scholarly journals Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio

Nanomaterials ◽  
2018 ◽  
Vol 8 (9) ◽  
pp. 669 ◽  
Author(s):  
Carol Olmos ◽  
Lidia Chinchilla ◽  
Andrea Cappella ◽  
Alberto Villa ◽  
Juan Delgado ◽  
...  
Keyword(s):  
Selective Oxidation ◽  
Photoelectron Spectroscopy ◽  
Inductively Coupled Plasma ◽  
Palladium Catalysts ◽  
Veratryl Alcohol ◽  
Dark Field ◽  
Molar Ratio ◽  
Pd Catalysts ◽  
X Ray ◽  
Wide Range

The selective oxidation of veratryl alcohol (VA), a model compound of lignin, with oxygen molecules to produce veratraldehyde (VAld) was studied over monometallic Au, Pd, and bimetallic Au:Pd nanoparticles supported on a Ce0.62Zr0.38O2 mixed oxide for the first time. These bimetallic Au-Pd catalysts with Au:Pd molar ratios from 0.4 to 4.3 were synthesized by the sol-immobilization method. Furthermore, all the catalysts were characterized by inductively coupled plasma-atomic emission spectroscopy (ICP-AES), N2 physisorption, X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy-high angle annular dark field (STEM-HAADF) imaging, energy dispersive X-ray spectroscopy (EDXS), and temperature programmed reduction (TPR) techniques. A synergistic effect between gold and palladium was observed over all the bimetallic catalysts in a wide range of studied Au:Pd ratios. Remarkably, the optimum Au:Pd ratio for this reaction was 1.4 with a turnover frequency of almost six times larger than for the monometallic gold and palladium catalysts. Selectivity to veratraldehyde was higher than 99% for the monometallic Au, Pd, and all the bimetallic Au-Pd catalysts, and stayed constant during the reaction time.

Effect of Aging Methods on CuZnAl Catalysts for Methyl Acetate Hydrogenation

2019 ◽  
Vol 72 (6) ◽  
pp. 417
Author(s):  
Changna Gan ◽  
Yunhao Wang ◽  
Chenliang Ye ◽  
Cuili Guo
Keyword(s):  
Photoelectron Spectroscopy ◽  
Inductively Coupled Plasma ◽  
Methyl Acetate ◽  
Copper Particle ◽  
Atomic Emission ◽  
Catalytic Performance ◽  
Precipitation Method ◽  
Molar Ratio ◽  
X Ray ◽  
Temperature Programmed

A series of CuZnAl catalysts derived from layered double hydroxide precursors with different Cu/Zn molar ratios were synthesised by a co-precipitation method for methyl acetate hydrogenation. The best catalytic performance was obtained when the Cu/Zn molar ratio reached 0.25:1. After fixing the Cu/Zn molar ratio at 0.25:1, the effect of aging methods, including ultrasound, high shear mixer stirring, and magnetic stirring, were investigated, which showed that 0.25CuZnAl-u and 0.25CuZnAl-h exhibited a higher conversion and selectivity than that of 0.25CuZnAl-m, especially under low reaction temperatures. The physicochemical properties of the CuZnAl catalysts were characterised by X-ray diffraction, inductively coupled plasma–atomic emission spectroscopy, N2 physisorption, N2O chemisorption, transmission electron microscopy, H2-temperature-programmed reduction, X-ray photoelectron spectroscopy, and H2-temperature-programmed desorption. It was found that compared with 0.25CuZnAl-m, 0.25CuZnAl-u and 0.25CuZnAl-h possessed a stronger interaction between Cu and the support, smaller copper particle size, and higher copper dispersion, which improved the catalytic performance.

scholarly journals Mechanochemical synthesis of CaO•ZnO.K2CO3 catalyst: Characterization and activity for methanolysis of sunflower oil

2015 ◽  
Vol 21 (1-1) ◽  
pp. 1-12 ◽  
Author(s):  
Zeljka Kesic ◽  
Ivana Lukic ◽  
Miodrag Zdujic ◽  
Cedomir Jovalekic ◽  
Hui Liu ◽  
...  
Keyword(s):  
Sunflower Oil ◽  
Photoelectron Spectroscopy ◽  
Inductively Coupled Plasma ◽  
Molar Ratio ◽  
Catalyst Characterization ◽  
Composite Powders ◽  
Indicator Method ◽  
X Ray ◽  
Air Atmosphere ◽  
Biodiesel Synthesis

The goal of this study was to prepare CaO.ZnO catalyst which contain small amount of K2CO3 and analyze its activity for biodiesel synthesis. Catalyst was prepared using the following procedure: CaO and ZnO (molar ratio of 1:2), water and K2CO3 (in various amounts) were mechanochemically treated and after milling heated at 700 oC in air atmosphere for obtaining mixed CaO?ZnO/xK2CO3 oxides (x = 0, 1, 2 and 4; mole of K2CO3 per 10 mole of CaO). All the samples were characterized by X-ray diffraction (XRD), inductively coupled plasma (ICP), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), infrared spectroscopy (FTIR), scanning electron microscopy/energy-dispersive spectroscopy (SEM/EDS), particle size laser diffraction (PSLD) distribution, solubility measurement of Ca, Zn and K ions in methanol as well as by determination of their alkalinity (Hammett indicator method). Prepared CaO?ZnO/xK2CO3 composite powders were tested as catalysts for methanolysis of sunflower oil at 70?C using molar ratio of sunflower oil to methanol of 1:10 and with 2 mas% of catalyst based on oil weight. The presence of K2CO3 in prepared samples was found to increase the activity of catalyst, and that such effect is caused by homogeneous-heterogeneous catalysis of biodiesel synthesis.

scholarly journals Selective Oxidation of Hydrogen Sulfide to Sulfur Using Vanadium Oxide Supported on Porous Clay Heterostructures (PCHs) Formed by Pillars Silica, Silica-Zirconia or Silica-Titania

Materials ◽  
2018 ◽  
Vol 11 (9) ◽  
pp. 1562 ◽  
Author(s):  
Juan Cecilia ◽  
M. Soriano ◽  
Alejandro Natoli ◽  
Enrique Rodríguez-Castellón ◽  
José López Nieto
Keyword(s):  
Vanadium Oxide ◽  
Selective Oxidation ◽  
Photoelectron Spectroscopy ◽  
Elemental Sulfur ◽  
Vanadium Content ◽  
Molar Ratio ◽  
X Ray ◽  
Porous Clay Heterostructures ◽  
Oxidation Of Hydrogen ◽  
Catalytic Stability

Vanadium oxide (V2O5) species has been supported on different porous clay heterostructures (with silica pillars, silica-zirconia with a molar ratio Si/Zr = 5 and silica-titania with a molar ratio Si/Ti = 5) by wetness incipient method. All catalysts were characterized by X-ray diffraction (XRD), N2 adsorption-desorption at −196 °C, NH3 thermoprogrammed desorption (NH3-TPD), Raman spectroscopy, diffuse reflectance UV-Vis and X-ray photoelectron spectroscopy (XPS). After that, the catalytic activity of the vanadium-based catalysts was evaluated in the selective oxidation of H2S to elemental sulfur. The catalytic data show that both the activity and the catalytic stability increase with the vanadium content, obtaining the highest conversion values and sulfur yield for the catalysts with vanadium content of 16 wt.%. The comparison among all supports reveals that the incorporation of TiO2 species in the pillars of the PCH improves the resistance to the deactivation, attaining as best results a H2S conversion of 89% for SiTi-PCH-16V catalyst and elemental sulfur is the only compound detected by gas chromatography.

scholarly journals Cu@Pd/C with Controllable Pd Dispersion as a Highly Efficient Catalyst for Hydrogen Evolution from Ammonia Borane

Nanomaterials ◽  
2020 ◽  
Vol 10 (9) ◽  
pp. 1850
Author(s):  
Yanliang Yang ◽  
Ying Duan ◽  
Dongsheng Deng ◽  
Dongmi Li ◽  
Dong Sui ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Photoelectron Spectroscopy ◽  
Inductively Coupled Plasma ◽  
Reduction Process ◽  
Ammonia Borane ◽  
Dark Field ◽  
Impregnation Method ◽  
Efficient Catalyst ◽  
X Ray ◽  
Transmission Electron

A series of Cu@Pd/C with different Pd contents was prepared using the galvanic reduction method to disperse Pd on the surface of Cu nanoparticles on Cu/C. The dispersion of Pd was regulated by the Cu(I) on the surface, which was introduced by pulse oxidation. The Cu2O did not react during the galvanic reduction process and restricted the Pd atoms to a specific area. The pulse oxidation method was demonstrated to be an effective process to control the oxidization degree of Cu on Cu/C and then to govern the dispersion of Pd. The catalysts were characterized by transmission electron microscopy (TEM), high-resolution transmission electron microscope (HRTEM), high angular annular dark field scanning TEM (HAADF-STEM), energy-dispersive spectroscopy (EDS) mapping, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), auger electron spectroscopy (AES), and inductively coupled plasma optical emission spectrometer (ICP-OES), which were used to catalyze the hydrogen evolution from ammonia borane. The Cu@Pd/C had much higher activity than the PdCu/C, which was prepared by the impregnation method. The TOF increased as the Cu2O in Cu/C used for the preparation of Cu@Pd/C increased, and the maximum TOF was 465 molH2 min−1 molPd−1 at 298 K on [email protected]/C-640 (0.5 wt % of Pd, 640 mL of air was pulsed during the preparation of Cu/C-640). The activity could be maintained in five continuous processes, showing the strong stability of the catalysts.

scholarly journals Photocatalytic Reduction of CO2 to Methanol Using a Copper-Zirconia Imidazolate Framework

Catalysts ◽  
2021 ◽  
Vol 11 (3) ◽  
pp. 346
Author(s):  
Sonam Goyal ◽  
Maizatul Shima Shaharun ◽  
Ganaga Suriya Jayabal ◽  
Chong Fai Kait ◽  
Bawadi Abdullah ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Catalyst Support ◽  
Oxidation Potential ◽  
Molar Ratio ◽  
X Ray Diffraction ◽  
X Ray ◽  
Molar Ratios ◽  
Optimum Parameters ◽  
Reduction Of Co2 ◽  
Enhanced Yield

A set of novel photocatalysts, i.e., copper-zirconia imidazolate (CuZrIm) frameworks, were synthesized using different zirconia molar ratios (i.e., 0.5, 1, and 1.5 mmol). The photoreduction process of CO2 to methanol in a continuous-flow stirred photoreactor at pressure and temperature of 1 atm and 25 °C, respectively, was studied. The physicochemical properties of the synthesized catalysts were studied using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and photoluminescence (PL) spectroscopy. The highest methanol activity of 818.59 µmol/L.g was recorded when the CuZrIm1 catalyst with Cu/Zr/Im/NH4OH molar ratio of 2:1:4:2 (mmol/mmol/mmol/M) was employed. The enhanced yield is attributed to the presence of Cu2+ oxidation state and the uniformly dispersed active metals. The response surface methodology (RSM) was used to optimize the reaction parameters. The predicted results agreed well with the experimental ones with the correlation coefficient (R2) of 0.99. The optimization results showed that the highest methanol activity of 1054 µmol/L.g was recorded when the optimum parameters were employed, i.e., stirring rate (540 rpm), intensity of light (275 W/m2) and photocatalyst loading (1.3 g/L). The redox potential value for the CuZrIm1 shows that the reduction potential is −1.70 V and the oxidation potential is +1.28 V for the photoreduction of CO2 to methanol. The current work has established the potential utilization of the imidazolate framework as catalyst support for the photoreduction of CO2 to methanol.

scholarly journals A Highly Sensitive Room Temperature CO2 Gas Sensor Based on SnO2-rGO Hybrid Composite

Materials ◽  
2021 ◽  
Vol 14 (3) ◽  
pp. 522
Author(s):  
Zhi Yan Lee ◽  
Huzein Fahmi bin Hawari ◽  
Gunawan Witjaksono bin Djaswadi ◽  
Kamarulzaman Kamarudin
Keyword(s):  
Electron Microscopy ◽  
Carbon Dioxide ◽  
Gas Sensor ◽  
Photoelectron Spectroscopy ◽  
Hybrid Composite ◽  
Room Temperature ◽  
Co2 Gas ◽  
X Ray ◽  
Wide Range ◽  
Co2 Gas Sensor

A tin oxide (SnO2) and reduced graphene oxide (rGO) hybrid composite gas sensor for high-performance carbon dioxide (CO2) gas detection at room temperature was studied. Since it can be used independently from a heater, it emerges as a promising candidate for reducing the complexity of device circuitry, packaging size, and fabrication cost; furthermore, it favors integration into portable devices with a low energy density battery. In this study, SnO2-rGO was prepared via an in-situ chemical reduction route. Dedicated material characterization techniques including field emission scanning electron microscopy (FESEM), high-resolution transmission electron microscopy (HRTEM), energy dispersive X-ray (EDX) spectroscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS) were conducted. The gas sensor based on the synthesized hybrid composite was successfully tested over a wide range of carbon dioxide concentrations where it exhibited excellent response magnitudes, good linearity, and low detection limit. The synergistic effect can explain the obtained hybrid gas sensor’s prominent sensing properties between SnO2 and rGO that provide excellent charge transport capability and an abundance of sensing sites.

Low-temperature route to nanoscale P3N5 hollow spheres

2003 ◽  
Vol 18 (10) ◽  
pp. 2359-2363 ◽  
Author(s):  
Hongzhou Gu ◽  
Yunle Gu ◽  
Zhefeng Li ◽  
Yongcheng Ying ◽  
Yitai Qian
Keyword(s):  
Photoelectron Spectroscopy ◽  
Hollow Spheres ◽  
Molar Ratio ◽  
Visible Absorption ◽  
X Ray ◽  
Transmission Electron ◽  
Influence Of Temperature On ◽  
Wide Gap ◽  
20 Nm ◽  
High Degree

Nanoscale hollow spheres of amorphous phosphorus nitride (P3N5) were synthesized by reacting PCl3 with NaN3 at 150–250 °C. Transmission electron microscope images show that the hollow spheres have a diameter of 150–350 nm, and the thickness of the shell is 20 nm. A very small amount of curly films were also found in the sample prepared at 150 °C. The infrared spectrum indicates a high degree of purity. X-ray photoelectron spectroscopy indicates the presence of P and N, with a molar ratio of 1:1.62 for P:N. Ultraviolet-visible absorption spectroscopy shows an absorption band at 265–315 nm. Under photoluminescent excitation at 230 nm, the P3N5 emits ultraviolet light at 305 nm. With a band gap of 4.28 eV, the products may be a wide gap semiconductor. A possible mechanism and the influence of temperature on the formation of the hollow spheres are also discussed.

scholarly journals The effect of cobalt on morphology, structure, and ORR activity of electrospun carbon fibre mats in aqueous alkaline environments

2021 ◽  
Vol 12 ◽  
pp. 1173-1186
Author(s):  
Markus Gehring ◽  
Tobias Kutsch ◽  
Osmane Camara ◽  
Alexandre Merlen ◽  
Hermann Tempel ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Inductively Coupled Plasma ◽  
Elevated Temperatures ◽  
Current Collector ◽  
Alkaline Media ◽  
Emission Spectrometry ◽  
Free Standing ◽  
X Ray ◽  
Turbostratic Carbon ◽  
Current Densities

An innovative approach for the design of air electrodes for metal–air batteries are free-standing scaffolds made of electrospun polyacrylonitrile fibres. In this study, cobalt-decorated fibres are prepared, and the influence of carbonisation temperature on the resulting particle decoration, as well as on fibre structure and morphology is discussed. Scanning electron microscopy, Raman spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, elemental analysis, and inductively coupled plasma optical emission spectrometry are used for characterisation. The modified fibre system is compared to a benchmark system without cobalt additives. Cobalt is known to catalyse the formation of graphite in carbonaceous materials at elevated temperatures. As a result of cobalt migration in the material the resulting overall morphology is that of turbostratic carbon. Nitrogen removal and nitrogen-type distribution are enhanced by the cobalt additives. At lower carbonisation temperatures cobalt is distributed over the surface of the fibres, whereas at high carbonisation temperatures it forms particles with diameters up to 300 nm. Free-standing, current-collector-free electrodes assembled from carbonised cobalt-decorated fibre mats display promising performance for the oxygen reduction reaction in aqueous alkaline media. High current densities at an overpotential of 100 mV and low overpotentials at current densities of 333 μA·cm−2 were found for all electrodes made from cobalt-decorated fibre mats carbonised at temperatures between 800 and 1000 °C.

scholarly journals Towards chemically neutral carbon cleaning processes: plasma cleaning of Ni, Rh and Al reflective optical coatings and thin Al filters for free-electron lasers and synchrotron beamline applications

2018 ◽  
Vol 25 (6) ◽  
pp. 1642-1649 ◽  
Author(s):  
Harol Moreno Fernández ◽  
Marco Zangrando ◽  
Guillaume Sauthier ◽  
Alejandro R. Goñi ◽  
Vincent Carlino ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Free Electron ◽  
Inductively Coupled Plasma ◽  
High Performance ◽  
Extreme Ultraviolet ◽  
Filter Material ◽  
Gas Mixture ◽  
Carbon Contamination ◽  
X Ray ◽  
Chemical Surface

The choice of a reflective optical coating or filter material has to be adapted to the intended field of application. This is mainly determined by the required photon energy range or by the required reflection angle. Among various materials, nickel and rhodium are common materials used as reflective coatings for (soft) X-ray mirrors. Similarly, aluminium is one of the most commonly used materials for extreme ultraviolet and soft X-ray transmission filters. However, both of these types of optics are subject to carbon contamination, which can be increasingly problematic for the operation of the high-performance free-electron laser and synchrotron beamlines. As an attempt to remove this type of contamination, an inductively coupled plasma source has been used in conjunction with N2/O2/H2 and N2/H2 feedstock gas plasmas. Results from the chemical surface analysis of the above materials before and after plasma treatment using X-ray photoelectron spectroscopy are reported. It is concluded that a favorable combination of an N2/H2 plasma feedstock gas mixture leads to the best chemical surface preservation of Ni, Rh and Al while removing the carbon contamination. However, this feedstock gas mixture does not remove C contamination as rapidly as, for example, an N2/O2/H2 plasma which induces the surface formation of NiO and NiOOH in Ni and RhOOH in Rh foils. As an applied case, the successful carbon removal from ultrathin Al filters previously used at the FERMI FEL1 using an N2/H2 plasma is demonstrated.

scholarly journals Graphitic Nitrogen in Carbon Catalysts Important for the Reduction of Nitrite Revealed by 15N NMR Spectroscopy at Natural Abundance

2020 ◽  
Author(s):  
Zheng Chen ◽  
Aleksander Jaworski ◽  
Jianhong Chen ◽  
Tetyana Budnyak ◽  
Ireneusz Szewczyk ◽  
...  
Keyword(s):  
Electron Microscopy ◽  
Photoelectron Spectroscopy ◽  
Reduction Reaction ◽  
Nitrite Reduction ◽  
15N Nmr ◽  
Carbon Catalyst ◽  
X Ray ◽  
Wide Range ◽  
Alkaline Conditions

Metal-free nitrogen-doped carbon is considered as a green functional material, but the structural determination of the atomic positions of nitrogen remains challenging. We recently demonstrated that directly-excited solid state <sup>15</sup>N NMR (ssNMR) spectroscopy is a powerful tool for the determination of such positions in an N-doped carbon at natural <sup>15</sup>N isotope abundance. Here we present a green chemistry approach to the synthesis of N-doped carbon using cellulose as precursor, and a study of the catalytic properties and atomic structures of the related catalyst. The N-doped carbon (NH<sub>3</sub>) was obtained by oxidation of cellulose with HNO<sub>3</sub> followed by ammonolysis at 800°C. It had a N content of 6.5 wt.% and a surface area of 557 m<sup>2 </sup>g<sup>–1</sup>, and <sup>15</sup>N ssNMR spectroscopy provided evidence for graphitic nitrogen besides of regular pyrrolic and pyridinic nitrogen. This structure determination enabled probing the role of graphitic nitrogen for electrocatalytic reactions, such as the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and nitrite reduction reaction. The N-doped carbon catalyst (NH<sub>3</sub>) had higher electrocatalytic activities in OER and HER under alkaline conditions and a higher activity for nitrite reduction, as compared with a catalyst prepared by carbonization of the HNO<sub>3</sub>-treated cellulose in N<sub>2</sub>. The electrocatalytic selectivity for nitrite reduction of the N-doped carbon catalyst (NH<sub>3</sub>) was directly related to the graphitic nitrogen functions. Complementary structural analysis by means of <sup>13</sup>C and <sup>1</sup>H ssNMR, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and low-temperature N<sub>2 </sub>adsorption were preformed and provided support to the findings. The results show that directly-excited <sup>15</sup>N ssNMR at natural <sup>15</sup>N abundance is generally capable to provide information on N-doped carbon materials, and it is expected that the approach can be applied to a wide range of solids with an intermediate amount of N atoms.

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