Charting the Metal-Dependent High-Pressure Stability of Bimetallic UiO-66 Materials

Rogge, Sven M. J.; Yot, Pascal G.; Jacobsen, Jannick; Muniz‐Miranda, Francesco; Vandenbrande, Steven; Gosch, Jonas; Ortiz, Vanessa; Collings, Ines E.; Devautour‐Vinot, Sabine; Maurin, Guillaume; Stock, Norbert; Speybroeck, Véronique Van

doi:10.1021/acsmaterialslett.0c00042

Cited by 32 publications

(25 citation statements)

References 66 publications

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“…106 In a different study, the onset pressure where amorphization occurs was studied as a function of metal node composition in UiO-66(Ce/Zr) and UiO-66(Hf/Zr) via experiment and computation, showing that cerium-based UiO-66 materials have lower mechanical stability compared to their Zr and Hf analogs; see Figure 4. 23 Likewise, and in agreement with previous studies, a large impact of defects on the mechanical stability of UiO-66 based materials was found. Therefore, the increase in catalytic activity through both catalytically active defects and cerium reduces the frameworks' mechanical stability, which agrees with trends in thermal stability.…”

Section: ■ Introductionsupporting

confidence: 91%

“…Here we would like to emphasize that existing high-pressure structural studies have shown that all the different chemical aspects of MOFs together define the pressure responsive properties, i.e. topology, 13,14,141 porosity, 74 linker length, 74,89 metal-node chemistry, 23,106,163 and the presence of defects. 107 The chemical diversity of MOFs provides a unique material platform to validate existing principles and to identify new guidelines and potentially new unexpected properties.…”

Section: ■ Introductionmentioning

confidence: 98%

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Structural Chemistry of Metal–Organic Frameworks under Hydrostatic Pressures

Vervoorts

Stebani

Méndez

et al. 2021

ACS Materials Lett.

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Studying the structural behavior of metal–organic frameworks (MOFs) under hydrostatic pressures is a steadily growing area. The goal of active research is identification of overarching composition–structure principles including both properties of technological relevance and material behavior of academic interest such as material stability criteria, mechanical properties, pressure-induced phase transitions, negative compressibilities, and guest-dependent high-pressure structural responses. Here the current literature on the high-pressure structural responses of MOFs is reviewed with focus on bulk moduli, pressure-transmitting medium dependent properties, pressure-induced phase transitions, and amorphization processesproperties that are derived from high-pressure X-ray diffraction studies. After highlighting topical examples, aspects of high-pressure diffraction studies on MOFs are summarized that are important to advance the field such as the rigorous reporting of experimental and analytical procedures, opportunities that come with custom-made high-pressure diffraction setups, the nature and impact of the pressure-transmitting medium, and the role of forging even closer ties between computation and experiment.

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Section: ■ Introductionsupporting

confidence: 91%

Section: ■ Introductionmentioning

confidence: 98%

Structural Chemistry of Metal–Organic Frameworks under Hydrostatic Pressures

Vervoorts

Stebani

Méndez

et al. 2021

ACS Materials Lett.

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“…While numerous reports support the notion that changes to the organic linker [21][22] and topology [23][24] can impact the compressibility of MOFs, systematic studies into the effect of changes to the metal node are less prevalent. 25 Herein, we investigate the role of the metal-carboxylate bond in the compression of UiO-66 by varying the identity of the metal node from Zr-UiO-66 to Hf-UiO-66 and Ce-UiO-66. By keeping the topology, linker, and experimental conditions constant, we isolate the coordination bond as the single structural variable that changes in this series of MOFs.…”

Section: Introductionmentioning

confidence: 99%

Isolating the Role of the Node-Linker Bond in the Compression of UiO-66 Metal–Organic Frameworks

et al. 2020

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Understanding the mechanical properties of metal-organic frameworks (MOFs) is essential to the fundamental advancement and practical implementations of porous materials. Recent computational and experimental efforts have revealed correlations between mechanical properties and pore size, topology, and defect density. These results demonstrate the important role of the organic linker in the response of these materials to physical stresses. However, the impact of the coordination bond between the inorganic node and organic linker on the mechanical stability of MOFs has not been thoroughly studied. Here, we isolate the role of this node-linker coordination bond to systematically study the effect it plays in the compression of a series of isostructural MOFs, M-UiO-66 (M = Zr, Hf, or Ce). The bulk modulus (i.e. the resistance to compression under hydrostatic pressure) of each MOF is determined by in situ diamond anvil cell (DAC) powder X-ray diffraction measurements and density functional theory (DFT) simulations. These experiments reveal distinctive behavior of Ce-UiO-66 in response to pressures under one GPa. In situ DAC Raman spectroscopy and DFT calculations support the observed differences in compressibility between Zr-UiO-66 and the Ceanalogue. Monitoring changes in bond lengths as a function of pressure through DFT simulations provides a clear picture of those which shorten more drastically under pressure and those which resist compression. This study demonstrates that changes to the node-linker bond can have significant ramifications on the mechanical properties of MOFs. File list (2) download file view on ChemRxiv Isolating the Role of the Node-Linker Bond in the Compr... (830.80 KiB) download file view on ChemRxiv Electronic supporting information.pdf (1.12 MiB)

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“…2B-2F). As shown in the spectra of the UiO-66-CdTe core, the typical Zr 3d, Cd 3d, Te 3d, O 1s and C 1s peaks were noted at 179.7, 402.2, 569.8, 529.2 and 284.8 eV, respectively 28 . In the spectra of the UiO-66-CdTe@ZIF-8 CSNCPs, there was a weak signal attributed to Zn 2p suggesting that ZIF-8 shell was successfully attached to the UiO-66-CdTe core.…”

Section: Discussionmentioning

confidence: 90%

A ratiometric fluorescence sensor based on UiO-66-CdTe@ZIF-8 core-shell nanocomposites for the highly selective detection of NO

Shi¹,

Zhang²

2021

Preprint

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In this work, a ratiometric fluorescence sensor based on UiO-66-CdTe@ZIF-8 core-shell nanocomposites (CSNCPs) was developed for the highly selective detection of NO. The yellow-emitting UiO-66-NH2 core was synthesised using the solvothermal method and then coated with red-emitting CdTe quantum dots (QDs). The resulting core UiO-66-CdTe nanocomposites served as the signal-displaying unit (UiO-66-CdTe). Next, the UiO-66-CdTe nanocomposite was encapsulated in a zeolitic imidazolate framework (ZIF-8), whereas large molecules such as substrate and oxidase have very little effect on its fluorescence. A detectable signal was obtained by monitoring the NO quenching fluorescence of UiO-66-NH2, and the CdTe QDs served as the reference signal. The fluorescence quenching ratio I442/I574 was proportional to the logarithm of NO concentration concentration in the range of 0-0.10 nM with the detection limit of 0.11 nM. The results demonstrate that the proposed UiO-66-CdTe@ZIF-8 CSNCPs-based sensor is suitable for quantitative purposes in various environmental and biological applications.

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Charting the Metal-Dependent High-Pressure Stability of Bimetallic UiO-66 Materials

Cited by 32 publications

References 66 publications

Structural Chemistry of Metal–Organic Frameworks under Hydrostatic Pressures

Structural Chemistry of Metal–Organic Frameworks under Hydrostatic Pressures

Isolating the Role of the Node-Linker Bond in the Compression of UiO-66 Metal–Organic Frameworks

A ratiometric fluorescence sensor based on UiO-66-CdTe@ZIF-8 core-shell nanocomposites for the highly selective detection of NO

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