scholarly journals Mechanochemical Synthesis of Nickel-Modified Metal–Organic Frameworks for Reduction Reactions

Catalysts ◽  
2021 ◽  
Vol 11 (5) ◽  
pp. 526
Author(s):  
Paulette Gómez-López ◽  
Martyna Murat ◽  
José M. Hidalgo-Herrador ◽  
Carolina Carrillo-Carrión ◽  
Alina M. Balu ◽  
...  

In this work, we report the incorporation of nickel oxide nanoparticles into a metal–organic framework (MOF) structure by a solvent-free mechanochemical strategy. In particular, the zirconium-based MOF UiO-66 was modified with different Ni loadings and characterized using complementary techniques including X-ray diffraction (XRD), N2 porosimetry and X-ray photoelectron spectroscopy (XPS). The catalytic potential of the as-prepared Ni/UiO-66 materials in the hydrogenation reaction of methyl levulinate using 2-propanol as hydrogen donor solvent has been investigated under flow conditions. Under optimized conditions, the 5%Ni/UiO-66 led to the best catalytic performance (70% yield, 100% selectivity to gamma-valerolactone), which could be attributed to the higher content of the Ni species within the MOF structure. The obtained results are promising and contribute to highlighting the great potential of MOFs in biomass upgrading processes, opening the path to the sustainable development of the chemical industry.

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.


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.


Author(s):  
Khaled Alshammari ◽  
Yubiao Niu ◽  
Richard E. Palmer ◽  
Nikolaos Dimitratos

A sol-immobilization method is used to synthesize a series of highly active and stable Au x Pd 1− x /TiO 2 catalysts (where x  = 0, 0.13, 0.25, 0.5, 0.75, 0.87 and 1) for wastewater remediation. The catalytic performance of the materials was evaluated for the catalytic reduction of 4-nitrophenol, a model wastewater contaminant, using NaBH 4 as the reducing agent under mild reaction conditions. Reaction parameters such as substrate/metal and substrate/reducing agent molar ratios, reaction temperature and stirring rate were investigated. Structure-activity correlations were studied using a number of complementary techniques including X-ray powder diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy. The sol-immobilization route provides very small Au–Pd alloyed nanoparticles, with the highest catalytic performance shown by the Au 0.5 Pd 0.5 /TiO 2 catalyst. This article is part of a discussion meeting issue ‘Science to enable the circular economy’.


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.


2017 ◽  
Vol 126 (1C) ◽  
pp. 21
Author(s):  
Võ Thị Thanh Châu ◽  
Hoàng Văn Đức

<p>In the present paper, a synthesis of MIL-101 by hydrothermal process was demonstrated. The obtained samples were characterized by powder X-ray diffraction (PXRD), transmission electron microscope (TEM), nitrogen adsorption/desorption isotherms at 77K, X-ray photoelectron spectroscopy (XPS). The results showed that MIL-101 synthesized by optimal conditions exhibited high crystallinity and surface area. The obtained MIL-101 possesses high stability in water and several organic solvents.</p><p><strong>Keywords:</strong> MIL-101, hydrothermal synthesis, metal organic framework-101. </p>


2018 ◽  
Author(s):  
Shawn Burdette ◽  
Jingjing Yan ◽  
Ron Grimm ◽  
Peter Mueller ◽  
Alexander Carl ◽  
...  

A metal organic framework containing an azobenzene chromophore exhibits luminescence that is quenched by nitro-phenol derivatives. The model system was used to develop an new analytical approach to differentiating between encapsulated guest molecules and those adsorbed on the outside of the MOF


Author(s):  
Song Wang ◽  
Genwang Zhu ◽  
Zhongchen Yu ◽  
Chenxi Li ◽  
Dan Wang ◽  
...  

Abstract As porous crystal materials, metal-organic frameworks (MOFs) have attracted wide attention in the field of environmental remediation. In this study, a trivalent iron-tartaric acid metal-organic framework (T2-MOF) was successfully synthesized using the inexpensive raw materials ferric chloride (FeCl3.6H2O) and tartaric acid (C4H6O6). The physical and chemical properties of T2-MOF were studied by using X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy and Brunauer–Emmett–Teller. After that, T2-MOF was used as a catalyst for catalytic ozonation of succinonitrile. The results show that T2-MOF has obvious crystal characteristics and uniform structure. In addition, T2-MOF exhibits strong catalytic performance in ozonation of succinonitrile. The results indicate that the chemical oxygen demand (COD) removal rate is affected by various operating parameters including catalyst characteristics dosages and initial pH values. In the ozonation with 30 mg L−1 T2-MOF, the COD removal rate of 100 mg L−1 succinonitrile reached 73.1% (±4.6%) within 180 min, which was 67.3% (±4.4%) higher than that obtained in the process without catalyst. T2-MOF maintained strong catalytic performance with the pH range of 3.0–7.0. By monitoring the Fe2+ concentration at different reaction time, it was found that the homogeneous catalysis occurred simultaneously with the heterogeneous catalysis.


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.


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