scholarly journals Highly Active Transition Metal-Promoted CuCeMgAlO Mixed Oxide Catalysts Obtained from Multicationic LDH Precursors for the Total Oxidation of Methane

Catalysts ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 613
Author(s):  
Hussein Mahdi S. Al-Aani ◽  
Mihaela M. Trandafir ◽  
Ioana Fechete ◽  
Lucia N. Leonat ◽  
Mihaela Badea ◽  
...  

To improve the catalytic performance of an active layered double hydroxide (LDH)-derived CuCeMgAlO mixed oxide catalyst in the total oxidation of methane, it was promoted with different transition-metal cations. Thus, two series of multicationic mixed oxides were prepared by the thermal decomposition at 750 °C of their corresponding LDH precursors synthesized by coprecipitation at constant pH of 10 under ambient atmosphere. The first series of catalysts consisted of four M(3)CuCeMgAlO mixed oxides containing 3 at.% M (M = Mn, Fe, Co, Ni), 15 at.% Cu, 10 at.% Ce (at.% with respect to cations), and with Mg/Al atomic ratio fixed to 3. The second series consisted of four Co(x)CuCeMgAlO mixed oxides with x = 1, 3, 6, and 9 at.% Co, while keeping constant the Cu and Ce contents and the Mg/Al atomic ratio. All the mixed oxides were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) coupled with X-ray energy dispersion analysis (EDX), X-ray photoelectron spectroscopy (XPS), nitrogen adsorption-desorption at −196 °C, temperature-programmed reduction under hydrogen (H2-TPR), and diffuse reflectance UV-VIS spectroscopy (DR UV-VIS), while thermogravimetric and differential thermal analyses (TG-DTG-DTA) together with XRD were used for the LDH precursors. The catalysts were evaluated in the total oxidation of methane, a test reaction for volatile organic compounds (VOC) abatement. Their catalytic performance was explained in correlation with their physicochemical properties and was compared with that of a reference Pd/Al2O3 catalyst. Among the mixed oxides studied, Co(3)CuCeMgAlO was found to be the most active catalyst, with a temperature corresponding to 50% methane conversion (T50) of 438 °C, which was only 19 °C higher than that of a reference Pd/Al2O3 catalyst. On the other hand, this T50 value was ca. 25 °C lower than that observed for the unpromoted CuCeMgAlO system, accounting for the improved performance of the Co-promoted catalyst, which also showed a good stability on stream.

Catalysts ◽  
2018 ◽  
Vol 8 (11) ◽  
pp. 505 ◽  
Author(s):  
Xiaoli Wang ◽  
Gongde Wu ◽  
Tongfa Jin ◽  
Jie Xu ◽  
Shihao Song

A series of transition metal oxides or mixed oxides supported nano-Au catalysts were prepared for the selective oxidation of glycerol to glyceric acid using 3% H2O2. It was found that the composition and structure of supports significantly influenced the catalytic performance of catalysts. The mesoporous trimetal mixed oxide (CuNiAlO) supported nano-Au catalysts were more active in comparison with the others. In the present catalytic system, the highest glycerol conversion was 90.5%, while the selectivity of glyceric acid could reach 72%. Moreover, the catalytic performance remained after 11 times of reaction.


Catalysts ◽  
2020 ◽  
Vol 10 (8) ◽  
pp. 870
Author(s):  
Hadi Dib ◽  
Rebecca El Khawaja ◽  
Guillaume Rochard ◽  
Christophe Poupin ◽  
Stéphane Siffert ◽  
...  

CuAlCe oxides were obtained from hydrotalcite-type precursors by coprecipitation using a M2+/M3+ ratio of 3. The collapse of the layered double hydroxide structure following the thermal treatment leads to the formation of mixed oxides (CuO and CeO2). The catalytic performance of the copper-based catalysts was evaluated in the total oxidation of two Volatile Organic Compounds (VOCs): ethanol and toluene. XRD, SEM Energy-Dispersive X-ray Spectrometry (EDX), H2-temperature programmed reduction (TPR) and XPS were used to characterize the physicochemical properties of the catalysts. A beneficial effect of combining cerium with CuAl-O oxides in terms of redox properties and the abatement of the mentioned VOCs was demonstrated. The sample with the highest content of Ce showed the best catalytic properties, which were mainly related to the improvement of the reducibility of the copper species and their good dispersion on the surface. The presence of a synergetic effect between the copper and cerium elements was also highlighted.


Catalysts ◽  
2019 ◽  
Vol 9 (4) ◽  
pp. 371 ◽  
Author(s):  
Maria Lykaki ◽  
Sofia Stefa ◽  
Sόnia Carabineiro ◽  
Pavlos Pandis ◽  
Vassilis Stathopoulos ◽  
...  

Ceria has been widely studied either as catalyst itself or support of various active phases in many catalytic reactions, due to its unique redox and surface properties in conjunction to its lower cost, compared to noble metal-based catalytic systems. The rational design of catalytic materials, through appropriate tailoring of the particles’ shape and size, in order to acquire highly efficient nanocatalysts, is of major significance. Iron is considered to be one of the cheapest transition metals while its interaction with ceria support and their shape-dependent catalytic activity has not been fully investigated. In this work, we report on ceria nanostructures morphological effects (cubes, polyhedra, rods) on the textural, structural, surface, redox properties and, consequently, on the CO oxidation performance of the iron-ceria mixed oxides (Fe2O3/CeO2). A full characterization study involving N2 adsorption at –196 °C, X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS), temperature programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS) was performed. The results clearly revealed the key role of support morphology on the physicochemical properties and the catalytic behavior of the iron-ceria binary system, with the rod-shaped sample exhibiting the highest catalytic performance, both in terms of conversion and specific activity, due to its improved reducibility and oxygen mobility, along with its abundance in Fe2+ species.


Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 490
Author(s):  
Rudaviro Garidzirai ◽  
Phillimon Modisha ◽  
Innocent Shuro ◽  
Jacobus Visagie ◽  
Pieter van Helden ◽  
...  

The effects of Mg and Zn dopants on the catalytic performance of Pt/Al2O3 catalyst were investigated for dehydrogenation of perhydrodibenzyltoluene (H18-DBT) as a liquid organic hydrogen carrier. Al2O3 supports were modified with Mg and Zn to produce Mg-Al2O3 and Zn-Al2O3 with a target loading of 3.8 wt.% for dopants. The modified supports were impregnated with chloroplatinic acid solution to produce the catalysts Pt/Al2O3, Pt/Mg-Al2O3 and Pt/Zn-Al2O3 of 0.5 wt.% Pt loading. Thereafter, the catalysts were characterised using inductively coupled plasma- optical emission spectrometry, scanning electron microscopy-energy dispersive X-ray spectroscopy, hydrogen temperature-programmed reduction, carbon-monoxide pulse chemisorption, ammonia temperature-programmed desorption, X-ray diffraction and transmission electron microscopy. The dehydrogenation experiments were performed using a horizontal plug flow reactor system and the catalyst time-on-stream was 22 h. Pt/Mg-Al2O3 showed the highest average hydrogen flowrate of 29 nL/h, while an average of 27 nL/h was obtained for both Pt/Al2O3 and Pt/Zn-Al2O3. This has resulted in a hydrogen yield of 80% for Pt/Mg-Al2O3, 71% for Pt/Zn-Al2O3 and 73% for Pt/Al2O3. In addition, the conversion of H18-DBT ranges from 99% to 92%, Pt 97–90% and 96–90% for Pt/Mg-Al2O3, Pt/Zn-Al2O3 and Pt/Al2O3, respectively. Following the latter catalyst order, the selectivity to dibenzyltoluene (H0-DBT) ranges from 78% to 57%, 75–51% and 71–45%. Therefore, Pt/Mg-Al2O3 showed improved catalytic performance towards dehydrogenation of H18-DBT.


Polymers ◽  
2021 ◽  
Vol 13 (11) ◽  
pp. 1712
Author(s):  
Appusamy Muthukrishnaraj ◽  
Salma Ahmed Al-Zahrani ◽  
Ahmed Al Otaibi ◽  
Semmedu Selvaraj Kalaivani ◽  
Ayyar Manikandan ◽  
...  

Towards the utilization of Cu2O nanomaterial for the degradation of industrial dye pollutants such as methylene blue and methyl orange, the graphene-incorporated Cu2O nanocomposites (GCC) were developed via a precipitation method. Using Hummers method, the grapheme oxide (GO) was initially synthesized. The varying weight percentages (1–4 wt %) of GO was incorporated along with the precipitation of Cu2O catalyst. Various characterization techniques such as Fourier-transform infra-red (FT-IR), X-ray diffraction (XRD), UV–visible diffused reflectance (UV-DRS), Raman spectroscopy, thermo gravimetric analysis (TGA), energy-dispersive X-ray analysis (EDX), and electro chemical impedance (EIS) were followed for characterization. The cabbage-like morphology of the developed Cu2O and its composites were ascertained from field-emission scanning electron microscopy (FESEM) and high-resolution transmission electron microscopy (HR-TEM). In addition, the growth mechanism was also proposed. The results infer that 2 wt % GO-incorporated Cu2O composites shows the highest value of degradation efficiency (97.9% and 96.1%) for MB and MO at 160 and 220 min, respectively. Further, its catalytic performance over visible region (red shift) was also enhanced to an appreciable extent, when compared with that of other samples.


2020 ◽  
Vol 15 (2) ◽  
pp. 490-500
Author(s):  
Neha Neha ◽  
Ram Prasad ◽  
Satya Vir Singh

A series of nickel-cobalt bimetal oxides in varying molar ratios and its single metal oxides were synthesized by reactive calcination of coprecipitated basic-carbonates. Several characterization techniques, such as: Bruneuer Emmett Teller (BET), X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Fourier Transform Infra Red (FTIR), and Hydrogen Temperature Programmed Reduction (H2-TPR), were performed over the oxides. Activities of oxides were evaluated in methane total oxidation in the presence or the absence of CO. The best catalytic performance was observed over NiCo catalyst with a Ni/Co molar ratio of 1:1, and the complete conversion of CO-CH4 mixture was achieved at 390 °C. Moreover, the presence of carbon monoxide improves CH4 total oxidation over nickel-cobalt mixed oxides. Structural analysis reveals that the insertion of nickel into the spinel lattice of cobalt oxide causes the structural disorder, which probably caused the increase of the amount of octahedrally coordinated divalent nickel cations that are responsible for catalytic activity. Stability of the best-performed catalyst has been tested in the two conditions, showing remarkable long-term stability and thermal stability, however, showed deactivation after thermally ageing at 700 °C. Copyright © 2020 BCREC Group. All rights reserved 


2009 ◽  
Vol 12 (1) ◽  
pp. 9 ◽  
Author(s):  
Z.R. Ismagilov ◽  
E.V. Matus ◽  
I.Z. Ismagilov ◽  
M.A. Kerzhentsev ◽  
V.I. Zailovskii ◽  
...  

<p>The structure changes of Mo/ZSM-5 catalysts with different Mo content (2 and 10 wt. % Mo) and Si/Al atomic ratio (17, 30 and 45) during the methane dehydroaromatization have been investigated by X-ray powder diffractometry, N<sub>2</sub> adsorption and transmission electron microscopy. The treatment of Mo/ZSM-5 catalysts in reducing atmosphere (CH<sub>4</sub> or H<sub>2</sub>) at about 700 °C promotes development of mesoporous system. The pores are open to the exterior of the zeolite grain and have an entrance diameter of ~ 4-10 nm. It is proposed that mesopore formation in Mo/ZSM-5 catalyst is connected with the dealumination of zeolite. The mesopore formation in the parent H-ZSM-5 zeolite by NaOH treatment does not improve the activity of /ZSM-5 catalyst.</p>


2020 ◽  
Vol 10 (6) ◽  
pp. 625
Author(s):  
Said Arhzaf ◽  
Mohammed Naciri Bennani ◽  
Sadik Abouarnadasse ◽  
Hamid Ziyat ◽  
Omar Qabaqous

<p>The fundamental character of the Mg-Al mixed oxide (Mg<sub>n</sub>(Al)O), derived from the Mg-Al hydrotalcite (Mg<sub>n</sub>Al-CO<sub>3</sub>-HT), where n corresponds to the Mg/Al molar ratio (n: 2, 2.5, 3, 3.5 and 4), was studied by using the adsorption of phenol as a probe acid molecule. The hydrotalcite precursors were prepared by the coprecipitation method. Their derived mixed oxides were obtained by thermal treatment at 450°C in a flow of air. The resulting solids were characterized by X-ray fluorescence spectroscopy (XRF), X-ray diffraction (XRD), infrared spectroscopy (FTIR), thermogravimetric and differential thermal analysis             (TG-DTA), nitrogen physisorption (BET) and phenol chemisorption. The phenol adsorption followed by UV-Visible spectrophotometry shows that the basicity increases with the Mg/Al molar ratio, such that maximum quantity of phenol adsorbed (Q<sub>ads</sub> = 0.54 mmol/g <sub>cat</sub>) was obtained with the mixed oxide derived from the Mg-Al hydrotalcite of Mg/Al molar ratio equal to 3.5.</p>


Catalysts ◽  
2019 ◽  
Vol 9 (7) ◽  
pp. 589 ◽  
Author(s):  
Mingliang Ma ◽  
Yuying Yang ◽  
Yan Chen ◽  
Fei Wu ◽  
Wenting Li ◽  
...  

In this manuscript, hollow flower-like ferric oxide/manganese dioxide/trimanganese tetraoxide (Fe3O4/MnO2/Mn3O4) magnetically separable microspheres were prepared by combining a simple hydrothermal method and reduction method. As the MnO2 nanoflower working as precursor was partially reduced, Mn3O4 nanoparticles were in situ grown from the MnO2 nanosheet. The composite microspheres were characterized in detail by employing scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), vibration sample magnetometer (VSM) and UV–visible spectrophotometer (UV–vis). Under visible light conditions, the test for degrading rhodamine B (RhB) was used to verify the photocatalytic activity of the photocatalyst. The results showed that the efficiency of the Fe3O4/MnO2/Mn3O4 photocatalyst in visible light for 130 min is 94.5%. The catalytic activity of photocatalyst far exceeded that of the Fe3O4/MnO2 component, and after four cycles, the catalytic performance of the catalyst remained at 78.4%. The superior properties of the photocatalyst came from improved surface area, enhanced light absorption, and efficient charge separation of the MnO2/Mn3O4 heterostructure. This study constructed a green and efficient valence heterostructure composite that created a promising photocatalyst for degrading organic contaminants in aqueous environments.


2019 ◽  
Vol 6 (9) ◽  
pp. 191019 ◽  
Author(s):  
Shang Wang ◽  
Zhaolian Han ◽  
Tingting Di ◽  
Rui Li ◽  
Siyuan Liu ◽  
...  

The pod-shaped TiO 2 nano burst tubes (TiO 2 NBTs) were prepared by the combination of electrospinning and impregnation calcination with oxalic acid (H 2 C 2 O 4 ), polystyrene (PS) and tetrabutyl titanate. The silver nanoparticles (AgNPs) were loaded onto the surface of TiO 2 NBTs by ultraviolet light reduction method to prepare pod-shaped Ag@TiO 2 NBTs. In this work, we analysed the effect of the amount of oxalic acid on the cracking degree of TiO 2 NBTs; the effect of the concentration of AgNO 3 solution on the particle size and loading of AgNPs on the surface of TiO 2 NBTs. Scanning electron microscopy and transmission electron microscopy investigated the surface morphology of samples. X-ray diffraction and X-ray photoelectron spectroscopy characterized the structure and composition of samples. Rhodamine B (RhB) solution was used to evaluate the photocatalytic activity of pod-shaped TiO 2 NBTs and Ag@TiO 2 NBTs. The results showed that TiO 2 NBTs degraded 91.0% of RhB under ultraviolet light, Ag@TiO 2 NBTs degraded 95.5% under visible light for 75 and 60 min, respectively. The degradation process of both samples was consistent with the Langmuir–Hinshelwood first-order kinetic equation. Therefore, the catalytic performance of the sample is: Ag@TiO 2 NBTs > TiO 2 NBTs > TiO 2 nanotubes.


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