scholarly journals PdZn catalysts for CO2 hydrogenation to methanol using chemical vapour impregnation (CVI)

2017 ◽  
Vol 197 ◽  
pp. 309-324 ◽  
Author(s):  
H. Bahruji ◽  
M. Bowker ◽  
W. Jones ◽  
J. Hayward ◽  
J. Ruiz Esquius ◽  
...  

The formation of PdZn bimetallic alloys on ZnO, TiO2 and Al2O3 supports was investigated, together with the effect of alloy formation on the CO2 hydrogenation reaction. The chemical vapour impregnation (CVI) method produced PdZn nanoparticles with diameters of 3–6 nm. X-ray photoelectron spectroscopy and X-ray diffraction revealed the changes in the structure of the PdZn alloy that help stabilise formate intermediates during methanol synthesis. PdZn supported on TiO2 exhibits high methanol productivity of 1730 mmol kgcat−1 h−1 that is associated with the high dispersion of the supported PdZn alloy.

Author(s):  
Tianlei Ma ◽  
Marek Nikiel ◽  
Andrew G. Thomas ◽  
Mohamed Missous ◽  
David J. Lewis

AbstractIn this report, we prepared transparent and conducting undoped and molybdenum-doped tin oxide (Mo–SnO2) thin films by aerosol-assisted chemical vapour deposition (AACVD). The relationship between the precursor concentration in the feed and in the resulting films was studied by energy-dispersive X-ray spectroscopy, suggesting that the efficiency of doping is quantitative and that this method could potentially impart exquisite control over dopant levels. All SnO2 films were in tetragonal structure as confirmed by powder X-ray diffraction measurements. X-ray photoelectron spectroscopy characterisation indicated for the first time that Mo ions were in mixed valence states of Mo(VI) and Mo(V) on the surface. Incorporation of Mo6+ resulted in the lowest resistivity of $$7.3 \times 10^{{ - 3}} \Omega \,{\text{cm}}$$ 7.3 × 10 - 3 Ω cm , compared to pure SnO2 films with resistivities of $$4.3\left( 0 \right) \times 10^{{ - 2}} \Omega \,{\text{cm}}$$ 4.3 0 × 10 - 2 Ω cm . Meanwhile, a high transmittance of 83% in the visible light range was also acquired. This work presents a comprehensive investigation into impact of Mo doping on SnO2 films synthesised by AACVD for the first time and establishes the potential for scalable deposition of SnO2:Mo thin films in TCO manufacturing. Graphical abstract


Materials ◽  
2021 ◽  
Vol 14 (19) ◽  
pp. 5490
Author(s):  
Nuria Jiménez-Arévalo ◽  
Eduardo Flores ◽  
Alessio Giampietri ◽  
Marco Sbroscia ◽  
Maria Grazia Betti ◽  
...  

Heterostructures formed by ultrathin borocarbonitride (BCN) layers grown on TiO2 nanoribbons were investigated as photoanodes for photoelectrochemical water splitting. TiO2 nanoribbons were obtained by thermal oxidation of TiS3 samples. Then, BCN layers were successfully grown by plasma enhanced chemical vapour deposition. The structure and the chemical composition of the starting TiS3, the TiO2 nanoribbons and the TiO2-BCN heterostructures were investigated by Raman spectroscopy, X-ray diffraction and X-ray photoelectron spectroscopy. Diffuse reflectance measurements showed a change in the gap from 0.94 eV (TiS3) to 3.3 eV (TiO2) after the thermal annealing of the starting material. Morphological characterizations, such as scanning electron microscopy and optical microscopy, show that the morphology of the samples was not affected by the change in the structure and composition. The obtained TiO2-BCN heterostructures were measured in a photoelectrochemical cell, showing an enhanced density of current under dark conditions and higher photocurrents when compared with TiO2. Finally, using electrochemical impedance spectroscopy, the flat band potential was determined to be equal in both TiO2 and TiO2-BCN samples, whereas the product of the dielectric constant and the density of donors was higher for TiO2-BCN.


2019 ◽  
Vol 10 ◽  
pp. 238-246 ◽  
Author(s):  
Arkadiusz Ciesielski ◽  
Lukasz Skowronski ◽  
Marek Trzcinski ◽  
Ewa Górecka ◽  
Wojciech Pacuski ◽  
...  

Noble metal nanolayers on flat substrates are often deposited with the use of semiconductor interlayers, which may strongly interact with the noble metal overlayer. We investigated the crystallinity, atomic concentration profile and optical parameters of ≈35 nm-thick silver and gold layers deposited on glass substrates with 2 nm-thick tellurium or selenium interlayers. Our study, based on X-ray reflectometry (XRR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and ellipsometric measurements, showed that using either of these interlayers introduces strain in nanocrystals of both plasmonic films. This, in turn, influences the migration of Se and Te into the metal layers. Selenium atoms migrate both in the silver and gold nanolayers, while tellurium atoms migrate only in silver. The Te concentration curve clearly suggests that this migration is an effect of the segregation of Te atoms in the silver structure. The differences in crystallinity, as well as the migration process, strongly influence the optical parameters of Ag and Au. In the permittivity of Ag deposited on either Te or Se, additional plasmonic bands originating from grain boundary segregation or diffusion occur, while for the Au layer, such resonances were not pronounced. In the permittivity of both materials, the intensity of the interband transition peaks is strongly altered, possibly due to the nano-alloy formation, but more likely due to the microstrain on metal grains.


2021 ◽  
Vol 11 (1) ◽  
Author(s):  
Bruna Teixeira da Fonseca ◽  
Eliane D’Elia ◽  
José Márcio Siqueira Júnior ◽  
Sanair Massafra de Oliveira ◽  
Kelly Leite dos Santos Castro ◽  
...  

AbstractThe SiO2/TiO2/Nb2O5 material was set by the sol–gel method and was characterized by several techniques through thermogravimetric, spectroscopic, and textural analyzes. For the two synthesized materials, the specific surface area was 350.0 and 494.0 m2 g−1 (SiTiNb-A and SiTiNb-B, respectively). An enhance of the crystalline order with the temperature increase of the thermal treatment was observed. Through X-ray Photoelectron Spectroscopy analysis, the binding energy values for the Ti 2p and Nb 3d levels showed the insertion of Ti and Nb atoms in the silica matrix. The Electron Dispersive Spectroscopy analyses also confirmed the high dispersion of the metals presented on the materials surface. The Thermogravimetric Analysis showed weight loss for the of 37.6% (SiTiNb-A) and 29.7% (SiTiNb-B). The presence of the crystalline phases TiO2-anatase and monoclinic-Nb2O5 in the materials was confirmed through the data obtained by association of powder X-ray Diffraction and FT-Raman. Values obtained from optical band-gap aimed the dependence of the oxides concentration and the calcination temperature. Finally, the pyridine adsorption studies have indicated the presence of Lewis and Brønsted acid sites.


2011 ◽  
Vol 1321 ◽  
Author(s):  
Balaji Rangarajan ◽  
Ihor Brunets ◽  
Peter Oesterlin ◽  
Alexey Y. Kovalgin ◽  
Jurriaan Schmitz

ABSTRACTGreen laser crystallization of a-Ge0.85Si0.15 films deposited using Low Pressure Chemical Vapour Deposition is studied. Large grains of 8x2 μm2 size were formed using a location-controlled approach. Characterization is done using Scanning Electron Microscopy, Atomic Force Microscopy, X-Ray Photoelectron Spectroscopy and X-Ray Diffraction.


2020 ◽  
Vol 73 (12) ◽  
pp. 1271
Author(s):  
Renata Lippi ◽  
Campbell J. Coghlan ◽  
Shaun C. Howard ◽  
Christopher D. Easton ◽  
Qinfen Gu ◽  
...  

Manganese-based metal–organic frameworks (MOFs) metalated with Rh were used as pre-catalysts for CO2 hydrogenation. Activated insitu (80% H2, 20% CO2, 350°C), the resulting templated catalysts displayed CO2 conversion of up to 20%, with CH4 as the main product. Used catalysts were compared with samples templated in 5% H2/Ar at 350°C using powder X-ray diffraction, electron microscopy, energy dispersive spectroscopy, and X-ray photoelectron spectroscopy. It was found that under reducing atmosphere Rh0 nanoparticles formed and organic MOF components decomposed, which allowed growth of MnO or MnCO3 and the formation of a mesh of catalytic Rh0 nanoparticles.


2003 ◽  
Vol 780 ◽  
Author(s):  
C. Essary ◽  
V. Craciun ◽  
J. M. Howard ◽  
R. K. Singh

AbstractHf metal thin films were deposited on Si substrates using a pulsed laser deposition technique in vacuum and in ammonia ambients. The films were then oxidized at 400 °C in 300 Torr of O2. Half the samples were oxidized in the presence of ultraviolet (UV) radiation from a Hg lamp array. X-ray photoelectron spectroscopy, atomic force microscopy, and grazing angle X-ray diffraction were used to compare the crystallinity, roughness, and composition of the films. It has been found that UV radiation causes roughening of the films and also promotes crystallization at lower temperatures.Furthermore, increased silicon oxidation at the interface was noted with the UVirradiated samples and was shown to be in the form of a mixed layer using angle-resolved X-ray photoelectron spectroscopy. Incorporation of nitrogen into the film reduces the oxidation of the silicon interface.


Polymers ◽  
2021 ◽  
Vol 13 (4) ◽  
pp. 581
Author(s):  
Gajanan S. Ghodake ◽  
Surendra K. Shinde ◽  
Ganesh D. Saratale ◽  
Rijuta G. Saratale ◽  
Min Kim ◽  
...  

The utilization of waste-paper-biomass for extraction of important α-cellulose biopolymer, and modification of extracted α-cellulose for application in enzyme immobilization can be extremely vital for green circular bio-economy. Thus, in this study, α-cellulose fibers were super-magnetized (Fe3O4), grafted with chitosan (CTNs), and thiol (-SH) modified for laccase immobilization. The developed material was characterized by high-resolution transmission electron microscopy (HR-TEM), HR-TEM energy dispersive X-ray spectroscopy (HR-TEM-EDS), X-ray diffraction (XRD), vibrating sample magnetometer (VSM), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FT-IR) analyses. Laccase immobilized on α-Cellulose-Fe3O4-CTNs (α-Cellulose-Fe3O4-CTNs-Laccase) gave significant activity recovery (99.16%) and laccase loading potential (169.36 mg/g). The α-Cellulose-Fe3O4-CTNs-Laccase displayed excellent stabilities for temperature, pH, and storage time. The α-Cellulose-Fe3O4-CTNs-Laccase applied in repeated cycles shown remarkable consistency of activity retention for 10 cycles. After the 10th cycle, α-Cellulose-Fe3O4-CTNs possessed 80.65% relative activity. Furthermore, α-Cellulose-Fe3O4-CTNs-Laccase shown excellent degradation of pharmaceutical contaminant sulfamethoxazole (SMX). The SMX degradation by α-Cellulose-Fe3O4-CTNs-Laccase was found optimum at incubation time (20 h), pH (3), temperatures (30 °C), and shaking conditions (200 rpm). Finally, α-Cellulose-Fe3O4-CTNs-Laccase gave repeated degradation of SMX. Thus, this study presents a novel, waste-derived, highly capable, and super-magnetic nanocomposite for enzyme immobilization applications.


Catalysts ◽  
2021 ◽  
Vol 11 (3) ◽  
pp. 346
Author(s):  
Sonam Goyal ◽  
Maizatul Shima Shaharun ◽  
Ganaga Suriya Jayabal ◽  
Chong Fai Kait ◽  
Bawadi Abdullah ◽  
...  

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.


Coatings ◽  
2021 ◽  
Vol 11 (8) ◽  
pp. 937
Author(s):  
Yingying Hu ◽  
Md Rasadujjaman ◽  
Yanrong Wang ◽  
Jing Zhang ◽  
Jiang Yan ◽  
...  

By reactive DC magnetron sputtering from a pure Ta target onto silicon substrates, Ta(N) films were prepared with different N2 flow rates of 0, 12, 17, 25, 38, and 58 sccm. The effects of N2 flow rate on the electrical properties, crystal structure, elemental composition, and optical properties of Ta(N) were studied. These properties were characterized by the four-probe method, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and spectroscopic ellipsometry (SE). Results show that the deposition rate decreases with an increase of N2 flows. Furthermore, as resistivity increases, the crystal size decreases, the crystal structure transitions from β-Ta to TaN(111), and finally becomes the N-rich phase Ta3N5(130, 040). Studying the optical properties, it is found that there are differences in the refractive index (n) and extinction coefficient (k) of Ta(N) with different thicknesses and different N2 flow rates, depending on the crystal size and crystal phase structure.


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