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使用O17O固态NMR探测UIO-66(Zr) MOF与水之间的氧气交换

Florian Venel¹, Raynald Giovine¹, Danielle Laurencin²

¹Univ. Lille, CNRS, Centrale Lille, ENSCL, Univ. Artois, UMR 8181 - UCCS - Unité de Catalyse et Chimie du Solide, F-59000, Lille, France.

Chemistry (Weinheim an der Bergstrasse, Germany)

|January 16, 2024

概括

这项研究揭示了基于的金属有机框架 (MOF) UiO-66与水的反应性. 在UiO-66 MOF位点中的氧原子可以与水交换,表明Zr-O键可变性.

科学领域:

材料科学材料科学材料科学
固态化学固态化学
核磁共振光谱学核磁共振光谱学

背景情况:

基于的金属有机框架 (MOF) UiO-66(Zr) 具有出色的热和化学稳定性.
虽然它的远程结构是水稳定的,但缺陷形成和反应性仍然不太清楚.
衍射技术不足以检测微妙的结构缺陷.

研究的目的:

用氧原子交换来研究UiO-66 (((Zr) 与水的反应性.
探测标准衍射方法无法检测到的缺陷形成机制.
在水热条件下阐明UiO-66 (((Zr) 中Zr-O键的可变性.

主要方法:

使用了17O固态NMR光谱仪在18.8 T.
用于通过机械化学制备的17O标记的甲酸,用于选择性同位素丰富碳酸盐群.
用 17O 丰富水进行了合成后的热水处理.

主要成果:

在UiO-66 (((Zr)) 中观察到碳酸盐 (COO-) 和μ3-O2-位点之间的氧原子交换,在暴露于水和随后脱水时.
通过使用 17O 丰富水,证明了所有三个不同的氧位点 (μ3-OH,μ3-O2-,COO-) 的成功丰富.
证实了Zr-O键的可变性和UiO-66 (((Zr) 与水的整体反应性.

结论:

UiO-66 (((Zr) 与水具有显著的反应性,涉及框架站点之间的氧气交换.
固态NMR光谱是研究MOF缺陷化学和反应性的强大工具.
这些发现突出了UiO-66中的Zr-O债券在特定条件下的动态性质.

关键词:

第170章没有了在UiO-66中使用.Zr−O 债券是一种债券.机械化学机械化学固态NMR是一种固态NMR.水水水的水水的水

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