How Reproducible is the Synthesis of Zr–Porphyrin Metal–Organic Frameworks? An Interlaboratory Study,Advanced Materials

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How Reproducible is the Synthesis of Zr–Porphyrin Metal–Organic Frameworks? An Interlaboratory Study
Advanced Materials ( IF 27.4 ) Pub Date : 2023-09-05 , DOI: 10.1002/adma.202304832
Hanna L B Boström _{1,

2} , Sebastian Emmerling ₁ , Fabian Heck ₁ , Charlotte Koschnick ₁ , Andrew J Jones ₃ , Matthew J Cliffe ₃ , Rawan Al Natour ₄ , Mickaële Bonneau ₄ , Vincent Guillerm ₄ , Osama Shekhah ₄ , Mohamed Eddaoudi ₄ , Javier Lopez-Cabrelles ₅ , Shuhei Furukawa _{5,

6} , María Romero-Angel ₇ , Carlos Martí-Gastaldo ₇ , Minliang Yan ₈ , Amanda J Morris _{8,

9} , Ignacio Romero-Muñiz ₁₀ , Ying Xiong ₁₀ , Ana E Platero-Prats _{10,

11,

12} , Jocelyn Roth ₁₃ , Wendy L Queen ₁₃ , Kalle S Mertin ₁₄ , Danielle E Schier ₁₅ , Neil R Champness ₁₅ , Hamish H-M Yeung ₁₅ , Bettina V Lotsch _{1,

16}

Affiliation

Max Planck Institute for Solid State Research, Heisenbergstraße 1, D-70569, Stuttgart, Germany.
Present address: Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, SE-106 91, Sweden.
School of Chemistry, University of Nottingham, University Park, Nottingham, NG7 2RD, UK.
King Abdullah University of Science and Technology (KAUST), Division of Physical Sciences and Engineering, Advanced Membranes & Porous Materials Center (AMPM), Functional Materials Design, Discovery & Development Research Group (FMD3), Thuwal, 23955-6900, Kingdom of Saudi Arabia.
Institute for Integrated Cell-Material Sciences (WPI-iCeMS), Kyoto University, Kyoto, 606-8501, Japan.
Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Kyoto, 615-8510, Japan.
Instituto de Ciencia Molecular (ICMol), Universitat de València, Catedrático José Beltrán-2, Paterna, 46980, Spain.
Macromolecules innovation institute, Virginia Tech, Blacksburg, VA, 24061, USA.
Department of Chemistry, Virginia Tech, Blacksburg, VA, 24061, USA.
Departamento de Química Inorgánica, Facultad de Ciencias, Universidad Autónoma de Madrid, Madrid, 28049, Spain.
Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, Madrid, 28049, Spain.
Institute for Advanced Research in Chemical Sciences (IAdChem), Universidad Autónoma de Madrid, Madrid, 28049, Spain.
Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Sion, CH-1950, Switzerland.
Institute of Inorganic Chemistry, Christian-Albrechts-University Kiel, 24118, Kiel, Germany.
School of Chemistry, University of Birmingham, Edgbaston, Birmingham, B15 2TT, UK.
Department of Chemistry, University of Munich (LMU), Butenandtstrasse 5-13, Haus D, 81377, Munich, Germany.

Metal–organic frameworks (MOFs) are a rapidly growing class of materials that offer great promise in various applications. However, the synthesis remains challenging: for example, a range of crystal structures can often be accessed from the same building blocks, which complicates the phase selectivity. Likewise, the high sensitivity to slight changes in synthesis conditions may cause reproducibility issues. This is crucial, as it hampers the research and commercialization of affected MOFs. Here, it presents the first-ever interlaboratory study of the synthetic reproducibility of two Zr–porphyrin MOFs, PCN-222 and PCN-224, to investigate the scope of this problem. For PCN-222, only one sample out of ten was phase pure and of the correct symmetry, while for PCN-224, three are phase pure, although none of these show the spatial linker order characteristic of PCN-224. Instead, these samples resemble dPCN-224 (disordered PCN-224), which has recently been reported. The variability in thermal behavior, defect content, and surface area of the synthesised samples are also studied. The results have important ramifications for field of metal–organic frameworks and their crystallization, by highlighting the synthetic challenges associated with a multi-variable synthesis space and flat energy landscapes characteristic of MOFs.

中文翻译：

Zr-卟啉金属有机骨架的合成重现性如何？实验室间研究

金属有机框架（MOF）是一类快速发展的材料，在各种应用中具有广阔的前景。然而，合成仍然具有挑战性：例如，通常可以从相同的构建块获得一系列晶体结构，这使相选择性变得复杂。同样，对合成条件的轻微变化的高敏感性可能会导致重现性问题。这一点至关重要，因为它阻碍了受影响 MOF 的研究和商业化。在此，它首次对两种 Zr-卟啉 MOF（PCN-222 和 PCN-224）的合成重现性进行了实验室间研究，以调查该问题的范围。对于 PCN-222，只有十分之一的样品是相位纯的并且具有正确的对称性，而对于 PCN-224，三个是相位纯的，尽管这些样品都没有显示出 PCN-224 的空间连接子顺序特征。相反，这些样本类似于最近报道的 dPCN-224（无序 PCN-224）。还研究了合成样品的热行为、缺陷含量和表面积的变化。通过强调与 MOF 的多变量合成空间和平坦能量景观特征相关的合成挑战，该结果对金属有机框架及其结晶领域具有重要影响。

更新日期：2023-09-05

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