scholarly journals Effect of Gold Electronic State on the Catalytic Performance of Nano Gold Catalysts in n-Octanol Oxidation

Nanomaterials ◽  
2020 ◽  
Vol 10 (5) ◽  
pp. 880 ◽  
Author(s):  
Ekaterina Pakrieva ◽  
Ekaterina Kolobova ◽  
Yulia Kotolevich ◽  
Laura Pascual ◽  
Sónia A. C. Carabineiro ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Density Functional ◽  
Co Adsorption ◽  
Nitrogen Adsorption ◽  
Dark Field ◽  
Gold Content ◽  
Drift Spectroscopy ◽  
X Ray ◽  
Nano Gold ◽  
Pretreatment Conditions

This study aims to identify the role of the various electronic states of gold in the catalytic behavior of Au/MxOy/TiO2 (where MxOy are Fe2O3 or MgO) for the liquid phase oxidation of n-octanol, under mild conditions. For this purpose, Au/MxOy/TiO2 catalysts were prepared by deposition-precipitation with urea, varying the gold content (0.5 or 4 wt.%) and pretreatment conditions (H2 or O2), and characterized by low temperature nitrogen adsorption-desorption, X-ray powder diffraction (XRD), energy dispersive spectroscopy (EDX), scanning transmission electron microscopy-high angle annular dark field (STEM HAADF), diffuse reflectance Fourier transform infrared (DRIFT) spectroscopy of CO adsorption, temperature-programmable desorption (TPD) of ammonia and carbon dioxide, and X-ray photoelectron spectroscopy (XPS). Three states of gold were identified on the surface of the catalysts, Au0, Au1+ and Au3+, and their ratio determined the catalysts performance. Based on a comparison of catalytic and spectroscopic results, it may be concluded that Au+ was the active site state, while Au0 had negative effect, due to a partial blocking of Au0 by solvent. Au3+ also inhibited the oxidation process, due to the strong adsorption of the solvent and/or water formed during the reaction. Density functional theory (DFT) simulations confirmed these suggestions. The dependence of selectivity on the ratio of Brønsted acid centers to Brønsted basic centers was revealed.

scholarly journals Effect of the Metal Deposition Order on Structural, Electronic and Catalytic Properties of TiO2-Supported Bimetallic Au-Ag Catalysts in 1-Octanol Selective Oxidation

Catalysts ◽  
2021 ◽  
Vol 11 (7) ◽  
pp. 799
Author(s):  
Yulia Kotolevich ◽  
Ekaterina Pakrieva ◽  
Ekaterina Kolobova ◽  
Mario H. Farías ◽  
Nina Bogdanchikova ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Density Functional ◽  
Catalytic Properties ◽  
Diffuse Reflectance Spectroscopy ◽  
Density Functional Theory Method ◽  
Nitrogen Adsorption ◽  
X Ray ◽  
A Charge ◽  
Adsorption Desorption ◽  
Ag Catalysts

Au and Ag were deposited on TiO2 modified with Ce, La, Fe or Mg in order to obtain bimetallic catalysts to be used for liquid-phase oxidation of 1-octanol. The effects of the deposition order of gold and silver, and the nature of the support modifying additives and redox pretreatments on the catalytic properties of the bimetallic Au-Ag catalysts were studied. Catalysts were characterized by low-temperature nitrogen adsorption–desorption, energy dispersive spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy and ultraviolet-visible diffuse reflectance spectroscopy. It was found that pretreatments with hydrogen and oxygen at 300 °C significantly decreased the activity of AuAg catalysts (silver was deposited first) and had little effect on the catalytic properties of AgAu samples (gold was deposited first). The density functional theory method demonstrated that the adsorption energy of 1-octanol increased for all positively charged AuxAgyq (x + y = 10, with a charge of q = 0 or +1) clusters compared with the neutral counterparts. Lanthanum oxide was a very effective promoter for both monometallic and bimetallic gold and silver catalysts in the studied process.

scholarly journals Pore Modification and Phosphorus Doping Effect on Phosphoric Acid-Activated Fe-N-C for Alkaline Oxygen Reduction Reaction

Nanomaterials ◽  
2021 ◽  
Vol 11 (6) ◽  
pp. 1519
Author(s):  
Jong Gyeong Kim ◽  
Sunghoon Han ◽  
Chanho Pak
Keyword(s):  
Phosphoric Acid ◽  
Photoelectron Spectroscopy ◽  
Structural Changes ◽  
Electronic States ◽  
Nitrogen Adsorption ◽  
Reduction Reaction ◽  
Phosphorus Doping ◽  
X Ray ◽  
Precious Metal Catalysts ◽  
Adsorption Desorption

The price and scarcity of platinum has driven up the demand for non-precious metal catalysts such as Fe-N-C. In this study, the effects of phosphoric acid (PA) activation and phosphorus doping were investigated using Fe-N-C catalysts prepared using SBA-15 as a sacrificial template. The physical and structural changes caused by the addition of PA were analyzed by nitrogen adsorption/desorption and X-ray diffraction. Analysis of the electronic states of Fe, N, and P were conducted by X-ray photoelectron spectroscopy. The amount and size of micropores varied depending on the PA content, with changes in pore structure observed using 0.066 g of PA. The electronic states of Fe and N did not change significantly after treatment with PA, and P was mainly found in states bonded to oxygen or carbon. When 0.135 g of PA was introduced per 1 g of silica, a catalytic activity which was increased slightly by 10 mV at −3 mA/cm2 was observed. A change in Fe-N-C stability was also observed through the introduction of PA.

scholarly journals Study of the Effect of TiO2 Layer on the Adsorption and Photocatalytic Activity of TiO2-MoS2 Heterostructures under Visible-Infrared Light

2020 ◽  
Vol 2020 ◽  
pp. 1-9 ◽  
Author(s):  
N. Cruz-González ◽  
O. Calzadilla ◽  
J. Roque ◽  
F. Chalé-Lara ◽  
J. K. Olarte ◽  
...  
Keyword(s):  
Electron Microscopy ◽  
Photocatalytic Activity ◽  
Photoelectron Spectroscopy ◽  
Diffuse Reflectance Spectroscopy ◽  
Nitrogen Adsorption ◽  
High Photocatalytic Activity ◽  
Infrared Light ◽  
Polluted Water ◽  
Light Spectrum ◽  
X Ray

In the last decade, the urgent need to environmental protection has promoted the development of new materials with potential applications to remediate air and polluted water. In this work, the effect of the TiO2 thin layer over MoS2 material in photocatalytic activity is reported. We prepared different heterostructures, using a combination of electrospinning, solvothermal, and spin-coating techniques. The properties of the samples were analyzed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), atomic force microscopy (AFM), X-ray diffraction (XRD), nitrogen adsorption-desorption isotherms, UV-Vis diffuse reflectance spectroscopy (UV-Vis-DRS), and X-ray photoelectron spectroscopy (XPS). The adsorption and photocatalytic activity were evaluated by discoloration of rhodamine B solution. The TiO2-MoS2/TiO2 heterostructure presented three optical absorption edges at 1.3 eV, 2.28 eV, and 3.23 eV. The high adsorption capacity of MoS2 was eliminated with the addition of TiO2 thin film. The samples show high photocatalytic activity in the visible-IR light spectrum.

Extraordinary Stability of Structural and Electronic Properties of Tin Oxide Nanoparticles Formed by Soft Chemistry

2010 ◽  
Vol 75 ◽  
pp. 36-42 ◽  
Author(s):  
Marina Rumyantseva ◽  
Irina Zhurbina ◽  
Elena Varechkina ◽  
Siranuysh Badalyan ◽  
Alexander Gaskov ◽  
...  
Keyword(s):  
Optical Properties ◽  
Photoelectron Spectroscopy ◽  
Tin Dioxide ◽  
Hydrogen Reduction ◽  
Nitrogen Adsorption ◽  
Ammonia Solution ◽  
Adsorption Method ◽  
X Ray ◽  
Wet Chemical Synthesis ◽  
Tin Chloride

Powders of tin dioxide (SnO2) have been prepared by two different modifications of wet chemical synthesis, i.e. (i) by conventional hydrolysis of tin chloride dissolved in aqueous ammonia solution and (ii) by precipitation from tin chloride dissolved in aqueous hydrazine monohydrate (N2H4*H2O) solution. The prepared gels were dried and then annealed at different temperatures varied from 300 to 700 oC in order to form nanocrystals. Structure and optical properties of the samples were investigated by using X-ray diffraction, transmission electron microscopy, thermoprogrammable hydrogen reduction, low temperature nitrogen adsorption method, photoluminescence, infra-red absorption, Raman spectroscopy, and X-ray photoelectron spectroscopy. The samples prepared by hydrazine-based method are characterized by surface area about 127-188 m2/g with high sintering resistance. The optical spectroscopy data revealed pure crystallinity and high defect concentration for the samples prepared by hydrazine-based method. The experimental results are discussed in view of different states of chemisorbed oxygen on SnO2 nanocrystal surfaces, which determine electronic and optical properties of the prepared samples.

scholarly journals Metal-Organic Framework MIL-101: Synthesis and Photocatalytic Degradation of Remazol Black B Dye

2019 ◽  
Vol 2019 ◽  
pp. 1-15 ◽  
Author(s):  
Pham Dinh Du ◽  
Huynh Thi Minh Thanh ◽  
Thuy Chau To ◽  
Ho Sy Thang ◽  
Mai Xuan Tinh ◽  
...  
Keyword(s):  
Photocatalytic Degradation ◽  
Photoelectron Spectroscopy ◽  
Metal Organic Framework ◽  
Nitrogen Adsorption ◽  
X Ray ◽  
Remazol Black B ◽  
Metal Organic ◽  
Degradation Reaction ◽  
Remazol Black ◽  
Organic Framework

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.

scholarly journals Bulk Versus Surface Modification of Alumina with Mn and Ce Based Oxides for CH4 Catalytic Combustion

Materials ◽  
2019 ◽  
Vol 12 (11) ◽  
pp. 1771 ◽  
Author(s):  
Stefan Neatu ◽  
Mihaela M. Trandafir ◽  
Adelina Stănoiu ◽  
Ovidiu G. Florea ◽  
Cristian E. Simion ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Catalytic Combustion ◽  
Mixed Oxides ◽  
Sol Gel ◽  
Nitrogen Adsorption ◽  
X Ray Diffraction ◽  
X Ray ◽  
Temperature Programmed ◽  
Catalytic Combustion Of Methane ◽  
Adsorption Desorption

This study presents the synthesis and characterization of lanthanum-modified alumina supported cerium–manganese mixed oxides, which were prepared by three different methods (coprecipitation, impregnation and citrate-based sol-gel method) followed by calcination at 500 °C. The physicochemical properties of the synthesized materials were investigated by various characterization techniques, namely: nitrogen adsorption-desorption isotherms, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and H2–temperature programmed reduction (TPR). This experimental study demonstrated that the role of the catalytic surface is much more important than the bulk one. Indeed, the incipient impregnation of CeO2–MnOx catalyst, supported on an optimized amount of 4 wt.% La2O3–Al2O3, provided the best results of the catalytic combustion of methane on our catalytic micro-convertors. This is mainly due to: (i) the highest pore size dimensions according to the Brunauer-Emmett-Teller (BET) investigations, (ii) the highest amount of Mn4+ or/and Ce4+ on the surface as revealed by XPS, (iii) the presence of a mixed phase (Ce2MnO6) as shown by X-ray diffraction; and (iv) a higher reducibility of Mn4+ or/and Ce4+ species as displayed by H2–TPR and therefore more reactive oxygen species.

scholarly journals Synthesis of nickel/gallium nanoalloys using a dual-source approach in 1-alkyl-3-methylimidazole ionic liquids

2019 ◽  
Vol 10 ◽  
pp. 1754-1767
Author(s):  
Ilka Simon ◽  
Julius Hornung ◽  
Juri Barthel ◽  
Jörg Thomas ◽  
Maik Finze ◽  
...  
Keyword(s):  
Electron Microscopy ◽  
Transmission Electron Microscopy ◽  
Photoelectron Spectroscopy ◽  
Dark Field ◽  
X Ray ◽  
Transmission Electron ◽  
Scanning Transmission ◽  
Annular Dark Field ◽  
Dual Source ◽  
Induced Decomposition

NiGa is a catalyst for the semihydrogenation of alkynes. Here we show the influence of different dispersion times before microwave-induced decomposition of the precursors on the phase purity, as well as the influence of the time of microwave-induced decomposition on the crystallinity of the NiGa nanoparticles. Microwave-induced co-decomposition of all-hydrocarbon precursors [Ni(COD)2] (COD = 1,5-cyclooctadiene) and GaCp* (Cp* = pentamethylcyclopentadienyl) in the ionic liquid [BMIm][NTf2] selectively yields small intermetallic Ni/Ga nanocrystals of 5 ± 1 nm as derived from transmission electron microscopy (TEM) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and supported by energy-dispersive X-ray spectrometry (EDX), selected-area energy diffraction (SAED) and X-ray photoelectron spectroscopy (XPS). NiGa@[BMIm][NTf2] catalyze the semihydrogenation of 4-octyne to 4-octene with 100% selectivity towards (E)-4-octene over five runs, but with poor conversion values. IL-free, precipitated NiGa nanoparticles achieve conversion values of over 90% and selectivity of 100% towards alkene over three runs.

Beta-Cyclodextrin-triggered fabrication of broccoli-like ZnO nanoaggregates with enhanced photocatalytic capability

2020 ◽  
Vol 13 (02) ◽  
pp. 2051004
Author(s):  
Jinyan Xiong ◽  
Wei Li ◽  
Kai Zhao ◽  
Weijie Li ◽  
Gang Cheng
Keyword(s):  
Electron Microscopy ◽  
Photoelectron Spectroscopy ◽  
Separation Efficiency ◽  
Nitrogen Adsorption ◽  
Electrochemical Measurement ◽  
X Ray ◽  
Recombination Efficiency ◽  
Beta Cyclodextrin ◽  
Composition And Structure ◽  
Pollution Removal

Nanocrystallite aggregates have great potential in semiconductor-based photocatalysis toward environmental pollution removal. In this work, we reported the fabrication of broccoli-like zinc oxide nanoaggregates in the presence of beta-cyclodextrin in ethylene glycol-H2O medium. The composition and structure of the as-obtained ZnO nanoaggregates were characterized by powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and nitrogen adsorption. It was observed that the beta-cyclodextrin played an important role in the fabrication of such broccoli-like structure. A plausible formation mechanism was discussed on the basis of the controllable experiments. The photocatalytic performance of the products was studied through the photodegradation of rhodamine B under simulated sunlight irradiation. Compared to the spherical ZnO nanoaggregates and ZnO broken spheres, the broccoli-like ZnO exhibited superior photocatalytic efficiency. Based on the photocurrent and electrochemical measurement results, the higher separation efficiency of the photogenerated carriers and lower recombination efficiency of the photoinduced electron–hole pairs over the broccoli-like ZnO nanoaggregates contributed to their remarkable photocatalytic activity.

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