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141.
  • Verwohlt, Jan, et al. (författare)
  • Low Dose X-Ray Speckle Visibility Spectroscopy Reveals Nanoscale Dynamics in Radiation Sensitive Ionic Liquids
  • 2018
  • Ingår i: Physical Review Letters. - 1079-7114 .- 0031-9007. ; 120:16
  • Tidskriftsartikel (refereegranskat)abstract
    • X-ray radiation damage provides a serious bottleneck for investigating microsecond to second dynamics on nanometer length scales employing x-ray photon correlation spectroscopy. This limitation hinders the investigation of real time dynamics in most soft matter and biological materials which can tolerate only x-ray doses of kGy and below. Here, we show that this bottleneck can be overcome by low dose x-ray speckle visibility spectroscopy. Employing x-ray doses of 22-438 kGy and analyzing the sparse speckle pattern of count rates as low as 6.7×10-3 per pixel, we follow the slow nanoscale dynamics of an ionic liquid (IL) at the glass transition. At the prepeak of nanoscale order in the IL, we observe complex dynamics upon approaching the glass transition temperature TG with a freezing in of the alpha relaxation and a multitude of millisecond local relaxations existing well below TG. We identify this fast relaxation as being responsible for the increasing development of nanoscale order observed in ILs at temperatures below TG.
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142.
  • Xiong, Shizhao, et al. (författare)
  • Analysis of the solid electrolyte interphase formed with an ionic liquid electrolyte for lithium-sulfur batteries
  • 2014
  • Ingår i: Journal of Power Sources. - 0378-7753. ; 252, s. 150-155
  • Tidskriftsartikel (refereegranskat)abstract
    • We have investigated the formation of the solid electrolyte interphase (SEI) on lithium electrodes in the presence of an ionic liquid electrolyte with a particular focus on the influence of polysulfides present in the electrolyte on the SEI. The electrochemical performance of symmetric cells with lithium electrodes and electrolytes composed of N-Methyl-(n-butyl)pyrrolidinium bis(trifluoromethanesulfonyl)imide (PYR14-TFSI) and LiTFSI, with and without the addition of polysulfides, were analyzed as well as the chemical composition of the SEI, before and after cycling. The cycling behavior of the symmetrical cells shows that the SEI films are relatively stable in the ionic liquid electrolyte, also in the presence of polysulfides. However, the presence of polysulfides results in a higher SEI layer resistance (R-SEI) and a higher activation energy. From X-ray photoelectron spectroscopy spectra (XPS), with argon-ion sputtering for depth profiling, we find that the SEI is formed by decomposition products from both cations and anions of the electrolyte. The XPS spectra show that the presence of polysulfides alters the decomposition process of the electrolyte, resulting in a SEI film with different chemical composition and structure, in line with the results from the electrochemical performance.
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143.
  • Xiong, Shizhao, 1985, et al. (författare)
  • Design of a Multifunctional Interlayer for NASCION-Based Solid-State Li Metal Batteries
  • 2020
  • Ingår i: Advanced Functional Materials. - 1616-301X. ; 30:22
  • Tidskriftsartikel (refereegranskat)abstract
    • NASCION-type Li conductors have great potential to bring high capacity solid-state batteries to realization, related to its properties such as high ionic conductivity, stability under ambient conditions, wide electrochemical stability window, and inexpensive production. However, their chemical and thermal instability toward metallic lithium (Li) has severely hindered attempts to utilize Li as anode material in NASCION-based battery systems. In this work, it is shown how a tailored multifunctional interlayer between the solid electrolyte and Li anode can successfully address the interfacial issues. This interlayer is designed by creating a quasi-solid-state paste in which the functionalities of LAGP (Li1.5Al0.5Ge1.5(PO4)3) nanoparticles and an ionic liquid (IL) electrolyte are combined. In a solid-sate cell, the LAGP-IL interlayer separates the Li metal from bulk LAGP and creates a chemically stable interface with low resistance (≈5 Ω cm2) and efficiently prevents thermal runaway at elevated temperatures (300 °C). Solid-state cells designed with the interlayer can be operated at high current densities, 1 mA cm−2, and enable high rate capability with high safety. Here developed strategy provides a generic path to design interlayers for solid-state Li metal batteries.
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144.
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145.
  • Xu, Xieyu, et al. (författare)
  • Role of Li-Ion Depletion on Electrode Surface: Underlying Mechanism for Electrodeposition Behavior of Lithium Metal Anode
  • 2020
  • Ingår i: Advanced Energy Materials. - 1614-6840 .- 1614-6832. ; 10:44
  • Tidskriftsartikel (refereegranskat)abstract
    • The application of lithium metal as an anode material for next generation high energy-density batteries has to overcome the major bottleneck that is the seemingly unavoidable growth of Li dendrites caused by non-uniform electrodeposition on the electrode surface. This problem must be addressed by clarifying the detailed mechanism. In this work the mass-transfer of Li-ions is investigated, a key process controlling the electrochemical reaction. By a phase field modeling approach, the Li-ion concentration and the electric fields are visualized to reveal the role of three key experimental parameters, operating temperature, Li-salt concentration in electrolyte, and applied current density, on the microstructure of deposited Li. It is shown that a rapid depletion of Li-ions on electrode surface, induced by, e.g., low operating temperature, diluted electrolyte and a high applied current density, is the underlying driving force for non-uniform electrodeposition of Li. Thus, a viable route to realize a dendrite-free Li plating process would be to mitigate the depletion of Li-ions on the electrode surface. The methodology and results in this work may boost the practical applicability of Li anodes in Li metal batteries and other battery systems using metal anodes.
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146.
  • Yaghini, Negin, 1976, et al. (författare)
  • Achieving enhanced ionic mobility in nanoporous silica by controlled surface interactions
  • 2017
  • Ingår i: Physical Chemistry Chemical Physics. - 1463-9084 .- 1463-9076.
  • Tidskriftsartikel (refereegranskat)abstract
    • We report a strategy to enhance the ionic mobility in an emerging class of gels, based on robust nanoporous silica micro-particles, by chemical functionalization of the silica surface. Two very different ionic liquids are used to fill the nano-pores of silica at varying pore filling factors, namely one aprotic imidazolium based (1-methyl-3-hexylimidazolium bis(trifluoromethanesulfonyl)imide, C6C1ImTFSI), and one protic ammonium based (diethylmethylammonium methanesulfonate, DEMAOMs) ionic liquid. Both these ionic liquids display higher ionic mobility when confined in functionalized silica as compared to untreated silica nano-pores, an improvement that is more pronounced at low pore filling factors (i.e. in the nano-sized pore domains) and observed in the whole temperature window investigated (i.e. from −10 to 140 °C). Solid-state NMR, diffusion NMR and dielectric spectroscopy concomitantly demonstrate this effect. The origin of this enhancement is explained in terms of weaker intermolecular interactions and a consequent flipped-ion effect at the silica interface strongly supported by 2D solid-state NMR experiments. The possibility to significantly enhance the ionic mobility by controlling the nature of surface interactions is extremely important in the field of materials science and highlights these structurally tunable gels as promising solid-like electrolytes for use in energy relevant devices. These include, but are not limited to, Li-ion batteries and proton exchange membrane (PEM) fuel cells.
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147.
  • Yaghini, Negin, 1976, et al. (författare)
  • Effect of Water on the Local Structure and Phase Behavior of Imidazolium-Based Protic Ionic Liquids
  • 2015
  • Ingår i: Journal of Physical Chemistry B. - 1520-5207 .- 1520-6106. ; 119:4, s. 1611-1622
  • Tidskriftsartikel (refereegranskat)abstract
    • We report on the effect of water on local structure and phase behavior of two protic ionic liquids, C(2)HImTFSI and C(2)HImTfO. Raman and infrared spectroscopy are employed to investigate the local coordination state. We find that water interacts weakly with TFSI- while more specifically with TfO- through the - SO3 group. Additionally, we observe that upon addition of water the - NH stretching frequency does not change in C(2)HImTFSI, while it red-shifts in C(2)HImTfO, indicative of different hydrogen bonding configurations. Supported by the appearance of some additional features in the 800-1000 cm(-1) frequency range where ring out-of-plane bending (?) modes are found, we hypothesize that in C(2)HImTFSI water interacts only with the cation coordinating to the ring C2H and the N3H sites, while it interacts with both cation and anion in C(2)HImTfO forming hydrogen bonds that involve the cationic N-H site as well as the anionic - SO3 group. These different local structures also reflect in the phase behavior investigated by DSC, which reveals a more homogeneous solution when water is added to C(2)HImTfO, as compared to H2O/C(2)HImTFSI mixtures. Finally we report that the addition of water also significantly affects both T-m and T-g.
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148.
  • Zhao, Peiyu, et al. (författare)
  • Stable lithium metal anode enabled by high-dimensional lithium deposition through a functional organic substrate
  • 2020
  • Ingår i: Energy Storage Materials. - 2405-8297. ; 33, s. 158-163
  • Tidskriftsartikel (refereegranskat)abstract
    • The growth of lithium dendrites severely restricts the development of lithium metal batteries. In order to achieve the goal of dendrites-free lithium in principle, it is crucial and urgent to control nucleation and growth of lithium. Here, a functional organic layer of perylene-3, 4, 9, 10-tetracarboxydiimide-lithium (PTCDI-Li) is built on the lithium anode surface by in-situ chemical reaction of PTCDI and Li metal. PTCDI-Li, with high surface energy (-10.19 eV) and low diffusion barrier (0.89 eV), efficiently promotes disk-shaped high-dimensional nucleation by regulation of lithium ion flux upon lithium plating, leading to a dendrites-free morphology. When operating under a relatively high current density of 10 mA cm−2, the Li | Li symmetrical cells with PTCDI-Li exhibit outstanding cyclic stability for 300 hours with ultralow overpotential of 400 mV, superior to the most of the reported lithium anode. The corresponding PTCDI-Li batteries show high specific capacity and enhanced cycle life. We anticipate that this strategy of regulation of lithium deposition from one-dimensional to high-dimensional opens a new horizon in the development of dendrites-free Li anodes.
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149.
  • Åkesson, Dan, 1970, et al. (författare)
  • Synthesis and Characterization of a cross-linkable polylactic acid based resin
  • 2010
  • Ingår i: Journal of Applied Polymer Science. - 1097-4628 .- 0021-8995. ; 115:1, s. 480-486
  • Tidskriftsartikel (refereegranskat)abstract
    • A new biobased polyester resin was developed for thermoset composite applications. The resin is potentially inexpensive and can be produced industrially by relatively simple means. The resin consists of star-shaped methacrylated oligomers of lactic acid (LA). LA oligomers were synthesized in a two-step process: in the first step, oligomers of LA were polymerized by direct condensation of LA. In the second step, the oligomers were end-functionalized by methacrylic anhydride. The resin was characterized by differential scanning calorimetry, Raman spectroscopy, NMR, rubber process analyzer, and TOF-SIMS. Tests show that the resin can be crosslinked into a rigid network within a couple of minutes upon thermal initiation.
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