Spin diffusion transfer difference (SDTD) NMR: An advanced method for the characterisation of water structuration within particle networks.

Spin diffusion transfer difference (SDTD) NMR: An advanced method for the characterisation of water structuration within particle networks.
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自旋扩散传递差 (SDTD) NMR:一种表征颗粒网络内水结构的先进方法。

DOI:
10.1016/j.jcis.2021.02.094
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发表时间:
2021
影响因子:
9.9
通讯作者:
Gabrielli V
Gabrielli V
中科院分区:
化学1区
文献类型:
--
作者:
Gabrielli V

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假设用于监测凝胶中溶剂相互作用的经典 STD NMR 方案强烈依赖于胶凝剂和溶剂浓度,并且不报告颗粒/溶剂界面处溶剂的结构化程度。我们假设,对于大胶凝剂颗粒的悬浮液,当使用一维扩散方程考虑颗粒到溶剂的 1H-1H 自旋扩散传递时,溶剂结构可以通过 STD NMR 来表征。实验我们对胶凝剂和溶剂浓度以及胶凝剂表面电荷的影响进行了系统研究,这些因素影响了经典 STD NMR 构建曲线的行为。为此,我们对在氘化水和酒精/D2O 混合物中制备的淀粉和类纤维素颗粒分散体中的溶剂相互作用进行了表征。研究结果自旋扩散传递差 (SDTD) NMR 协议与胶凝剂和溶剂浓度无关,因此可以估计不同颗粒网络内溶剂结构化的程度。此外,使用一般一维扩散方程模拟 SDTD 构建曲线可以确定颗粒/溶剂界面处的最小距离 (r) 和自旋扩散速率 (D)。这种新颖的 NMR 协议可以轻松扩展,以表征由大颗粒构成的任何类型的胶体系统中的溶剂组织。
HypothesisThe classical STD NMR protocol to monitor solvent interactions in gels is strongly dependent on gelator and solvent concentrations and does not report on the degree of structuration of the solvent at the particle/solvent interface. We hypothesised that, for suspensions of large gelator particles, solvent structuration could be characterised by STD NMR when taking into account the particle-to-solvent1H–1H spin diffusion transfer using the 1D diffusion equation.ExperimentsWe have carried out a systematic study on effect of gelator and solvent concentrations, and gelator surface charge, affecting the behaviour of the classical STD NMR build-up curves. To do so, we have characterised solvent interactions in dispersions of starch and cellulose-like particles prepared in deuterated water and alcohol/D2O mixtures.FindingsThe Spin Diffusion Transfer Difference (SDTD) NMR protocol is independent of the gelator and solvent concentrations, hence allowing the estimation of the degree of solvent structuration within different particle networks. In addition, the simulation of SDTD build-up curves using the general one–dimensional diffusion equation allows the determination of minimum distances (r) and spin diffusion rates (D) at the particle/solvent interface. This novel NMR protocol can be readily extended to characterise the solvent(s) organisation in any type of colloidal systems constituted by large particles.
液相聚合物体系中的自旋扩散理论
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