近表面中性电荷调节热力学
Thermodynamics of Charge Regulation Near Surface Neutrality
摘要：
已知浸入水溶液中的两个相邻带电表面之间的相互作用受到电荷调节的影响-当两个带电表面彼此接近时表面电荷的调制。这种现象在接近表面中性的地方特别重要，在那里物体如胶体或生物分子的稳定性受到危害。集中在这个无处不在的情况下，我们阐明了基本的热力学，并表明，在这种情况下，电荷调节由表面熵。我们推导出明确的表达式，电荷调节和制定一个新的普遍的限制法律的离子吸附到表面的自由能。后者与$k_{B}T$成正比，与离子与表面基团的缔合能无关。这些新的结果适用于分析单极以及两性表面，如氧化物附近的零电荷点或蛋白质附近的等电点。
英文摘要：
The interaction between two adjacent charged surfaces immersed in aqueous solution is known to be affected by charge regulation - the modulation of surface charge as two charged surfaces approach each other. This phenomenon is particularly important near surface neutrality where the stability of objects such as colloids or biomolecules is jeopardized. Focusing on this ubiquitous case, we elucidate the underlying thermodynamics and show that charge regulation is governed in this case by surface entropy. We derive explicit expressions for charge regulation and formulate a new universal limiting law for the free energy of ion adsorption to the surfaces. The latter turns out to be proportional to $k_{B}T$, and independent of the association energy of ions to surface groups. These new results are applied to the analysis of unipolar as well as amphoteric surfaces such as oxides near their point of zero charge or proteins near their isoelectric point.
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