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| 2. |
- Annamalai, Alagappan, et al.
(författare)
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Influence of Sb5+ as a Double Donor on Hematite (Fe3+) Photoanodes for Surface-Enhanced Photoelectrochemical Water Oxidation
- 2018
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 10:19, s. 16467-16473
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Tidskriftsartikel (refereegranskat)abstract
- To exploit the full potential of hematite (α-Fe2O3) as an efficient photoanode for water oxidation, the redox processes occurring at the Fe2O3/electrolyte interface need to be studied in greater detail. Ex situ doping is an excellent technique to introduce dopants onto the photoanode surface and to modify the photoanode/electrolyte interface. In this context, we selected antimony (Sb5+) as the ex situ dopant because it is an effective electron donor and reduces recombination effects and concurrently utilize the possibility to tuning the surface charge and wettability. In the presence of Sb5+ states in Sb-doped Fe2O3 photoanodes, as confirmed by X-ray photoelectron spectroscopy, we observed a 10-fold increase in carrier concentration (1.1 × 1020 vs 1.3 × 1019 cm–3) and decreased photoanode/electrolyte charge transfer resistance (∼990 vs ∼3700 Ω). Furthermore, a broad range of surface characterization techniques such as Fourier-transform infrared spectroscopy, ζ-potential, and contact angle measurements reveal that changes in the surface hydroxyl groups following the ex situ doping also have an effect on the water splitting capability. Theoretical calculations suggest that Sb5+ can activate multiple Fe3+ ions simultaneously, in addition to increasing the surface charge and enhancing the electron/hole transport properties. To a greater extent, the Sb5+- surface-doped determines the interfacial properties of electrochemical charge transfer, leading to an efficient water oxidation mechanism.
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| 3. |
- Barbero, David R., et al.
(författare)
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Ultralow Percolation Threshold in Nanoconfined Domains
- 2017
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 11:10, s. 9906-9913
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Tidskriftsartikel (refereegranskat)abstract
- Self-assembled percolated networks play an important role in many advanced electronic materials and devices. In nanocarbon composites, decreasing the percolation threshold phi(c) is of paramount importance to reduce nanotube bundling, minimize material resources and costs, and enhance charge transport. Here we demonstrate that three-dimensional nanoconfinement in single-wall carbon nanotube/polymer nanocomposites produces a strong reduction in phi(c) reaching the lowest value ever reported in this system of phi(c) approximate to 1.8 X 10(-5) wt % and 4-5 orders of magnitude lower than the theoretical statistical percolation threshold oh phi(stat) Moreover, a change in network resistivity and electrical conduction was observed with increased confinement, and a simple resistive model is used to accurately estimate the difference in is in the confined networks. These results are explained in terms of networks' size, confinement, and tube orientation as determined by atomic force microscopy, electrical conductivity measurements, and polarized Raman spectroscopy. Our findings provide important insight into nanoscale percolated networks and should find application in electronic nanocomposites and devices.
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| 4. |
- Barzegar, Hamid Reza, et al.
(författare)
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Self-assembled PCBM nanosheets : a facile route to electronic layer-on-Layer heterostructures
- 2018
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Ingår i: Nano letters (Print). - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 18:2, s. 1442-1447
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Tidskriftsartikel (refereegranskat)abstract
- We report on the self-assembly of semicrystalline [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) nanosheets at the interface between a hydrophobic solvent and water, and utilize this opportunity for the realization of electronically active organic/organic molecular heterostructures. The self-assembled PCBM nanosheets can feature a lateral size of >1 cm2 and be transferred from the water surface to both hydrophobic and hydrophilic surfaces using facile transfer techniques. We employ a transferred single PCBM nanosheet as the active material in a field-effect transistor (FET) and verify semiconductor function by a measured electron mobility of 1.2 × 10–2 cm2 V–1 s–1 and an on–off ratio of ∼1 × 104. We further fabricate a planar organic/organic heterostructure with the p-type organic semiconductor poly(3-hexylthiophene-2,5-diyl) as the bottom layer and the n-type PCBM nanosheet as the top layer and demonstrate ambipolar FET operation with an electron mobility of 8.7 × 10–4 cm2 V–1 s–1 and a hole mobility of 3.1 × 10–4 cm2V–1 s–1.
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| 5. |
- Boulanger, Nicolas, 1986-
(författare)
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Carbon nanotubes and graphene polymer composites for opto-electronic applications
- 2016
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Carbon nanotubes are carbon based structures with outstanding electronical and mechanical properties. They are used in a wide range of applications, usually embedded in polymer in the form of composites, in order to affect the electronic behavior of the matrix material. However, as the nanotubes properties are directly dependent on their intrinsic structure, it is necessary to select specific nanotubes depending on the application, which can be a complicated and inefficient process. This makes it attractive to be able to reduce the amount of material used in the composites.In this thesis, focus is placed on the electrical properties of the composites. A simple patterning method is presented which allows the use of extremely low amounts of nanotubes in order to increase the electrical conductivity of diverse polymers such as polystyrene (PS) or poly(3-hexylthiophene) (P3HT). This method is called nanoimprint lithography and uses a flexible mold in order to pattern composite films, leading to the creation of conducting nanotube networks, resulting in vertically conducting samples (from the bottom of the film to the top of the imprinted patterns).In parallel, X-ray diffraction measurements have been conducted on thin P3HT polymer films. These were prepared on either silicon substrate or on graphene, and the influence of the processing conditions as well as of the substrate on the crystallinity of the polymer have been investigated. The knowledge of the crystalline structure of P3HT is of great importance as it influences its electronic properties. Establishing a link between the processing conditions and the resulting crystallinity is therefore vital in order to be able to make opto-electronic devices such as transistor or photovoltaic cells.
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| 6. |
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| 7. |
- Boulanger, Nicolas, et al.
(författare)
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Graphene induced electrical percolation enables more efficient charge transport at a hybrid organic semiconductor/graphene interface
- 2018
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 20:6, s. 4422-4428
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Tidskriftsartikel (refereegranskat)abstract
- Self-assembly of semiconducting polymer chains during crystallization from a liquid or melt dictates to a large degree the electronic properties of the resulting solid film. However, it is still unclear how charge transport pathways are created during crystallization. Here, we performed complementary in situ electrical measurements and synchrotron grazing incidence X-ray diffraction (GIXD), during slow cooling from the melt of highly regio-regular poly(3-hexylthiophene) (P3HT) films deposited on both graphene and on silicon. Two different charge transport mechanisms were identified, and were correlated to the difference in crystallites' orientations and overall amount of crystallites in the films on each surface as molecular self-assembly proceeded. On silicon, a weak charge transport was enabled as soon as the first edge-on lamellae formed, and further increased with the higher amount of crystallites (predominantly edge-on and randomly oriented lamellae) during cooling. On graphene however, the current remained low until a minimum amount of crystallites was reached, at which point interconnection of conducting units (face-on, randomly oriented lamellae and tie-chains) formed percolated conducting pathways across the film. This lead to a sudden rapid increase in current by approximate to 10 fold, and strongly enhanced charge transport, despite a much lower amount of crystallites than on silicon.
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| 8. |
- Boulanger, Nicolas, et al.
(författare)
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In situ probing of the crystallization kinetics of rr-P3HT on single layer graphene as a function of temperature
- 2017
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 19:12, s. 8496-8503
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Tidskriftsartikel (refereegranskat)abstract
- We studied the molecular packing and crystallization of a highly regio-regular semiconducting polymer poly(3-hexylthiophene) (P3HT) on both single layer graphene and silicon as a function of temperature, during cooling from the melt. The onset of crystallization, crystallites' size, orientation, and kinetics of formation were measured in situ by synchrotron grazing incidence X-ray diffraction (GIXD) during cooling and revealed a very different crystallization process on each surface. A favored crystalline orientation with out of plane pi-pi stacking formed at a temperature of 200 degrees C on graphene, whereas the first crystallites formed with an edge-on orientation at 185 degrees C on silicon. The crystallization of face-on lamellae revealed two surprising effects during cooling: (a) a constant low value of the pi-pi spacing below 60 degrees C; and (b) a reduction by half in the coherence length of face-on lamellae from 100 to 30 degrees C, which corresponded with the weakening of the 2nd or 3rd order of the in-plane (k00) diffraction peak. The final ratio of face-on to edge-on orientations was 40% on graphene, and 2% on silicon, revealing the very different crystallization mechanisms. These results provide a better understanding of how surfaces with different chemistries and intermolecular interactions with the polythiophene polymer chains lead to different crystallization processes and crystallites orientations for specific electronic applications.
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| 9. |
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| 10. |
- Ekspong, Joakim, et al.
(författare)
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Surface activation of graphene nanoribbons for oxygen reduction reaction by nitrogen doping and defect engineering : An ab initio study
- 2018
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Ingår i: Carbon. - : Elsevier. - 0008-6223 .- 1873-3891. ; 137, s. 349-357
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Tidskriftsartikel (refereegranskat)abstract
- Introducing heteroatoms and creating structural defects on graphene is a common and rather successful strategy to transform its inert basal plane into an efficient metal-free electrocatalyst for oxygen reduction reaction (ORR). However, the intricate atomic configuration of defective graphenes difficult their optimization as ORR electrocatalysts, where not only a large density of active sites is desirable, but also excellent electrical conductivity is required. Therefore, we used density functional theory to investigate the current-voltage characteristics and the catalytic active sites towards ORR of nitrogen-doped and defective graphene by using 8 zig-zag graphene nanoribbons as model systems. Detailed ORR catalytic activity maps are created for ten different systems showing the distribution of catalytic hot spots generated by each defect. Subsequently, the use of both current-voltage characteristics and catalytic activity maps allow to exclude inefficient systems that exhibit either low electrical conductivity or have adsorption energies far from optimal. Our study highlights the importance of considering not only the interaction energy of reaction intermediates to design electrocatalysts, but also the electrical conductivity of such configurations. We believe that this work is important for future experimental studies by providing insights on the use of graphene as a catalyst towards the ORR reaction.
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