| 1. |
- Enghag, Margareta, 1952-, et al.
(författare)
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Student evaluations of themselves as disciplinary practitioners
- 2009
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Ingår i: Paper presented at the GIREP-EPEC (International Research Group on Physics Teaching) Conference, University of Leicester, Great Britain, 17-21 August.
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Konferensbidrag (övrigt vetenskapligt/konstnärligt)
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| 2. |
- Le Breton, Michael, 1986, et al.
(författare)
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Chlorine oxidation of VOCs at a semi-rural site in Beijing: significant chlorine liberation from ClNO2 and subsequent gas- and particle-phase Cl-VOC production
- 2018
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:17, s. 13013-13030:18, s. 13013-13030
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Tidskriftsartikel (refereegranskat)abstract
- Nitryl chloride (ClNO2) accumulation at night acts as a significant reservoir for active chlorine and impacts the following day's photochemistry when the chlorine atom is liberated at sunrise. Here, we report simultaneous measurements of N2O5 and a suite of inorganic halogens including ClNO2 and reactions of chloride with volatile organic compounds (Cl-VOCs) in the gas and particle phases utilising the Filter Inlet for Gas and AEROsols time-of-flight chemical ionisation mass spectrometer (FIGAERO-ToF-CIMS) during an intensive measurement campaign 40 km northwest of Beijing in May and June 2016. A maximum mixing ratio of 2900 ppt of ClNO2 was observed with a mean campaign nighttime mixing ratio of 487 ppt, appearing to have an anthropogenic source supported by correlation with SO2, CO and benzene, which often persisted at high levels after sunrise until midday. This was attributed to such high mixing ratios persisting after numerous e-folding times of the photolytic lifetime enabling the chlorine atom production to reach 2.3 x 10(5) molecules cm(-3) from ClNO2 alone, peaking at 09:30 LT and up to 8.4 x 10(5) molecules cm(-3) when including the supporting inorganic halogen measurements. Cl-VOCs were observed in the particle and gas phases for the first time at high time resolution and illustrate how the iodide ToF-CIMS can detect unique markers of chlorine atom chemistry in ambient air from both biogenic and anthropogenic sources. Their presence and abundance can be explained via time series of their measured and steady-state calculated precursors, enabling the assessment of competing OH and chlorine atom oxidation via measurements of products from both of these mechanisms and their relative contribution to secondary organic aerosol (SOA) formation.
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| 3. |
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| 4. |
- Rocha, Luis E C, 1981-
(författare)
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Exploring patterns of empirical networks
- 2011
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- We are constantly struggling to understand how nature works, trying to identify recurrent events and looking for analogies and relations between objects or individuals. Knowing patterns of behavior is powerful and fundamental for survival of any species. In this thesis, datasets of diverse systems related to transportation, economics, sexual and social contacts, are characterized by using the formalisms of time series and network theory. Part of the results consists on the collection and analyzes of original network data, the rest focuses on the simulation of dynamical processes on these networks and to study how they are affected by the particular structures. The majority of the thesis is about temporal networks, i.e. networks whose structure changes in time. The new temporal dimension reveals structural dynamical properties that help to understand the feedback mechanisms responsible to make the network structure to adapt and to understand the emergence and inhibition of diverse phenomena in dynamic systems, as epidemics in sexual and contact networks.
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| 5. |
- Borsato, M., et al.
(författare)
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Unleashing the full power of LHCb to probe stealth new physics
- 2022
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Ingår i: Reports on Progress in Physics. - : IOP Publishing. - 0034-4885 .- 1361-6633. ; 85:2
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Tidskriftsartikel (refereegranskat)abstract
- In this paper, we describe the potential of the LHCb experiment to detect stealth physics. This refers to dynamics beyond the standard model that would elude searches that focus on energetic objects or precision measurements of known processes. Stealth signatures include long-lived particles and light resonances that are produced very rarely or together with overwhelming backgrounds. We will discuss why LHCb is equipped to discover this kind of physics at the Large Hadron Collider and provide examples of well-motivated theoretical models that can be probed with great detail at the experiment.
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| 6. |
- Lindahl, Niklas, 1981, et al.
(författare)
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Aluminum Metal-Organic Batteries with Integrated 3D Thin Film Anodes
- 2020
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Ingår i: Advanced Functional Materials. - : Wiley. - 1616-301X .- 1616-3028. ; 30:51
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Tidskriftsartikel (refereegranskat)abstract
- Aluminum 3D thin film anodes fully integrated with a separator are fabricated by sputtering and enable rechargeable aluminum metal batteries with high power performance. The 3D thin film anodes have an approximately four to eight times larger active surface area than a metal foil, which significantly both reduces the electrochemical overpotential, and improves materials utilization. In full cells with organic cathodes, that is, aluminum metal-organic batteries, the 3D thin film anodes provide 165 mAh g(-1)at 0.5 C rate, with a capacity retention of 81% at 20 C, and 86% after 500 cycles. Post-mortem analysis reveals structural degradation to limit the long-term stability at high rates. As the multivalent charge carrier active here is AlCl2+, the realistic maximal specific energy, and power densities at cell level are approximate to 100 Wh kg(-1)and approximate to 3100 W kg(-1), respectively, which is significantly higher than the state-of-the-art for Al batteries.
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| 7. |
- Waltersson, Erik, 1979-, et al.
(författare)
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Controlled operations in a strongly correlated two-electron quantum ring
- 2009
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Ingår i: Physical Review B. Condensed Matter and Materials Physics. - : American Physical Society. - 1098-0121 .- 1550-235X. ; 79:11, s. 115318-
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Tidskriftsartikel (refereegranskat)abstract
- We have analyzed the electronic spectrum and wave-function characteristics of a strongly correlated two-electron quantum ring with model parameters close to those observed in experiments. The analysis is based on an exact diagonalization of the Hamiltonian in a large B-spline basis. We propose a qubit pair for storing quantum information, where one component is stored in the total electron spin and one multivalued “quMbit” is represented by the total angular momentum. In this scheme the controlled-NOT quantum gate is demonstrated with near 100% fidelity for a realistic far-infrared electromagnetic pulse.
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| 8. |
- Fan, Qunping, 1989, et al.
(författare)
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Over 14% efficiency all-polymer solar cells enabled by a low bandgap polymer acceptor with low energy loss and efficient charge separation
- 2020
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Ingår i: Energy & Environmental Science. - : Royal Society of Chemistry. - 1754-5692 .- 1754-5706. ; 13:12, s. 5017-5027
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Tidskriftsartikel (refereegranskat)abstract
- Obtaining both high open-circuit voltage (V-oc) and short-circuit current density (J(sc)) has been a major challenge for efficient all-polymer solar cells (all-PSCs). Herein, we developed a polymer acceptor PF5-Y5 with excellent optical absorption capability (onset extending to similar to 880 nm and maximum absorption coefficient exceeding 105 cm(-1) in a film), high electron mobility (3.18 x 10(3) cm(2) V-1 s(-1)) and high LUMO level (-3.84 eV) to address such a challenge. As a result, the PBDB-T:PF5-Y5-based all-PSCs achieved a high power conversion efficiency of up to 14.45% with both a high Voc (0.946 V) and a high Jsc (20.65 mA cm(-2)), due to the high and broad absorption coverage, small energy loss (0.57 eV) and efficient charge separation and transport in the device, which are among the best values in the all-PSC field. In addition, the all-PSC shows a similar to 15% improvement in PCE compared to its counterpart small molecule acceptor (Y5)-based device. Our results suggest that PF5-Y5 is a very promising polymer acceptor candidate for applications in efficient all-PSCs.
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| 9. |
- Castelain, Mickaël, et al.
(författare)
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Fast uncoiling kinetics of F1C pili expressed by uropathogenic Escherichia coli are revealed on a single pilus level using force-measuring optical tweezers
- 2011
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Ingår i: European Biophysics Journal. - : Springer Science and Business Media LLC. - 0175-7571 .- 1432-1017. ; 40:3, s. 305-316
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Tidskriftsartikel (refereegranskat)abstract
- Uropathogenic Escherichia coli (UPEC) expressvarious kinds of organelles, so-called pili or fimbriae, thatmediate adhesion to host tissue in the urinary tract throughspecific receptor-adhesin interactions. The biomechanicalproperties of these pili have been considered important forthe ability of bacteria to withstand shear forces from rinsingurine flows. Force-measuring optical tweezers have beenused to characterize individual organelles of F1C typeexpressed by UPEC bacteria with respect to such properties.Qualitatively, the force-versus-elongation response wasfound to be similar to that of other types of helix-like piliexpressed by UPEC, i.e., type 1, P, and S, with force-inducedelongation in three regions, one of which represents theimportant uncoiling mechanism of the helix-like quaternarystructure. Quantitatively, the steady-state uncoiling forcewas assessed as 26.4 ±1.4 pN, which is similar to those ofother pili (which range from 21 pN for SI to 30 pN for type 1).The corner velocity for dynamic response (1,400 nm/s) wasfound to be larger than those of the other pili (400–700 nm/sfor S and P pili, and 6 nm/s for type 1). The kinetics werefound to be faster, with a thermal opening rate of 17 Hz, afew times higher than S and P pili, and three orders ofmagnitude higher than type 1. These data suggest that F1Cpili are, like P and S pili, evolutionarily selected to primarilywithstand the conditions expressed in the upper urinary tract.
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| 10. |
- Dissanayake, Makl, et al.
(författare)
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Optimizing the size and amount of CdS quantum dots for efficiency enhancement in CdS/N719 co-sensitized solar cells
- 2022
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Ingår i: Physica E-Low-Dimensional Systems & Nanostructures. - : Elsevier BV. - 1386-9477. ; 144
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Tidskriftsartikel (refereegranskat)abstract
- Co-sensitization of TiO2 photoanodes in solar cells with Ruthenium dye and quantum dots offer better photovoltaic performance compared to the sensitization by the dye only. In the present study, TiO2 nanostructured photoanode was co-sensitized with CdS quantum dots and N719 dye. CdS quantum dots were deposited using successive ionic layer adsorption and reaction (SILAR). A suitable thin ZnS interfacial layer has been introduced between two sensitizers to prevent the corrosion of CdS quantum dots by the iodide-based liquid electrolyte. In order to get the highest efficiency, the number of SILAR cycles for CdS quantum dot deposition has been optimized. A power conversion efficiency of 6.79% with short-circuit current density of 15.55 mA cm-2 and open circuit voltage of 764.5 mV have been obtained for the co-sensitized solar cell made with TiO2/CdS/ZnS/N719 co-sensitized photoanode under the illumination of 100 mW cm-2 with AM 1.5 spectral filter. Efficiency and short-circuit current density of the solar cell have been enhanced by 11.31% and 6.58% respectively due to the co-sensitization. The optimized co-sensitized solar cell shows a higher incident photon to current conversion efficiency and a reduced electron recombination compared to the solar cell with dye-sensitized photoanode. Higher recombination resistance and longer electron lifetime of the solar cell with CdS/ZnS/N719 co-sensitized TiO2 photoanode have contributed to the increased short circuit current and open circuit voltage leading to the enhanced efficiency of 6.79% which is among the highest for a co-sensitized dye sensitized solar cell.
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| 11. |
- Manzetti, Sergio, et al.
(författare)
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A Korteweg-DeVries type model for helical soliton solutions for quantum and continuum phenomena
- 2021
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Ingår i: International Journal of Modern Physics C. - : World Scientific. - 0129-1831. ; 32:03
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Tidskriftsartikel (refereegranskat)abstract
- Quantum mechanical states are normally described by the Schrödinger equation, which generates real eigenvalues and quantizable solutions which form a basis for the estimation of quantum mechanical observables, such as momentum and kinetic energy. Studying transition in the realm of quantum physics and continuum physics is however more difficult and requires different models. We present here a new equation which bears similarities to the Korteweg–DeVries (KdV) equation and we generate a description of transitions in physics. We describe here the two- and three-dimensional form of the KdV like model dependent on the Plank constant ℏ and generate soliton solutions. The results suggest that transitions are represented by soliton solutions which arrange in a spiral-fashion. By helicity, we propose a conserved pattern of transition at all levels of physics, from quantum physics to macroscopic continuum physics.
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| 12. |
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| 13. |
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| 14. |
- Andersson, Ole, et al.
(författare)
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Device-independent certification of two bits of randomness from one entangled bit and Gisin's elegant Bell inequality
- 2018
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - : American Physical Society. - 1050-2947 .- 1094-1622. ; 97:1
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Tidskriftsartikel (refereegranskat)abstract
- We prove that as conjectured by Acín et al. [Phys. Rev. A 93, 040102(R) (2016)], two bits of randomness can be certified in a device-independent way from one bit of entanglement using the maximal quantum violation of Gisin's elegant Bell inequality. This suggests a surprising connection between maximal entanglement, complete sets of mutually unbiased bases, and elements of symmetric informationally complete positive operator-valued measures, on one side, and the optimal way of certifying maximal randomness, on the other.
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| 15. |
- Parafilo, A. V., et al.
(författare)
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Kondo effect in a Aharonov-Casher interferometer
- 2019
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Ingår i: Physical Review B. - 2469-9950 .- 2469-9969. ; 100:23
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Tidskriftsartikel (refereegranskat)abstract
- We consider a model describing a spin field-effect transistor based on a quantum nanowire with a tunable spin-orbit interaction embedded between two ferromagnetic leads with anticollinear magnetization. We investigate a regime of a strong interplay between resonance Kondo scattering and interference associated with the Aharonov-Casher effect. Using the Keldysh technique at a weak-coupling regime we calculate perturbatively the charge current. It is predicted that the effects of the spin-orbit interaction result in a nonvanishing current for any spin polarization of the leads including the case of fully polarized anticollinear contacts. We analyze the influence of the Aharonov-Casher phase and degree of spin polarization in the leads onto a Kondo temperature.
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| 16. |
- Erhart, Paul, 1978
(författare)
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A first-principles study of helium storage in oxides and at oxide-iron interfaces
- 2012
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Ingår i: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 111:11
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Tidskriftsartikel (refereegranskat)abstract
- Density-functional theory calculations based on conventional as well as hybrid exchange-correlation functionals have been carried out to study the properties of helium in various oxides (Al2O3, TiO2, Y2O3, YAP, YAG, YAM, MgO, CaO, BaO, SrO) as well as at oxide-iron interfaces. Helium interstitials in bulk oxides are shown to be energetically more favorable than substitutional helium, yet helium binds to existing vacancies. The solubility of He in oxides is systematically higher than in iron and scales with the free volume at the interstitial site nearly independently of the chemical composition of the oxide. In most oxides, He migration is significantly slower and He-He binding is much weaker than in iron. To quantify the solubility of helium at oxide-iron interfaces two prototypical systems are considered (Fe-MgO, Fe-FeO-MgO). In both cases, the He solubility is markedly enhanced in the interface compared to either of the bulk phases. The results of the calculations allow to construct a schematic energy landscape for He interstitials in iron. The implications of these results are discussed in the context of helium sequestration in oxide dispersion strengthened steels, including the effects of interfaces and lattice strain.
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| 17. |
- Bahrova, O. M., et al.
(författare)
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Cooling of nanomechanical vibrations by Andreev injection
- 2022
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Ingår i: Low Temperature Physics. - : AIP Publishing. - 1063-777X .- 1090-6517. ; 48:6, s. 476-482
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Tidskriftsartikel (refereegranskat)abstract
- A nanoelectromechanical weak link composed of a carbon nanotube suspended between two normal electrodes in a gap between two superconducting leads is considered. The nanotube is treated as a movable single level quantum dot in which the position-dependent superconducting order parameter is induced due to the Cooper pair tunneling. We show that electron tunneling processes significantly affect the state of the mechanical subsystem. We found that at a given direction of the applied voltage between the electrodes, the stationary state of the mechanical subsystem has a Boltzmann form with an effective temperature dependent on the parameters of the device. As this takes place, the effective temperature can reach significantly small values (cooling effect). We also demonstrate that nanotube fluctuations strongly affect the dc current through the system. The latter can be used to probe the predicted effects in an experiment. Published under an exclusive license by AIP Publishing.
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| 18. |
- Jiao, Yang, 1985, et al.
(författare)
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Signatures of van der Waals binding: A coupling-constant scaling analysis
- 2018
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Ingår i: Physical Review B. - 2469-9969 .- 2469-9950. ; 97:8
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Tidskriftsartikel (refereegranskat)abstract
- The van der Waals (vdW) density functional (vdW-DF) method [Rep. Prog. Phys. 78, 066501 (2015)RPPHAG0034-488510.1088/0034-4885/78/6/066501] describes dispersion or vdW binding by tracking the effects of an electrodynamic coupling among pairs of electrons and their associated exchange-correlation holes. This is done in a nonlocal-correlation energy term Ecnl, which permits density functional theory calculation in the Kohn-Sham scheme. However, to map the nature of vdW forces in a fully interacting materials system, it is necessary to also account for associated kinetic-correlation energy effects. Here, we present a coupling-constant scaling analysis, which permits us to compute the kinetic-correlation energy Tcnl that is specific to the vdW-DF account of nonlocal correlations. We thus provide a more complete spatially resolved analysis of the electrodynamical-coupling nature of nonlocal-correlation binding, including vdW attraction, in both covalently and noncovalently bonded systems. We find that kinetic-correlation energy effects play a significant role in the account of vdW or dispersion interactions among molecules. Furthermore, our mapping shows that the total nonlocal-correlation binding is concentrated to pockets in the sparse electron distribution located between the material fragments.
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| 19. |
- Parafilo, A. V., et al.
(författare)
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Pumping and Cooling of Nanomechanical Vibrations Generated by Cooper-Pair Exchange
- 2022
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Ingår i: Journal of Low Temperature Physics. - : Springer Science and Business Media LLC. - 0022-2291 .- 1573-7357. ; 210:1-2, s. 150-65
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Tidskriftsartikel (refereegranskat)abstract
- We consider a nanoelectromechanical system composed of a carbon nanotube suspended between two normal leads and coupled to a superconducting scanning tunneling microscope (STM) tip via vacuum tunnel barrier. Treating the nanotube as a single-level quantum dot, it is shown that an applied voltage between the superconducting STM tip and normal leads gives rise to a pumping or a cooling of the mechanical subsystem depending on the direction of the electronic flow. It is also demonstrated that the transition between these two regimes is controlled by the strength of the tunnel coupling between the nanotube and superconducting STM tip and the relative position of the electronic level. Such phenomena are realized due to a specific electromechanical coupling that is fully governed by the quantum dynamics of the Cooper pairs. The amplitude of the self-sustained oscillations in the pumping regime is analyzed numerically, and the effective temperature of the mechanical subsystem in the cooling regime is obtained.
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| 20. |
- Sjöqvist, Erik, et al.
(författare)
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Conceptual aspects of geometric quantum computation
- 2016
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Ingår i: Quantum Information Processing. - : Springer Science and Business Media LLC. - 1570-0755 .- 1573-1332. ; 15:10, s. 3995-4011
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Tidskriftsartikel (refereegranskat)abstract
- Geometric quantum computation is the idea that geometric phases can be used to implement quantum gates, i.e., the basic elements of the Boolean network that forms a quantum computer. Although originally thought to be limited to adiabatic evolution, controlled by slowly changing parameters, this form of quantum computation can as well be realized at high speed by using nonadiabatic schemes. Recent advances in quantum gate technology have allowed for experimental demonstrations of different types of geometric gates in adiabatic and nonadiabatic evolution. Here, we address some conceptual issues that arise in the realizations of geometric gates. We examine the appearance of dynamical phases in quantum evolution and point out that not all dynamical phases need to be compensated for in geometric quantum computation. We delineate the relation between Abelian and non-Abelian geometric gates, and find an explicit physical example where the two types of gates coincide. We identify differencies and similarities between adiabatic and nonadiabatic realizations of quantum computation based on non-Abelian geometric phases.
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| 21. |
- Lee, Kyuho, et al.
(författare)
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Benchmarking van der Waals density functionals with experimental data: potential-energy curves for H2 molecules on Cu(111), (100) and (110) surfaces
- 2012
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Ingår i: Journal of Physics: Condensed Matter. - : IOP Publishing. - 0953-8984 .- 1361-648X. ; 24:42
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Tidskriftsartikel (refereegranskat)abstract
- Detailed physisorption data from experiment for the H2 molecule on low-index Cu surfaces challenge theory. Recently, density functional theory (DFT) has been developed to account for nonlocal correlation effects, including van der Waals (dispersion) forces. We show that the functional vdW-DF2 gives a potential-energy curve, potential-well energy levels and difference in lateral corrugation promisingly close to the results obtained by resonant elastic backscattering–diffraction experiments. The backscattering barrier is sensitive to the choice of exchange functional approximation. Further, the DFT-D3 and TS-vdW corrections to traditional DFT formulations are also benchmarked, and deviations are analyzed.
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| 22. |
- Isaksson, Oscar, et al.
(författare)
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An optical levitation system for a physics teaching laboratory
- 2018
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Ingår i: American Journal of Physics. - : American Association of Physics Teachers (AAPT). - 0002-9505 .- 1943-2909. ; 86:2, s. 135-142
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Tidskriftsartikel (refereegranskat)abstract
- We describe an experimental system based on optical levitation of an oil droplet. When combined with an applied electric field and a source of ionizing radiation, the setup permits the investigation of physical phenomena such as radiation pressure, light diffraction, the motion of a charged particle in an oscillating electric field, and the interaction of ionizing radiation with matter. The trapping occurs by creating an equilibrium between a radiation pressure force and the force of gravity. We have found that an oil droplet can be trapped for at least nine hours. The system can be used to measure the size and total electric charge on the trapped droplet. The intensity of the light from the trapping laser that is scattered by the droplet is sufficient to allow the droplet to be easily seen with the naked eye, covered by laser alignment goggles. When oscillating under the influence of an ac electric field, the motion of the droplet can be described as that of a driven, damped harmonic oscillator. The magnitude and polarity of the charge can be altered by exposing the droplet to ionizing radiation from a low-activity radioactive source. Our goal was to design a hands-on setup that allows undergraduate and graduate students to observe and better understand fundamental physical processes. (C) 2018 American Association of Physics Teachers.
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| 23. |
- Windelius, Olle, 1972, et al.
(författare)
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Photoelectron angular distributions in photodetachment from P
- 2021
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Ingår i: Physical Review A. - 2469-9926 .- 2469-9934. ; 103:3
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Tidskriftsartikel (refereegranskat)abstract
- The angular distributions of electrons ejected in laser photodetachment of the P- ion have been studied in the photon energy range of 0.95-3.28 eV using a photoelectron spectrometer designed to accommodate a source consisting of collinearly overlapping photon and negative ion beams. We observe the value of the asymmetry parameter beta starting at zero near the threshold, falling to almost -1 about 0.5 eV above the threshold and eventually rising to a positive value. The experimental data has been fitted to a simplified model of the Cooper-Zare formula which yields a qualitative understanding of the quantum interference between the outgoing s and d waves representing the free electron. The present results are also compared with previous results for other elements involving p-electron photodetachment.
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| 24. |
- Scott, Pat, 1982-
(författare)
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Searches for Particle Dark Matter : Dark stars, dark galaxies, dark halos and global supersymmetric fits
- 2010
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The identity of dark matter is one of the key outstanding problems in both particle and astrophysics. In this thesis, I describe a number of complementary searches for particle dark matter. I discuss how the impact of dark matter on stars can constrain its interaction with nuclei, focussing on main sequence stars close to the Galactic Centre, and on the first stars as seen through the upcoming James Webb Space Telescope. The mass and annihilation cross-section of dark matter particles can be probed with searches for gamma rays produced in astronomical targets. Dwarf galaxies and ultracompact, primordially-produced dark matter minihalos turn out to be especially promising in this respect. I illustrate how the results of these searches can be combined with constraints from accelerators and cosmology to produce a single global fit to all available data. Global fits in supersymmetry turn out to be quite technically demanding, even with the simplest predictive models and the addition of complementary data from a bevy of astronomical and terrestrial experiments; I show how genetic algorithms can help in overcoming these challenges.
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| 25. |
- van den Bossche, Maxime, 1989
(författare)
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Methane oxidation over palladium oxide. From electronic structure to catalytic conversion
- 2017
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Understanding how catalysts work down to the atomic level can provide ways to improve chemical processes on which our contemporary economy is heavily reliant. The oxidation of methane is one such example, which is important from an environmental point of view. Methane is a potent greenhouse gas and natural and biogas vehicles need efficient catalysts to prevent slip of uncombusted fuel into the exhaust. Commercial catalysts for methane oxidation are often based on palladium or platinum. Metallic palladium, however, is easily converted to palladium oxide when the engine is operated at oxygen rich conditions. In this thesis, various aspects of complete methane oxidation over PdO(101) are investigated with computational methods based on density functional theory (DFT). PdO(101) is the active surface for methane oxidation, and firstly, the reaction intermediates CO and H are studied in detail. Possible pathways for H2 adsorption, dissociation and eventual water formation are investigated, in connection to core-level spectroscopy experiments. Similarly, the adsorption configurations for carbon monoxide on clean and oxidized palladium are examined with a combination of DFT calculations, core-level and infrared spectroscopy. Secondly, a detailed kinetic model is constructed that describes the catalytic conversion of CH4 to CO2 and H2O over PdO(101). This is done in a first-principles microkinetics framework, where the kinetic parameters are obtained by applying density functional and transition state theory. The kinetic model provides a fundamental understanding of findings from reactor experiments, such as the rate limiting steps and poisoning behaviour, and shows qualitatively different behaviour of adsorbates on oxide as compared to metal surfaces. Lastly, limitations of the commonly used class of generalized gradient functionals are illustrated in the computation of several properties of adsorbates on metal oxide surfaces. These include core-level shifts and thermodynamic and reactive properties of adsorbates on the PdO(101) surface. Similarly, the description of several molecular and cooperative adsorption processes are also found to be sensitive to the applied exchange-correlation functional on the BaO(100), TiO2(110) and CeO2(111) surfaces.
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