scholarly journals Promoting Effect of Copper Loading and Mesoporosity on Cu-MOR in the Carbonylation of Dimethyl Ether to Methyl Acetate

Catalysts ◽  
2021 ◽  
Vol 11 (6) ◽  
pp. 696
Author(s):  
Raju Poreddy ◽  
Susanne Mossin ◽  
Anker Degn Jensen ◽  
Anders Riisager
Keyword(s):  
Dimethyl Ether ◽  
Photoelectron Spectroscopy ◽  
Gas Flow ◽  
Methyl Acetate ◽  
Coke Formation ◽  
Acid Property ◽  
Promoting Effect ◽  
Paramagnetic Resonance ◽  
X Ray ◽  
Temperature Programmed

Cu-mordenite (Cu-MOR) catalysts with different copper loadings were prepared, characterized and examined in continuous, gas-flow synthesis of methyl acetate (MA) by dimethyl ether (DME) carbonylation. Improved activity and selectivity were observed for Cu-MOR catalysts with up to 1 wt% Cu and X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR) spectroscopy and temperature-programmed reduction with hydrogen (H2-TPR) were used to elucidate the state of copper in the catalysts. Moreover, mesoporous MOR catalysts (RHMs) were prepared by mild stepwise recrystallization with X-ray powder diffraction (XRPD) and ammonia temperature-programmed desorption (NH3-TPD) demonstrating the retained MOR structure and the acid property of the catalysts, respectively. The RHM catalysts showed improved lifetime compared to pristine MOR giving a yield up to 78% MA with 93% selectivity after 5 h on stream (GHSV = 6711 h−1). Under identical reaction conditions, 1 wt% Cu-RHM catalysts had an even higher catalytic activity and durability resulting in a MA yield of 90% with 97% selectivity for 7–8 h of operation as well as a lower coke formation.

scholarly journals Propane and Naphthalene Oxidation over Gold-Promoted Cobalt Catalysts Supported on Zirconia

Catalysts ◽  
2020 ◽  
Vol 10 (4) ◽  
pp. 387
Author(s):  
María Silvia Leguizamón Aparicio ◽  
María Lucia Ruiz ◽  
Marco Antonio Ocsachoque ◽  
Marta Isabel Ponzi ◽  
Enrique Rodríguez-Castellón ◽  
...  
Keyword(s):  
Electron Microscopy ◽  
Photoelectron Spectroscopy ◽  
Cobalt Catalysts ◽  
Bet Surface Area ◽  
Promoting Effect ◽  
Propane Combustion ◽  
X Ray ◽  
Transmission Electron ◽  
Temperature Programmed ◽  
Supported Gold

Zirconia-supported gold-promoted cobalt catalysts were synthesized and tested for the complete oxidation of propane and naphthalene. The catalysts were characterized by BET surface area, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), powder X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS). In both propane and naphthalene combustion reactions, the results obtained indicate that catalysts formulated with Co3O4 are more active than those containing only Au. Catalysts prepared using the deposit/precipitation (DP) method have better activity than those in which the traditional technique is used. Gold addition using the DP methods generates a promoting effect on the activity of cobalt-containing catalysts. The AuDpCoZt catalyst was found to be the most active for both propane and naphthalene combustion. The catalytic behavior of this sample is associated with a synergic effect between gold, cobalt, and the support, which is also evidenced by an increase in the reducibility of this catalytic system. The effect of the presence of NO in the feed was also analyzed for propane combustion.

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 Active Site of O2 and Its Improvement Mechanism over Ce-Ti Catalyst for NH3-SCR Reaction

Catalysts ◽  
2018 ◽  
Vol 8 (8) ◽  
pp. 336 ◽  
Author(s):  
Dong Jiang ◽  
Shule Zhang ◽  
Yiqing Zeng ◽  
Pengfei Wang ◽  
Qin Zhong
Keyword(s):  
Active Site ◽  
Photoelectron Spectroscopy ◽  
Oxygen Vacancies ◽  
Catalytic Reduction ◽  
Supported Catalyst ◽  
Temperature Programmed Desorption ◽  
Paramagnetic Resonance ◽  
X Ray ◽  
Adsorption Sites ◽  
Temperature Programmed

The current study on Ce-Ti catalyst was mainly focused on the function of NH3 and NO adsorption sites. In our study, by comparing Ce-Ti (doped catalyst) to Ce/Ti (supported catalyst), the active site of O2 and its improvement mechanism over Ce-Ti catalyst for NH3-Selective catalytic reduction (SCR) reactions were investigated. For Ce-Ti catalyst, a cerium atom was confirmed entering a TiO2 crystal lattice by X-ray diffraction (XRD) and Raman; the structure of Ce-□-Ti (□ represents oxygen vacancy) in Ce-Ti catalyst was confirmed by X-ray photoelectron spectroscopy (XPS) and Photoluminescence spectra (PL spectra). The nature of this structure was characterized by electron paramagnetic resonance (EPR), Ammonia temperature-programmed desorption (NH3-TPD), hydrogen temperature-programmed reduction (H2-TPR), Nitric oxide temperature-programmed desorption (NO-TPD) and In situ DRIFT. The results indicated that oxygen vacancies had a promotive effect on the adsorption and activation of oxygen, and oxygen was converted to superoxide ions in large quantities. Also, because of adsorption and activation of NO and NH3, electrons were transferred to adsorbed oxygen via oxygen vacancies, which also promoted the formation of superoxide ions. We expected that our study could promote understanding of the active site of O2 and its improvement mechanism for doped catalyst.

scholarly journals Regeneration of Pt-Sn/Al2O3 Catalyst for Hydrogen Production through Propane Dehydrogenation Using Hydrochloric Acid

Catalysts ◽  
2020 ◽  
Vol 10 (8) ◽  
pp. 898
Author(s):  
Yi Sun Choi ◽  
Kyeongseok Oh ◽  
Kwang-Deog Jung ◽  
Won-Il Kim ◽  
Hyoung Lim Koh
Keyword(s):  
Hydrochloric Acid ◽  
Photoelectron Spectroscopy ◽  
Coke Formation ◽  
Propane Dehydrogenation ◽  
Pure Hydrogen ◽  
X Ray ◽  
Air Atmosphere ◽  
Sustainable Operation ◽  
Temperature Programmed ◽  
Calcination Atmosphere

Compared with dehydrogenation in conventional petroleum refinery processes, relatively pure hydrogen can be produced by propane dehydrogenation (PDH) without innate contaminants like sulfur and metals. Among the existing catalysts for PDH, Pt catalysts are popular and are often used in conjunction with Sn as a co-catalyst. Coke formation is a major concern in PDH, where catalyst regeneration is typically achieved by periodic coke burning to achieve sustainable operation. In this study, Pt-Sn/Al2O3 catalysts were regenerated after coke burning in three stages: mixing the catalyst with liquid hydrochloric acid, drying, and calcining under air atmosphere. In this process, the optimum concentration of hydrochloric acid was found to be 35% w/w. HCl treatment was effective for enhancing redispersion of the metal catalysts and aiding the formation of the Pt3Sn alloy, which is considered to be effective for PDH reaction. HCl treatment may provide oxychlorination-like conditions under the calcination atmosphere. The characteristics of the catalysts were examined by X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), and CO chemisorption.

scholarly journals Reduction of NOx by H2 on WOx-Promoted Pt/Al2O3/SiO2 Catalysts Under O2-Rich Conditions

2021 ◽  
Author(s):  
Enno Eßer ◽  
Daniel Schröder ◽  
Anna V. Nartova ◽  
Aleksey M. Dmitrachkov ◽  
Sven Kureti
Keyword(s):  
Photoelectron Spectroscopy ◽  
Laser Raman Spectroscopy ◽  
Promoting Effect ◽  
X Ray ◽  
Laser Raman ◽  
Supported Pt Catalysts ◽  
Metal Support Interaction ◽  
Metal Support ◽  
Temperature Programmed ◽  
Diffuse Reflectance Infrared

AbstractThis work addresses the reduction of NOx by H2 under O2-rich conditions using Al2O3/SiO2-supported Pt catalysts with different loads of WOx promotor. The samples were thoroughly characterised by N2 physisorption, temperature-programmed desorption of CO, scanning electron microscopy, X-ray diffraction, laser raman spectroscopy, X-ray photoelectron spectroscopy and diffuse reflectance infrared fourier transform spectroscopy with probe molecule CO. The catalytic studies of the samples without WOx showed pronounced NOx conversion below 200 °C, whereas highest efficiency was related to small Pt particles. The introduction of WOx provided increasing deNOx activity as well as N2 selectivity. This promoting effect was referred to an additional reaction path at the Pt-WOx/Al2O3/SiO2 interface, whereas an electronic activation of Pt by strong metal support interaction was excluded. Graphic Abstract

Interactions of Ge Atoms with High- ê Oxide Dielectric Surfaces

2005 ◽  
Vol 879 ◽  
Author(s):  
Scott K. Stanley ◽  
John G. Ekerdt
Keyword(s):  
Oxide Layer ◽  
Photoelectron Spectroscopy ◽  
Chemical Vapor ◽  
Temperature Programmed Desorption ◽  
Tungsten Filament ◽  
X Ray ◽  
Dielectric Surfaces ◽  
Temperature Programmed ◽  
The Stability ◽  
Ge Nanocrystals

AbstractGe is deposited on HfO2 surfaces by chemical vapor deposition (CVD) with GeH4. 0.7-1.0 ML GeHx (x = 0-3) is deposited by thermally cracking GeH4 on a hot tungsten filament. Ge oxidation and bonding are studied at 300-1000 K with X-ray photoelectron spectroscopy (XPS). Ge, GeH, GeO, and GeO2 desorption are measured with temperature programmed desorption (TPD) at 400-1000 K. Ge initially reacts with the dielectric forming an oxide layer followed by Ge deposition and formation of nanocrystals in CVD at 870 K. 0.7-1.0 ML GeHx deposited by cracking rapidly forms a contacting oxide layer on HfO2 that is stable from 300-800 K. Ge is fully removed from the HfO2 surface after annealing to 1000 K. These results help explain the stability of Ge nanocrystals in contact with HfO2.

Highly active carbon nanotube–promoted Rh-Mn-Li/SiO2 catalysts for the synthesis of C2+ oxygenates from syngas

2021 ◽  
pp. 174751982098472
Author(s):  
Jun Yu ◽  
Ying Han ◽  
Guoqing Chen ◽  
Xiuzhen Xiao ◽  
Haifang Mao ◽  
...  
Keyword(s):  
Carbon Nanotubes ◽  
Photoelectron Spectroscopy ◽  
Co Hydrogenation ◽  
X Ray ◽  
Highly Active ◽  
Transmission Electron ◽  
Co Insertion ◽  
Temperature Programmed Surface Reaction ◽  
Temperature Programmed ◽  
Oxygenate Synthesis

The effect of carbon nanotubes on the catalytic properties of Rh-Mn-Li/SiO2 catalysts was investigated for CO hydrogenation. The catalysts were comprehensively characterized by means of X-ray power diffraction, N2 sorption, transmission electron microscope, H2–temperature-programmed reduction, CO–temperature-programmed desorption, temperature-programmed surface reaction, and X-ray photoelectron spectroscopy. The results showed that an appropriate amount of carbon nanotubes can be attached to the surface of the SiO2 sphere and can improve the Rh dispersion. Moderate Rh-Mn interaction can be obtained by doping with the appropriate amount of carbon nanotubes, which promotes the formation of strongly adsorbed CO and facilitates the progress of CO insertion, resulting in the increase in the selectivity of C2+ oxygenate synthesis.

Jellyfish-like few-layer graphene nanoflakes: high paramagnetic response alongside increased interlayer interaction

2021 ◽  
Vol 0 (0) ◽  
Author(s):  
Alexander Ulyanov ◽  
Dmitrii Stolbov ◽  
Serguei Savilov
Keyword(s):  
Photoelectron Spectroscopy ◽  
High Sensitivity ◽  
Paramagnetic Centers ◽  
Interlayer Interaction ◽  
Paramagnetic Resonance ◽  
X Ray ◽  
Graphene Nanoflakes ◽  
Few Layer Graphene ◽  
Electron Paramagnetic ◽  
Hydrocarbon Pyrolysis

Abstract Jellyfish-like graphene nanoflakes (GNF), prepared by hydrocarbon pyrolysis, are studied with electron paramagnetic resonance (EPR) method. The results are supported by X-ray photoelectron spectroscopy (XPS) data. Oxidized (GNFox) and N-doped oxidized (N-GNFox) flakes exhibit an extremely high EPR response associated with a large interlayer interaction which is caused by the structure of nanoflakes and layer edges reached by oxygen. The GNFox and N-GNFox provide the localized and mobile paramagnetic centers which are silent in the pristine (GNF p ) and N-doped (N-GNF) samples. The change in the relative intensity of the line corresponding to delocalized electrons is parallel with the number of radicals in the quaternary N-group. The environment of localized and mobile electrons is different. The results can be important in GNF synthesis and for explanation of their features in applications, especially, in devices with high sensitivity to weak electromagnetic field.

scholarly journals Biodiesel Production on Monometallic Pt, Pd, Ru, and Ag Catalysts Supported on Natural Zeolite

Materials ◽  
2020 ◽  
Vol 14 (1) ◽  
pp. 48
Author(s):  
Pawel Mierczynski ◽  
Magdalena Mosińska ◽  
Lukasz Szkudlarek ◽  
Karolina Chalupka ◽  
Misa Tatsuzawa ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Natural Zeolite ◽  
Noble Metals ◽  
Methyl Esters ◽  
Physicochemical Characteristics ◽  
Biodiesel Production ◽  
X Ray Diffraction ◽  
X Ray ◽  
Yield Values ◽  
Temperature Programmed

Biodiesel production from rapeseed oil and methanol via transesterification reaction facilitated by various monometallic catalyst supported on natural zeolite (NZ) was investigated. The physicochemical characteristics of the synthesized catalysts were studied by X-ray diffraction (XRD), Brunauer–Emmett–Teller method (BET), temperature-programmed-reduction in hydrogen (H2-TPR), temperature-programmed-desorption of ammonia (NH3-TPD), Scanning Electron Microscope equipped with EDX detector (SEM-EDS), and X-ray photoelectron spectroscopy (XPS) methods. The highest activity and methyl ester yields were obtained for the Pt/NZ catalyst. This catalyst showed the highest triglycerides conversion of 98.9% and fatty acids methyl esters yields of 94.6%. The activity results also confirmed the high activity of the carrier material (NZ) itself in the investigated reaction. Support material exhibited 90.5% of TG conversion and the Fatty Acid Methyl Esters yield (FAME) of 67.2%. Introduction of noble metals improves the TG conversion and FAME yield values. Increasing of the metal loading from 0.5 to 2 wt.% improves the reactivity properties of the investigated catalysts.

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