| 1. |
- Haridas, Anupriya K., et al.
(författare)
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A flexible and free-standing FeS/sulfurized polyacrylonitrile hybrid anode material for high-rate sodium-ion storage
- 2020
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Ingår i: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947. ; 385:1 April
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Tidskriftsartikel (refereegranskat)abstract
- Sodium-ion based energy storage systems have attracted extensive attention due to the similarities in the mechanism of operation with lithium-ion batteries along with the additional benefit of low cost and high abundance of sodium resources. Iron sulfide-based electrodes that operate via conversion mechanism have shown ample potential for high energy sodium-ion storage. However, the problems related with tremendous volume changes and the dissolution of sodium polysulfides in the electrolyte deteriorate the cycle life and limit their application in sodium-ion batteries (SIBs). Herein, a hybrid anode material, FeS/SPAN-HNF, with iron sulfide (FeS) nanoparticles decorated in a sulfurized polyacrylonitrile (SPAN) fiber matrix is demonstrated as flexible and free-standing anode material for high-rate SIBs. Unlike previous strategies in which FeS is encapsulated in an electrochemically inactive carbon matrix, this study utilizes SPAN, an electrochemically active material, as a dual functional matrix that can efficiently buffer volume expansion and sulfur dissolution of FeS nanoparticles as well as provide significant capacity improvement. The as-designed electrode is self-standing and flexible, without current collectors, binders or additional conductive agents, thus rendering enhanced practical capacity and energy density. This electrode showed a high reversible capacity of 782.8 mAh g−1 at 200 mA g−1 with excellent high rate capability, maintaining 327.5 mAh g−1 after 500 cycles at 5 A g−1, emphasizing promising prospects for the development of flexible and high energy density SIBs.
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| 2. |
- Calcagno, Giulio, 1990, et al.
(författare)
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Effect of Nitrogen Doping on the Performance of Mesoporous CMK-8 Carbon Anodes for Li-Ion Batteries
- 2020
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Ingår i: Energies. - : MDPI AG. - 1996-1073 .- 1996-1073. ; 13:19
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Tidskriftsartikel (refereegranskat)abstract
- Designing carbonaceous materials with heightened attention to the structural properties such as porosity, and to the functionalization of the surface, is a growing topic in the lithium-ion batteries (LIBs) field. Using a mesoporous silica KIT-6 hard template, mesoporous carbons belonging to the OMCs (ordered mesoporous carbons) family, namely 3D cubic CMK-8 and N-CMK-8 were synthesized and thoroughly structurally characterized. XPS analysis confirmed the successful introduction of nitrogen, highlighting the nature of the different nitrogen atoms incorporated in the structure. The work aims at evaluating the electrochemical performance of N-doped ordered mesoporous carbons as an anode in LIBs, underlining the effect of the nitrogen functionalization. The N-CMK-8 electrode reveals higher reversible capacity, better cycling stability, and rate capability, as compared to the CMK-8 electrode. Coupling the 3D channel network with the functional N-doping increased the reversible capacity to similar to 1000 mAh center dot g(-1) for the N-CMK-8 from similar to 450 mAh center dot g(-1) for the undoped CMK-8 electrode. A full Li-ion cell was built using N-CMK-8 as an anode, commercial LiFePO4, a cathode, and LP30 commercial electrolyte, showing stable performance for 100 cycles. The combination of nitrogen functionalization and ordered porosity is promising for the development of high performing functional anodes.
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| 3. |
- Calcagno, Giulio, 1990, et al.
(författare)
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Fast charging negative electrodes based on anatase titanium dioxide beads for highly stable Li-ion capacitors
- 2020
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Ingår i: Materials Today Energy. - : Elsevier BV. - 2468-6069. ; 16
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Tidskriftsartikel (refereegranskat)abstract
- Hybrid energy storage systems aim to achieve both high power and energy densities by combining supercapacitor-type and battery-type electrodes in tandem. The challenge is to find sustainable materials as fast charging negative electrodes, which are characterized by high capacity retention. In this study, mesoporous anatase beads are synthetized with tailored morphology to exploit fast surface redox reactions. The TiO2-based electrodes are properly paired with a commercial activated carbon cathode to form a Li-ion capacitor. The titania electrode exhibits high capacity and rate performance. The device shows extremely stable performance with an energy density of 27 mWh g-1 at a specific current of 2.5 A g−1 for 10,000 cycles. The remarkable stability is associated with a gradual shift of the potential during cycling as result of the formation of cubic LiTiO2 on the surface of the beads. This phenomenon renews the interest in using TiO2 as negative electrode for Li-ion capacitors.
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| 4. |
- Cavallo, Carmen, 1986, et al.
(författare)
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Effect of the Niobium Doping Concentration on the Charge Storage Mechanism of Mesoporous Anatase Beads as an Anode for High-Rate Li-Ion Batteries
- 2021
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 4:1, s. 215-225
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Tidskriftsartikel (refereegranskat)abstract
- A promising strategy to improve the rate performance of Li-ion batteries is to enhance and facilitate the insertion of Li ions into nanostructured oxides like TiO2. In this work, we present a systematic study of pentavalent-doped anatase TiO2 materials for third-generation high-rate Li-ion batteries. Mesoporous niobium-doped anatase beads (Nb-doped TiO2) with different Nb5+ doping (n-type) concentrations (0.1, 1.0, and 10% at.) were synthesized via an improved template approach followed by hydrothermal treatment. The formation of intrinsic n-type defects and oxygen vacancies under RT conditions gives rise to a metallic-type conduction due to a shift of the Fermi energy level. The increase in the metallic character, confirmed by electrochemical impedance spectroscopy, enhances the performance of the anatase bead electrodes in terms of rate capability and provides higher capacities both at low and fast charging rates. The experimental data were supported by density functional theory (DFT) calculations showing how a different n-type doping can be correlated to the same electrochemical effect on the final device. The Nb-doped TiO2 electrode materials exhibit an improved cycling stability at all the doping concentrations by overcoming the capacity fade shown in the case of pure TiO2 beads. The 0.1% Nb-doped TiO2-based electrodes exhibit the highest reversible capacities of 180 mAh g-1 at 1C (330 mA g-1) after 500 cycles and 110 mAh g-1 at 10C (3300 mA g-1) after 1000 cycles. Our experimental and computational results highlight the possibility of using n-type doped TiO2 materials as anodes in high-rate Li-ion batteries.
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| 5. |
- Cengiz, Elif Ceylan, 1986, et al.
(författare)
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Review - Reference Electrodes in Li-Ion and Next Generation Batteries: Correct Potential Assessment, Applications and Practices
- 2021
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Ingår i: Journal of the Electrochemical Society. - : The Electrochemical Society. - 1945-7111 .- 0013-4651. ; 168:12
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Forskningsöversikt (refereegranskat)abstract
- This review provides an accessible analysis of the processes on reference electrodes and their applications in Li-ion and next generation batteries research. It covers fundamentals and definitions as well as specific practical applications and is intended to be comprehensible for researchers in the battery field with diverse backgrounds. It covers fundamental concepts, such as two- and three-electrodes configurations, as well as more complex quasi- or pseudo- reference electrodes. The electrode potential and its dependance on the concentration of species and nature of solvents are explained in detail and supported by relevant examples. The solvent, in particular the cation solvation energy, contribution to the electrode potential is important and a largely unknown issue in most the battery research. This effect can be as high as half a volt for the Li/Li+ couple and we provide concrete examples of the battery systems where this effect must be taken into account. With this review, we aim to provide guidelines for the use and assessment of reference electrodes in the Li-ion and next generation batteries research that are comprehensive and accessible to an audience with a diverse scientific background.
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| 6. |
- Eliasen, K. L., et al.
(författare)
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High-frequency dynamics and test of the shoving model for the glass-forming ionic liquid Pyr14-TFSI
- 2021
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Ingår i: Physical Review Materials. - 2475-9953. ; 5:6
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Tidskriftsartikel (refereegranskat)abstract
- In studies of glass-forming liquids, one of the important questions is to understand to which degree chemically different classes of liquids have the same type of dynamics. In this context, room-temperature ionic liquids are interesting because they exhibit both van der Waals and Coulomb interactions. In this work we study the α relaxation and faster relaxation dynamics in the room-temperature ionic liquid 1-butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (Pyr14-TFSI). The paper presents quasielastic neutron and shear mechanical spectroscopy data measured over seven decades in frequency (10-3-104 Hz). The use of these two methods in combination reveal the α relaxation and four separate, faster modes. Two of these faster modes, based on the partial deuterations, can be assigned to the methyl group and the methyl end of the butyl chain of the cation. The neutron data are also used to determine the mean-square displacement (MSD) on the nanosecond timescale. It is shown that the temperature dependence of the MSD can account for the super-Arrhenius behavior of the α relaxation as predicted by the shoving model [Dyre, Rev. Mod. Phys. 78, 953 (2006)RMPHAT0034-686110.1103/RevModPhys.78.953], similarly to what is seen in simpler glass-forming liquids.
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| 7. |
- Fretz, Samuel Joseph, 1987, et al.
(författare)
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Amine- and Amide-Functionalized Mesoporous Carbons: A Strategy for Improving Sulfur/Host Interactions in Li-S Batteries
- 2020
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Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 3:8, s. 757-765
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Tidskriftsartikel (refereegranskat)abstract
- Lithium-sulfur (Li-S) batteries are of great interest due to their potentially high energy density, but the low electronic conductivity of both the sulfur (S-8) cathode active material and the final discharge product lithium sulfide (Li2S) require the use of a conductive host. Usually made of relatively hydrophobic carbon, such hosts are typically ill-suited to retain polar discharge products such as the intermediate lithium polysulfides (LiPs) and the final Li2S. Herein, we propose a route to increase the sulfur utilization by functionalizing the surface of ordered mesoporous carbon CMK3 with polar groups. These derivatized CMK3 materials are made using a simple two-step procedure of bromomethylation and subsequent nucleophilic substitution with amine or amide nucleophiles. We demonstrate that, compared to the unfunctionalized control, these modified CMK3 surfaces have considerably larger binding energies with LiPs and Li2S, which are proposed to aid the electrochemical conversion between S-8 and Li2S by keeping the LiPs species in close proximity to the carbon surface during Li-S battery cycling. As a result, the functionalized cathodes exhibit significantly improved specific capacities relative to their unmodified precursor.
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| 8. |
- Izzo, M. G., et al.
(författare)
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Rayleigh scattering and disorder-induced mixing of polarizations in amorphous solids at the nanoscale: 1-octyl-3-methylimidazolium chloride glass
- 2020
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Ingår i: Physical Review B. - 2469-9969 .- 2469-9950. ; 102:21
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Tidskriftsartikel (refereegranskat)abstract
- Acousticlike excitations in topologically disordered media at mesocale/nanoscale present anomalous features with respect to the Debye's theory. The so-called Rayleigh scattering manifests in a strong increase of the attenuation of the acousticlike excitations and a softening of the phase velocity with respect to its continuum limit value. Mean field models developed in the random media theory framework can successfully predict the occurrence, at the proper length scale, of Rayleigh scattering. The overall attenuation in the Rayleigh region is, however, underestimated. In the framework of random media theory we developed an analytical model, which permits a quantitative description of the acousticlike excitations in topological glasses in the whole first pseudo-Brillouin zone. The underestimation of the Rayleigh scattering is avoided and, importantly, the model allows to account also for the polarization properties of the acousticlike excitations. In a three-dimensional medium an acoustic wave is characterized by its phase velocity, intensity, and polarization. Rayleigh scattering emphasizes how the topological disorder affects the first two properties. The topological disorder is, however, expected to influence also the third one. In common with the Rayleigh scattering, hallmarks possibly related to the mixing of polarizations have been traced in different classes of amorphous solids at nanoscale. The quantitative theoretical approach developed permits to demonstrate how the mixing of polarizations generates a distinctive feature in the dynamic structure factor of amorphous solids. The modeling capability of the proposed mean field theory is tested on glassy 1-octyl-3-methylimidazolium chloride, whose spatial distribution of the elastic moduli is well assessed and can be experimentally characterized. Contrast between theoretical and experimental features for the selected glass reveals an excellent agreement. The mean field approach we present retains a certain degree of generality and can be possibly extended to different stochastic media or different wave fields.
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| 9. |
- Lee, Suyeong, et al.
(författare)
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Recent developments and future challenges in designing rechargeable potassium-sulfur and potassium-selenium batteries
- 2020
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Ingår i: Energies. - : MDPI AG. - 1996-1073 .- 1996-1073. ; 13:11
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Tidskriftsartikel (refereegranskat)abstract
- The use of chalcogenide elements, such as sulfur (S) and selenium (Se), as cathode materials in rechargeable lithium (Li) and sodium (Na) batteries has been extensively investigated. Similar to Li and Na systems, rechargeable potassium-sulfur (K-S) and potassium-selenium (K-Se) batteries have recently attracted substantial interest because of the abundance of K and low associated costs. However, K-S and K-Se battery technologies are in their infancy because K possesses overactive chemical properties compared to Li and Na and the electrochemical mechanisms of such batteries are not fully understood. This paper summarizes current research trends and challenges with regard to K-S and K-Se batteries and reviews the associated fundamental science, key technological developments, and scientific challenges to evaluate the potential use of these batteries and finally determine effective pathways for their practical development.
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| 10. |
- Lindberg, Simon, 1985, et al.
(författare)
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Electrochemical Behaviour of Nb-Doped Anatase TiO2 Microbeads in an Ionic Liquid Electrolyte
- 2020
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Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 3:11, s. 1233-1238
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Tidskriftsartikel (refereegranskat)abstract
- TiO(2)is a promising material for high-power battery and supercapacitor applications. However, in general TiO(2)suffers from an initial irreversible capacity that limits its use in different applications. A combination of a microbead morphology, Nb-doping, and the use of an ionic liquid electrolyte is shown to significantly decrease the irreversible capacity loss. A change in the electrochemical response in the first cycles indicates formation of a solid-electrolyte interphase (SEI) or a modification of the structure of the surface layer of the TiO2/Nb microbeads, which apparently stabilises the performance. The change in the response is manifested in an increased charge transfer resistance and the presence of two charge transfer contributions. During prolonged cycling the TiO2/Nb electrode shows an excellent stability over 5000 cycles. Ex situ analysis after cycling shows that the overall microbead morphology is intact and that there are no changes in the crystal structure. However, a decrease in the intensity of the XRD pattern can point to a decrease in size of the nanocrystals building up the microbeads or the formation of amorphous phases.
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