Klika Václav, Krause Andrew L
Department of Mathematics, FNSPE , Czech Technical University in Prague , Trojanova 13 , Prague 2 12000 , Czech Republic.
Mathematical Institute, University of Oxford , Andrew Wiles Building, Radcliffe Observatory Quarter, Woodstock Road , Oxford OX2 6GG , United Kingdom.
J Phys Chem Lett. 2018 Dec 20;9(24):7021-7025. doi: 10.1021/acs.jpclett.8b03281. Epub 2018 Dec 5.
Phenomenological coefficients in linear nonequilibrium thermodynamics have been considered to be independent, apart from restrictions due to the Onsager-Casimir reciprocal relations and the requirement to have non-negative entropy production. Recently, it has been shown that functional constraints between these coefficients may hold, restricting their dependence on state variables, especially in the case of coupled phenomena. Here we demonstrate that such restrictions require only mild assumptions on the system of interest and are, in fact, much more constraining than previously reported. Such constraints vastly reduce the set of plausible models for constitutive relations and allow for simpler experimental determinations of dependencies in coupled systems. These results may also clarify inconsistencies in the literature regarding constitutive models used that do not obey these thermodynamic constraints.
线性非平衡态热力学中的唯象系数一直被认为是相互独立的,除了受昂萨格 - 卡西米尔互易关系的限制以及非负熵产生的要求。最近,研究表明这些系数之间可能存在函数约束,限制了它们对状态变量的依赖,特别是在耦合现象的情况下。在此,我们证明这种约束仅需要对所关注的系统做一些温和的假设,并且实际上比先前报道的约束要强得多。这种约束极大地减少了本构关系的合理模型集,并允许在耦合系统中更简单地通过实验确定依赖关系。这些结果也可能澄清文献中关于不遵守这些热力学约束的本构模型的不一致之处。