scholarly journals A Facile Method for Preparing UiO-66 Encapsulated Ru Catalyst and its Application in Plasma-Assisted CO2 Methanation

Nanomaterials ◽  
2019 ◽  
Vol 9 (10) ◽  
pp. 1432 ◽  
Author(s):  
Weiwei Xu ◽  
Mengyue Dong ◽  
Lanbo Di ◽  
Xiuling Zhang

With increasing applications of metal-organic frameworks (MOFs) in the field of gas separation and catalysis, the preparation and performance research of encapsulating metal nanoparticles (NPs) into MOFs (M@MOF) have attracted extensive attention recently. Herein, an Ru@UiO-66 catalyst is prepared by a one-step method. Ru NPs are encapsulated in situ in the UiO-66 skeleton structure during the synthesis of UiO-66 metal-organic framework via a solvothermal method, and its catalytic activity for CO2 methanation with the synergy of cold plasma is studied. The crystallinity and structural integrity of UiO-66 is maintained after encapsulating Ru NPs according to the X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM). As illustrated by X-ray photoelectron spectroscopy (XPS), high resolution transmission electron microscopy (HRTEM), and mapping analysis, the Ru species of the hydration ruthenium trichloride precursor are reduced to metallic Ru NPs without additional reducing processes during the synthesis of Ru@UiO-66, and the Ru NPs are uniformly distributed inside the Ru@UiO-66. Thermogravimetric analysis (TGA) and N2 sorption analysis show that the specific surface area and thermal stability of Ru@UiO-66 decrease slightly compared with that of UiO-66 and was ascribed to the encapsulation of Ru NPs in the UiO-66 skeleton. The results of plasma-assisted catalytic CO2 methanation indicate that Ru@UiO-66 exhibits excellent catalytic activity. CO2 conversion and CH4 selectivity over Ru@UiO-66 reached 72.2% and 95.4% under 13.0 W of discharge power and a 30 mL·min−1 gas flow rate ( V H 2 : V C O 2 = 4 : 1 ), respectively. Both values are significantly higher than pure UiO-66 with plasma and Ru/Al2O3 with plasma. The enhanced performance of Ru@UiO-66 is attributed to its unique framework structure and excellent dispersion of Ru NPs.

Sensors ◽  
2021 ◽  
Vol 21 (13) ◽  
pp. 4352
Author(s):  
Yanli Kang ◽  
Lu Zhang ◽  
Wenhao Wang ◽  
Feng Yu

It is of great significance to develop ethanol sensors with high sensitivity and low detection temperature. Hence, we prepared Au-supported material on mesoporous ZnO composites derived from a metal-organic framework ZIF-8 for the detection of ethanol gas. The obtained Au/ZnO materials were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (SEM), field emission transmission electron microscopy (TEM) and nitrogen adsorption and desorption isotherms. The results showed that the Au/ZnO-1.0 sample maintains a three-dimensional (3D) dodecahedron structure with a larger specific surface area (22.79 m2 g−1) and has more oxygen vacancies. Because of the unique ZIF structure, abundant surface defects and the formation of Au-ZnO Schottky junctions, an Au/ZnO-1.0 sensor has a response factor of 37.74 for 100 ppm ethanol at 250 °C, which is about 6 times that of pure ZnO material. In addition, the Au/ZnO-1.0 sensor has good selectivity for ethanol. According to density functional theory (DFT) calculations, the adsorption energy of Au/ZnO for ethanol (−1.813 eV) is significantly greater than that of pure ZnO (−0.217 eV). Furthermore, the adsorption energy for ethanol is greater than that of other gases.


NANO ◽  
2019 ◽  
Vol 14 (01) ◽  
pp. 1950005 ◽  
Author(s):  
Zhongfei Liu ◽  
Jiangtao Yuan ◽  
Hui Zhang ◽  
Kuangwei Xiong ◽  
Shaowei Jin ◽  
...  

In this paper, the MOFs-derived carbonaceous ZnO and RGO (carbonaceous ZnO/RGO) composites have been prepared by the wet chemical method and carbonization process. The as-prepared products are characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy (TEM), Raman spectra, thermogravimetric (TG) analysis and X-ray photoelectron spectroscopy (XPS). The electromagnetic parameters of carbonaceous ZnO/RGO composites are investigated by the vector network analyzer. The results exhibit carbonaceous ZnO/RGO composites have a maximum absorption of [Formula: see text][Formula: see text]dB at 6[Formula: see text]GHz with thickness of 3.5[Formula: see text]mm and the effective absorption (below [Formula: see text][Formula: see text]dB) bandwidth is up to 1.92[Formula: see text]GHz (from 5.28 to 7.2[Formula: see text]GHz). Thus, the carbonaceous ZnO/RGO composites have great potential in the field of electromagnetic wave absorption.


2021 ◽  
Vol 2021 ◽  
pp. 1-13
Author(s):  
Pham Dinh Du ◽  
Pham Ngoc Hoai

The iron (III) benzene dicarboxylate metal-organic framework material (MIL-53(Fe)) was synthesized with either the solvent-thermal or hydrothermal method under different conditions. The influence of the type of solvents, molar ratio of precursors and solvent, temperature, and reaction time on the structure of MIL-53(Fe) was investigated. The material was characterized by using X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), and N2 adsorption/desorption isotherm. The MIL-53(Fe) structure formed in N′, N-dimethylformamide (DMF) and methanol (MeOH) but not in water. In DMF, the molar ratio of precursors and solvent, temperature, and reaction time had a significant effect on the crystal structure of MIL-53(Fe). Under optimal conditions, MIL-53(Fe) has high crystallinity and a large specific surface area ( S BET  = 88.2 m2/g). The obtained MIL-53(Fe) could serve as a potential heterogeneous catalyst to oxidize phenol (PhN), rhodamine B (RhB), and methylene blue (MtB) in the Fenton-like reaction system at the different solution pHs.


2016 ◽  
Vol 2016 ◽  
pp. 1-9 ◽  
Author(s):  
José María Rivera ◽  
Susana Rincón ◽  
Cherif Ben Youssef ◽  
Alejandro Zepeda

Mesoporous metal-organic framework-5 (MOF-5), with the composition Zn4O(BDC)3, showed a high capacity for the adsorptive removal of Pb(II) from 100% aqueous media. After the adsorption process, changes in both morphology and composition were detected using a scanning electron microscope (SEM) equipped with an energy dispersive X-ray (EDX) system, Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS) analysis. The experimental evidence showed that Zn(II) liberation from MOF-5 structure was provoked by the water effect demonstrating that Pb(II) removal is not due to ionic exchange with Zn. A kinetic study showed that Pb(II) removal was carried out in 30 min with a behavior of pseudo-second-order kinetic model. The experimental data on Pb(II) adsorption were adequately fit by both the Langmuir and BET isotherm models with maximum adsorption capacities of 658.5 and 412.7 mg/g, respectively, at pH 5 and 45°C. The results of this work demonstrate that the use of MOF-5 has great potential for applications in environmental protection, especially regarding the removal of the lead present in industrial wastewaters and tap waters.


2019 ◽  
Vol 2019 ◽  
pp. 1-15 ◽  
Author(s):  
Pham Dinh Du ◽  
Huynh Thi Minh Thanh ◽  
Thuy Chau To ◽  
Ho Sy Thang ◽  
Mai Xuan Tinh ◽  
...  

In the present paper, the synthesis of metal-organic framework MIL-101 and its application in the photocatalytic degradation of Remazol Black B (RBB) dye have been demonstrated. The obtained samples were characterized by X-ray diffraction (XRD), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption/desorption isotherms at 77 K. It was found that MIL-101 synthesized under optimal conditions exhibited high crystallinity and specific surface area (3360 m2·g-1). The obtained MIL-101 possessed high stability in water for 14 days and several solvents (benzene, ethanol, and water at boiling temperature). Its catalytic activities were evaluated by measuring the degradation of RBB in an aqueous solution under UV radiation. The findings show that MIL-101 was a heterogeneous photocatalyst in the degradation reaction of RBB. The mechanism of photocatalysis was considered to be achieved by the electron transfer from photoexcited organic ligands to metallic clusters in MIL-101. The kinetics of photocatalytic degradation reaction were analyzed by using the initial rate method and Langmuir-Hinshelwood model. The MIL-101 photocatalyst exhibited excellent catalytic recyclability and stability and can be a potential catalyst for the treatment of organic pollutants in aqueous solutions.


Catalysts ◽  
2020 ◽  
Vol 10 (4) ◽  
pp. 375
Author(s):  
Adele R. Latypova ◽  
Maxim D. Lebedev ◽  
Evgeniy V. Rumyantsev ◽  
Dmitry V. Filippov ◽  
Olga V. Lefedova ◽  
...  

The article describes the synthesis of aminoorgano-functionalized silica as a prospective material for catalysis application. The amino groups have electron donor properties which are valuable for the metal chemical state of palladium. Therefore, the presence of electron donor groups is important for increasing catalysts’ stability. The research is devoted to the investigation of silica amino-modified support influence on the activity and stability of palladium species in 4-nitroaniline hydrogenation process. A series of catalysts with different supports such as SiO2, SiO2-C3H6-NH2 (amino-functionalized silica), γ-Al2O3 and activated carbon were studied. The catalytic activity was studied in the hydrogenation of 4-nitroaniline to 1,4-phenylenediamine. The catalysts were characterized by scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and chemisorption of hydrogen by the pulse technique. The 5 wt.% Pd/SiO2-C3H6-NH2 catalyst exhibited the highest catalytic activity for 4-nitroaniline hydrogenation with 100% conversion and 99% selectivity with respect to 1,4-phenylenediamine.


2019 ◽  
Vol 79 (12) ◽  
pp. 2357-2365 ◽  
Author(s):  
Huaisu Guo ◽  
Weilin Guo ◽  
Yang Liu ◽  
Xiaohua Ren

Abstract In this work, quinone-modified metal-organic framework MIL-101(Fe)(Q-MIL-101(Fe)), as a novel heterogeneous Fenton-like catalyst, was synthesized for the activation of persulfate (PS) to remove bisphenol A (BPA). The synthetic Q-MIL-101(Fe) was characterized via X-ray diffraction, scanning electron microscope, Fourier transform infrared, electrochemical impedance spectroscopy, cyclic voltammetry and X-ray photoelectron spectroscopy. As compared to the pure MIL-101(Fe), Q-MIL-101(Fe) displayed better catalytic activity and reusability. The results manifested that the Q-MIL-101(Fe) kept quinone units, which successfully promoted the redox cycling of Fe3+/Fe2+ and enhanced the removal efficiency. In addition, the reaction factors of Q-MIL-101(Fe) were studied (e.g. pH, catalyst dosage, PS concentration and temperature), showing that the optimum conditions were [catalyst] = 0.2 g/L, [BPA] = 60 mg/L, [PS] = 4 mmol/L, pH = 6.79, temperature = 25 °C. On the basis of these findings, the probable mechanism on the heterogeneous activation of PS by Q-MIL-101(Fe) was proposed.


2019 ◽  
Vol 75 (8) ◽  
pp. 1053-1059 ◽  
Author(s):  
Lin-Lu Qian ◽  
Zhi-Xiang Wang ◽  
Hai-Xin Tian ◽  
Min Li ◽  
Bao-Long Li ◽  
...  

Metal–organic frameworks (MOFs) have attracted much interest in the fields of gas separation and storage, catalysis synthesis, nonlinear optics, sensors, luminescence, magnetism, photocatalysis gradation and crystal engineering because of their diverse properties and intriguing topologies. A Cu–MOF, namely poly[[(μ2-succinato-κ2 O:O′){μ2-tris[4-(1,2,4-triazol-1-yl)phenyl]amine-κ2 N:N′}copper(II)] dihydrate], {[Cu(C4H4O4)(C24H18N10)]·2H2O} n or {[Cu(suc)(ttpa)]·2H2O} n , (I), was synthesized by the hydrothermal method using tris[4-(1,2,4-triazol-1-yl)phenyl]amine (ttpa) and succinate (suc2−), and characterized by IR, powder X-ray diffraction (PXRD), luminescence, optical band gap and valence band X-ray photoelectron spectroscopy (VB XPS). Cu–MOF (I) shows a twofold interpenetrating 4-coordinated three-dimensional CdSO4 topology with point symbol {65·8}. It presents good photocatalytic degradation of methylene blue (MB) and rhodamine B (RhB) under visible-light irradiation. A photocatalytic mechanism was proposed and confirmed.


Applied Nano ◽  
2021 ◽  
Vol 2 (4) ◽  
pp. 344-358
Author(s):  
Daiana A. Bravo Fuchineco ◽  
Angélica C. Heredia ◽  
Sandra M. Mendoza ◽  
Enrique Rodríguez-Castellón ◽  
Mónica E. Crivello

The massive use of petroleum and its possible exhaustion are driving the current research trend to study alternative raw materials from biomass for organic reactions. In this context, the present article presents a study of the catalytic esterification of levulinic acid, a platform molecule, with ethanol. Metal-organic framework (MOF) type compounds UiO-66-NH2 have been synthesized. Zirconium was incorporated, using zirconium chloride as a metal precursor, together with 2-aminoterephthalic acid as an organic binding agent. An alternative route of synthesis was proposed using more favorable conditions from an economic and environmental point of view, replacing dimethylformamide by 50 and 75% acetone as substitute solvent. The physicochemical properties of the materials were evaluated by X-ray diffraction (XRD), Infrared Spectrometry with Fourier Transform (FTIR), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), microwave plasma atomic emission spectroscopy (MP-AES) and N2 adsorption to understand their morphology, crystalline, chemical and pore structure. The progress of the reaction was followed by gas chromatography and mass spectroscopy. The catalytic activity result of MOF25% in autoclave reactor, showed 100% of selectivity to ethyl levulinate and a turnover number (TON) of 66.18 moles of product/moles of Zr. This good catalytic performance obtained by partial solvent replacement in the synthetic material provides a more economical and eco-friendly process for ethyl levulinate generation.


Sign in / Sign up

Export Citation Format

Share Document