| 51. |
- Jiao, Xingxing, et al.
(author)
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Morphology evolution of electrodeposited lithium on metal substrates
- 2023
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In: Energy Storage Materials. - 2405-8297. ; 61
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Journal article (peer-reviewed)abstract
- Lithium (Li) metal is deemed to be the high-energy-density anode material for next generation batteries, but its practical application is impeded by the uneven electrodeposition during charge of battery, which leads to the low Coulombic efficiency and potential safety issue. Here, multiscale modeling is fabricated to understand the morphology evolution of Li during electrodeposition process, from the self-diffusion of Li adatoms on electrode surface, to the nucleation process, and to the formation of Li microstructures, revealing the correlation between final morphology and deposition substrates. Energy batteries and self-diffusion of Li adatom on various substrates (lithium, copper, nickel, magnesium, and silver) result in the different nucleation size, which is calculated by kinetic Monte Carlo simulation based on classical nucleation theory. Formation of Li substructures that are grown from Li nuclei, is revealed by phase field modeling coupled with cellular automaton method. Our results show that larger Li nuclei is obtained under faster self-diffusion of Li adatom, leading to the low aspect ratio of Li substructures and the subsequent morphology evolution of electrodeposited Li. Furthermore, the electrodeposition of Li is strongly regulated by the selection of substrates, giving the practical guideline of anode design in rechargeable Li metal batteries. It is worthy to mention that this method to investigate the electro-crystallization process involving nucleation and growth can be transplanted to the other metallic anode, such as sodium, potassium, zinc, magnesium, calcium and the like.
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| 52. |
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| 53. |
- Johansson, Patrik, 1969, et al.
(author)
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The conductivity of pyrrolidinium and sulfonylimide based ionic liquids: A combined experimental and computational study
- 2010
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In: Journal of Power Sources. - : Elsevier BV. - 0378-7753. ; 195:7, s. 2074-2076
-
Journal article (peer-reviewed)abstract
- Ionic conductivity is a fundamental property of ionic liquids with its origin and exact nature under debate. Using a specially selected system of pyrrolidinium cations (PYR1x, x = 3,4) and sulfonylimide anions (FSI, TFSI, BETI, and IM14)-based ionic liquids we observe a simple and accurate connection between ab initio computed cation and anion volumes and measured molar ionic conductivities.
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| 54. |
- Karlsson, Maths, 1978, et al.
(author)
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Alkali-ion concentration dependence of the structure of proton-conducting alkali thio-hydroxogermanates investigated with neutron diffraction
- 2015
-
In: Solid State Ionics. - : Elsevier BV. - 0167-2738. ; 274, s. 40-45
-
Journal article (peer-reviewed)abstract
- The proton-conducting hydrated alkali thio-hydroxogermanate's MxGeSx(OH)(4) - x center dot yH(2)O (M = Na and K; x = 1 - 4,y approximate to 0.5 - 2) were investigated by means of neutron diffraction with the aim to elucidate how the structure changes as a function of alkali-ion concentration, x, type of alkali ion, M, and water content, y. For x = 1 - 3 we find that the materials are amorphous and composed of thio-hydroxogermanate anions, water molecules, and charge balancing alkali ions, whereas for x = 4 we find that the materials contain also a crystalline phase, suggesting that it is difficult to prepare purely amorphous materials for the highest alkali-ion concentration, for both the Na and K based materials. For x = 1 - 3, the structure is reflected by an intermediate-range ordering, with a characteristic length-scale ranging from approximately 6 to 9 angstrom, which is dependent on both x and M and which may be related to the separation distance between dimers of thio-hydroxogermanate anions. As x increases, the intermediate-range ordering shortens, possibly as the result of an increasing level of hydration water that may act as a dielectric medium that reduces the repulsive interaction between the negatively charged thio-hydroxogermanate anions and/or between the positively charged alkali ions. A comparison of the structural results to the reported conductivities of the same materials indicates a non-trivial relationship, which depends on both the type and concentration of alkali ions, as well as on the level of hydration water.
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| 55. |
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| 56. |
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| 57. |
- Karlsson, Maths, 1978, et al.
(author)
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Quasielastic neutron scattering of hydrated BaZr0.90A0.10O2.95 (A = Y and Sc)
- 2009
-
In: Solid State Ionics. - : Elsevier BV. - 0167-2738. ; 180:1, s. 22-28
-
Journal article (peer-reviewed)abstract
- Proton motions in hydrated proton conducting perovskites BaZr 0.90 A 0.10 O 2.95 (A = Y and Sc) have been investigated using quasielastic neutron scattering. The results reveal a localized motion on the ps time scale and with an activation energy of ~ 10-30 meV, in both materials. The temperature dependence of the total mean square displacement of the protons shows an onset of this motion at a temperature of about 300 K. The low activation energy, much lower than the activation energy for the macroscopic proton conductivity, suggests that this motion is not the rate-limiting process for the long-range proton diffusion, i.e. it is not linked to the two materials significantly different proton conductivities. In fact, a comparison of the QENS results with density functional theory calculations indicates that for both materials the observed motion may be ascribed to intra-octahedral proton transfers occurring close to a dopant atom. © 2008 Elsevier B.V. All rights reserved.
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| 58. |
- Karlsson, Maths, et al.
(author)
-
Short-range structure of proton-conducting BaM0.10Zr0.90O2.95 (M = Y, In, Sc and Ga) investigated with vibrational spectroscopy
- 2010
-
In: Solid State Ionics. - : Elsevier BV. - 0167-2738 .- 1872-7689. ; 181:3-4 (Sp. Iss.), s. 126-129
-
Journal article (peer-reviewed)abstract
- The short-range structures of hydrated and dry samples of the proton-conducting, cubic-structured, acceptor-doped perovskites BaM0.10Zr0.90O2.95 (M=Y, In, Sc and Ga), and, for comparison, BaZrO3, have been investigated using infrared and Raman spectroscopy. The results show that the acceptor-doping leads to local structural distortions of the average cubic structure, most likely related to tilts of (M/Zr)O-6 octahedra, and that the distortions are most pronounced in the Ga-doped material for which we also find additional distortions upon hydration. For the Y-, In- and Sc-doped equivalents the distortions are somewhat weaker and hydration is found to have a reversed, although weak, effect. A comparison of the spectroscopic results to the reported proton diffusivities of the investigated materials would suggest that the much lower proton diffusivity in the Ga-doped material is associated to its stronger structural distortions. (C) 2009 Elsevier B.V. All rights reserved.
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| 59. |
- Karlsson, Maths, et al.
(author)
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Short-range structure of proton-conducting perovskite BaInxZr1-xO3-x/2 (x=0-0
- 2009
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In: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 20:10, s. 3480-3486
-
Journal article (peer-reviewed)abstract
- In a systematic study, we investigate the effect of dopant level and hydration on the short-range structure of the proton-conducting perovskite-type oxide BaInxZr1-xO3-x/2 (x = 0 - 0.75), using infrared and Raman spectroscopy. The results show that the doping leads to significant local distortions of the average cubic structure of these materials. By increasing the In concentration from x = 0 to x = 0.75, new bands appear and grow in intensity in both the IR and the Raman spectra, showing that the local distortions become successively more and more pronounced. The structural distortions are largely uncorrelated to the presence of oxygen vacancies, but instead are mainly driven by the size and charge difference between the In3+ and Zr4+ ions, which leads to displacements of the cations and to tilting of the (In/Zr)O-6 octahedra. On the basis of our results, we suggest that there is a threshold between x = 0.10 and x = 0.25 where the structural distortions propagate throughout the whole perovskite structure. Comparison of our spectroscopic data with the proton conductivity for the same materials indicates that the presence of extended structural distortions is favorable for fast proton transport.
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| 60. |
- Karlsson, Maths, 1978, et al.
(author)
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Structural Origin of the Mixed Glass Former Effect in Sodium Borophosphate Glasses Investigated with Neutron Diffraction and Reverse Monte Carlo Modeling
- 2015
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In: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 119:49, s. 27275-27284
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Journal article (peer-reviewed)abstract
- The mixed glass former systems 0.35Na(2)O + 0.65[xB(2)O(3) + (1 - x)P2O5] and 0.5Na(2)O + 0.5[xB(2)O(3) + (1 - x)P2O5] with x = 0-1 were investigated with neutron diffraction (ND) together with reverse Monte Carlo (RMC) modeling of 0.35Na(2)O + 0.65[xB(2)O(3) + (1 - x)P2O5]. The results show that the structure of both systems is reflected by an intermediate-range ordering, with a characteristic x-dependent length scale of about 4-6 angstrom and which contracts slightly with the increase of the Na concentration. Results obtained from RMC modeling of the 0.35Na(2)O + 0.65[xB(2)O(3) + (1 - x)P2O5] system, using both previously reported X-ray diffraction (XRD) data as well as the here obtained ND data as independent constraints in the modeling, show that the intermediate-range structural features, notably the Na coordination and volume fraction of the conducting pathways, are only weakly dependent on the choice of the constraints used. In particular, we observe that the volume fraction of the conducting pathways and the activation energy for ionic conduction are only weakly correlated to each other, as opposed to what is found for binary alkali borate and phosphate glasses.
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