| 1. |
- Abrahams, I., et al.
(författare)
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A Combined Total Scattering and Simulation Approach to Analyzing Defect Structure in Bi3YO6
- 2010
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 1520-5002 .- 0897-4756. ; 22:15, s. 4435-4445
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Tidskriftsartikel (refereegranskat)abstract
- The defect structure and electrical properties of the fast oxide ion-conducting solid electrolyte delta-Bi3YO6 have been studied using a combination of total neutron scattering analysis, energy minimization methods, and AC impedance spectroscopy. Conventional structural analysis using the Rietveld method reveals the oxide ions to be distributed over three crystallographic sites at room temperature, with a small change in this distribution at 800 degrees C. Analysis of short-range correlations using a total neutron scattering approach yields information on Bi and Y coordination environments. Careful analysis of the angular distribution functions derived from reverse Monte Carlo modeling of the total scattering data reveals physical evidence for a predominance of vacancy ordering in this system. This ordering is confirmed as the lowest energy configuration in parallel energy minimization simulations.
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| 2. |
- Agostini, M., et al.
(författare)
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Polysulfide-containing Glyme-based Electrolytes for Lithium Sulfur Battery
- 2015
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 1520-5002 .- 0897-4756. ; 27:13, s. 4604-4611
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Tidskriftsartikel (refereegranskat)abstract
- A new comparative investigation of lithium sulfur cells employing a tetraethylene glycol dimethyl ether-lithium trifluoromethanesulfonate (TEGDME-LiCF3SO3) electrolyte charged by various polysulfide species (Li2S2, Li2S4, Li2S6, and Li2S8) is here reported. We carefully detect the effects of lithium polysulfide addition by originally combining X-ray photoelectron spectroscopy (XPS) and electrochemical impedance spectroscopy (EIS). The measurements clearly reveal how the polysulfide addition affects the nature and composition of the solid electrolyte interphase (SEI) in terms of precipitated S-based species determined by XPS. The study demonstrates that the SEI layer formed on the Li anode decreases in impedance and stabilizes by the presence of polysulfide. This, together with a buffer effect strongly mitigating the sulfur-cathode dissolution and the shuttle reaction, significantly improves the stability of the lithium-sulfur cell. The data here reported clearly suggest the polysulfide as an effective additive to enhance the performance of the lithium-sulfur battery (Graph Presented).
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| 3. |
- Agrios, Alexander George, et al.
(författare)
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Nanostructured composite films for dye-sensitized solar cells by electrostatic layer-by-layer deposition
- 2006
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 18:23, s. 5395-5397
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Tidskriftsartikel (refereegranskat)abstract
- The possibilities for making nanocomposite semiconductor films for DSC using the ELBL method was investigated. Coated slides were cut in half vertically giving two strips that can be subjected to different treatments for comparison. The electrode was heated to 450 °C for 30 min and then Cooled to 80 °C. Scanning electron microscopy of a sintered film with 5 cycles of TiO2 nanoparticles shows that the particles are well distributed and completely cover the transparent conducting oxide substrate. Spectroscopic measurements of a dye-coated film in acetonitrile found a dye concentration within the film of 0.15 mM based on an extinction coefficient. The solar cell including a scattering layer had more than double the current of the transparent layer-only cell. It was observed that ELBL method can produce TiO2 films for DSC with high efficiencies at low thickness.
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| 4. |
- Andrén, Oliver C. J., et al.
(författare)
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Therapeutic Nanocarriers via Cholesterol Directed Self-Assembly of Well-Defined Linear-Dendritic Polymeric Amphiphiles
- 2017
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 29:9, s. 3891-3898
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Tidskriftsartikel (refereegranskat)abstract
- A novel platform of fluorescently labeled nanocarriers (NCs) is herein proposed based on amphiphilic linear-dendritic polymeric hybrids. These sophisticated polymers were synthesized with a high degree of structural control at a macro-molecular level, displayed hydrophobic cholesterol compartments as chain-terminus groups of the dendritic block and hydrophilic bifunctional linear poly(ethylene glycol) (PEG) block. Spherical supramolecular assemblies with therapeutically relevant properties were successfully achieved including (i) sizes in the region of 100 to 200 nm; (ii) narrow dispersity profile with values close to 0.12; and (iii) self-assembly down to nanomolar concentrations. The modular nature of the NCs permitted the encapsulation of single or dual anticancer drugs and in parallel provide intracellular fluorescent traceability. As polymer therapeutics, the NCs were proven to penetrate the cancerous cell membranes and deliver the cargo of drugs into the nuclei as well as the cytoplasm and mitochondria. The dual drug delivery of both doxorubicin (DOX) and triptolide substantially enhanced the therapeutic efficacy with a 63% significant increase against resistant breast cancer cells when compared to free DOX.
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| 5. |
- Anselmo, Ana Sofia, 1980-, et al.
(författare)
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Tuning the Vertical Phase Separation in Polyfluorene: Fullerene Blend Films by Polymer Functionalization
- 2011
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Ingår i: Chemistry of Materials. - Washington : American Chemical Society (ACS). - 1520-5002 .- 0897-4756. ; 23:9, s. 2295-2302
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Tidskriftsartikel (refereegranskat)abstract
- Achieving control over the nanomorphology of blend films of the fullerene derivative [6,6]-phenyl C61-butyric acid methyl ester, PCBM, with light-absorbing conjugated polymers is an important challenge in the development of efficient solution-processed photovoltaics. Here, three new polyfluorene copolymers are presented, tailored for enhanced miscibility with the fullerene through the introduction of polymer segments with modified side chains, which enhance the polymer's polar character. The composition of the spincoated polymer:PCBM films is analyzed with dynamic secondary ion mass spectrometry (dSIMS). The dSIMS depth profiles demonstrate compositional variations perpendicular to the surface plane, as a result of vertical phase separation, directed by the substrate. These variations propagate to a higher degree through the film for the polymers with a larger fraction of modified side chains. The surface composition of the films is studied by Near-edge X-ray absorption fine structure spectroscopy (NEXAFS). Quantitative analysis of the NEXAFS spectra through a linear combination fit with the spectra of the pure components yields the surface composition. The resulting blend ratios reveal polymer-enrichment of the film surface for all three blends, which also becomes stronger as the polar character of the polymer increases. Comparison of the NEXAFS spectra collected with two different sampling depths shows that the vertical composition gradient builds up already in the first nanometers underneath the surface of the films. The results obtained with this new series of polymers shed light on the onset of formation of lamellar structures in thin polymer:PCBM films prepared from highly volatile solvents.
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| 6. |
- Arcos, D., et al.
(författare)
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Ordered Mesoporous Microspheres for Bone Grafting and Drug Delivery
- 2009
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 21:6, s. 1000-1009
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Tidskriftsartikel (refereegranskat)abstract
- Bioactive microspheres with ordered mesoporous structure have been synthesized by means of the evaporation-induced self-assembly (EISA) method and following an aerosol-assisted route. The bioactive microspheres belong to the SiO2-CaO-P2O5 systems, and the mesoporous structure closely depends on the structure-directing agent as well as its interaction with the Ca2+ cations during the mesophase formation. Among the different tested surfactants, the triblock copolymer F127 leads to hexagonal ordered structures for low CaO contents, P123 leads to wormlike mesoporous structures for any CaO content, whereas the ionic surfactant cetyltrimethyl ammonium bromide (C16TAB) does not produce accessible mesopores at the external surface, for any CaO content. All the mesoporous SiO2-CaO-P2O5 microspheres develop an apatite like layer when reacting with simulated body fluid. Preliminary tests indicate the capability to load and release triclosan with kinetic profiles that depend on the pore structure, thus showing interesting features to be used in periodontal regenerative surgery and infection profilaxis.
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| 7. |
- Arnbjerg, Lene M., et al.
(författare)
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Structure and Dynamics for LiBH4-LiCl Solid Solutions
- 2009
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 21:24, s. 5772-5782
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Tidskriftsartikel (refereegranskat)abstract
- A Surprisingly high degree of structural and compositional dynamics is observed in the system LiBH4-LiCl as a function of temperature and time. Rietveld refinement of synchrotron radiation powder X-ray diffraction (SR-PXD) data reveals that Cl- readily substitutes for BH4- in the Structure of LiBH4. Prolonged heating a sample of LiBH4-LiCl (1:1 molar ratio) above the phase transition temperature and below the melting point (108 < T < 275 degrees C) can produce highly chloride substituted hexagonal lithium borohydride, h-Li(BH4)(l-x)Cl-x, e.g., x similar to 0.42, after heating from room temperature (RT) to 224 degrees C at 2.5 degrees C/min. LiCl has a higher solubility in h-LiBH4 its compared to orthorhombic lithium borohydride, o-LiBH4, which is illustrated by a LiBH4-LiCl (1:1) sample equilibrated at 245 degrees C for 24 days and left at RT for another 13 months. Rietveld refinement reveals that this sample contains o-Li(BH4)(0.91)Cl-0.09 and LiCl. This illustrates a significantly faster dissolution of LiCl in h-LiBH4 its compared to a slower segregation of LiCl from o-LiBH4, which is also demonstrated by in situ SR-PXD from three cycles of heating and cooling of the same Li(BH4)(0.91)Cl-0.09 sample. The substitution of the smaller Cl- for the larger BH4- ion is clearly observed as a reduction in the unit cell volume as a function of time and temperature. A significant stabilization of h-LiBH4 is found to depend on the degree of anion substitution. Variable temperature solid-state magic-angle spinning (MAS) Li-7 and B-13 NMR experiments oil pure LiBH4 show an increase in full width at half maximum (fwhm) when approaching the phase transition from o- to h-LiBH4, which indicates an increase of the relaxation rate (i.e. T-2 decreases). A less pronounced effect is observed for ion-substituted Li(BH4)(1-x)Cl-x, 0.09 < x < 0.42. The MAS NMR experiments also demonstrate a higher degree of motion in the hexagonal phase, i.e., fwhm is reduced by more than a Factor of 10 at the o- to h-LiBH4 phase transition.
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| 8. |
- Arvizu, Miguel A, et al.
(författare)
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Electrochromic W(1-x-y)Ti(x)lo(y)O(3) Thin Films Made by Sputter Deposition : Large Optical Modulation, Good Cycling Durability, and Approximate Color Neutrality
- 2017
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 29:5, s. 2246-2253
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Tidskriftsartikel (refereegranskat)abstract
- Tungsten oxide thin films are used in electrochromic devices such as variable-transmittance "smart windows" for energy efficient buildings with good indoor comfort. Two long-standing issues for WO3 thin films are their limited durability under electrochemical cycling and their blue color in transmission. Here, we show that both of these problems can be significantly alleviated by additions of titanium and molybdenum. We found that similar to 300 nm-thick films of sputter deposited W1-x-yTixMoyO3 are able to combine a midluminous transmittance modulation of 0.4 similar to 70% with good color neutrality and durability under extended electrochemical cycling. The Ti content should be similar to 10 at. % in order to achieve durability without impairing transmittance modulation significantly, and the Mo content preferably should be no larger than 6 at. % in order to maintain durability. Hence, our results give clear guidelines for making three-component mixed-oxide thin films that are suitable for electrochromic "smart windows".
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| 9. |
- Atluri, Rambabu, 1981-, et al.
(författare)
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Hydrothermal Phase Transformation of Bicontinuous Cubic Mesoporous Material AMS-6
- 2008
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 20:12, s. 3857–3866-
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Tidskriftsartikel (refereegranskat)abstract
- The controlled synthesis of ordered anionic surfactant templated mesoporous silica with cubic Ia3d̅ structure (AMS-6) is reported via prolonged periods of hydrothermal treatment (HT). The cubic Ia3d̅ mesophase transforms to hexagonal p6mm after 8 days of HT at 100 °C. Surprisingly, the hexagonal phase is stable only for a limited period after which a reversal to the cubic Ia3d̅ mesostructure is observed. Characterization methods such as powder X-ray diffraction (XRD), electron microscopy (SEM, TEM), N2-isotherms, magic-angle spinning (MAS) 29Si NMR spectroscopy, and thermogravimetric analysis (TGA) have been employed to follow structural and textural changes of the materials prepared. Data show that the resultant mesostructure and its textural properties are highly dependent on the period of HT with less unit-cell shrinkage on calcination after extensive HT. Furthermore, evidence of two different solid−solid phase mechanisms during HT is presented. The initial transition is consistent with a restructuring of the surfactant packing and a depletion of the organic moieties from the organo-silica wall as evident from 29Si NMR spectroscopy. The return to the bicontinuous cubic phase is driven by changes in charge matching at the organic−inorganic interface as a result of increases in the polymerization of the silica wall. The textural properties, and in particular the presence or absence of surface porosity, has been controlled through variations in hydrothermal treatment. These are associated with specific growth directions of cubic AMS-6 crystals. The synthetic method described allows us to easily prepare phase pure and intermediate mesostructured nanoparticles.
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| 10. |
- Bai, Sai, et al.
(författare)
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Reproducible Planar Heterojunction Solar Cells Based on One-Step Solution-Processed Methylammonium Lead Halide Perovskites
- 2017
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Ingår i: Chemistry of Materials. - : AMER CHEMICAL SOC. - 0897-4756 .- 1520-5002. ; 29:1, s. 462-473
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Tidskriftsartikel (refereegranskat)abstract
- Metal halide perovskites have been demonstrated as one of the most promising materials for low-cost and high-performance photovoltaic applications. However, due to the susceptible crystallization process of perovskite films on planar substrates and the high sensitivity of the physical and optoelectronic nature of the internal interfaces within the devices, researchers in different laboratories still experience poor reproducibility in fabricating efficient perovskite solar cells with planar heterojunction device structures. In this method paper, we present detailed information on the reagents, equipment, and procedures for the fabrication of planar perovskite solar cells in both "regular" n-i-p and "inverted" p-i-n architectures based on one-step solution-processed methylammonium lead triiodide (MAPbI(3)) perovskite films. We discuss key parameters affecting the crystallization of perovskite and the device interfaces. This method paper will provide a guideline for the reproducible fabrication of planar heterojunction solar cells based on MAPbI3 perovskite films. We believe that the shared experience on MA-based perovskite films and planar solar cells will be also useful for the optimization process of perovskites with varied compositions, and other emerging perovskite-based optoelectronic devices.
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| 11. |
- Banerjee, Hrishit, et al.
(författare)
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Cationic Effect on Pressure Driven Spin-State Transition and Cooperativity in Hybrid Perovskites
- 2016
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 28:22, s. 8379-8384
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Tidskriftsartikel (refereegranskat)abstract
- Hybrid or metal organic framework (MOP) perovskites of general composition, ABX(3), are known to show interesting properties that can lead to a variety of technological applications. Our first-principles study shows they are also potential candidates for exhibiting cooperative spin-state transitions upon application of external stimuli. We demonstrate this by considering two specific Fe-based MOF perovskites, namely dimethylammonium iron formate, [CH3NH2CH3][Fe(HCOO)(3)], and hydroxylammonium iron formate, [NH3OH][Fe(HCOO)(3)]. Both the compounds are found to undergo high-spin (S = 2) to low-spin (S = 0) transition at Fe(II) site upon application of moderate strength of hydrostatic pressure, along with large hysteresis. This spin-state transition is signaled by the changes in electronic, magnetic, and optical properties. We find both the transition pressure and the width of the hysteresis to be strongly dependent on the choice of A-site cation, dimethylammonium or hydroxylammonium, implying that tuning of spin-switching properties is achievable by chemical variation of the amine cation in the structure. Our findings open up novel functionalities in this family of materials of recent interest, which can have important usage in sensors and memory devices.
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| 12. |
- Bellani, Sebastiano, et al.
(författare)
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Graphene-Based Electrodes in a Vanadium Redox Flow Battery Produced by Rapid Low-Pressure Combined Gas Plasma Treatments
- 2021
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 33:11, s. 4106-4121
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Tidskriftsartikel (refereegranskat)abstract
- The development of high-power density vanadium redox flow batteries (VRFBs) with high energy efficiencies (EEs) is crucial for the widespread dissemination of this energy storage technology. In this work, we report the production of novel hierarchical carbonaceous nanomaterials for VRFB electrodes with high catalytic activity toward the vanadium redox reactions (VO2+/VO2+ and V2+/V3+). The electrode materials are produced through a rapid (minute timescale) low-pressure combined gas plasma treatment of graphite felts (GFs) in an inductively coupled radio frequency reactor. By systematically studying the effects of either pure gases (O-2 and N-2) or their combination at different gas plasma pressures, the electrodes are optimized to reduce their kinetic polarization for the VRFB redox reactions. To further enhance the catalytic surface area of the electrodes, single-/fewlayer graphene, produced by highly scalable wet-jet milling exfoliation of graphite, is incorporated into the GFs through an infiltration method in the presence of a polymeric binder. Depending on the thickness of the proton-exchange membrane (Nafion 115 or Nafion XL), our optimized VRFB configurations can efficiently operate within a wide range of charge/discharge current densities, exhibiting energy efficiencies up to 93.9%, 90.8%, 88.3%, 85.6%, 77.6%, and 69.5% at 25, 50, 75, 100, 200, and 300 mA cm(-2), respectively. Our technology is cost-competitive when compared to commercial ones (additional electrode costs < 100 (sic) m(-2)) and shows EEs rivalling the record-high values reported for efficient systems to date. Our work remarks on the importance to study modified plasma conditions or plasma methods alternative to those reported previously (e.g., atmospheric plasmas) to improve further the electrode performances of the current VRFB systems.
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| 13. |
- Bi, Chenghao, et al.
(författare)
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Stable CsPb1- xZn xI3Colloidal Quantum Dots with Ultralow Density of Trap States for High-Performance Solar Cells
- 2020
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 32:14, s. 6105-6113
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Tidskriftsartikel (refereegranskat)abstract
- All inorganic halide perovskites in the form of colloidal quantum dots (QDs) have come into people's view as one of the potential materials for the high-efficiency solar cells; nevertheless, the high surface trap density and poor stability of QDs restrict the performance improvement and application. Here, we obtain colloidal inorganic perovskite CsPb1-xZnxI3 QDs by the hot-injection synthesis process with the addition of ZnCl2. Synchrotron-based X-ray absorption fine structures demonstrate that the guest Zn2+ ions are doped into the CsPbI3 structure to improve the local ordering of the lattice of the perovskite, reducing the octahedral distortions. The increase of the Goldschmidt tolerance factor and the Pb-I bond energy also enhance the stability of the perovskite structure. Furthermore, the Cl- ions from ZnCl2 occupy the iodide vacancies of the perovskite to decrease the nonradiative recombination. The synergistic effect of doping and defect passivation makes for stable colloidal CsPb0.97Zn0.03I3 QDs with ultralow density of trap states. The champion solar cell based on the QDs shows a power conversion efficiency of 14.8% and a largely improved stability under ambient conditions.
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| 14. |
- Bilousov, Oleksandr V., et al.
(författare)
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Atomic Layer Deposition of Cubic and Orthorhombic Phase Tin Monosulfide
- 2017
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Ingår i: Chemistry of Materials. - : AMER CHEMICAL SOC. - 0897-4756 .- 1520-5002. ; 29:7, s. 2969-2978
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Tidskriftsartikel (refereegranskat)abstract
- Tin monosulfide (SnS) is a promising light-absorbing material with weak environmental constraints for application in thin film solar cells. In this paper, we present low-temperature atomic layer deposition (ALD) of high-purity SnS of both cubic and orthorhombic phases. Using tin(II) 2,4-pentanedionate [Sn(acac)(2)] and hydrogen sulfide (H2S) as precursors, controlled growth of the two polymorphs is achieved. Quartz crystal microbalance measurements are used to establish saturated conditions and show that the SnS ALD is self-limiting over temperatures from at least 80 to 160 degrees C. In this temperature window, a stable mass gain of 19 ng cm(-2) cycle(-1) is observed. The SnS thin film crystal structure and morphology undergo significant changes depending on the conditions. High-resolution transmission electron microscopy and X-ray diffraction demonstrate that fully saturated growth requires a large H2S dose and results in the cubic phase. Smaller H2S doses and higher temperatures favor the orthorhombic phase. The optical properties of the two polymorphs differ significantly, as demonstrated by spectroscopic ellipsometry. The orthorhombic phase displays a wide (0.3-0.4 eV) Urbach tail in the near-infrared region, ascribed to its nanoscale structural disorder and/or to sulfur vacancy-induced gap states. In contrast, the cubic phase is smooth and void-free and shows a well-defined, direct forbidden-type bandgap of 1.64 eV.
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| 15. |
- Bilousov, Oleksandr V., et al.
(författare)
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Substrate Effects on Crystal Phase in Atomic Layer Deposition of Tin Monosulfide
- 2021
-
Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 33:8, s. 2901-2912
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Tidskriftsartikel (refereegranskat)abstract
- Obtaining single-phase tin monosulfide (SnS) films at low temperatures is challenging since cubic (π-SnS) and orthorhombic (α-SnS) polymorphs have similar energies of formation and grow under similar conditions. Here, we show that in atomic layer deposition (ALD) of polycrystalline SnS using tin(II) acetylacetonate and H2S precursors, the substrate surface greatly influences the SnS phase evolution. For example, a silicon (100) substrate, with a highly hydroxylated surface, favors the growth of α-SnS. Meanwhile, ozone treatment or preannealing of the same substrate leads to mainly π-SnS. Just a few ALD cycles of another oxide or sulfide can even more substantially alter the outcome. Substrates that favor α-SnS growth typically produce initially enhanced growth rates, while those promoting π-SnS are partially surface-poisoned by the acetylacetonate precursor ligands. Growth of either polymorph is self-sustained after its initiation, and the sustaining factor appears to be the surface–ligand interaction; π-SnS preferentially evolves on substrates and π-SnS surfaces that are rich in highly reactive dangling bonds, while chemically inert substrates and α-SnS surfaces promote α-SnS. While lattice matching is less central, the role of ligand bonding in SnS ALD also helps explain the previously reported phase dependence on growth temperature and H2S precursor dose and shows promise for area-selective ALD of SnS.
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| 16. |
- Björk, Jonas, et al.
(författare)
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Functionalizing MXenes by Tailoring Surface Terminations in Different Chemical Environments
- 2021
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Ingår i: Chemistry of Materials. - : American Chemical Society. - 0897-4756 .- 1520-5002. ; 33:23, s. 9108-9118
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Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional metal carbides and nitrides-MXenes-represent a group of materials which have attained growing attention over the last decade due to their chemical versatility, making them highly promising in areas such as energy storage, superconductivity, and heterogenous catalysis. Surface terminations are a natural consequence of the MXene synthesis, conventionally consisting of O, OH, and F. However, recent studies have extended the chemical domain of the surface terminations to other elements, and they should be considered as an additional parameter governing the MXene properties. There is a shortfall in the understanding of how various chemical species could act as terminations on different MXenes. In particular, there is limited comprehension in which chemical environments different terminations are stable. Here, we present an extensive theoretical study of the surface terminations of MXenes in different atmospheres by considering in total six experimentally achieved MXenes (Ti2C, Nb2C, V2C, Mo2C, Ti3C2, and Nb4C3) and twelve surface terminations (O, OH, N, NH, NH2, S, SH, H, F, Cl, Br, and I). We consider fully terminated (single termination) MXenes and also the impact of substituting individual terminations. Our study provides insights into what terminations are stable on which MXenes in different chemical environments, with predictions of how to obtain single-termination MXenes and which MXenes are resilient under ambient conditions. In addition, we propose synthesis protocols of MXenes which have not yet been realized in experiments. It is anticipated that alongside the development of new synthesis routes, our study will provide design rules for how to tailor the surface terminations of MXenes.
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| 17. |
- Blidberg, Andreas, 1987-, et al.
(författare)
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Monitoring LixFeSO4F (x = 1, 0.5, 0) Phase Distributions in Operando To Determine Reaction Homogeneity in Porous Battery Electrodes
- 2017
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Ingår i: Chemistry of Materials. - : American Chemical Society. - 0897-4756 .- 1520-5002. ; 29:17, s. 7159-7169
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Tidskriftsartikel (refereegranskat)abstract
- Increasing the energy and power density simultaneously remains a major challenge for improving electrochemical energy storage devices such as Li-ion batteries. Understanding the underlying processes in operating electrodes is decisive to improve their performance. Here, an extension of an in operando X-ray diffraction technique is presented, wherein monitoring the degree of coexistence between crystalline phases in multiphase systems is used to investigate reaction homogeneity in Li-ion batteries. Thereby, a less complicated experimental setup using commercially available laboratory equipment could be employed. By making use of the intrinsic structural properties of tavorite type LiFeSO4F, a promising cathode material for Li-ion batteries, new insights into its nonequilibrium behavior are gained. Differences in the reaction mechanism upon charge and discharge are shown; the influence of adequate electronic wiring for the cycling stability is demonstrated, and the effect of solid state transport on rate performance is highlighted. The methodology is an alternative and complementary approach to the expensive and demanding techniques commonly employed for time-resolved studies of structural changes in operating battery electrodes. The multiphase behavior of LiFeSO4F is commonly observed for other insertion type electrode materials, making the methodology transferable to other new energy storage materials. By expanding the possibilities for investigating complex processes in operating batteries to a larger community, faster progress in both electrode development and fundamental material research can be realized.
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| 18. |
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| 19. |
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| 20. |
- Brandell, Daniel, et al.
(författare)
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Conduction Mechanisms in Crystalline LiPF6·PEO6 Doped with SiF62- and SF6
- 2005
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Ingår i: Chem. Mater. - : American Chemical Society (ACS). ; 17:14, s. 3673-3680
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Tidskriftsartikel (refereegranskat)abstract
- Molecular dynamics (MD) simulations have been made under imposed electric fields for crystalline LiPF6·PEO6, (LiPF6)1-x(Li2SiF6)x·PEO6, and (LiPF6)1-x(SF6)x·PEO6 for x = 0.01 under standard pressure and temperature conditions with the aim of identifying the conduction mechanisms in the systems. Contrary to the results of earlier experimental investigations where only cation mobility was observed, ionic transport is here found to occur in regions between the polymer hemi-helices, with a high transference number (0.9-1.0) for the PF6- anions.
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| 21. |
- Brant, William, et al.
(författare)
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Selective Control of Composition in Prussian White for Enhanced Material Properties
- 2019
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Ingår i: Chemistry of Materials. - : AMER CHEMICAL SOC. - 0897-4756 .- 1520-5002. ; 31:18, s. 7203-7211
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Tidskriftsartikel (refereegranskat)abstract
- Sodium-ion batteries based on Prussian blue analogues (PBAs) are ideal for large-scale energy storage applications due to the ability to meet the huge volumes and low costs required. For Na2-xFe[Fe(CN)(6)](1-y)center dot zH(2)O, realizing its commercial potential means fine control of the concentration of sodium, Fe(CN)(6) vacancies, and water content. To date, there is a huge variation in the literature of composition leading to variable electrochemical performance. In this work, we break down the synthesis of PBAs into three steps for controlling the sodium, vacancy, and water content via an inexpensive, scalable synthesis method. We produce rhombohedral Prussian white Na1.88(5)Fe[Fe-(CN)(6)]center dot 0.18(9)H2O with an initial capacity of 158 mAh/g retaining 90% capacity after 50 cycles. Subsequent characterization revealed that the increased polarization on the 3 V plateau is coincident with a phase transition and reduced utilization of the high-spin Fe(III)/Fe(II) redox couple. This reveals a clear target for subsequent improvements of the material to boost long-term cycling stability. These results will be of great interest for the myriad of applications of PBAs, such as catalysis, magnetism, electrochromics, and gas sorption.
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| 22. |
- Brorsson, Joakim, 1988, et al.
(författare)
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Order-Disorder Transition in Inorganic Clathrates Controls Electrical Transport Properties
- 2021
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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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| 23. |
- Bryngelsson, Hanna, et al.
(författare)
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Electrodeposited Sb and Sb/Sb2O3 nanoparticle coatings as anode materials for Li-ion batteries
- 2007
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 19:5, s. 1170-1180
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Tidskriftsartikel (refereegranskat)abstract
- Galvanostatically electrodeposited coatings of pure Sb or co-deposited Sb and Sb2O3 nanoparticles, prepared from antimony tartrate solutions, were studied as anode materials in Li-ion batteries. It is demonstrated that the co-deposition of 20-25% (w/w) Sb2O3 results from a local pH increase at the cathode (due to protonation of liberated tartrate) in poorly buffered solutions. This causes precipitation of Sb2O3 nanoparticles and inclusion of some of the particles in the deposit where they become coated with a protecting layer of Sb. Chronopotentiometric cycling of the deposits, which also were characterized using, e.g., SEM, TEM, and XRD, clearly showed that the Sb2O3-containing deposits were superior as anode materials. While the Sb/Sb2O3 coatings exhibited a specific capacity close to the Sb theoretical value of 660 mA·h·g -1 during more than 50 cycles, the capacity for the Sb coatings gradually decreased to about 250 mA·h·g-1. This indicates that the influence of the significant volume changes present upon the formation and oxidation of Li3Sb was much smaller for the Sb/Sb2O3 nanoparticle coatings. The improved performance can be explained by significant formation of Sb2O3 during the reoxidation, the presence of smaller Sb particles in the Sb/Sb2O3 coatings, and the formation of buffering nanoparticles of Li2O in a matrix of Sb during the first reduction cycle for the Sb/Sb2O3 deposits.
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| 24. |
- Burbano, M., et al.
(författare)
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Oxygen Vacancy Ordering and the Conductivity Maximum in Y(2)O(3)-Doped CeO(2)
- 2012
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 1520-5002 .- 0897-4756. ; 24:1, s. 222-229
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Tidskriftsartikel (refereegranskat)abstract
- The defect structure and ionic diffusion processes within the anion-deficient, fluorite structured system Ce(1-x)Y(x)O(2-x/2) have been investigated at high temperatures (873 K-1073 K) as a function of dopant concentration, x, using a combination of neutron diffraction studies, impedance spectroscopy measurements, and molecular dynamics (MD) simulations using interionic potentials developed from ab initio calculations. Particular attention is paid to the short-range ion-ion correlations, with no strong evidence that the anion vacancies prefer, at high temperature, to reside in the vicinity of either cationic species. However, the vacancy-vacancy interactions play a more important role, with preferential ordering of vacancy pairs along the directions, driven by their strong repulsion at closer distances, becoming dominant at high values of x. This effect explains the presence of a maximum in the ionic conductivity in the intermediate temperature range as a function of increasing x. The wider implications of these conclusions for understanding the structure property relationships within anion-deficient fluorite structured oxides are briefly discussed, with reference to complementary studies of yttria and/or scandia doped zirconia published previously.
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| 25. |
- Buscaglia, Maria Teresa, et al.
(författare)
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Fe2O3@BaTiO3 Core−Shell Particles as Reactive Precursors for the Preparation of Multifunctional Composites Containing Different Magnetic Phases
- 2010
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Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 22:16, s. 4740-4748
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Tidskriftsartikel (refereegranskat)abstract
- Well-designed reactive precursors and templates allow for careful control of solid-state reactions at the nanoscale level, thus enabling the fabrication of materials with specific microstructures and properties. In this study, Fe2O3@BaTiO3 core−shell particles have been used as precursors for the in situ fabrication of multifunctional composites containing a dielectric/ferroelectric phase and two magnetic phases with contrasting coercivities (Fe2O3/Fe3O4, BaFe12O19/Ba12Fe28Ti15O84). The formation of new magnetic phases occurs during sintering or post-annealing via reaction between BaTiO3 and Fe2O3. The starting powders have been prepared using a multistep process that combines colloidal chemistry methods and a solid-state reaction. The nature and the amount of the magnetic phases and, consequently, the final magnetic properties of the composite can be controlled by varying the relative amount of Fe2O3 (30 or 50 vol %), the densification method (conventional or spark plasma sintering), and the processing temperature. The composites show constricted magnetic hysteresis loops with a coercivity of 0.1−2.5 kOe and a saturation magnetization of 5−16 emu/g. Composites obtained from powders containing 30 vol % Fe2O3 show, at temperatures of 20−80 °C and frequencies between 10 kHz and 1 MHz, a relative dielectric constant of 50 and dielectric losses of <10%.
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