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Salt-Screened Transition toward Bulk-Like Water Dynamics near Polymeric Zwitterions
ACS Macro Letters ( IF 5.1 ) Pub Date : 2024-07-12 , DOI: 10.1021/acsmacrolett.4c00347 Shawn D Mengel 1 , Audra J DeStefano 1 , Thomas Webber 1 , Anton Semerdjiev 1 , Songi Han 2 , Rachel A Segalman 1, 3, 4
ACS Macro Letters ( IF 5.1 ) Pub Date : 2024-07-12 , DOI: 10.1021/acsmacrolett.4c00347 Shawn D Mengel 1 , Audra J DeStefano 1 , Thomas Webber 1 , Anton Semerdjiev 1 , Songi Han 2 , Rachel A Segalman 1, 3, 4
Affiliation
The superior antifouling performance of zwitterionic materials is commonly linked to their hydration structure, in which tight surface binding of water molecules inhibits solute adsorption. However, there is comparatively little direct experimental data on the hydration water structure and dynamics around zwitterionic moieties, including the longer-range behavior of the hydration shell that modulates the approach of solutes to the polymer surface. This work experimentally probes the dynamics of the diffusing hydration water molecules around a series of zwitterion chemistries using Overhauser dynamic nuclear polarization relaxometry. Surprisingly, water dynamics measured within ∼1 nm of the zwitterions were minimally inhibited compared to those near uncharged hydrophilic or cationic side chains. Specific dissolved ions further enhance the water diffusivity near the zwitterions, rendering the hydration shell bulk water-like. These results that the hydration of a zwitterion surface is nearly indistinguishable from bulk water suggest that these surfaces are “invisible” to biological constituents in a manner tunable by the ionic environment and the chemical design of the zwitterionic surface.
中文翻译:
聚合物两性离子附近向类块状水动力学的盐筛选转变
两性离子材料优异的防污性能通常与其水化结构有关,其中水分子的紧密表面结合抑制了溶质吸附。然而,关于两性离子部分周围的水合水结构和动力学的直接实验数据相对较少,包括调节溶质接近聚合物表面的水合壳的长程行为。这项工作使用 Overhauser 动态核极化弛豫测量法,通过实验探讨了一系列两性离子化学物质周围扩散水合水分子的动力学。令人惊讶的是,与靠近不带电的亲水性或阳离子侧链的水动力学相比,在约 1 nm 的两性离子内测量的水动力学受到最小程度的抑制。特定的溶解离子进一步增强了两性离子附近的水扩散率,使水合壳整体呈水状。这些结果表明,两性离子表面的水合与散装水几乎没有区别,这表明这些表面对生物成分来说是“不可见的”,其方式可通过离子环境和两性离子表面的化学设计进行调节。
更新日期:2024-07-12
中文翻译:
聚合物两性离子附近向类块状水动力学的盐筛选转变
两性离子材料优异的防污性能通常与其水化结构有关,其中水分子的紧密表面结合抑制了溶质吸附。然而,关于两性离子部分周围的水合水结构和动力学的直接实验数据相对较少,包括调节溶质接近聚合物表面的水合壳的长程行为。这项工作使用 Overhauser 动态核极化弛豫测量法,通过实验探讨了一系列两性离子化学物质周围扩散水合水分子的动力学。令人惊讶的是,与靠近不带电的亲水性或阳离子侧链的水动力学相比,在约 1 nm 的两性离子内测量的水动力学受到最小程度的抑制。特定的溶解离子进一步增强了两性离子附近的水扩散率,使水合壳整体呈水状。这些结果表明,两性离子表面的水合与散装水几乎没有区别,这表明这些表面对生物成分来说是“不可见的”,其方式可通过离子环境和两性离子表面的化学设计进行调节。