UiO-66 (Zr) MOF中丁烷异构体的迁移率和骨架动力学:氧化锆簇中羟基的影响

IF 1.8 3区 化学 Q4 CHEMISTRY, PHYSICAL Solid state nuclear magnetic resonance Pub Date : 2022-04-01 DOI:10.1016/j.ssnmr.2022.101784
Alexander E. Khudozhitkov , Sergei S. Arzumanov , Daniil I. Kolokolov , Alexander G. Stepanov
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引用次数: 2

摘要

UiO-66 (Zr)是一种金属有机骨架(MOF),以其热稳定性和化学稳定性以及广泛的吸附应用而闻名。该MOF对丁烷异构体具有较高的分离选择性。早先已经推断,材料的分离性能取决于氧化锆簇的羟基化状态。在这篇文章中,我们应用2H固态核磁共振来表征MOF有机框架本身和羟基化和去羟基化形式的UiO-66的丁烷异构体的动力学。结果表明,在脱羟基形式下,骨架内的π翻转速率和苯基环平面振动幅度较大。对两种形式的UiO-66的丁烷异构体的自扩散系数进行了估计。脱羟基形式的正丁烷的扩散率更高,而异丁烷的扩散不受MOF氧化锆簇中OH基团存在的影响。脱羟基形式下正丁烷的高扩散率是由于该形式下相邻笼间窗口的有效直径较大,这是由更快的旋转和更大的框架连接体振动幅度引起的。这使得UiO-66(Zr)材料的脱羟基形式分离丁烷异构体的效率更高。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Butane isomers mobility and framework dynamics in UiO-66 (Zr) MOF: Impact of the hydroxyl groups in zirconia cluster

UiO-66 (Zr) is a metal-organic framework (MOF) known for its thermal and chemical stability and wide range of adsorption-based applications. This MOF exhibits high separation selectivity for butane isomers. It has been earlier inferred that the separation performance of the material depends on the hydroxylation state of the zirconia cluster. In this contribution, we apply 2H solid-state NMR to characterize the dynamics of both the MOF organic framework itself and butane isomers in hydroxylated and dehydroxylated forms of UiO-66. It is established that the rate of π-flipping and the amplitude of the phenylene ring plane librations in the framework are higher for the dehydroxylated form. Self-diffusion coefficients of butane isomers have been estimated for both forms of UiO-66. The diffusivity is higher for n-butane in the dehydroxylated form, whereas the diffusion of isobutane is not affected by the presence of OH groups in the zirconia cluster of the MOF. Higher diffusivity of n-butane in dehydroxylated form is accounted for by the larger effective diameter of the window between the adjacent cages in this form, which arises from faster rotation and larger amplitude of framework linker libration. This rationalizes the higher efficiency of the dehydroxylated form of UiO-66(Zr) material for butane isomers separation.

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来源期刊
CiteScore
5.30
自引率
9.40%
发文量
42
审稿时长
72 days
期刊介绍: The journal Solid State Nuclear Magnetic Resonance publishes original manuscripts of high scientific quality dealing with all experimental and theoretical aspects of solid state NMR. This includes advances in instrumentation, development of new experimental techniques and methodology, new theoretical insights, new data processing and simulation methods, and original applications of established or novel methods to scientific problems.
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