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通过 PGSE ESR 研究多孔介质中的分子扩散。

Molecular diffusion in porous media by PGSE ESR.

机构信息

Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, Israel.

出版信息

Phys Chem Chem Phys. 2010 Jun 21;12(23):5998-6007. doi: 10.1039/b922060g. Epub 2010 Apr 6.

Abstract

Diffusion in porous media is a general subject that involves many fields of research, such as chemistry (e.g. porous catalytic pallets), biology (e.g. porous cellular organelles), and materials science (e.g. porous polymer matrixes for controlled-release and gas-storage materials). Pulsed-gradient spin-echo nuclear magnetic resonance (PGSE NMR) is a powerful technique that is often employed to characterize complex diffusion patterns inside porous media. Typically it measures the motion of at least approximately 10(15) molecules occurring in the milliseconds-to-seconds time scale, which can be used to characterize diffusion in porous media with features of approximately 2-3 mum and above (in common aqueous environments). Electron Spin Resonance (ESR), which operates in the nanoseconds-to-microseconds time scale with much better spin sensitivity, can in principle be employed to measure complex diffusion patterns in porous media with much finer features (down to approximately 10 nm). However, up to now, severe technical constraints precluded the adaptation of PGSE ESR to porous media research. In this work we demonstrate for the first time the use of PGSE ESR in the characterization of molecular restricted diffusion in common liquid solutions embedded in a model system for porous media made of sub-micron glass spheres. A unique ESR resonator, efficient gradient coils and fast gradient current drivers enable these measurements. This work can be further extended in the future to many applications that involve dynamical processes occurring in porous media with features in the deep sub-micron range down to true nanometric length scales.

摘要

多孔介质中的扩散是一个普遍的主题,涉及许多研究领域,如化学(例如多孔催化托盘)、生物学(例如多孔细胞细胞器)和材料科学(例如用于控制释放和气体存储材料的多孔聚合物基质)。脉冲梯度自旋回波核磁共振(PGSE NMR)是一种强大的技术,常用于表征多孔介质内部复杂的扩散模式。它通常测量至少大约 10^15 个分子在毫秒到秒的时间尺度内的运动,这可用于表征具有大约 2-3 µm 及以上特征的多孔介质中的扩散(在常见的水相环境中)。电子顺磁共振(ESR)在纳秒到微秒的时间尺度内具有更好的自旋灵敏度,原则上可以用于测量具有更精细特征(低至大约 10 nm)的多孔介质中的复杂扩散模式。然而,到目前为止,严重的技术限制使得 PGSE ESR 无法应用于多孔介质研究。在这项工作中,我们首次展示了 PGSE ESR 在嵌入多孔介质模型系统的常见液体溶液中分子受限扩散表征中的应用,该模型系统由亚微米玻璃球组成。独特的 ESR 谐振器、高效的梯度线圈和快速的梯度电流驱动器使得这些测量成为可能。这项工作将来可以进一步扩展到许多涉及在深亚微米范围内到真正纳米尺度的特征的多孔介质中发生的动态过程的应用中。

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