Experimental Measurement of Surface Charge Effects on the Stability of a Surface-Bound Biopolymer.

Experimental Measurement of Surface Charge Effects on the Stability of a Surface-Bound Biopolymer.
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表面电荷对表面结合生物聚合物稳定性影响的实验测量。

DOI:
10.1021/acs.langmuir.8b01004
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发表时间:
2018
期刊:
Langmuir : the ACS journal of surfaces and colloids
影响因子:
--
通讯作者:
Plaxco,KevinW
Plaxco,KevinW
中科院分区:
--
文献类型:
--
作者:
Watkins,HerschelM;Ricci,Francesco;Plaxco,KevinW

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生物聚合物与特定表面相互作用的热力学的定量实验研究仍然非常有限。作为回应,在这里,我们描述了实验和理论研究的折叠自由能的变化时发生的一个简单的生物聚合物,DNA茎环,是位点特异性连接到一系列的化学上不同的表面通过自组装单层形成的金电极。毫不奇怪,表面附着改变生物聚合物的折叠自由能的程度强烈依赖于表面的电荷,带负电荷的表面越来越多,导致不稳定性增加。一个简单的模型,只考虑排除的体积和静电排斥产生的表面和模型的离子环境以上的表面作为一个连续定量恢复所观察到的自由能变化与附件带弱电荷的负表面。对于更强的负电荷表面的模型,考虑到所涉及的离子的离散尺寸是必需的。因此,我们的研究突出了静电学在表面生物分子相互作用物理学中的重要作用。
Quantitative experimental studies of the thermodynamics with which biopolymers interact with specific surfaces remain quite limited. In response, here we describe experimental and theoretical studies of the change in folding free energy that occurs when a simple biopolymer, a DNA stem-loop, is site-specifically attached to a range of chemically distinct surfaces generated via self-assembled monolayer formation on a gold electrode. Not surprisingly, the extent to which surface attachment alters the biopolymer’s folding free energy depends strongly on the charge of the surface, with increasingly negatively charged surfaces leading to increased destabilization. A simple model that considers only the excluded volume and electrostatic repulsion generated by the surface and models the ionic environment above the surface as a continuum quantitatively recovers the observed free energy change associated with attachment to weakly charged negative surfaces. For more strongly charged negative surfaces a model taking into account the discrete size of the involved ions is required. Our studies thus highlight the important role that electrostatics can play in the physics of surface–biomolecule interactions.
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