| 1. |
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| 2. |
- 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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| 3. |
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| 4. |
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| 5. |
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| 6. |
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| 7. |
- Berggrund, Malin, 1966, et al.
(författare)
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Influence of Synthesis Conditions for ZSM-5 on the Hydrothermal Stability of Cu-ZSM-5
- 2009
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Ingår i: Catalysis Letters. - : Springer Science and Business Media LLC. - 1572-879X .- 1011-372X. ; 130:1-2, s. 79-85
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Tidskriftsartikel (refereegranskat)abstract
- The influence of syntheses parameters of zeolite ZSM-5 on the lean NO (x) reduction activity and hydrothermal stability of Cu-ZSM-5 has been investigated. The hydrothermal stability of Cu-ZSM-5 was found to depend on the aluminium source used and on the presence of Ca(OH)(2) in the synthesis mixture for ZSM-5.
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| 8. |
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| 9. |
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| 10. |
- 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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| 11. |
- 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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| 12. |
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| 13. |
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| 14. |
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| 15. |
- 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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| 16. |
- 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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| 17. |
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| 18. |
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| 19. |
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| 20. |
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| 21. |
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| 22. |
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| 23. |
- Andersson, Martin, 1974, et al.
(författare)
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Use of Self-Assembled Surfactants for Nanomaterials Synthesis
- 2009
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Ingår i: Particulate Systems in Nano- and Biotechnologies. ; , s. 27-51
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Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- Synthesis of inorganic materials with nanosized dimensions can take advantage of the ability of surfactants to self-assemble into well-defined structures. These structures are used as a kind of template for the synthesis. This approach of nanomaterials preparation has triggered substantial interest both in the surface chemistry and the materials chemistry community. The accuracy and reproducibility of the self-assembly process has been seen as means of achieving control of materials architecture on the nanometer scale. This is a biomimetic approach; a wide variety of biological structural materials are made by a templating process with the use of surface active compounds—primarily surface active polymers but also low molecular weight polar lipids. The number of papers dealing with surfactant-templated synthesis of inorganic materials has increased dramatically in recent years and several review papers deal with various aspects of the technique (1-12). Existing and potential applications for the synthesized materials range from biomaterials (e.g., artificial bone), to technical products such as catalysts, magnetic particles, and pigments.
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| 24. |
- Bergek, Jonatan, 1984, et al.
(författare)
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Formation of titanium dioxide core-shell microcapsules through a binary-phase spray technique
- 2017
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Ingår i: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9084 .- 1463-9076. ; 19:35, s. 23878-23886
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Tidskriftsartikel (refereegranskat)abstract
- Core-shell microcapsules consisting of a titanium dioxide shell and a hydrophobic solvent core have been prepared with diameters of a few micrometers and a narrow size distribution using a simple and fast airbrush technique. These microcapsules were prepared at room temperature in a single-step process in which an oil with a dissolved titanium alkoxide precursor was forced together with an aqueous solution, containing a surface-active polymer, through a narrow spray nozzle using a nitrogen gas propellant. Several different parameters of chemical, physical, and processing origin were investigated to find an optimal recipe. Two different alkanes, one ketone, and four alcohols were tested and evaluated as core materials, alone or together with the antifungal biocide 2-n-octyl-4-isothiazolin-3-one (OIT). Long-chain alcohols were found suitable as core oil due to their low solubility in water and surface activity. The addition of the surface-active polymers in the water phase was important in aiding the formation and stabilization of the titanium dioxide shell. An impressive loading of 50 wt%of the semi-hydrophobic OIT was possible to encapsulate using this simple and applicable procedure.
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| 25. |
- Berggren, Andreas, 1979, et al.
(författare)
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Particle Size Control in Colloidal Suspensions of Mesostructured Silica
- 2008
-
Ingår i: Journal of Physical Chemistry C. ; 112:3, s. 732-737
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Tidskriftsartikel (refereegranskat)abstract
- Stable colloidal suspensions of ordered mesostructured silica have been prepared in a concentrated reaction solution under mild acidic conditions using an inorganic silica source and Pluronic P123. This synthesis method results in a high yield, and it is also suitable for studies of formation and growth mechanisms of colloidal mesostructured silica particles. The size of the obtained particles can be controlled within the range of 50−300 nm by varying the amount of water used in the synthesis or addition of salt to the synthesis solution. The pH of the solution is important since it affects the mesoorder of the material, colloidal stability, and product yield. Ordered material was obtained at pH 1.7−5, whereas stable colloidal suspensions were obtained in the range 3−8. A mechanism for formation of the colloidal particles based on a burst nucleation process followed by growth through aggregation is also proposed.
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| 26. |
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| 27. |
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| 28. |
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| 29. |
- Björkegren, Sanna, 1984, et al.
(författare)
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Clouding observed for surface active, mPEG-grafted silica nanoparticles
- 2019
-
Ingår i: RSC Advances. - : Royal Society of Chemistry (RSC). - 2046-2069. ; 9:23, s. 13297-13303
-
Tidskriftsartikel (refereegranskat)abstract
- Temperature-dependent phase-separation, clouding, has been observed in suspensions of silica nanoparticles surface-functionalized with methyl-poly(ethylene glycol) silane. Interparticle interactions and conformational changes of the grafted poly(ethylene glycol) chains influence the observed cloud points, and can be controlled by electrolyte concentration and pH. These findings open new routes to tailoring properties of Pickering emulsions.
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| 30. |
- Björkegren, Sanna, 1984, et al.
(författare)
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Hydrophilic and hydrophobic modifications of colloidal silica particles for Pickering emulsions
- 2017
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Ingår i: Journal of Colloid and Interface Science. - : Elsevier BV. - 1095-7103 .- 0021-9797. ; 487, s. 250-257
-
Tidskriftsartikel (refereegranskat)abstract
- Colloidal silica particles, functionalized with hydrophilic and hydrophobic groups, have been studied for utilization in particle-stabilized emulsions, so called Pickering emulsions. The amounts of attached groups have been characterized using NMR spectroscopy and elemental analysis. A range of particles were prepared, with sizes from around 13 to 70 nm in diameter. Hydrophilic functionalization of the silica sols was achieved by attaching methyl poly(ethylene glycol) (mPEG) silane to the silica particle surface. This provides a reduction of surface charge density, a pH dependent and controllable flocculation behavior and surface activity. The hydrophobic functionalization of the silica sols was accomplished by attaching organosilanes containing mainly propyl and methyl groups. The emulsification abilities were evaluated by preparing Pickering emulsions using particles, with varying degrees and combinations of surface functionalization, as stabilizers and comparing the obtained emulsion droplet size distributions. It was found that colloidal silica functionalized with hydrophobic groups produced emulsions with smaller droplets compared to using unmodified silica. The emulsification performance was further improved by the combination of both hydrophilic and hydrophobic groups. All particles having this heterogeneous modification were found to generate emulsions with high stability towards coalescence (from five weeks to 1.5 years).
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| 31. |
- Björkegren, Sanna, 1984, et al.
(författare)
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Phase Inversions Observed in Thermoresponsive Pickering Emulsions Stabilized by Surface Functionalized Colloidal Silica
- 2020
-
Ingår i: Langmuir. - : American Chemical Society (ACS). - 1520-5827 .- 0743-7463. ; 36:9, s. 2357-2367
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Tidskriftsartikel (refereegranskat)abstract
- In this study, the emulsification performance of functionalized colloidal silica is explored with the aim to achieve phase inversion of particle-stabilized (Pickering) emulsion systems. An increased understanding of inversion conditions can facilitate surfactant-free emulsion fabrication and expand its use in industrial applications. Phase inversion was achieved by adjusting the temperature but without changing the composition of the emulsion formulation. Silica nanoparticles modified with hydrophobic propyl groups and hydrophilic methyl poly(ethylene)glycol (mPEG) groups are used as emulsifiers, enabling control of the wettability of the particles and exploration of phase inversion phenomena, the latter due to the thermoresponsiveness of the attached PEG chains. The phase inversion conditions as well as the reversibility of the emulsion systems were examined at varying electrolyte concentrations and pH values of the suspensions. Transitional phase inversions, from oil-in-water and water-in-oil and back, were observed in functionalized silica particle-stabilized butanol emulsions at distinct temperatures. The phase inversion temperature was affected by electrolyte concentration and pH conditions due to salting-out effects, PEG-silica interactions, and the effects of the particle surface charge. Investigations of phase inversion conditions, temperature, and hysteresis effects in Pickering emulsions can improve the theoretical understanding of these phenomena and facilitate the implementation of low-energy emulsion preparation.
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| 32. |
- Brorsson, Joakim, 1988, et al.
(författare)
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First-Principles Study of Order-Disorder Transitions in Pseudobinary Clathrates
- 2021
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 125:41, s. 22817-22826
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Tidskriftsartikel (refereegranskat)abstract
- It has been recently demonstrated that the pseudoternary Ba8AlxGayGe46-x-y clathrate undergoes an order-disorder transition with increasing temperature that can be observed via site occupation factors (SOFs) and manifests itself, e.g., in electrical transport properties. Here, we generalize this result and analyze the characteristics of this order-disorder transition in the pseudobinary clathrates Ba8GaxGe46-x, Ba8GaxSi46-x, Ba8AlxGe46-x, and Ba8AlxSi46-x. To this end, we employ atomistic simulations that combine alloy cluster expansions trained against density functional theory calculations with Wang-Landau and ensemble Monte Carlo simulations. The simulations show that all four systems studied here display order-disorder transitions for at least some composition range. Based on an extensive literature survey, we also provide evidence for signatures of the transition in earlier experimental studies that to the best of our knowledge have hitherto not been related to such transitions. The predicted transition temperatures are lower for Ba8GaxGe46-x and Ba8GaxSi46-x than for Ba8AlxGe46-x and Ba8AlxSi46-x, although it appears that the simulations underestimate the transition temperatures for Ga-containing systems compared to the experiment. This nonetheless provides a sensible explanation for why the experimentally determined Al SOFs agree better with the simulated higherature disordered configurations, while the Ga SOFs more closely agree with the simulated ground-state configurations. As a result of stronger interactions, the SOFs vary substantially, especially near the stoichiometric 16:30 composition, providing an indication of why it has proved difficult to synthesize Ba8AlxGe46-x and Ba8AlxSi46-x samples at this ratio. The present study thereby yields detailed atomic-scale insights into the ordering in inorganic clathrates that, given the connection to transport properties established earlier, are not only useful from a fundamental perspective but also relevant for applications.
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| 33. |
- Brorsson, Joakim, 1988, et al.
(författare)
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Order-Disorder Transition in Inorganic Clathrates Controls Electrical Transport Properties
- 2021
-
Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 1520-5002 .- 0897-4756. ; 33:12, s. 4500-4509
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Tidskriftsartikel (refereegranskat)abstract
- Inorganic clathrates have been extensively investigated owing to their unique and intriguing atomic structure as well as their potential as thermoelectric materials. The connection between the chemical ordering and the physical properties has, however, remained elusive. Here, this relation is uncovered through a combination of first-principles calculations, atomistic simulations, and experimental measurements of thermodynamic as well as electrical transport properties. This approach is, specifically, used to reveal the existence of an order-disorder transition in the quaternary clathrate series Ba8AlxGa16-xGe30. The results, furthermore, demonstrate that this phenomenon is responsible for the discontinuity in the heat capacity that has been observed previously. Moreover, the unusual temperature dependence of both Seebeck coefficient and electrical conductivity can be fully explained by the alterations of the band structure brought about by the phase transformation. It is finally argued that the phenomenology described here is not limited to this particular material but should be present in a wide range of inorganic clathrates and could even be observed in other materials that exhibit chemical ordering on at least one sublattice.
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| 34. |
- Brorsson, Joakim, 1988, et al.
(författare)
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Strategic Optimization of the Electronic Transport Properties of Pseudo-Ternary Clathrates
- 2022
-
Ingår i: Advanced Electronic Materials. - : Wiley. - 2199-160X .- 2199-160X. ; 8:3
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Tidskriftsartikel (refereegranskat)abstract
- While alloying is a powerful handle for materials engineering, it is an ongoing challenge to navigate the large and complex parameter space of these materials. This applies in particular for thermoelectrics and even more so clathrates. Here, a combination of density functional theory calculations, alloy cluster expansions, Monte Carlo simulations, and Boltzmann transport theory calculations is used to identify compositions that yield high power factors in the pseudo-ternary clathrates Ba8AlxGayGe46−x−y and Ba8GaxGeySi46−x−y, while accounting for weight and raw material costs. The results show how a cost-efficient performance can be achieved by reducing the number of Al and Ga atoms per unit cell, while compensating the resulting increase in the carrier concentration via an extrinsic dopant. The approach used in this study is transferable and can be a useful tool for mapping the thermodynamic and transport properties of other multinary systems.
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| 35. |
- Brown, D. R., et al.
(författare)
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Relating phase transition heat capacity to thermal conductivity and effusivity in Cu2Se
- 2016
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Ingår i: Physica Status Solidi - Rapid Research Letetrs. - : Wiley. - 1862-6254 .- 1862-6270. ; 10:8, s. 618-621
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Tidskriftsartikel (refereegranskat)abstract
- Accurate measurement of thermal conductivity is essential to determine the thermoelectric figure-of-merit, zT. Near the phase transition of Cu2Se at 410 K, the transport properties change rapidly with temperature, and there is a concurrent peak in measured heat capacity from differential scanning calorimetry (DSC). Interpreting the origin as a broad increase in heat capacity or as a transient resulted in a three-fold difference in the reported zT in two recent publications. To resolve this discrepancy, thermal effusivity was deduced from thermal conductivity and diffusivity measurements via the transient plane source (TPS) method and compared with that calculated from thermal diffusivity and the two interpretations of the DSC data for heat capacity. The comparison shows that the DSC measurement gave the heat capacity relevant for calculation of the thermal conductivity of Cu2Se. The thermal conductivity calculated this way follows the electronic contribution to thermal conductivity closely, and hence the main cause of the zT peak is concluded to be the enhanced Seebeck coefficient.
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| 36. |
- Calcagno, Giulio, 1990, et al.
(författare)
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Effect of Nitrogen Doping on the Performance of Mesoporous CMK-8 Carbon Anodes for Li-Ion Batteries
- 2020
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Ingår i: Energies. - : MDPI AG. - 1996-1073 .- 1996-1073. ; 13:19
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Tidskriftsartikel (refereegranskat)abstract
- Designing carbonaceous materials with heightened attention to the structural properties such as porosity, and to the functionalization of the surface, is a growing topic in the lithium-ion batteries (LIBs) field. Using a mesoporous silica KIT-6 hard template, mesoporous carbons belonging to the OMCs (ordered mesoporous carbons) family, namely 3D cubic CMK-8 and N-CMK-8 were synthesized and thoroughly structurally characterized. XPS analysis confirmed the successful introduction of nitrogen, highlighting the nature of the different nitrogen atoms incorporated in the structure. The work aims at evaluating the electrochemical performance of N-doped ordered mesoporous carbons as an anode in LIBs, underlining the effect of the nitrogen functionalization. The N-CMK-8 electrode reveals higher reversible capacity, better cycling stability, and rate capability, as compared to the CMK-8 electrode. Coupling the 3D channel network with the functional N-doping increased the reversible capacity to similar to 1000 mAh center dot g(-1) for the N-CMK-8 from similar to 450 mAh center dot g(-1) for the undoped CMK-8 electrode. A full Li-ion cell was built using N-CMK-8 as an anode, commercial LiFePO4, a cathode, and LP30 commercial electrolyte, showing stable performance for 100 cycles. The combination of nitrogen functionalization and ordered porosity is promising for the development of high performing functional anodes.
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| 37. |
- Calcagno, Giulio, 1990, et al.
(författare)
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Fast charging negative electrodes based on anatase titanium dioxide beads for highly stable Li-ion capacitors
- 2020
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Ingår i: Materials Today Energy. - : Elsevier BV. - 2468-6069. ; 16
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Tidskriftsartikel (refereegranskat)abstract
- Hybrid energy storage systems aim to achieve both high power and energy densities by combining supercapacitor-type and battery-type electrodes in tandem. The challenge is to find sustainable materials as fast charging negative electrodes, which are characterized by high capacity retention. In this study, mesoporous anatase beads are synthetized with tailored morphology to exploit fast surface redox reactions. The TiO2-based electrodes are properly paired with a commercial activated carbon cathode to form a Li-ion capacitor. The titania electrode exhibits high capacity and rate performance. The device shows extremely stable performance with an energy density of 27 mWh g-1 at a specific current of 2.5 A g−1 for 10,000 cycles. The remarkable stability is associated with a gradual shift of the potential during cycling as result of the formation of cubic LiTiO2 on the surface of the beads. This phenomenon renews the interest in using TiO2 as negative electrode for Li-ion capacitors.
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| 38. |
- Calcagno, Giulio, 1990, et al.
(författare)
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Understanding the Operating Mechanism of Aqueous Pentyl Viologen/Bromide Redox-Enhanced Electrochemical Capacitors with Ordered Mesoporous Carbon Electrodes
- 2022
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Ingår i: ACS Applied Materials & Interfaces. - : American Chemical Society (ACS). - 1944-8252 .- 1944-8244. ; 14:18, s. 20349-20357
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Tidskriftsartikel (refereegranskat)abstract
- Compared to traditional electric double-layer capacitors, redox-enhanced electrochemical capacitors (redox-ECs) show increased energy density and steadier power output thanks to the use of redox-active electrolytes. The aim of this study is to understand the electrochemical mechanisms of the aqueous pentyl viologen/bromide dual redox system at the interface of an ordered mesoporous carbon (CMK-8) and improve the device performance. Cells with CMK-8 carbon electrodes were investigated in several configurations using different charging rates and potential windows. The pentyl viologen electrochemistry shows a mixed behavior between solution-based diffusion and adsorption phenomena, with the reversible formation of an adsorbed layer. The extension of the voltage window allows for full reduction of the viologen molecules during charge and a consequent increase in the specific discharge energy delivered by the cell. Investigation of the mechanism indicates that a 1.5 V charging voltage with a 0.5 A g-1 charging rate and fast discharge rate produces the best overall performance.
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| 39. |
- Cavallo, Carmen, 1986, et al.
(författare)
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Effect of the Niobium Doping Concentration on the Charge Storage Mechanism of Mesoporous Anatase Beads as an Anode for High-Rate Li-Ion Batteries
- 2021
-
Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 4:1, s. 215-225
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Tidskriftsartikel (refereegranskat)abstract
- A promising strategy to improve the rate performance of Li-ion batteries is to enhance and facilitate the insertion of Li ions into nanostructured oxides like TiO2. In this work, we present a systematic study of pentavalent-doped anatase TiO2 materials for third-generation high-rate Li-ion batteries. Mesoporous niobium-doped anatase beads (Nb-doped TiO2) with different Nb5+ doping (n-type) concentrations (0.1, 1.0, and 10% at.) were synthesized via an improved template approach followed by hydrothermal treatment. The formation of intrinsic n-type defects and oxygen vacancies under RT conditions gives rise to a metallic-type conduction due to a shift of the Fermi energy level. The increase in the metallic character, confirmed by electrochemical impedance spectroscopy, enhances the performance of the anatase bead electrodes in terms of rate capability and provides higher capacities both at low and fast charging rates. The experimental data were supported by density functional theory (DFT) calculations showing how a different n-type doping can be correlated to the same electrochemical effect on the final device. The Nb-doped TiO2 electrode materials exhibit an improved cycling stability at all the doping concentrations by overcoming the capacity fade shown in the case of pure TiO2 beads. The 0.1% Nb-doped TiO2-based electrodes exhibit the highest reversible capacities of 180 mAh g-1 at 1C (330 mA g-1) after 500 cycles and 110 mAh g-1 at 10C (3300 mA g-1) after 1000 cycles. Our experimental and computational results highlight the possibility of using n-type doped TiO2 materials as anodes in high-rate Li-ion batteries.
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| 40. |
- 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
-
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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| 41. |
- Cederkrantz, Daniel, 1979, et al.
(författare)
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Thermal stability and thermoelectric properties of p-type Ba8Ga16Ge30 clathrates
- 2009
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Ingår i: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 106:7, s. 074509 (artno)-
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Tidskriftsartikel (refereegranskat)abstract
- The thermal stability of p-type Ba(8)Ga(16)Ge(3)0 clathrates grown from gallium flux has been tested by heat treatment in low pressure Ar atmosphere at 400, 600, and 800 degrees C. Significant gallium loss was observed for all samples during heat treatment. The treatment at 400 degrees C does not significantly change the sample properties, and the samples remain p-type and comparable to the untreated, as-prepared, sample. At 600 degrees C the sample switches from extrinsic p-type to extrinsic n-type, presumably due to significant loss of Ga, and shows a high thermopower but a reduced electrical conductivity compared to as-made n-type samples. Surprisingly, after a thermal treatment at 800 degrees C, the crystal structure seemingly loses less Ga, only reducing the hole concentration to near intrinsic levels and thus has a negative impact on ZT. Regardless of the heat treatment temperature of the p-type samples the thermal conductivity remained exceptionally low, for some samples 0.9 W/m K. Heat treatment can thus greatly affect the thermoelectric properties of p-type Ba(8)Ga(16)Ge(3)0, but the crystal structure remains intact. (C) 2009 American Institute of Physics. [doi: 10.1063/1.3236635]
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| 42. |
- Cederkrantz, Daniel, 1979, et al.
(författare)
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Thermoelectric properties of partly Sb- and Zn-substituted Ba8Ga16Ge30 clathrates
- 2010
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Ingår i: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 108:11, s. 113711-
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Tidskriftsartikel (refereegranskat)abstract
- The effects on the thermoelectric properties of n-Ba8Ga16Ge30 when substituting small amounts of the Ga or Ge with Sb or Zn have been investigated. A number of syntheses were prepared in quaternary systems of Ba8Ga16Ge30 substituted with either Sb or Zn but only three samples were found to yield single phase products with nominal compositions of Ba8Ga15Sb1Ge30, Ba8Ga15Zn1Ge30 and Ba8Ga16Ge28Zn2, respectively. When Ge was substituted for Zn the resulting sample remained n-type and an increase in thermopower and a decrease in thermal conductivity were achieved. These positive effects were accompanied with an increased electrical resistivity and thus the ZT was only somewhat improved up to about 400 °C. When substituting Ga with either Sb or Zn samples remained n-type but showed decreased thermopower and increased electrical resistivity and thermal conductivity. It is thus concluded that substitution of Ga with Zn or Sb is detrimental for the thermoelectric properties of Ba8Ga16Ge30, whereas substitution of Ge with Zn appears a potent method for improving its performance.
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| 43. |
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| 44. |
- DAWODY, JAZAER, 1959, et al.
(författare)
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An integrated system for energy-efficient exhaust aftertreatment for heavy-duty vehicles
- 2015
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Ingår i: Renewable Energy in the Service of Mankind. - Cham : Springer International Publishing. - 9783319177779 - 9783319177762 ; 1, s. 133-143
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Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- © Springer International Publishing Switzerland 2015. This chapter presents a unique system approach applied in a joint academic- industrial research programme, E4 Mistra, to attain the goals of high energy efficiency and low emissions in an exhaust aftertreatment system for heavy-duty vehicles. The high energy efficiency is achieved by heat recuperation, onboard hydrogen production for NOx reduction, and by finding new solutions for making the aftertreatment system active at low exhaust temperatures. To reach low particulate emissions, a mechanical filter using a sintered metal powder is developed and coated with catalytic material to improve the soot oxidation efficiency. Low NOx emissions are achieved by an efficient NOx reduction catalyst. The integrated E4 Mistra system comprises four technological advances: thermoelectric (TE) materials for heat recuperation, catalytic reduction of NOx over innovative catalyst substrates using either the onboard diesel or biodiesel, H2 from a high-efficiency fuel reformer, and particulate filtration over a porous metal filter. The TE materials are used in a TE generator (TEG) which converts thermal energy into electricity. The TEG is used to recuperate heat from the exhaust-gas recirculation (EGR) circuit of heavy-duty trucks and is expected to generate ~1 kW electric power from 20 kW heat in the exhaust gas. The TEG is integrated in a plate heat exchanger (HEX) designed particularly for this application. Apart from the knowledge and experiences in TEG and heat exchange technologies, a thorough fluid dynamics and TE analysis are performed in this project to understand the governing processes and optimize the system accordingly. The components of the E4 Mistra system are explained in the chapter in addition to test results, which show the system's capacity for H2 production, NOx conversion, particulate matter filtration and soot oxidation, and finally electric power generation via heat recuperation from the exhaust gas using the developed TEG-HEX system.
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| 45. |
- DAWODY, JAZAER, 1959, et al.
(författare)
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E4-Mistra, a research program for the development of an energy efficient low emission exhaust aftertreatment system for heavy duty vehicles
- 2012
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Ingår i: World Renewable Energy Forum, WREF 2012, Including World Renewable Energy Congress XII and Colorado Renewable Energy Society (CRES) Annual Conference. - : American Solar Energy Society. - 9781622760923 ; , s. 4530-4536
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Konferensbidrag (refereegranskat)abstract
- This paper presents a unique system approach applied in a joint academic - industrial research program, E4 Mistra, to reach the goals of energy efficiency and low emissions exhaust aftertreatment system for heavy duty vehicles. The high energy efficiency is achieved by heat recuperation, on-board hydrogen production for use in both an auxiliary power unit and for NOx reduction and by finding new solutions for making the after-treatment system active at low exhaust temperatures. To reach low particulate emissions a mechanical filter using a sintered metal filter is developed. Low NOx emissions are achieved by an efficient NOx reduction catalyst. The system is based on four technological advances: Thermoelectric material s for heat recuperation, catalytic reduction of NOx over innovative catalyst substrates using hydrocarbons from the fuel and H2 from a high efficiency fuel reformer, and particulate filtration over a porous metal filter.
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| 46. |
- Dombrovskis, Johanna, 1986, et al.
(författare)
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One-pot synthesis of transition metal ion-chelating ordered mesoporous carbon/carbon nanotube composites for active and durable fuel cell catalysts
- 2017
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Ingår i: Journal of Power Sources. - : Elsevier BV. - 0378-7753. ; 357, s. 87-96
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Tidskriftsartikel (refereegranskat)abstract
- Development of non-precious metal catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane (PEM) fuel cells with high activity and durability and with optimal water management properties is of outmost technological importance and highly challenging. Here we study the possibilities offered through judicious selection of small molecular precursors used for the formation of ordered mesoporous carbon-based non-precious metal ORR catalysts. By combining two complementary precursors, we present a one-pot synthesis that leads to a composite material consisting of transition metal ion-chelating ordered mesoporous carbon and multi-walled carbon nanotubes (TM-OMC/CNT). The resulting composite materials show high specific surface areas and a carbon structure that exhibits graphitic signatures. The synthesis procedure allows for tuning of the carbon structure, the surface area, the pore volume and the ratio of the two components of the composite. The TM-OMC/CNT composites were processed into membrane electrode assemblies and evaluated in single cell fuel cell measurements where they showed a combination of good ORR activity and very high durability.
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| 47. |
- Dombrovskis, Johanna, 1986, et al.
(författare)
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Optimization of fuel cell membrane electrode assemblies for transition metal ion-chelating ordered mesoporous carbon cathode catalysts
- 2014
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Ingår i: APL Materials. - : AIP Publishing. - 2166-532X. ; 2:12, s. Art. no. 121102-
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Tidskriftsartikel (refereegranskat)abstract
- Transition metal ion-chelating ordered mesoporous carbon (TM-OMC) materials were recently shown to be efficient polymer electrolyte membrane fuel cell (PEMFC) catalysts. The structure and properties of these catalysts are largely different from conventional catalyst materials, thus rendering membrane electrode assembly (MEA) preparation parameters developed for conventional catalysts not useful for applications of TM-OMC catalysts. This necessitates development of a methodology to incorporate TM-OMC catalysts in the MEA. Here, an efficient method for MEA preparation using TM-OMC catalyst materials for PEMFC is developed including effects of catalyst/ionomer loading and catalyst/ionomer-mixing and application procedures. An optimized protocol for MEA preparation using TM-OMC catalysts is described.
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| 48. |
- Dombrovskis, Johanna, 1986, et al.
(författare)
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Recent Progress in Synthesis, Characterization and Evaluation of Non-Precious Metal Catalysts for the Oxygen Reduction Reaction
- 2016
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Ingår i: Fuel Cells. - : Wiley. - 1615-6846 .- 1615-6854. ; 16:1, s. 4-22
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Forskningsöversikt (refereegranskat)abstract
- The oxygen reduction reaction (ORR) is usually catalyzed by precious metals. As the kinetics of the reaction are sluggish comparatively large amounts of precious metal are needed to achieve satisfactory reaction rates. This results in high cost of technologies utilizing the ORR, like low temperature fuel cells. Recent years have seen tremendous research efforts in the development of non-precious metal catalysts (NPMCs) with a wide range of newly developed materials resulting in improved catalyst materials, an increased understanding of the ORR mechanism on NPMC materials and better knowledge of the active site structure. Here we summarize the developments from 2011 and onwards with a special focus on carbon-based NPMCs developed for use in acid environments. We include explicit comparisons of PEMFC measurement results in all referenced studies and detailed information on the physical characterization methods used in various publications.
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| 49. |
- Dombrovskis, Johanna, 1986, et al.
(författare)
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The Active Site Structure of Transition Metal Ion-Chelating Ordered Mesoporous Carbon Fuel Cell Catalysts
- 2016
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Ingår i: Fuel Cells. - : Wiley. - 1615-6846 .- 1615-6854. ; 16:1, s. 23-31
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Tidskriftsartikel (refereegranskat)abstract
- Transition metal ion-chelating ordered mesoporous carbons (TM-OMCs) were studied as polymer electrolyte membrane fuel cell cathode catalysts. The active site structure of the TM-OMCs was studied by X-ray absorption spectroscopy in combination with variations of a range of synthesis variables of the TM-OMCs. The variations were found to have significant influence on the catalyst structure both in the mesoscale and on the atomic local structure allowing for detailed conclusions on the nature of the active sites. The main active site was found to be FeNx chelates. An additional highly active site was found and proposed to be a FeNx-dioxygen site. It was further found that the catalytic activity could be increased threefold by acid washing and subsequent heat treatment of the as-synthesized TM-OMC materials.
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| 50. |
- Dombrovskis, Johanna, 1986, et al.
(författare)
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Transition Metal Ion-Chelating Ordered Mesoporous Carbons as Noble Metal-Free Fuel Cell Catalysts
- 2013
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 1520-5002 .- 0897-4756. ; 25:6, s. 856-861
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Tidskriftsartikel (refereegranskat)abstract
- A new concept for noble metal-free polymer electrolyte membrane fuel cell catalysts has been developed. The catalysts consist of chelated transition metal ions incorporated in a nitrogen-functionalized ordered mesoporous carbon matrix, which is evidenced by a combination of X-ray absorption fine structure analysis and high-resolution transmission electron microscopy. The ordered mesoporous carbon matrix of the catalyst offers an exceptionally high specific surface area and allows conceptually for a high degree of tuning, enabling controlled variability of, e.g., pore size and curvature and thickness of the pore walls of the catalysts. Single cell fuel cell tests of membrane electrode assemblies prepared with a cathode made of iron- or cobalt-based versions of the catalyst show high power densities, reaching up to one-third of a commercial Pt/C catalyst at 0.6 V.
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