论文标题
建模纳米固定反应动力学：融合平衡程度波动的替代方法
Modeling nanoconfined reaction kinetics: Alternative methodology incorporating equilibrium extent fluctuations
论文作者
论文摘要
这项研究表明，最近在统计力学框架中得出的纳米结合反应的平衡常数微分方程（ECDE）可用于建模随机化学动力学。假定和验证，如果将纳米反应商的瞬态值视为平衡常数，则相应的平衡反应范围及其波动（方差函数）与相应的瞬态值一致。由ECDE计算的方差函数促进了随机动力学方程（SKE）的溶液，这是对化学计量交换反应所证明的。这种原始方法获得的结果与化学主方程提供的结果完全一致。与基于后者和需要大量计算机存储器且耗时的吉莱斯皮算法的常用方法相反，所提出的SKE-ECDE方法只需要求解ECDE和单个随机动力学差异方程。
This study reveals that Equilibrium Constant Differential Equations (ECDE) for nanoconfined reactions derived recently in the frameworks of statistical mechanics are useful in modeling stochastic chemical kinetics. It is assumed and verified that if the transient value of the nano-reaction quotient is treated as being an equilibrium constant, the corresponding equilibrium reaction extent and its fluctuations (the variance function) coincide with the respective transient values. The ECDE-computed variance function facilitates the solution of the stochastic kinetics equations (SKE), as is demonstrated for a stoichiometric exchange reaction. The results obtained by this original methodology are in full agreement with those provided by the chemical master equations. Contrary to the commonly used approaches based on the latter and the Gillespie algorithm, which need a lot of computer memory and are time-consuming, the proposed SKE-ECDE method requires to solve only the ECDE and a single stochastic kinetics differential equation.
