Mechanistic Insight into Nanoparticle Surface Adsorption by Solution NMR Spectroscopy in an Aqueous Gel,Angewandte Chemie International Edition

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Mechanistic Insight into Nanoparticle Surface Adsorption by Solution NMR Spectroscopy in an Aqueous Gel
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2017-07-17 08:17:35 , DOI: 10.1002/anie.201704471
Timothy K. Egner ₁ , Pranjali Naik _{1,

2} , Nicholas C. Nelson _{1,

2} , Igor I. Slowing _{1,

2} , Vincenzo Venditti ₁

Affiliation

Engineering nanoparticle (NP) functions at the molecular level requires a detailed understanding of the dynamic processes occurring at the NP surface. Herein we show that a combination of dark-state exchange saturation transfer (DEST) and relaxation dispersion (RD) NMR experiments on gel-stabilized NP samples enables the accurate determination of the kinetics and thermodynamics of adsorption. We used the former approach to describe the interaction of cholic acid (CA) and phenol (PhOH) with ceria NPs with a diameter of approximately 200 nm. Whereas CA formed weak interactions with the NPs, PhOH was tightly bound to the NP surface. Interestingly, we found that the adsorption of PhOH proceeds via an intermediate, weakly bound state in which the small molecule has residual degrees of rotational diffusion. We believe the use of aqueous gels for stabilizing NP samples will increase the applicability of solution NMR methods to the characterization of nanomaterials.

中文翻译：

溶液NMR光谱在水凝胶中对纳米粒子表面吸附的机理的洞察力。

在分子水平上工程纳米颗粒（NP）功能需要对NP表面发生的动态过程有详细的了解。本文中，我们证明了在凝胶稳定的NP样品上进行暗态交换饱和转移（DEST）和弛豫分散（RD）NMR实验的组合，可以准确确定吸附的动力学和热力学。我们使用前一种方法来描述胆酸（CA）和苯酚（PhOH）与直径约200 nm的二氧化铈NP的相互作用。CA与NP之间形成弱相互作用，而PhOH与NP表面紧密结合。有趣的是，我们发现PhOH的吸附通过中间的弱结合状态进行，其中小分子具有残留的旋转扩散度。

更新日期：2017-07-17

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