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Dynamics of Benzene Adsorbed on Ca-LSX Zeolite Studied by Solid-State Two-Dimensional Exchange ~(13)C NMR

机译:固态二维交换〜(13)C NMR研究Ca-LSX沸石上苯的吸附动力学

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摘要

Transport of molecular guest species in confined environments is central to the performance of many permeable materials, including porous catalysts, adsorbents, membranes, and polymers, which are heterogeneous systems characterized by appreciable disorder and complexity. Neutron and X-ray diffraction investigations can provide local structural information for guest configurations that possess sufficiently long range periodic order, while complementary structural measurements over much shorter length scales are provided by nuclear magnetic resonance (NMR) techniques. Information on local guest species dynamics, however, is often difficult to infer from such studies, although over longer length scales (ca. 1 μm) molecular self-diffusion can be measured by means of pulsed-field-gradient NMR methods. Solid-state two-dimensional (2D) exchange NMR strategies pioneered by Spiess and co-workers for studying reorientation geometries and time scales of slow dynamic processes in polymers are powerful probes of local environment and dynamics. We report here the first solid-state ~(13)C NMR measurement of analogous transport dynamics of adsorbed hydrocarbon guest molecules on a microporous molecular sieve, specifically, benzene adsorbed on Ca-LSX zeolite.
机译:在密闭环境中分子客体物种的运输对于许多可渗透材料的性能至关重要,这些材料包括多孔催化剂,吸附剂,膜和聚合物,这些材料是非均相的系统,其特征在于明显的无序性和复杂性。中子和X射线衍射研究可以为拥有足够长距离周期性顺序的客体结构提供局部结构信息,而核磁共振(NMR)技术则可以在更短的长度范围内提供互补的结构测量结果。尽管可以通过脉冲场梯度NMR方法测量更长的分子尺度(约1μm)分子自扩散,但是通常难以从此类研究中推断出本地客体动力学的信息。 Spiess及其同事率先研究的固态二维(2D)交换NMR策略,用于研究聚合物中慢动态过程的重新定向几何形状和时标,是局部环境和动力学的有力探索者。我们在这里报告的第一个固态〜(13)C NMR测量的微孔分子筛上吸附的烃客体分子,特别是吸附在Ca-LSX沸石上的苯的类似传输动力学。

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