A critical transition rule for broadening exponent of fluctuation and its effect on dissipation in chemical reaction-heat conduction coupling systems

A critical transition rule for broadening exponent of fluctuation and its effect on dissipation in chemical reaction-heat conduction coupling systems
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化学反应-热传导耦合系统涨落指数展宽的关键转变规则及其对耗散的影响

DOI:
10.1007/s11426-011-4254-6
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发表时间:
2011-05
期刊:
Science China Chemistry
影响因子:
--
通讯作者:
Luo JiuLi
Luo JiuLi
中科院分区:
其他
文献类型:
--
作者:
Lin Feng;Zhao NanRong;Luo JiuLi

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本文提出了一维气体系统在Dirichlet或零通量边界条件下的化学反应-热传导-扩散的随机模型。基于该模型,我们将临界涨落的展宽指数理论推广到化学反应-热传导耦合系统,作为相应的马尔可夫主方程(ME)的渐近性质,并建立了这类系统的有效的随机热力学。作为说明,对非等温、非齐次Schlögl模型进行了显式研究。通过有序分析漂移和扩散对相应的Fokker-Planck方程(FPE)中几率分布演化的贡献,我们确定了化学反应和热传导耦合引起的涨落展宽指数的临界跃迁规则。结果表明,临界涨落引起的耗散达到了确定性水平,导致了非平衡物理化学过程的热力学效应。
A stochastic model of chemical reaction-heat conduction-diffusion for a one-dimensional gaseous system under Dirichlet or zero-fluxes boundary conditions is proposed in this paper. Based on this model, we extend the theory of the broadening exponent of critical fluctuations to cover the chemical reaction-heat conduction coupling systems as an asymptotic property of the corresponding Markovian master equation (ME), and establish a valid stochastic thermodynamics for such systems. As an illustration, the non-isothermal and inhomogeneous Schlögl model is explicitly studied. Through an order analysis of the contributions from both the drift and diffusion to the evolution of the probability distribution in the corresponding Fokker-Planck equation(FPE) in the approach to bifurcation, we have identified the critical transition rule for the broadening exponent of the fluctuations due to the coupling between chemical reaction and heat conduction. It turns out that the dissipation induced by the critical fluctuations reaches a deterministic level, leading to a thermodynamic effect on the nonequilibrium physico-chemical processes.
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