scholarly journals CO Total and Preferential Oxidation over Stable Au/TiO2 Catalysts Derived from Preformed Au Nanoparticles

Catalysts ◽  
2020 ◽  
Vol 10 (9) ◽  
pp. 1028
Author(s):  
Núria J. Divins ◽  
Eduardo López ◽  
Inmaculada Angurell ◽  
Stefan Neuberg ◽  
Ralf Zapf ◽  
...  

CO preferential oxidation (PROX) is an effective method to clean reformate H2 streams to feed low-temperature fuel cells. In this work, the PROX and CO oxidation reactions were studied on preformed Au nanoparticles (NPs) supported on TiO2 anatase. Preformed Au NPs were obtained from gold cores stabilized by dodecanethiols or trimethylsilane-dendrons. A well-controlled size of ca. 2.6 nm and narrow size distributions were achieved by this procedure. The catalysts were characterized by high-resolution transmission electron microscopy and ex situ and in situ X-ray photoelectron spectroscopy (XPS). The XPS results showed that the preformed Au NPs exhibited high thermal stability. The different ligand-derived Au catalysts, as well as a conventional gold catalyst for comparison purposes, were loaded onto cordierite supports with 400 cells per square inch. The activity and selectivity of the samples were evaluated for various operation conditions. The catalyst prepared using dodecanethiol-capped Au NPs showed the best performance. In fact, CO conversions of up to 70% at 40% CO2 selectivity and 90% O2 conversion were observed operating at 363 K in H2-rich atmospheres. The performance of the best catalysts was subsequently tested on stainless steel microreactors. A 500-hour stability test was carried out under a real post-reformate stream, including 18 vol.% CO2 and 29 vol.% H2O. A mean CO conversion of ca. 24% was measured for the whole test operating at 453 K and a gas hourly space velocity (GHSV) of 1.3 × 104 h−1. These results reveal our dodecanethiol- and carbosilane-derived Au catalysts as extremely promising candidates to conduct a PROX reaction while avoiding deactivation, which is one of the major drawbacks of Au/TiO2 catalysts.

Micromachines ◽  
2019 ◽  
Vol 10 (4) ◽  
pp. 254 ◽  
Author(s):  
Yuxiang Yan ◽  
Hua Yang ◽  
Zao Yi ◽  
Ruishan Li ◽  
Xiangxian Wang

Using P25 as the titanium source and based on a hydrothermal route, we have synthesized CaTiO3 nanocuboids (NCs) with the width of 0.3–0.5 μm and length of 0.8–1.1 μm, and systematically investigated their growth process. Au nanoparticles (NPs) of 3–7 nm in size were assembled on the surface of CaTiO3 NCs via a photocatalytic reduction method to achieve excellent Au@CaTiO3 composite photocatalysts. Various techniques were used to characterize the as-prepared samples, including X-ray powder diffraction (XRD), scanning/transmission electron microscopy (SEM/TEM), diffuse reflectance spectroscopy (UV-vis DRS), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). Rhodamine B (RhB) in aqueous solution was chosen as the model pollutant to assess the photocatalytic performance of the samples separately under simulated-sunlight, ultraviolet (UV) and visible-light irradiation. Under irradiation of all kinds of light sources, the Au@CaTiO3 composites, particularly the 4.3%Au@CaTiO3 composite, exhibit greatly enhanced photocatalytic performance when compared with bare CaTiO3 NCs. The main roles of Au NPs in the enhanced photocatalytic mechanism of the Au@CaTiO3 composites manifest in the following aspects: (1) Au NPs act as excellent electron sinks to capture the photoexcited electrons in CaTiO3, thus leading to an efficient separation of photoexcited electron/hole pairs in CaTiO3; (2) the electromagnetic field caused by localized surface plasmon resonance (LSPR) of Au NPs could facilitate the generation and separation of electron/hole pairs in CaTiO3; and (3) the LSPR-induced electrons in Au NPs could take part in the photocatalytic reactions.


2020 ◽  
Author(s):  
Jennifer A. Rudd ◽  
Ewa Kazimierska ◽  
Louise B. Hamdy ◽  
Odin Bain ◽  
Sunyhik Ahn ◽  
...  

The utilization of carbon dioxide is a major incentive for the growing field of carbon capture. Carbon dioxide could be an abundant building block to generate higher value products. Herein, we describe the use of porous copper electrodes to catalyze the reduction of carbon dioxide into higher value products such as ethylene, ethanol and, notably, propanol. For <i>n</i>-propanol production, faradaic efficiencies reach 4.93% at -0.83 V <i>vs</i> RHE, with a geometric partial current density of -1.85 mA/cm<sup>2</sup>. We have documented the performance of the catalyst in both pristine and urea-modified foams pre- and post-electrolysis. Before electrolysis, the copper electrode consisted of a mixture of cuboctahedra and dendrites. After 35-minute electrolysis, the cuboctahedra and dendrites have undergone structural rearrangement. Changes in the interaction of urea with the catalyst surface have also been observed. These transformations were characterized <i>ex-situ</i> using scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. We found that alterations in the morphology, crystallinity, and surface composition of the catalyst led to the deactivation of the copper foams.


Author(s):  
Xinyue Li ◽  
Marco Fortunato ◽  
Anna Maria Cardinale ◽  
Angelina Sarapulova ◽  
Christian Njel ◽  
...  

AbstractNickel aluminum layered double hydroxide (NiAl LDH) with nitrate in its interlayer is investigated as a negative electrode material for lithium-ion batteries (LIBs). The effect of the potential range (i.e., 0.01–3.0 V and 0.4–3.0 V vs. Li+/Li) and of the binder on the performance of the material is investigated in 1 M LiPF6 in EC/DMC vs. Li. The NiAl LDH electrode based on sodium alginate (SA) binder shows a high initial discharge specific capacity of 2586 mAh g−1 at 0.05 A g−1 and good stability in the potential range of 0.01–3.0 V vs. Li+/Li, which is better than what obtained with a polyvinylidene difluoride (PVDF)-based electrode. The NiAl LDH electrode with SA binder shows, after 400 cycles at 0.5 A g−1, a cycling retention of 42.2% with a capacity of 697 mAh g−1 and at a high current density of 1.0 A g−1 shows a retention of 27.6% with a capacity of 388 mAh g−1 over 1400 cycles. In the same conditions, the PVDF-based electrode retains only 15.6% with a capacity of 182 mAh g−1 and 8.5% with a capacity of 121 mAh g−1, respectively. Ex situ X-ray photoelectron spectroscopy (XPS) and ex situ X-ray absorption spectroscopy (XAS) reveal a conversion reaction mechanism during Li+ insertion into the NiAl LDH material. X-ray diffraction (XRD) and XPS have been combined with the electrochemical study to understand the effect of different cutoff potentials on the Li-ion storage mechanism. Graphical abstract The as-prepared NiAl-NO3−-LDH with the rhombohedral R-3 m space group is investigated as a negative electrode material for lithium-ion batteries (LIBs). The effect of the potential range (i.e., 0.01–3.0 V and 0.4–3.0 V vs. Li+/Li) and of the binder on the material’s performance is investigated in 1 M LiPF6 in EC/DMC vs. Li. Ex situ X-ray photoelectron spectroscopy (XPS) and ex situ X-ray absorption spectroscopy (XAS) reveal a conversion reaction mechanism during Li+ insertion into the NiAl LDH material. X-ray diffraction (XRD) and XPS have been combined with the electrochemical study to understand the effect of different cutoff potentials on the Li-ion storage mechanism. This work highlights the possibility of the direct application of NiAl LDH materials as negative electrodes for LIBs.


2020 ◽  
Vol 9 (1) ◽  
pp. 734-743
Author(s):  
Ran Zhao ◽  
ZiChen Tian ◽  
Zengwu Zhao

AbstractBayan Obo tailings are rich in rare earth elements (REEs), iron, and other catalytic active substances. In this study, mine tailings were calcined at different temperatures and tested for the catalytic combustion of low-concentration methane. Upon calcination at 600°C, high catalytic activity was revealed, with 50% CH4 conversion at 587°C (space velocity of 12,000 mL/g h). The physicochemical properties of catalysts were characterized using thermogravimetric analysis, X-ray diffraction, scanning electron microscopy, hydrogen temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS). Compared to the raw ore sample, the diffraction peak intensity of Fe2O3 increased post calcination, whereas that of CeCO3F decreased. A porous structure appeared after the catalyst was calcined at 600°C. Additionally, Fe, Ce, Ti, and other metal elements were more highly dispersed on the catalyst surface. H2-TPR results revealed a broadening of the reduction temperature range for the catalyst calcined at 600°C and an increase in the reduction peak. XPS analysis indicated the presence of Ce in the form of Ce3+ and Ce4+ oxidation states and the coexistence of Fe in the form of Fe2+ and Fe3+. Moreover, XPS revealed a higher surface Oads/Olatt ratio. This study provides evidence for the green reuse of Bayan Obo mine tailings in secondary resources.


Polymers ◽  
2021 ◽  
Vol 13 (13) ◽  
pp. 2142
Author(s):  
Shengjun Wang ◽  
Jiaqi Guo ◽  
Yibo Ma ◽  
Alan X. Wang ◽  
Xianming Kong ◽  
...  

The flexible SERS substrate were prepared base on regenerated cellulose fibers, in which the Au nanoparticles were controllably assembled on fiber through electrostatic interaction. The cellulose fiber was regenerated from waste paper through the dry-jet wet spinning method, an eco-friendly and convenient approach by using ionic liquid. The Au NPs could be controllably distributed on the surface of fiber by adjusting the conditions during the process of assembling. Finite-difference time-domain theoretical simulations verified the intense local electromagnetic fields of plasmonic composites. The flexible SERS fibers show excellent SERS sensitivity and adsorption capability. A typical Raman probe molecule, 4-Mercaptobenzoicacid (4-MBA), was used to verify the SERS cellulose fibers, the sensitivity could achieve to 10−9 M. The flexible SERS fibers were successfully used for identifying dimetridazole (DMZ) from aqueous solution. Furthermore, the flexible SERS fibers were used for detecting DMZ from the surface of fish by simply swabbing process. It is clear that the fabricated plasmonic composite can be applied for the identifying toxins and chemicals.


2001 ◽  
Vol 696 ◽  
Author(s):  
R. Würz ◽  
W. Bohne ◽  
W. Fuhs ◽  
J. Röhrich ◽  
M. Schmidt ◽  
...  

AbstractCaF2 films with thicknesses in the monolayer range (<20 Å) were grown on Si(111) by evaporation from a CaF2 source at UHV conditions. They were characterized ex-situ by Heavy-Ion Elastic Recoil Detection Analysis (HI-ERDA), RBS/Channeling, X-ray Photoelectron Spectroscopy (XPS) and Atomic Force Microscopy (AFM). The F/Ca ratio of the films was found to depend on the growth temperature Ts and to deviate appreciably from the stoichiometric composition (F/Ca=2). Due to an interface reaction which leads to a CaF-interface layer a change from polycrystalline to epitaxial growth occurs at Ts=450°C. At higher temperature film growth started with a closed layer of CaF on top of which CaF2 layers with an increasing fraction of pinholes were formed. By means of a two-step process at different temperatures, the amount of pinholes could be strongly reduced. It was found, that buffer layers of CaF2 with a CaF interface layer introduced in Au/p-Si contacts enhance the barrier height by as much as 0.36eV to values of 0.64eV.


1995 ◽  
Vol 416 ◽  
Author(s):  
L. C. Chen ◽  
C. C. Juan ◽  
J. Y. Wu ◽  
K. H. Chen ◽  
J. W. Teng

ABSTRACTNear-single-crystal diamond films have been obtained in a number of laboratories recently. The optimization of nucleation density by using a bias-enhanced nucleation (BEN) method is believed to be a critical step. However, the condition of optimized nucleation has never been clearly delineated. In the present report, a novel quantitative technique was established to monitor the nucleation of diamond in-situ. Specifically, the induced current was measured as a function of nucleation time during BEN. The timedependence of induced current was studied under various methane concentrations as well as substrate temperatures. The optimized nucleation condition can be unambiguously determined from the current-time plot. Besides the in-situ current probe, ex-situ x-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM) were also used to investigate the chemical and morphological evolution. Characteristic XPS and AFM features of optimized nucleation is discussed.


2012 ◽  
Vol 1376 ◽  
Author(s):  
P. Silva-Bermudez ◽  
S. Muhl ◽  
M. Rivera ◽  
S. E. Rodil

ABSTRACTIn the present work, the adsorption of albumin and fibrinogen on Ta, Nb, Ti and Zr oxidesthin films deposited on Si (100) wafers by magnetron sputtering was studied in order to get a better understanding of the correlation among the surface properties of these oxides and the protein adsorption phenomena on their surfaces. The surface energy, hydrophobicity, chemical composition, roughness and atomic order of the films were characterized. The films were immersedfor 45 minutes in single protein solutions; either albumin or fibrinogenand the adsorbed protein layer on the films was studied ex-situ in a dry ambient using bothX-ray photoelectron spectroscopy and atomic force microscopy.The adsorption of albumin and fibrinogen on the films modified the surface morphology and decreased the surface roughness for all the four different metal oxides. The XPS results confirmed the presence of the protein on the surface of the films and showed that the two proteins studied were adsorbed without undergoing a major chemical decomposition. A correlation between the surface roughness,the polar component of the surface energy of the films and the atomic percentage of nitrogen on the films after protein adsorption, an indirect signal of the amount of protein adsorbed, was found for albumin and fibrinogen adsorption on Ta, Nb and Ti oxides; the largest the roughness or the polar component the largest amount of adsorbed protein.


2009 ◽  
Vol 1171 ◽  
Author(s):  
Marco Bonato ◽  
Kristin Vala Ragnarsdottir ◽  
Geoffrey C. Allen

AbstractTiO2 anatase nanotubes synthesised via anodic oxidation were used as adsorbent for the uptake of U and Pb from aqueous solution and the photoremoval of As(III). An X-ray photoelectron spectroscopy study of the sorbent medium surface revealed a high adsorption of U and Pb at pH 8. The adsorption of the uranyl ion was enhanced in an anoxy (N2) atmosphere, because this prevents the formation of very stable carbonyl complexes. As(III) was adsorbed on TiO2 but in the presence of O2 and UV light was oxidized to As(V). XPS analysis revealed that in the pH range 3-9 As(V) was always the major species detected at the surface of the titania photocatalyst.


2021 ◽  
Vol 314 ◽  
pp. 23-28
Author(s):  
Seungjun Oh ◽  
Sunyoung Lee ◽  
Heehwan Kim ◽  
Donggeon Kwak ◽  
Chulwoo Bae ◽  
...  

Technological control over ultra-trace level contaminants is important for semiconductor development. Despite technological developments, defects remain in the single wafer wet cleaning process. In this paper, the source of the contamination is explained via trace analytical methods. Fluorine resin materials of polytetrafluoroethylene (PTFE) and ethylene tetrafluoroethylene (ETFE) are commonly used in semiconductor equipment. Isopropyl alcohol (IPA) oxidation reactions occur at high temperature below the boiling point due to impurities. IPA changed to different alcohol forms from gas chromatography (GCMS) analysis. The oxygen concentration in the X-ray photoelectron spectroscopy (XPS) results increased and formed new bonds in IPA with fluorine resin. These reactions confirmed that cations were a catalyst from the time-of-flight secondary ion mass spectrometry (TOF-SIMS) results. Representative ions were Fe+, K+, and Na+ with different concentrations for each material.


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