Long‐Term Photostability in Terephthalate Metal–Organic Frameworks

Mateo, Diego; Santiago‐Portillo, Andrea; Albero, Josep; Navalón, Sergio; Álvaro, Mercedes; Garcı́a, Hermenegildo

doi:10.1002/ange.201911600

Cited by 21 publications

(14 citation statements)

References 39 publications

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“…The powder XRD patterns of Zr-MOFs are shown in Figure 2. The positions of their diffraction peaks are very similar, which are consistent with the XRD patterns of typical UIO-66 MOF, [40] indicating that a large amount of hydrochloric acid does not affect the synthesis of UiO-66 (Zr). As the extension of prepared time, the intensity of XRD diffraction peak increases correspondingly (Figure 2a), which indicates that the degree of crystallite increases gradually, and this is consistent with the results of SEM.…”

Section: Characterization Of the Uio-66 (Zr) Catalystssupporting

confidence: 77%

Synthesis of defected UIO‐66 with boosting the catalytic performance via rapid crystallization

Chu

Guo

Wang

et al. 2021

Applied Organom Chemis

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Due to environmental and health concerns, it is very important to develop high activity oxidative desulfurization (ODS) catalyst for petroleum purification. Recently, defect engineering of metal organic frameworks (MOFs) to generate a large number of unsaturated catalytic active sites is a very promising approach. Defective MOF has good research value as ODS catalyst. Here, UIO‐66 with lots of defects can be prepared by rapid crystallization using concentrated hydrochloric acid as a modulator. The prepared UIO‐66 material has good industrial applicability due to its low synthesis temperature (100°C), short synthesis time (20–30 min), large‐scale preparation, and excellent catalytic performance (dibenzothiophene can be entirely removed in 6 min under the optimal catalytic conditions [25‐mg catalyst, 60°C, O/S 7.5]). The obtained material exhibits not only extraordinary ODS activity of 37.6 mmol h−1 g−1 but also good cycle stability for the removal of DBT (in 7 cycles without significant loss of activity, greater than 90.2%). And for large space volume 4,6‐DMDBT, it also shows excellent catalytic performance. The ODS mechanism of defect UIO‐66 for DBT is explored, and it proves that hydroxyl radicals and superoxide radicals are generated and play a critical role in ODS reaction. The excellent catalytic performance of defect UIO‐66 gives mainly the credit to the abundant defect sites, large specific surface area, and pore volume.

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Section: Characterization Of the Uio-66 (Zr) Catalystssupporting

confidence: 77%

Synthesis of defected UIO‐66 with boosting the catalytic performance via rapid crystallization

Chu

Guo

Wang

et al. 2021

Applied Organom Chemis

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“…The detailed synthetic procedures are presented in Supporting Information. It is established that the nodes of MIL-101 are constituted by three octahedra sharing a µ 3 -O corner and one Fe at the center [ 45 ]. As shown in Fig.…”

Section: Resultsmentioning

confidence: 99%

Tuning Atomically Dispersed Fe Sites in Metal–Organic Frameworks Boosts Peroxidase-Like Activity for Sensitive Biosensing

Kang

Jiao

et al. 2020

Nano-Micro Lett.

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Although nanozymes have been widely developed, accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant challenges. Herein, two functional groups with opposite electron modulation abilities (nitro and amino) were introduced into the metal–organic frameworks (MIL-101(Fe)) to tune the atomically dispersed metal sites and thus regulate the enzyme-like activity. Notably, the functionalization of nitro can enhance the peroxidase (POD)-like activity of MIL-101(Fe), while the amino is poles apart. Theoretical calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active sites. Benefiting from both geometric and electronic effects, the nitro-functionalized MIL-101(Fe) with a low reaction energy barrier for the HO* formation exhibits a superior POD-like activity. As a concept of the application, a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−1. Moreover, the detection of organophosphorus pesticides was also achieved. This work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors.

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“…This small CO 2 evolution from MIP-208@RuO x compares favourably with the stability of the most robust MOFs reported as photocatalysts under similar irradiation conditions. 81 The crystallinity of the MIP-208@RuO x sample after seven times cycling in catalysis was well-maintained, as no notable change in the PXRD pattern was observed (Figure S14). Furthermore, the solid-state 13 C-NMR spectra of the fresh and seven-time reused MIP-208@RuO x were coincident (Figure S15).…”

Section: Resultsmentioning

confidence: 95%

A Robust Titanium Isophthalate Metal-Organic Framework for Visible-Light Photocatalytic CO2 Methanation

Wang

Cabrero-Antonino

Navalón

et al. 2020

Chem

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Isophthalic acid (IPA), a feedstock linker, has been considered so far to build series of topical metal-organic frameworks (MOFs) of diverse structures with various di-and trivalent metal ions, such as CAU-10(Al), owing to its facile availability, unique connection angle/mode and a wide scope of functional groups attached. Constructing MOFs from IPA and tetravalent metals, typically Group 4 metals, would be of a great interest due to expected higher chemical stability. In particular, titanium-IPA frameworks possessing photoresponse is alluring, in relation to the known challenge of synthesizing new Ti-MOFs. Here, we have synthesized the first Ti-IPA MOF, denoted as MIP-208, via a solvothermal process that efficiently combines the use of preformed Ti 8 oxoclusters and in situ acetylation of 5-NH 2 -IPA linker. MIP-208 has helical chains of cis-connected corner-sharing TiO 6 polyhedra as the inorganic building units, which are interconnected to each other leading to a 3D ultramicroporous framework. Solid-solution mixed linkers strategy was then successfully applied resulting in a series of multivariate MIP-208 structures with tunable chemical environment and sizable porosity. Finally, the excellent thermal and hydrolytic stabilities of MIP-208 allowed its use for the photocatalytic carbon dioxide (CO 2 ) methanation, showing the best result among the pure MOF catalysts. Ruthenium oxide nanoparticles were further photodeposited on MIP-208 forming a highly active and selective composite catalyst, MIP-208@RuO x , to largely improve the photocatalytic performance, which features a notable visible light response, an excellent stability and recycling ability.

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Long‐Term Photostability in Terephthalate Metal–Organic Frameworks

Cited by 21 publications

References 39 publications

Synthesis of defected UIO‐66 with boosting the catalytic performance via rapid crystallization

Synthesis of defected UIO‐66 with boosting the catalytic performance via rapid crystallization

Tuning Atomically Dispersed Fe Sites in Metal–Organic Frameworks Boosts Peroxidase-Like Activity for Sensitive Biosensing

A Robust Titanium Isophthalate Metal-Organic Framework for Visible-Light Photocatalytic CO2 Methanation

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