Laboratoire de Physico-Chimie Théorique-UMR CNRS Gulliver 7083, PSL Research University, ESPCI, 10 Rue Vauquelin, F-75231 Paris, France.
Center for Nonlinear Phenomena and Complex Systems, Université Libre de Bruxelles (U.L.B.), Campus Plaine, Code Postal 231, B-1050 Brussels, Belgium.
J Chem Phys. 2018 Apr 14;148(14):144902. doi: 10.1063/1.5022697.
Kinetic theory and thermodynamics of reaction networks are extended to the out-of-equilibrium dynamics of continuous-flow stirred tank reactors (CSTR) and serial transfers. On the basis of their stoichiometry matrix, the conservation laws and the cycles of the network are determined for both dynamics. It is shown that the CSTR and serial transfer dynamics are equivalent in the limit where the time interval between the transfers tends to zero proportionally to the ratio of the fractions of fresh to transferred solutions. These results are illustrated with a finite cross-catalytic reaction network and an infinite reaction network describing mass exchange between polymers. Serial transfer dynamics is typically used in molecular evolution experiments in the context of research on the origins of life. The present study is shedding a new light on the role played by serial transfer parameters in these experiments.
将反应网络的动理学理论和热力学扩展到连续搅拌釜式反应器 (CSTR) 和连续转移的非平衡动力学。基于它们的化学计量矩阵，确定了这两种动力学的守恒定律和网络循环。结果表明，当转移之间的时间间隔与新鲜溶液与转移溶液的分数之比成比例地趋近于零时，CSTR 和连续转移动力学是等效的。这些结果通过一个有限的交叉催化反应网络和一个描述聚合物之间质量交换的无限反应网络来说明。连续转移动力学通常用于生命起源研究背景下的分子进化实验。本研究为这些实验中连续转移参数所扮演的角色提供了新的视角。
