| 1. |
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| 2. |
- Besharat, Zahra, et al.
(författare)
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Se-C Cleavage of Hexane Selenol at Steps on Au(111)
- 2018
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Ingår i: Langmuir. - : American Chemical Society (ACS). - 0743-7463 .- 1520-5827. ; 34:8, s. 2630-2636
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Tidskriftsartikel (refereegranskat)abstract
- Selenols are considered as an alternative to thiols in self-assembled monolayers, but the Se-C bond is one limiting factor for their usefulness. In this study, we address the stability of the Se-C bond by a combined experimental and theoretical investigation of gas phase-deposited hexane selenol (CH3(CH2)(5)SeH) on Au(111) using photoelectron spectroscopy, scanning tunneling microscopy, and density functional theory (DFT). Experimentally, we find that initial adsorption leaves atomic Se on the surface without any carbon left on the surface, whereas further adsorption generates a saturated selenolate layer. The Se 3d component from atomic Se appears at 0.85 eV lower binding energy than the selenolate-related component. DFT calculations show that the most stable structure of selenols on Au(111) is in the form of RSe-Au-SeR complexes adsorbed on the unreconstructed Au(111) surface. This is similar to thiols on Au(111). Calculated Se 3d core-level shifts between elemental Se and selenolate in this structure nicely reproduce the experimentally recorded shifts. Dissociation of RSeH and subsequent formation of RH are found to proceed with high barriers on defect-free Au(111) terraces, with the highest barrier for scissoring R-Se. However, at steps, these barriers are considerably lower, allowing for Se-C bond breaking and hexane desorption, leaving elemental Se at the surface. Hexane is the selenol to selenolate formed by replacing the Se-C bond with a H-C bond by using the hydrogen liberated from transformation.
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| 3. |
- Ghadami Yazdi, Milad, et al.
(författare)
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Naphthalene on Ni(111) : experimental and theoretical insights into adsorption, dehydrogenation and carbon passivation
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- An attractive solution to mitigate tars and also to decompose lighter hydrocarbons in biomass gasification is secondary catalytic reforming, converting hydrocarbons to useful permanent gases. Albeit in use for long time in fossil feedstock catalytic steam reforming, the understanding of the catalytic processes is still limited. Naphthalene is typically present in the biomass gasification gas and to further understand the elementary steps of naphthalene transformation, we investigated the temperature dependent naphthalene adsorption, dehydrogenation and passivation on Ni(111). TPD (temperature programmed desorption) and STM (scanning tunneling microscopy) in ultra-high vacuum environment from 110 K up to 780 K, combined with DFT (density functional theory) were used in the study. Room temperature adsorption results in a flat naphthalene monolayer. DFT favors the di-bridge[7] geometry but the potential energy surface is rather smooth. DFT also reveals a pronounced dearomatization and charge transfer from the adsorbed molecule into the nickel surface. Dehydrogenation occurs in two steps, with two desorption peaks at approximately 450 K and 600 K. The first step is due to partial dehydrogenation generating active hydrocarbon species that at higher temperatures migrates over the surface forming graphene. The graphene formation is accompanied by desorption of hydrogen in the high temperature TPD peak. The formation of graphene effectively passivates the surface both for hydrogen adsorption and naphthalene dissociation. In conclusion, the obtained results on the model naphthalene and Ni(111) system, provides insight into elementary steps of naphthalene adsorption, dehydrogenation and carbon passivation, which may serve as a good starting point for rational design, development and optimization of the Ni catalyst surface, as well as process conditions, for the aromatic hydrocarbon reforming process.
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| 4. |
- Ghadami Yazdi, Milad, et al.
(författare)
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Structure dependent effect of silicon on the oxidation of Al(111) and Al(100)
- 2019
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Ingår i: Surface Science. - : Elsevier. - 0039-6028 .- 1879-2758. ; 684, s. 1-11
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Tidskriftsartikel (refereegranskat)abstract
- The effect of sub-monolayer silicon on the oxidation of Al(111) and Al(100) surfaces was investigated using X-ray Photoelectron Spectroscopy (XPS) and density functional theory (DFT) calculations. On both surfaces the adatom site is preferred over substituting Si into the Al-lattice; on Al(100) the four fold hollow site is vastly favored whereas on Al(111) bridge and hollow sites are almost equal in energy. Upon O 2 exposure, Si is not oxidized but buried at the metal/oxide interface under the growing aluminum oxide. On Al(111), Si has a catalytic effect on both the initial oxidation by aiding in creating a higher local oxygen coverage in the early stages of oxidation and, in particular, at higher oxide coverages by facilitating lifting Al from the metal into the oxide. The final oxide, as measured from the Al2p intensity, is 25–30% thicker with Si than without. This observation is valid for both 0.1 monolayer (ML) and 0.3 ML Si coverage. On Al(100), on the other hand, at 0.16 ML Si coverage, the initial oxidation is faster than for the bare surface due to Si island edges being active in the oxide growth. At 0.5 ML Si coverage the oxidation is slower, as the islands coalesce and he amount of edges reduces. Upon oxide formation the effect of Si vanishes as it is overgrown by Al 2 O 3 , and the oxide thickness is only 6% higher than on bare Al(100), for both Si coverages studied. Our findings indicate that, in addition to a vanishing oxygen adsorption energy and Mott potential, a detailed picture of atom exchange and transport at the metal/oxide interface has to be taken into account to explain the limiting oxide thickness.
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| 5. |
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| 6. |
- Marks, Kess, et al.
(författare)
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Investigation of the surface species during temperature dependent dehydrogenation of naphthalene on Ni(111)
- 2019
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 150:24
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Tidskriftsartikel (refereegranskat)abstract
- The temperature dependent dehydrogenation of naphthalene on Ni(111) has been investigated using vibrational sum-frequency generation spectroscopy, X-ray photoelectron spectroscopy, scanning tunneling microscopy, and density functional theory with the aim of discerning the reaction mechanism and the intermediates on the surface. At 110 K, multiple layers of naphthalene adsorb on Ni(111); the first layer is a flat lying chemisorbed monolayer, whereas the next layer(s) consist of physisorbed naphthalene. The aromaticity of the carbon rings in the first layer is reduced due to bonding to the surface Ni-atoms. Heating at 200 K causes desorption of the multilayers. At 360 K, the chemisorbed naphthalene monolayer starts dehydrogenating and the geometry of the molecules changes as the dehydrogenated carbon atoms coordinate to the nickel surface; thus, the molecule tilts with respect to the surface, recovering some of its original aromaticity. This effect peaks at 400 K and coincides with hydrogen desorption. Increasing the temperature leads to further dehydrogenation and production of H-2 gas, as well as the formation of carbidic and graphitic surface carbon. Published under license by AIP Publishing.
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| 7. |
- Marks, Kess, 1987-, et al.
(författare)
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Naphthalene Dehydrogenation on Ni(111) in the Presence of Chemisorbed Oxygen and Nickel Oxide
- 2024
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Ingår i: Catalysts. - : MDPI AG. - 2073-4344. ; 14:2
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Tidskriftsartikel (refereegranskat)abstract
- Catalyst passivation through carbon poisoning is a common and costly problem as it reduces the lifetime and performance of the catalyst. Adding oxygen to the feed stream could reduce poisoning but may also affect the activity negatively. We have studied the dehydrogenation, decomposition, and desorption of naphthalene co-adsorbed with oxygen on Ni(111) by combining temperature-programmed desorption (TPD), sum frequency generation spectroscopy (SFG), photoelectron spectroscopy (PES), and density functional theory (DFT). Chemisorbed oxygen reduces the sticking of naphthalene and shifts H2 production and desorption to higher temperatures by blocking active Ni sites. Oxygen increases the production of CO and reduces carbon residues on the surface. Chemisorbed oxygen is readily removed when naphthalene is decomposed. Oxide passivates the surface and reduces the sticking coefficient. But it also increases the production of CO dramatically and reduces the carbon residues. Ni2O3 is more active than NiO.
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| 8. |
- Saleemi, Mohsin, et al.
(författare)
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Effect of particles size and surface modification on thermal conductivity and viscosity of alumina nanofluids
- 2013
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Konferensbidrag (refereegranskat)abstract
- Electronics industry growing faster and it demands ultrahigh performance cooling systems to manage the heat loses in terms of energy and money. Conventional cooling fluids are approaching to its limit due to the poor thermal transport performance and a new era for the heat transfer fluids had been initiated about two decades ago. When nanoparticles dispersed in conventional heat transfer fluid (like water, oil, glycols), the mixture is called as nanofluids. Alumina suspensions are well known class of nanofluids, which have been investigated in many recent studies to determine the non-classical behavior of the suspensions. The aim of this study is to investigate optimized particle size and suitable surface modification for the improved dispersion properties of nanofluids with enhanced thermal performance and low viscosity. We have utilized two different types of alumina crystal phases; one is Boehmite (γ-AlOOH) and clay type (α -Al2O3) and the nanofluids were prepare d by suspending different size of nanoparticles in water and water/ethylene glycol (EG) mixtures. Dynamic light scattering (DLS) was used to determine the agglomerate size and scanning electron microscope (SEM) used to study the particle size and morphology. Zeta potential was measured to determine the electrostatic stability for the dispersed nanoparticles. Thermal conductivity was estimated by using KD2 Pro setup and up to 10 % enhancement in TC was observed as compared to the base fluid. Viscosity was measured by capillary viscometer, which shows the significant effect from the addition of additives and surfactants. Possible mechanisms contributing in reducing the viscosity and increasing the thermal conductivity are described in details.
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| 9. |
- Sassa, Yasmine, 1981, et al.
(författare)
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Kagome-like silicene: A novel exotic form of two-dimensional epitaxial silicon
- 2020
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Ingår i: Applied Surface Science. - : Elsevier BV. - 0169-4332 .- 1873-5584. ; 530
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Tidskriftsartikel (refereegranskat)abstract
- Since the discovery of graphene, intensive efforts have been made in search of novel two-dimensional (2D) materials. Decreasing the materials dimensionality to their ultimate thinness is a promising route to unveil new physical phenomena, and potentially improve the performance of devices. Among recent 2D materials, analogs of graphene, the group IV elements have attracted much attention for their unexpected and tunable physical properties. Depending on the growth conditions and substrates, several structures of silicene, germanene, and stanene can be formed. Here, we report the synthesis of a Kagome-like lattice of silicene on aluminum (1 1 1) substrates. We provide evidence of such an exotic 2D Si allotrope through scanning tunneling microscopy (STM) observations, high-resolution core-level (CL) and angle-resolved photoelectron spectroscopy (ARPES) measurements, along with Density Functional Theory calculations.
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| 10. |
- Soldemo, Markus, et al.
(författare)
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The Surface Structure of Cu2O(100)
- 2016
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 120:8, s. 4373-4381
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Tidskriftsartikel (refereegranskat)abstract
- Despite the industrial importance of copper oxides, the nature of the (100) surface of Cu2O has remained poorly understood. The surface has previously been subject to several theoretical and experimental studies, but has until now not been investigated by atomically resolved microscopy or high-resolution photoelectron spectroscopy. Here we determine the atomic structure and electronic properties of Cu2O(100) by a combination of multiple experimental techniques and simulations within the framework of density functional theory (DFT). Low-energy electron diffraction (LEED) and scanning tunneling microscopy (STM) characterized the three ordered surface structures found. From DFT calculations, the structures are found to be energetically ordered as (3,0;1,1), c(2 x 2), and (1 x 1) under ultrahigh vacuum conditions. Increased oxygen pressures induce the formation of an oxygen terminated (1 x 1) surface structure. The most common termination of Cu2O(100) has previously been described by a (3 root 2 x root 2)R45 degrees unit cell exhibiting a LEED pattern with several missing spots. Through atomically resolved STM, we show that this structure instead is described by the matrix (3,0;1,1). Both simulated STM images and calculated photoemission core level shifts compare favorably with the experimental results.
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