Institute for Molecules and Materials, Radboud University Nijmegen, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands.
J Am Chem Soc. 2023 Apr 5;145(13):7559-7568. doi: 10.1021/jacs.3c00908. Epub 2023 Mar 24.
Prebiotic environments are dynamic, containing a range of periodic and aperiodic variations in reaction conditions. However, the impact of the temporal dynamics of environmental conditions upon prebiotic chemical reaction networks has not been investigated. Here, we demonstrate how the magnitude and rate of temporal fluctuations of the catalysts Ca and hydroxide control the product distributions of the formose reaction. Surprisingly, the product compositions of the formose reaction under dynamic conditions deviate significantly from those under steady state conditions. We attribute these compositional changes to the non-uniform propagation of fluctuations through the network, thereby shaping reaction outcomes. An examination of temporal concentration patterns showed that collections of compounds responded collectively to perturbations, indicating that key gating reactions branching from the Breslow cycle may be important responsive features of the formose reaction. Our findings show how the compositions of prebiotic reaction networks were shaped by sequential environmental events, illustrating the necessity for considering the temporal traits of prebiotic environments that supported the origin of life.
前生物环境是动态的，包含一系列周期性和非周期性的反应条件变化。然而，环境条件的时间动态对前生物化学反应网络的影响尚未得到研究。在这里，我们展示了催化剂 Ca 和氢氧根的时间波动幅度和速率如何控制类糖醛酸反应的产物分布。令人惊讶的是，动态条件下的类糖醛酸反应产物组成与稳态条件下的产物组成有很大的不同。我们将这些组成变化归因于波动在网络中的非均匀传播，从而影响了反应结果。对时间浓度模式的研究表明，化合物的集合对干扰有集体响应，这表明从 Breslow 环分支的关键门控反应可能是类糖醛酸反应的重要响应特征。我们的发现表明，前生物化学反应网络的组成是如何受到连续环境事件的影响的，这说明了考虑支持生命起源的前生物环境的时间特征的必要性。
