Building Stable Pillar-Layered Metal–Organic Frameworks: Introduction of Unsaturated Bonds for Enhanced Efficiency in C2H2/CO2 Separation

IF 9.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Materials Letters Pub Date : 2024-07-26 DOI:10.1021/acsmaterialslett.4c01150

Wenke Yuan, Panyue Guo, Weize Wang, Peipei Cen, Xiu-Yuan Li, Bo Liu, Huifang Zhou

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Abstract

Pillar-layered structures represent a significant category within MOFs; however, the exploration of their chemical stability and systematic functionalization has been largely neglected. Herein, we fabricated a pillar-layered MOF (Zn-L_C–C) with fsc topology, utilizing a tetradentate carboxylic ligand with bipyridine and Zn(II) ions via the pillar-layered approach. Notably, this topological structure displays markedly superior stability compared with typical pillar-layered MOFs with pcu topology. In addition, by introducing unsaturated bonds to modify and increase the length of the pillars, three additional pillar-layered MOFs (Zn-L_N=N, Zn-L_C=C, and Zn-L_C≡C) were obtained. Compared with those of Zn-L_C–C, the adsorption capacities for C₂H₂ of the other three structures have been improved. Strikingly, the dynamic adsorption uptake of Zn-L_N=N for C₂H₂ is as high as 53.7 cm³ g^–1, and the dynamic separation ratio of C₂H₂/CO₂ is 3.2. These results demonstrate that the introduction of diazo groups in the pillar can enhance the adsorption capacities of pillar-layered MOFs to C₂H₂.

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构建稳定的柱层金属有机框架：引入不饱和键以提高 C2H2/CO2 分离效率

柱层结构是 MOF 中的一个重要类别；然而，对其化学稳定性和系统功能化的探索在很大程度上被忽视了。在此，我们利用四价羧酸配体与联吡啶和 Zn（II）离子，通过柱层方法制备了一种具有 fsc 拓扑结构的柱层 MOF（Zn-LC-C）。值得注意的是，与具有 pcu 拓扑结构的典型柱层 MOF 相比，这种拓扑结构显示出明显优越的稳定性。此外，通过引入不饱和键来改变和增加支柱的长度，还获得了另外三种支柱层状 MOF（Zn-LN=N、Zn-LC=C 和 Zn-LC≡C）。与 Zn-LC-C 相比，其他三种结构对 C2H2 的吸附容量都有所提高。引人注目的是，Zn-LN=N 对 C2H2 的动态吸附量高达 53.7 cm3 g-1，C2H2/CO2 的动态分离比为 3.2。这些结果表明，在柱中引入重氮基团可以提高柱层 MOFs 对 C2H2 的吸附能力。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.