Gulliver Laboratory, UMR CNRS 7083, PSL Research University, ESPCI, 10 rue Vauquelin, F-75231 Paris, France.
J Chem Phys. 2017 Sep 7;147(9):094905. doi: 10.1063/1.5001021.
We describe the kinetics and thermodynamics of copolymers undergoing recombination reactions, which are important for prebiotic chemistry. We use two approaches: the first one, based on chemical rate equations and the mass-action law describes the infinite size limit, while the second one, based on the chemical master equation, describes systems of finite size. We compare the predictions of both approaches for the relaxation of thermodynamic quantities towards equilibrium. We find that for some choice of initial conditions, the entropy of the sequence distribution can be lowered at the expense of increasing the entropy of the length distribution. We consider mainly energetically neutral reactions, except for one simple case of non-neutral reactions.
我们描述了经历重组反应的共聚物的动力学和热力学，这对于前生物化学很重要。我们使用了两种方法：第一种方法基于化学速率方程和质量作用定律，描述了无限大尺寸的极限情况，而第二种方法基于化学主方程，描述了有限尺寸的系统。我们比较了这两种方法对热力学量向平衡态松弛的预测。我们发现，对于某些初始条件的选择，序列分布的熵可以降低，而长度分布的熵则会增加。我们主要考虑能量中性反应，除了一个简单的非中性反应情况。
