Isolation of the Secondary Building Unit of a 3D Metal–Organic Framework through Clip-Off Chemistry, and Its Reuse To Synthesize New Frameworks by Dynamic Covalent Chemistry

IF 15.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2024-09-30 DOI:10.1021/jacs.4c0907710.1021/jacs.4c09077

Dongsik Nam, Jorge Albalad, Roberto Sánchez-Naya, Sara Ruiz-Relaño, Alba Cortés-Martínez, Yunhui Yang, Judith Juanhuix, Inhar Imaz* and Daniel Maspoch*,

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引用次数: 0

Abstract

Herein, we present a novel methodology for synthesizing metal clusters or secondary building units (SBUs) that are subsequently employed to construct innovative metal–organic frameworks (MOFs) via dynamic covalent chemistry. Our approach entails extraction of SBUs from preformed MOFs through complete disassembly by clip-off chemistry. The initial MOF precursor is designed to incorporate the desired SBU, connected exclusively by cleavable linkers (in this study, with olefinic bonds). Cleavage of all the organic linkers (in this study, via ozonolysis under reductive conditions) liberates the SBUs functionalized with aldehyde groups. Once synthesized, these SBUs can be further reacted with amines in dynamic covalent chemistry to build new, rationally designed MOFs.

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通过剪切化学分离三维金属有机框架的二级构建单元，并通过动态共价化学将其重新用于合成新框架

在此，我们提出了一种合成金属簇或二级构建单元（SBU）的新方法，随后通过动态共价化学将其用于构建创新的金属有机框架（MOF）。我们的方法是通过剪切化学将 SBU 从预成的 MOF 中完全拆解提取出来。最初的 MOF 前体是为了加入所需的 SBU 而设计的，完全由可裂解的连接体（在本研究中为烯烃键）连接。在本研究中，通过还原条件下的臭氧裂解）裂解所有有机连接体后，就能得到醛基官能化的 SBU。合成后，这些 SBU 可进一步与胺进行动态共价化学反应，从而构建出设计合理的新型 MOF。

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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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.