocells. However, experimentally testing the influence of coacervates on different reactions is challenging and time-consuming. We therefore use a numerical model to explore the effect of phase-separated droplets on the kinetics and outcome of different chemical reaction systems, where we vary the coacervate volume and partitioning of reactants. We find that the rate of bimolecular reactions has an optimal dilute/coacervate phase volume ratio for a given reactant partitioning. Furthermore, coacervates can accelerate polymerization and self-replication reactions and lead to formation of longer polymers. Lastly, we find that coacervates can ‘rescue’ oscillating reaction networks in concentration regimes where sustained oscillations do not occur in a single-phase system. Our results indicate that coacervates can direct the outcome of a wide range of reactions and impact fundamental aspects such as yield, reaction pathway selection, product length and emergent functions. This may have far-reaching implications for origins of life, synthetic cells and the fate and function of biological condensates.

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