Stability of UiO-66 under acidic treatment: Opportunities and limitations for post-synthetic modifications

Piscopo, Calogero G.; Polyzoidis, Angelos; Schwarzer, M.; Loebbecke, S.

doi:10.1016/j.micromeso.2015.01.032

Cited by 173 publications

(66 citation statements)

References 35 publications

(30 reference statements)

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“…Calcination processes are not compatible with the reduced thermal stability of MOFs relative to that of zeolites and other robust materials. Furthermore, intensive washing procedures such as solvent extraction often lead to leaching of both linkers and metals, despite not affecting the crystal structure of the network …”

Section: Figuresupporting

confidence: 61%

Batch versus Flow Acetalization of Benzaldehyde with HKUST‐1: Diffusion Pathways and Performance Comparison

et al. 2016

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Understanding the poisoning and deactivation pathways of metal–organic frameworks (MOFs) is an essential goal to boost their application as robust and efficient catalysts in chemical transformations relevant to industrial processes. Herein, the acetalization reaction of benzaldehyde with methanol was investigated by using [Cu3(BTC)2] (BTC=1,3,5‐benzenetricarboxylate) as a catalyst. The reaction was performed under batch and continuous flow conditions, and the conversion of benzaldehyde into 1,1‐dimethoxytoluene proceeded efficiently in the presence of a modest amount of water. Nevertheless, a drastic reduction in the catalytic activity was observed after recycling the MOF for repetitive batch experiments and after prolonged continuous flow tests. Pore clogging of the MOF and partial crystal‐structure modifications, gathered from XRD and pore analyses, suggested grinding the catalyst prior to application; the ground catalyst showed a considerable enhancement in catalytic performance.

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Section: Figuresupporting

confidence: 61%

Batch versus Flow Acetalization of Benzaldehyde with HKUST‐1: Diffusion Pathways and Performance Comparison

et al. 2016

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“…It should be noted that the choice of reagents for acidic functionalization of MOFs is very important. For example, using chlorosulfonic acid as a sulfonating agent may results in decomposition of the crystal structure of MOF support . Therefore, installation of SO 3 H groups on the MOF support under mild conditions would be very favorable.…”

Section: Introductionmentioning

confidence: 99%

Sulfonic Acid Functionalized MIL‐101(Cr) Metal‐Organic Framework for Catalytic Production of Acetals

et al. 2019

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A simple and green process for acetalization of benzaldehyde derivatives in the presence of a new solid acid nanocatalyst is reported. For this purpose, MIL-101(Cr) was synthesized in the absence of HF and then sulfonic acid functionalized MOF was prepared under mild conditions without using hazardous chemicals. First, the MIL-101(Cr) was functionalized with cysteamine as a non-toxic material to afford MIL-101(Cr)-SH. Then, reaction of the MIL-101(Cr)-SH with hydrogen peroxide as a clean oxidant followed by acidification with diluted sulfuric acid produced MIL-101(Cr)-SO 3 H solid acid nanocatalyst. Characterization of the prepared nanocatalyst was carried out with various physicochemical methods. The results of elemental analysis and FT-IR spectroscopy confirmed the stepwise functionalization of MIL-101(Cr) with sulfonic acid groups. Nitrogen adsorption-desorption analysis indicated the reduction of surface area after functionalization of pristine MIL-101 (Cr). X-ray diffraction (XRD) analysis showed that the MIL-101 (Cr) kept its crystal structure during the modification steps. Finally, the activity of prepared catalyst was evaluated in the clean acetalization of benzaldehyde derivatives with ethylene glycol which exhibited excellent efficiencies and produced water as the only byproduct. The nanocatalyst was consecutively recovered and applied 5-times without notable loss of its activity.[a] Dr.

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“…studied the effect of different synthesis parameters of UiO‐66 on its catalytic activity, concluding that the defects in the crystalline structure have a beneficial effect on the oxidation performances . Nevertheless, although these studies highlight the recyclability of the MOFs, it is well‐known that the defects in the UiO‐66 structure are associated with a lower structural stability, compromising a long‐term catalyst utilization.…”

Section: Figurementioning

confidence: 99%

Continuous Flow Desulfurization of a Model Fuel Catalysed by Titanium Functionalized UiO‐66

et al. 2019

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The porous material UiO‐66 is one of the most stable MOFs, retaining its properties under a relatively wide range of chemical and physical conditions, making it attractive for post‐synthetic modifications and catalytic applications. A Titanium functionalization of UiO‐66 has been carried out and the synthesized material has been efficiently used as catalyst in the continuous oxidative desulfurization of a model fuel with aqueous H2O2. Using dibenzothiophene as sulfur source, only a partial desulfurization has been achieved, nevertheless the functionalized MOF showed better performances compared to the standard UiO‐66. The titanium containing MOF allowed to completely removing thioanisole from the oil phase within only eight minutes. The pore sizes of UiO‐66 are playing an important role in allowing a fast oxidation of the thioanisole compared to dibenzothiophene.

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Stability of UiO-66 under acidic treatment: Opportunities and limitations for post-synthetic modifications

Cited by 173 publications

References 35 publications

Batch versus Flow Acetalization of Benzaldehyde with HKUST‐1: Diffusion Pathways and Performance Comparison

Batch versus Flow Acetalization of Benzaldehyde with HKUST‐1: Diffusion Pathways and Performance Comparison

Sulfonic Acid Functionalized MIL‐101(Cr) Metal‐Organic Framework for Catalytic Production of Acetals

Continuous Flow Desulfurization of a Model Fuel Catalysed by Titanium Functionalized UiO‐66

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