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解读UiO-66金属有机框架结晶的机制

Olesya O Semivrazhskaya¹, Daniil Salionov², Adam H Clark³

¹Laboratory for Organic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 3, 8093, Zurich, Switzerland.

Small (Weinheim an der Bergstrasse, Germany)

|August 27, 2023

概括

了解UiO-66等含有的金属有机框架 (MOF) 的形成至关重要. 这项研究揭示了UiO-66核化通过自催化水解发生,晶体生长是限制速度的步骤.

科学领域:

材料科学材料科学材料科学
纳米技术纳米技术
化学工程是化学工程的重要组成部分.

背景情况:

含有的金属有机框架 (MOF) 与UiO-66拓是非常通用的材料.
尽管有广泛的应用,但UiO-66核和生长的分子层次机制仍然不太清楚.
自从关于这个MOF的最初报告以来,已经进行了十多年的研究.

研究的目的:

阐明控制UiO-66.6核化和生长的分子层次机制.
确定参与UIO-66合成的关键中间体和反应途径.
了解控制晶体大小和形态的因素.

主要方法:

在现场时间解析的高分辨率质谱仪.
Zr K-边缘X射线吸收光谱学
魔法角度旋转的核磁共振光谱学
在X射线中,X射线的衍射效果是不同的.

主要成果:

UiO-66的核形成是通过基甲酸盐的溶液介导水解进行的,表现出自催化行为.
氧结的形成迅速且直接;没有观察到预先形成的集群或稳定的非静态度介质.
原子核具有与晶体相同的局部环境,但缺乏在结晶过程中获得的远程秩序.
晶体生长是决定速度的步骤,而快速核化产生小的UiO-66晶体 (~200 nm) 具有狭窄的尺寸分布.

结论:

UiO-66的合成机制涉及通过自催化水解直接形成氧节点.
晶体的生长,而不是核形成,决定了整体的过程速率和最终的晶体特性.
这些发现为MOF形成提供了关键的见解,使得针对特定应用的定制合成成为可能.

关键词:

晶体的生长晶体的生长在现场的光谱学.金属有机框架的框架.核化的核化.时间分辨率光谱学.

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