2H-NMR as a Practical Tool for Following MOF Formation: A Case Study of UiO-66

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Amanda P. Parsons, Céline M. Schneider, Michael J. Katz
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引用次数: 0

Abstract

Developing the mechanism for MOF formation is crucial for the rapid development of new materials. This work demonstrates that Deuterium-NMR spectroscopy is the optimal inter-laboratory methodology for understanding the in-situ kinetics of metal-organic framework (MOF) formation. This method is facile, affordable, and allows for the isolation and monitoring of individual reagents by using one deuterated component while the remaining components are protonated. This study utilizes 2H-NMR, via the spectrometer’s lock channel, to investigate the formation of UiO-66 as influenced by different modulators: acetic acid, benzoic acid, and hydrochloric acid. By monitoring the concentration of the deuterated linker and observing the chemical shift and peak width of deuterated water over time, key elements of the mechanism are unraveled. Paradoxically, conditions that cause the ligand to be consumed more slowly result in MOFs forming more quickly and with fewer defects. This phenomenon is attributed to the dissociative mechanism associated with the Zr(IV)-containing node.
2H-NMR作为跟踪MOF形成的实用工具:以UiO-66为例
开发 MOF 的形成机理对于快速开发新材料至关重要。这项研究表明,氘-核磁共振光谱法是了解金属有机框架(MOF)原位形成动力学的最佳实验室间方法。这种方法简便易行、经济实惠,可通过使用一种氘化成分而同时使用质子化的其余成分来分离和监测单个试剂。本研究通过光谱仪的锁定通道利用 2H-NMR 来研究 UiO-66 的形成受不同调制剂(醋酸、苯甲酸和盐酸)的影响。通过监测氘化连接体的浓度和观察氘化水随时间变化的化学位移和峰宽,揭示了该机制的关键要素。矛盾的是,在配体消耗较慢的条件下,MOF 的形成速度更快,缺陷更少。这一现象归因于与含 Zr(IV) 节点相关的离解机制。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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