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Microwaves induced epitaxial growth of urchin like MIL-53(Al) crystals on ceramic supports.

ABSTRACT: Shaping Metal-Organic Frameworks (MOFs) poses a significant challenge for their widespread application on a large scale. In particular, a precise control over crystal orientation and arrangement on substrates are expected to provide exiting opportunities for novel materials with customized characteristics and enhanced performance in catalysis, gas storage, sensing, optics and electronics. Here we demonstrated for the first time that microwave irradiation can induce well controlled epitaxial growth of urchin-like MIL-53(Al) crystals via the hydrothermal conversion of Atomic Layer Deposition alumina layers on SiC foams. The resulting large, ordered crystals feature specific size, homogeneity, dispersion, and quantity that strongly correlate with the nature of the ceramic support and its ability to absorb microwaves. Furthermore, the supported MIL-53(Al) urchins were considered as templates for generating nanostructured alumina fibers on SiC foams, providing attractive catalyst carriers with high specific surface areas.

SUBMITTER: Ben Neon L

PROVIDER: S-EPMC11362168 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature

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Microwaves induced epitaxial growth of urchin like MIL-53(Al) crystals on ceramic supports.

Ben Neon Limor L Drobek Martin M Bechelany Mikhael M Rebiere Bertrand B Julbe Anne A

Scientific reports 20240829 1

Shaping Metal-Organic Frameworks (MOFs) poses a significant challenge for their widespread application on a large scale. In particular, a precise control over crystal orientation and arrangement on substrates are expected to provide exiting opportunities for novel materials with customized characteristics and enhanced performance in catalysis, gas storage, sensing, optics and electronics. Here we demonstrated for the first time that microwave irradiation can induce well controlled epitaxial grow ...[more]

PMID: 39209977

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Project description:In this study, hybrids of nanoporous MIL-101(Cr) and MIL-53(Al) were synthesized using a hydrothermal method for various time periods, ranging from 8 to 40 h. The prepared materials were characterized by powder X-ray diffraction (PXRD) and elemental analysis, and their specific surface areas were measured by N2 sorption at 77 K using the Brunauer-Emmett-Teller (BET) method. To investigate the practical application of these materials, the pure carbon dioxide and methane adsorption capacities of the samples were determined using the volumetric method. The Langmuir model was used to fit the CO2 and CH4 isotherms. Extended Langmuir (EL) equations and the ideal adsorbed solution theory (IAST) models were used to obtain the CO2/CH4 selectivity. The sample with the highest BET specific surface area was selected as a candidate for further investigations. The thermal stability of the selected sample was investigated by thermogravimetric analysis (TGA). Scanning electron microscopy (SEM) was used to characterize the sample morphology. XRD results showed that the sample synthesized over the shortest time corresponded to MIL-101(Cr), while the sample synthesized over the longest time was in agreement with MIL-53(Al). Samples synthesized for time periods between these two limits were assumed to be composites of both MIL-53(Al) and MIL-101(Cr). TGA results indicated that the hybrid materials were thermally stable at temperatures about 100 °C higher than for pure MIL-101(Cr). The BET specific surface area (1746 m2 g-1) and CO2 adsorption capacity (16 mmol g-1) of the selected hybrid sample were about 50% and 35% higher, respectively, compared with those of pure MIL-53(Al), but 30% and 20% lower, respectively, compared with those of pure MIL-101(Cr). Binary adsorption modeling showed the high selectivity of the MIL-101(Cr) and MIL-53(Al) hybrid material for CO2 with a minimum separation factor of about 60 at 298 K. This value was much higher than those reported previously and those observed in this work for the original MIL-101(Cr) or MIL-53(Al). These results demonstrated that the hybrid of MIL-101(Cr) and MIL-53(Al) was a promising material for selective CO2 capture from natural and biogas.

Project description:The application of metal-organic frameworks (MOFs) has attracted increasing attention in organic synthesis. The modification of MOFs can efficiently tailor the structure and improve the property for meeting ongoing demand in various applications, such as the alteration of gas adsorption and separation, catalytic activity, stability, and sustainability or reusability. In this study, carboxyethylsilanetriol (CEST) disodium salt was used as a dual-functional ligand for modified Al-MIL-53 to fabricate CEST-functionalized Al-MIL-53 samples through a hydrothermal reaction of aluminum nitrate, terephthalic acid, and CEST disodium salt by varying the molar ratio of CEST to terephthalic acid and keeping a constant molar ratio of Al3+/-COOH of 1:1. The structure, composition, morphology, pore feature, and stability were characterized by XRD, different spectroscopies, electron microscopy, N2 physisorption, and thermogravimetric analysis. With increasing CEST content, CEST-Al-MIL-53 still preserves an Al-MIL-53-like structure, but the microstructure changed compared with pure Al-MIL-53 due to the integration of CEST. Such a CEST-Al-MIL-53 was used as the support to load Pd particles and afford a catalyst Pd/CEST-Al-MIL-53 for Suzuki-Miyaura C-C cross-coupling reaction of aryl halides and phenylboronic acid under basic conditions. The resulting Pd/CEST-Al-MIL-53 showed a high catalytic activity compared with Pd/Al-MIL-53, due to the nanofibrous structure of silicon species-integrated CEST-Al-MIL-53. The nanofiber microstructure undergoes a remarkable transformation into intricate 3D cross-networks during catalytic reaction, which enables the leachable Pd particles to orientally redeposit and inlay into these networks as the monodisperse spheres and thereby effectively preventing Pd particles from aggregation and leaching, therefore demonstrating a high catalytic performance, long-term stability, and enhanced reusability. Obviously, the integration of CEST into MOFs can effectively prevent the leaching of active Pd species and ensure the re-deposition during catalysis. Moreover, catalytic performance strongly depended on catalyst dosage, temperature, time, solvent, and the type of the substituted group on benzene ring. This work further extends the catalytic application of hybrid metal-organic frameworks.

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Microwaves induced epitaxial growth of urchin like MIL-53(Al) crystals on ceramic supports.

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Microwaves induced epitaxial growth of urchin like MIL-53(Al) crystals on ceramic supports.

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