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| 2. |
- Carlsson, Per-Anders, 1972, et al.
(författare)
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A transient in situ FTIR and XANES study of CO oxidation over Pt/Al2O3 catalysts
- 2004
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 226:2, s. 422-434
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Tidskriftsartikel (refereegranskat)abstract
- We report experimental results for the oxidation of CO over supported Pt/Al2O3 catalysts operating in oxygen excess at atmospheric pressure. To study the reaction kinetics under transient conditions we have employed step changes of the O2 concentration by intermittently switching off the O2 supply at various temperatures ranging from 523 to 623 K. Detailed in situ FTIR and XANES data for CO coverage and the chemical state of Pt, respectively, are presented together with the CO conversion, which in both cases was monitored by mass spectrometry. A red-shift of the vibrational frequency of linearly bonded CO which correlates with a blue-shift of the Pt LIII binding energy indicates that the Pt catalyst initially is partially oxidised and gradually reduced when the O2 supply is switched off. Control experiments with a NO2 oxidised Pt/Al2O3 catalyst support these findings. A hysteresis in the catalytic activity due to the different rates whereby Pt is oxidised and reduced as a function of gas-phase composition is observed. The activation energy for the Pt oxide reduction (decomposition) process is estimated to be about 50 kJ/mol. The results further emphasise that the conventional three-step Langmuir-Hinshelwood (LH) scheme used to interpret CO oxidation on Pt surfaces must be complemented by a Pt oxidation and reduction mechanism during transient conditions. Moreover, FTIR data suggest that during the extinction, the partially oxidised platinum surface is reduced by chemisorbed CO which should be explicitly accounted for in the modeling of the reaction mechanism.
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| 3. |
- von Kraemer, Sophie, et al.
(författare)
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Evaluation of TiO2 as catalyst support in Pt-TiO2/C composite cathodes for the proton exchange membrane fuel cell
- 2008
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Ingår i: Journal of Power Sources. - : Elsevier BV. - 0378-7753 .- 1873-2755. ; 180:1, s. 185-190
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Tidskriftsartikel (refereegranskat)abstract
- Anatase TiO2 is evaluated as catalyst support material in authentic Pt-TiO2/C composite gas diffusion electrodes (GDEs), as a different approach in the context of improving the proton exchange membrane fuel cell (PEMFC) cathode stability. A thermal stability study shows high carbon stability as Pt nanoparticles are supported on TiO2 instead of carbon in the Pt-TiO2/C composite material, presumably due to a reduced direct contact between Pt and C. The performance of Pt-TiO2/C cathodes is investigated electrochemically in assembled membrane-electrode assemblies (MEAs) considering the added carbon fraction and Pt concentration deposited on TiO2. The O-2 reduction current for the Pt-TiO2 alone is expectedly low due to the low electronic conductivity in bulk TiO2. However, the Pt-TiO2/C composite cathodes show enhanced fuel cell cathode performance with growing carbon fraction and increasing Pt concentration deposited on TiO2. The proposed reasons for these observations are improved macroscopic and local electronic conductivity, respectively. Electron micrographs of fuel cell tested Pt-TiO2/C composite cathodes illustrate only a minor Pt migration in the Pt-TiO2/C structure, in which anatase TiO2 is used as Pt support. On the whole, the study demonstrates a stable Pt-TiO2/C Composite material possessing a performance comparable to conventional Pt-C materials when incorporated in a PEMFC cathode.
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| 4. |
- Arnby, Karl, 1974, et al.
(författare)
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The effect of platinum distribution in monolithic catalysts on the oxidation of CO and hydrocarbons
- 2005
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 233:1, s. 176-185
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Tidskriftsartikel (refereegranskat)abstract
- Monolithic Pt/gamma-Al2O3 catalysts were prepd. by depositing of the platinum phase, either homogeneously or heterogeneously (i.e., local high platinum concn.), in the washcoat. The influence of the platinum distribution on the ignition and extinction processes for oxidn. of CO, propene, and propane, resp., was investigated by both temp.-programmed and oxygen step-response flow-reactor expts. In addn., in situ XANES spectroscopy was used to follow changes in the chem. state of platinum during propane oxidn. For samples with heterogeneous platinum distribution, the results show an improved low-temp. activity for CO oxidn., whereas no clear improvement is obsd. for oxidn. of propene or propane. Comparison of the results for CO and hydrocarbon oxidn. shows that the improved activity cannot be explained by thermal effects. Moreover, calcns. indicate that the enhanced activity for CO oxidn. can be due to mass-transfer phenomena. This could not be confirmed by our expts., however. Instead, the improved activity for CO oxidn. can be due to varying platinum particle size between the samples. Furthermore, the oxidn. of propane is shown to be highly influenced by the oxygen concn., showing an activity max. for gas compositions close to the stoichiometric. High oxygen levels result most probably in a predominantly oxygen-covered surface, which inhibits the reaction and, as supported by the in situ XANES experiments, passivates the surface by forming platinum oxide.
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| 7. |
- Björkegren, Sanna, 1984, et al.
(författare)
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Surface activity and flocculation behavior of polyethylene glycol-functionalized silica nanoparticles
- 2015
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Ingår i: Journal of Colloid and Interface Science. - : Elsevier BV. - 1095-7103 .- 0021-9797. ; 452, s. 215-223
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Tidskriftsartikel (refereegranskat)abstract
- Colloidal silica nanoparticles have been functionalized with methyl polyethylene glycol silane (mPEG silane) and the PEGylated particles have been characterized with focus on exploring their surface chemical properties. The degree of surface functionalization was quantified using NMR diffusometry, and the measurements showed that the silane binds covalently to the silica surface. Samples with surface coverages ranging from 0.068 to 0.315 gmol silane/m(2) have been analyzed. The functionalized particles proved to be surface active and showed a significant reduction in surface charge and zeta potential with increasing degree of PEG functionalization. All samples showed colloidal stability at neutral pH and above within the range studied. At lower pH, the samples with low surface coverage displayed a reversible flocculation behavior, while samples with a high surface coverage and samples without functionalization remained stable. This suggests that steric stabilization is effective at low pH when the surface coverage is high enough; electrostatic stabilization is effective for samples without functionalization; and that inter-particle PEG-silica interactions cause flocculation of particles with too low degrees of PEG functionalization.
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| 8. |
- Saramat, Ali, 1977, et al.
(författare)
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Thermoelectric Properties of YMn4+xAl8-x, -2 ≤ x ≤ 2.5
- 2009
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Ingår i: Journal of Alloys and Compounds. - : Elsevier BV. - 0925-8388. ; 477:1-2, s. 51-54
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Tidskriftsartikel (refereegranskat)abstract
- Seven samples within the series YMn 4+x Al 8 - x (-2.0 ≤ x ≤ 2.5) were synthesized using direct reaction of the elements. The thermoelectric properties of the samples were characterized by measurements of resistivity, thermal conductivity and thermopower. According to transport measurements, slight Mn-deficiency influences the electronic conductivity of the YMn 4+x Al 8 - x system, implying that the electronic structure is marginal to the metal-semiconductor boundary. Furthermore, the ZT values of the samples prepared in this study were low. Experimental results indicated that structurally ordered YMn 4 Al 8 shows metallic conductivity, whereas off-stoichiometric compounds displayed semiconductor-like behavior, at low temperatures. © 2008 Elsevier B.V. All rights reserved.
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| 9. |
- Zhang, Yifei, 1992, et al.
(författare)
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Investigating the Chemical Ordering in Quaternary Clathrate Ba₈AlₓGa₁₆₋ₓGe₃₀
- 2021
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 60:22, s. 16977-16985
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Tidskriftsartikel (refereegranskat)abstract
- Recently, there has been an increased interest in quaternary clathrate systems as promising thermoelectric materials. Because of their increased complexity, however, the chemical ordering in the host framework of quaternary clathrates has not yet been comprehensively analyzed. Here, we have synthesized a prototypical quaternary type-I clathrate Ba8AlxGa16-xGe30 by Czochralski and flux methods, and we employed a combination of X-ray and neutron diffraction along with atomic scale simulations to investigate chemical ordering in this material. We show that the site occupancy factors of trivalent elements at the 6c site differ, depending on the synthesis method, which can be attributed to the level of equilibration. The flux-grown samples are consistent with the simulated high-temperature disordered configuration, while the degree of ordering for the Czochralski sample lies between the ground state and the high-temperature state. Moreover, we demonstrate that the atomic displacement parameters of the Ba atoms in the larger tetrakaidecahedral cages are related to chemical ordering. Specifically, Ba atoms are either displaced toward the periphery or localized at the cage centers. Consequently, this study reveals key relationships between the chemical ordering in the quaternary clathrates Ba8AlxGa16-xGe30 and the structural properties, thereby offering new perspectives on designing these materials and optimizing their thermoelectric properties.
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| 10. |
- Cederkrantz, Daniel, 1979, et al.
(författare)
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Enhanced thermoelectric properties of Mg2Si by addition of TiO2 nanoparticles
- 2012
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Ingår i: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 111:2
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Tidskriftsartikel (refereegranskat)abstract
- The effects on the thermoelectric properties of Mg2Si when adding TiO2 nanoparticles have been evaluated experimentally. A batch of Mg2Si was prepared through direct solid state reaction and divided into portions which were mechanically mixed with different amounts of TiO2 nanoparticles ranging from 0.5 to 3 vol% and subsequently sintered to disks. All materials showed n-type conduction and the absolute value of the Seebeck coefficient was reduced with increasing amount of TiO2 added, while the electrical resistivity was greatly reduced. The thermal conductivity was surprisingly little affected by the addition of the nanoparticles. An optimum value of the thermoelectric figure-of-merit ZT = TS2 sigma/k was found for the addition of 1 vol% TiO2, showing almost three times higher ZT value than that of the pure Mg2Si. Larger TiO2 additions resulted in lower ZT values and with 3 vol% added TiO2 the ZT was comparable to the pure Mg2Si. The sintering process resulted in reduction or chemical reaction of all TiO2 to TiSi2 and possibly elemental titanium as well as reduced TiOx. The increased electrical conductivity and the decreased Seebeck coefficient were found due to an increased charge carrier concentration, likely caused by the included compounds or titanium-doping of the Mg2Si matrix. The low observed effect on the thermal conductivity of the composites may be explained by the relatively higher thermal conductivity of the included compounds, counter-balancing the expected increased grain boundary scattering. Alternatively, the introduction of compounds does not significantly increase the concentration of scattering grain boundaries.
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