scholarly journals Sulfur stabilizing metal nanoclusters on carbon at high temperatures

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Peng Yin ◽  
Xiao Luo ◽  
Yanfu Ma ◽  
Sheng-Qi Chu ◽  
Si Chen ◽  
...  
Keyword(s):  
High Temperatures ◽  
Supported Catalysts ◽  
Carbon Matrix ◽  
Carbon Support ◽  
Metal Nanoclusters ◽  
Electronic Effects ◽  
Atom Diffusion ◽  
Surface Areas ◽  
Metal Nanocluster ◽  
Thermal Sintering

AbstractSupported metal nanoclusters consisting of several dozen atoms are highly attractive for heterogeneous catalysis with unique catalytic properties. However, the metal nanocluster catalysts face the challenges of thermal sintering and consequent deactivation owing to the loss of metal surface areas particularly in the applications of high-temperature reactions. Here, we report that sulfur—a documented poison reagent for metal catalysts—when doped in a carbon matrix can stabilize ~1 nanometer metal nanoclusters (Pt, Ru, Rh, Os, and Ir) at high temperatures up to 700 °C. We find that the enhanced adhesion strength between metal nanoclusters and the sulfur-doped carbon support, which arises from the interfacial metal-sulfur bonding, greatly retards both metal atom diffusion and nanocluster migration. In catalyzing propane dehydrogenation at 550 °C, the sulfur-doped carbon supported Pt nanocluster catalyst with interfacial electronic effects exhibits higher selectivity to propene as well as more stable durability than sulfur-free carbon supported catalysts.

In situ REM imaging of surface processes on ceramic bulk crystals from 300 to 1670 K in a conventional TEM

1991 ◽  
Vol 49 ◽  
pp. 660-661
Author(s):  
Z. L. Wang ◽  
J. Bentley
Keyword(s):  
High Temperatures ◽  
Image Resolution ◽  
Atomic Processes ◽  
Crystal Surfaces ◽  
Beam Radiation ◽  
Surface Areas ◽  
Transmission Electron ◽  
Reflection Electron Microscopy ◽  
Gas Reactions

Studying the behavior of surfaces at high temperatures is of great importance for understanding the properties of ceramics and associated surface-gas reactions. Atomic processes occurring on bulk crystal surfaces at high temperatures can be recorded by reflection electron microscopy (REM) in a conventional transmission electron microscope (TEM) with relatively high resolution, because REM is especially sensitive to atomic-height steps.Improved REM image resolution with a FEG: Cleaved surfaces of a-alumina (012) exhibit atomic flatness with steps of height about 5 Å, determined by reference to a screw (or near screw) dislocation with a presumed Burgers vector of b = (1/3)<012> (see Fig. 1). Steps of heights less than about 0.8 Å can be clearly resolved only with a field emission gun (FEG) (Fig. 2). The small steps are formed by the surface oscillating between the closely packed O and Al stacking layers. The bands of dark contrast (Fig. 2b) are the result of beam radiation damage to surface areas initially terminated with O ions.

scholarly journals Towards High Efficacy of Pd-Au/C Catalyst for Tetrachloromethane Hydrodechlorination

Chemistry ◽  
2021 ◽  
Vol 3 (1) ◽  
pp. 338-359
Author(s):  
Magdalena Bonarowska ◽  
Zbigniew Kaszkur ◽  
Krzysztof Matus ◽  
Alicja Drelinkiewicz ◽  
Tomasz Szumełda ◽  
...  
Keyword(s):  
Microwave Irradiation ◽  
Gas Phase ◽  
Thermal Activation ◽  
Supported Catalysts ◽  
Carbon Support ◽  
Thermal Reduction ◽  
Microwave Oven ◽  
Optimal Conditions ◽  
Catalyst Activation ◽  
Critical Part

We present an efficient strategy for synthesising the PdAu catalysts with a homogeneous PdAu alloy phase for environmentally important hydrodechlorination of tetrachloromethane in the gas phase. The synthesis of carbon-supported catalysts involved two major steps: (i) incorporation of palladium and gold nanoparticles into carbon support and (ii) activation of the catalysts. The critical part of this work was to find the optimal conditions for both steps. Thus, the incorporation of the nanoparticles was carried out in two ways, by impregnation and direct redox reaction method using acetone solutions of metal precursor salts. The activation was performed either by a conventional thermal reduction in hydrogen or flash irradiation in a microwave oven. The homogeneity and structure of the PdAu alloy were found to depend on the catalyst activation method critically. In all cases, we observed better homogeneity for catalysts that were subject to microwave irradiation. Moreover, the flash microwave irradiation of prepared catalysts provided catalysts of better stability and selectivity towards the desired products (hydrocarbons) in the hydrodechlorination of tetrachloromethane as compared to the catalyst obtained by conventional thermal activation in hydrogen.

scholarly journals Nickel Phosphide Catalysts as Efficient Systems for CO2 Upgrading via Dry Reforming of Methane

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 446
Author(s):  
Miriam González-Castaño ◽  
Estelle le Saché ◽  
Cameron Berry ◽  
Laura Pastor-Pérez ◽  
Harvey Arellano-García ◽  
...  
Keyword(s):  
Supported Catalysts ◽  
Lower Surface ◽  
Catalytic Performance ◽  
Dry Reforming Of Methane ◽  
Oxidation Reactions ◽  
Surface Areas ◽  
Ceo2 Sample ◽  
Conversion Rates ◽  
Ni Oxidation ◽  
Catalytic Behaviour

This work establishes the primordial role played by the support’s nature when aimed at the constitution of Ni2P active phases for supported catalysts. Thus, carbon dioxide reforming of methane was studied over three novel Ni2P catalysts supported on Al2O3, CeO2 and SiO2-Al2O3 oxides. The catalytic performance, shown by the catalysts’ series, decreased according to the sequence: Ni2P/Al2O3 > Ni2P/CeO2 > Ni2P/SiO2-Al2O3. The depleted CO2 conversion rates discerned for the Ni2P/SiO2-Al2O3 sample were associated to the high sintering rates, large amounts of coke deposits and lower fractions of Ni2P constituted in the catalyst surface. The strong deactivation issues found for the Ni2P/CeO2 catalyst, which also exhibited small amounts of Ni2P species, were majorly associated to Ni oxidation issues. Along with lower surface areas, oxidation reactions might also affect the catalytic behaviour exhibited by the Ni2P/CeO2 sample. With the highest conversion rate and optimal stabilities, the excellent performance depicted by the Ni2P/Al2O3 catalyst was mostly related to the noticeable larger fractions of Ni2P species established.

Novel Carbon Structure as Highly Stable Support for Electro-catalyst in Acid Media: Regulating Oxygen Functionalization Behavior of Carbon

2021 ◽  
Author(s):  
Guokang Han ◽  
Yongrong Sun ◽  
Yuxin Liu ◽  
Lingfeng Li ◽  
Xudong Li ◽  
...  
Keyword(s):  
Precious Metal ◽  
Catalytic Properties ◽  
Supported Catalysts ◽  
Carbon Support ◽  
Carbon Structure ◽  
Acid Media

The nature of carbon support has huge effects on the catalytic properties of supported catalysts. When utilized for electrochemical purposes as support for precious metal in acid media, the oxygen...

A Study of Nanosize Fe3O4 Deposited on Carbon Matrix

2008 ◽  
Vol 8 (2) ◽  
pp. 591-594 ◽  
Author(s):  
B. Banov ◽  
L. Ljutzkanov ◽  
I. Dimitrov ◽  
A. Trifonova ◽  
H. Vasilchina ◽  
...  
Keyword(s):  
Average Particle Size ◽  
Carbon Matrix ◽  
Reversible Capacity ◽  
Carbon Support ◽  
Test Sample ◽  
Constant Current ◽  
Average Particle ◽  
Scanning Electron Micrographs ◽  
Lithium Secondary Batteries ◽  
Electrochemical Tests

Nanosized crystalline Fe3O4 (with an average particle size of 16 nm) was successfully synthesized on a carbon matrix surface. The prepared sample was heat-treated in the temperature range 300 °C–750 °C to remove residual impurities and to obtain a final product with a 77:23 ratio between magnetite and the carbon support. The sample was subjected to physicochemical and electrochemical tests. The purity of the phase and the particles size was determined by X-ray diffraction analysis and confirmed by field emission scanning electron micrographs. The specific surface area of the sample measured by the B.E.T method was 120 m2 g−1. A series of electrochemical tests including EIS, CV and long-term constant current cycling have been performed. The obtained reversible capacity within 15 cycles was in the range 400–550 mA h · g−1. The electrochemical behavior of the test sample and its possible practical use as an anode material in lithium secondary batteries are discussed.

scholarly journals Surfactant-Free Colloidal Strategies for Highly Dispersed and Active Supported IrO2 Catalysts: Synthesis and Performance Evaluation for the Oxygen Evolution Reaction

2021 ◽  
Author(s):  
Francesco Bizzotto ◽  
Jonathan Quinson ◽  
Johanna Schröder ◽  
Alessandro Zana ◽  
Matthias Arenz
Keyword(s):  
Supported Catalysts ◽  
Active Phase ◽  
Carbon Support ◽  
Colloidal Dispersions ◽  
Catalyst Design ◽  
Transition Electron Microscopy ◽  
Highly Active ◽  
X Ray Scattering ◽  
And Performance ◽  
Transition Electron

Supported Ir oxide catalysts obtained from surfactant-free colloidal Ir nanoparticles (NPs) synthesized in alkaline methanol (MeOH), ethanol (EtOH), and ethylene glycol (EG) are investigated and compared. The comparison of independent techniques such as transition electron microscopy (TEM), small angle X-ray scattering (SAXS), and electrochemistry allows shedding light on the parameters that affect the dispersion of the active phase as well as the catalytic activity. The colloidal dispersions obtained are suitable to develop supported catalysts with little NP agglomeration on a carbon support leading to highly active catalysts with more than 400 A g<sup>-1</sup><sub>Ir</sub> reached at 1.5 V<sub>RHE</sub> for the OER. While the more common surfactant-free alkaline EG synthesis requires flocculation and re-dispersion leading to Ir loss, the main difference between methanol and ethanol as solvent is related to the dispersibility of the support material. The choice of the suitable monoalcohol determines the maximum achieved Ir loading on the support without detrimental particle agglomeration. This simple consideration on catalyst design can readily lead to significantly improved catalysts.

Carbon nanopore and anchoring site–assisted general construction of encapsulated metal (Rh, Ru, Ir) nanoclusters for highly efficient hydrogen evolution in pH–universal electrolytes and natural seawater

2021 ◽  
Author(s):  
Rong Ding ◽  
Tingting Yan ◽  
Yi Wang ◽  
Yan Long ◽  
Guangyin Fan
Keyword(s):  
Hydrogen Evolution ◽  
Water Splitting ◽  
General Construction ◽  
Natural Seawater ◽  
Metal Nanoclusters ◽  
Hydrogen Economy ◽  
Ligand Free ◽  
Metal Nanocluster ◽  
Substantial Interest ◽  
Free Metal

Metal–nanocluster–catalyzed hydrogen evolution through water splitting has received substantial interest toward the implementation of hydrogen economy. However, the general and efficient fabrication of well–defined and ligand–free metal nanoclusters (NCs) with...

scholarly journals Thermal Modification Effect on Supported Cu-Based Activated Carbon Catalyst in Hydrogenolysis of Glycerol

Materials ◽  
2020 ◽  
Vol 13 (3) ◽  
pp. 603 ◽  
Author(s):  
Juan Seguel ◽  
Rafael García ◽  
Ricardo José Chimentão ◽  
José Luis García-Fierro ◽  
I. Tyrone Ghampson ◽  
...  
Keyword(s):  
Activated Carbon ◽  
Specific Surface ◽  
Hydrogen Adsorption ◽  
Carbon Support ◽  
Catalytic Performance ◽  
Homogeneous Distribution ◽  
Surface Groups ◽  
Carbon Supports ◽  
Surface Areas ◽  
Oxygen Surface

Glycerol hydrogenolysis to 1,2-propanediol (1,2-PDO) was performed over activated carbon supported copper-based catalysts. The catalysts were prepared by impregnation using a pristine carbon support and thermally-treated carbon supports (450, 600, 750, and 1000 °C). The final hydrogen adsorption capacity, porous structure, and total acidity of the catalysts were found to be important descriptors to understand catalytic performance. Oxygen surface groups on the support controlled copper dispersion by modifying acidic and adsorption properties. The amount of oxygen species of thermally modified carbon supports was also found to be a function of its specific surface area. Carbon supports with high specific surface areas contained large amount of oxygen surface species, inducing homogeneous distribution of Cu species on the carbon support during impregnation. The oxygen surface groups likely acted as anchorage centers, whereby the more stable oxygen surface groups after the reduction treatment produced an increase in the interaction of the copper species with the carbon support, and determined catalytic performances.

scholarly journals H2 Production from Catalytic Methane Decomposition Using Fe/x-ZrO2 and Fe-Ni/(x-ZrO2) (x = 0, La2O3, WO3) Catalysts

Catalysts ◽  
2020 ◽  
Vol 10 (7) ◽  
pp. 793
Author(s):  
Fahad Al-Mubaddel ◽  
Samsudeen Kasim ◽  
Ahmed A. Ibrahim ◽  
Abdulrhman S. Al-Awadi ◽  
Anis H. Fakeeha ◽  
...  
Keyword(s):  
Supported Catalysts ◽  
Thermo Gravimetric Analysis ◽  
Space Velocity ◽  
H2 Production ◽  
Methane Decomposition ◽  
Gravimetric Analysis ◽  
Impregnation Method ◽  
Carbon Deposits ◽  
Surface Areas ◽  
H2 Yield

An environmentally-benign way of producing hydrogen is methane decomposition. This study focused on methane decomposition using Fe and Fe-Ni catalysts, which were dispersed over different supports by the wet-impregnation method. We observed the effect of modifying ZrO2 with La2O3 and WO3 in terms of H2 yield and carbon deposits. The modification led to a higher H2 yield in all cases and WO3-modified support gave the highest yield of about 90% and was stable throughout the reaction period. The reaction conditions were at 1 atm, 800 °C, and 4000 mL(hgcat)−1 space velocity. Adding Ni to Fe/x-ZrO2 gave a higher H2 yield and stability for ZrO2 and La2O3 + ZrO2-supported catalysts whose prior performances and stabilities were very poor. Catalyst samples were analyzed by characterization techniques like X-ray diffraction (XRD), nitrogen physisorption, temperature-programmed reduction (TPR), thermo-gravimetric analysis (TGA), and Raman spectroscopy. The phases of iron and the supports were identified using XRD while the BET revealed a significant decrease in the specific surface areas of fresh catalysts relative to supports. A progressive change in Fe’s oxidation state from Fe3+ to Fe0 was observed from the H2-TPR results. The carbon deposits on Fe/ZrO2 and Fe/La2O3 + ZrO2 are mainly amorphous, while Fe/WO3 + ZrO2 and Fe-Ni/x-ZrO2 are characterized by graphitic carbon.

XRD characterization of highly dispersed metal catalysts on carbon support

1993 ◽  
Vol 8 (8) ◽  
pp. 1829-1835 ◽  
Author(s):  
Paolo Scardi ◽  
Pier Luigi Antonucci
Keyword(s):  
Particle Size ◽  
Supported Catalysts ◽  
Profile Analysis ◽  
Rietveld Method ◽  
Carbon Support ◽  
Lattice Parameter ◽  
Microstructural Parameters ◽  
Transmission Electron ◽  
Supported Pt Catalysts ◽  
Highly Dispersed

Carbon-supported Pt catalysts were prepared from H2PtCl6 or K2PtCl6 aqueous solutions. Particle size and structure after several thermal activation treatments were studied by X-Ray Diffraction (XRD), Transmission Electron Microscopy (TEM), and Cyclic Voltammetry (CV), and the results of the three techniques were compared. As the catalysts were highly dispersed on an amorphous support, a conventional XRD profile analysis for crystallite size determination could not be performed properly, because of the strong overlapping between the broad Pt peaks superposed to the halos of the amorphous phase. Thus, a new procedure of whole XRD pattern fitting, based on the Rietveld method, was used to have reliable data of Pt particle size (surface area) and lattice parameter. All structural and microstructural parameters were refined within the same procedure, also considering the transparency of the carbon supported catalysts and minimizing the effect of the amorphous background. The method can also take into account the presence of bimodal particle size distributions, which is difficult to study by CV or TEM.

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