Raymond and Beverly Sackler School of Physics and Astronomy, Tel Aviv University, Ramat Aviv 69978, Tel Aviv, Israel.
Soft Matter. 2018 Jul 25;14(29):6058-6069. doi: 10.1039/c8sm00728d.
We revisit the charge-regulation mechanism of macro-ions and apply it to mobile macro-ions in a bathing salt solution. In particular, we examine the effects of correlation between various adsorption/desorption sites and analyze the collective behavior in terms of the solution effective screening properties. We show that such a behavior can be quantified in terms of the charge asymmetry of the macro-ions, defined by their preference for a non-zero effective charge, and their donor/acceptor propensity for exchanging salt ions with the bathing solution. Asymmetric macro-ions tend to increase the screening, while symmetric macro-ions can in some cases decrease it. Macro-ions that are classified as donors display a rather regular behavior, while those that behave as acceptors exhibit an anomalous non-monotonic Debye length. The screening properties, in their turn, engender important modifications to the disjoining pressure between two charged surfaces. Our findings are in particular relevant for solutions of proteins, whose exposed amino acids can undergo charge dissociation/association processes to/from the bathing solution, and can be considered as a solution of charged regulated macro-ions, as analyzed here.
我们重新审视了大分子离子的电荷调节机制,并将其应用于浴盐溶液中的可移动大分子离子。具体来说,我们研究了各种吸附/解吸位点之间相关性的影响,并根据溶液的有效屏蔽特性分析了集体行为。我们表明,可以根据大分子离子的电荷不对称性来定量描述这种行为,其定义为它们对非零有效电荷的偏好,以及它们与浴盐溶液交换盐离子的施主/受体倾向。不对称大分子离子往往会增加屏蔽作用,而对称大分子离子在某些情况下则会降低屏蔽作用。被归类为施主的大分子离子表现出相当规则的行为,而表现为受体的大分子离子则表现出反常的非单调德拜长度。屏蔽特性反过来又会对两个带电表面之间的离差压力产生重要的影响。我们的发现对于蛋白质溶液尤其重要,因为蛋白质中暴露的氨基酸可以经历与浴盐溶液的电荷解离/结合过程,并可以被视为这里分析的带电调节大分子离子的溶液。