液滴、气泡和厚膜在开孔和闭孔中的热力学稳定性
Thermodynamic stability of droplets, bubbles and thick films in open and closed pores
摘要：
孔隙中的流体可以形成多种非均质结构。我们结合毛细管的描述，加上协会状态方程研究的热力学稳定性的液滴，气泡和薄膜的水在358 K的圆柱对称孔。平衡结构强烈地依赖于孔的大小以及孔是封闭的还是连接到颗粒储存器。提出了一种新的方法来分析薄膜的热力学稳定性，其中描述系统的总能量的积分近似的求积规则。我们表明，对于大孔隙，热力学稳定性限制的吸附液滴和气泡在开放和封闭的孔隙是由它们的机械稳定性，这是密切相关的孔隙形状。对于闭孔中的膜也是如此。在开孔中，除了非常低的膜相接触角和有限的外部压力范围外，膜是化学不稳定的。这一结果强调需要调用一个完整的热力学稳定性分析，而不是限制讨论机械稳定性。一个共同的特点，大多数的异质结构检查是外观的结构是亚稳态相对于一个充满均匀流体的孔隙的区域。在封闭的孔隙中，当孔隙变小时，这些区域的尺寸显著地增长。[...]完整的相图，比较所有的调查结构。在平衡状态下的开孔中，最稳定的结构是均相或吸附的液滴和气泡，这取决于外部储层中的相类型。较小的孔隙允许液滴和气泡吸附较大的压力跨度。在闭孔中，根据总密度、接触角和孔形状，可以出现大多数研究的构型。[...]
英文摘要：
A fluid in a pore can form diverse heterogeneous structures. We combine a capillary description with the cubic-plus-association equation of state to study the thermodynamic stability of droplets, bubbles and films of water at 358 K in a cylindrically symmetric pore. The equilibrium structure depends strongly on the size of the pore and whether the pore is closed or connected to a particle reservoir. A new methodology is presented to analyze the thermodynamic stability of films, where the integral that describes the total energy of the system is approximated by a quadrature rule. We show that, for large pores, the thermodynamic stability limit of adsorbed droplets and bubbles in both open and closed pores is governed by their mechanical stability, which is closely linked to the pore shape. This is also the case for a film in a closed pore. In open pores, the film is chemically unstable except for very low film-phase contact angles and for a limited range in external pressure. This result emphasizes the need to invoke a complete thermodynamic stability analysis, and not restrict the discussion to mechanical stability. A common feature for most of the heterogeneous structures examined is the appearance of regions where the structure is metastable with respect to a pore filled with a homogeneous fluid. In the closed pores, these regions grow considerably in size when the pores become smaller. [...] Complete phase diagrams are presented that compare all the investigated structures. In open pores at equilibrium, the most stable structure is either the homogeneous phase or adsorbed droplets and bubbles, depending on the type of phase in the external reservoir. Smaller pores allow for droplets and bubbles to adsorb for a larger span in pressure. In closed pores, most of the investigated configurations can occur depending on the total density, the contact angle and the pore shape. [...]
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