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1.
Study of Li-S batteries by S K-edge RIXS spectroscopy
Robert Dominko, Iztok Arčon, Marko Petrič, Klemen Bučar, Matjaž Žitnik, Matjaž Kavčič, Alen Vižintin, 2016, published scientific conference contribution abstract

Abstract: Li-S batteries are considered as one of the most promising candidates for future batteries in applications where high energy density is required [1]. Despite that the general principle of operation is known for a long time [2], the lack of detailed understanding of relevant operation mechanisms has so far prevented their extensive use. A Li-S battery is composed of a lithium metal anode and a sulfur based cathode, separated by a porous separator wetted with electrolyte. During the battery cycle the reduction and oxidation of S to Li2S and back proceeds through a complicated equilibrium mixture of compounds that are typically dissolved in the electrolyte in the form of long and short chain polysulfides. In order to improve our understanding of polysulfide formation and its interactions within electrode, which are essential to achieve the long term cycling stability, development and application of new analytical tools is required. In this work sulfur K-edge resonant X-ray emission (RXES) measurements were performed on the Li-S battery in operando mode. The experiment was performed at the ID26 beamline at ESRF using the Johansson type tender x-ray emission spectrometer [3]. Full K-L RIXS maps were recorded on a set of chemically prepared Li2Sx sample standards characterized by different Li:S stoichiometric ratio, followed by the operando measurements on Li-S battery. Using the spectra recorded on Li2Sx standards two excitation energies were chosen and RXES spectra from the back of the battery cathode were sequentially acquired during one discharge cycle (C20). The relative amounts of each sulfur compound in the cathode during the discharge cycle were determined from the linear combination fit using measured reference standard spectra. Because of resonant excitation conditions the sensitivity for the polysulfide detection was significantly enhanced. Our work sets up S K-edge RIXS spectroscopy as an important analytical tool to study the mechanism of Li-polysulfide formation in the cathode and their interaction with the host matrix and electrolyte.
Found in: ključnih besedah
Summary of found: ...were performed on the Li-S battery in operando mode. The experiment was performed at the... ...RIXS, RXES, Li-S battery, operando, Sulphur K-edge XANES, Lithium polysulphides, Li2S...
Keywords: RIXS, RXES, Li-S battery, operando, Sulphur K-edge XANES, Lithium polysulphides, Li2S
Published: 28.06.2016; Views: 3785; Downloads: 0
.pdf Fulltext (60,50 KB)

2.
Polysulfides formation in different electrolytes from the perspective of X-ray absorption spectroscopy
Robert Dominko, Alen Vižintin, Giuliana Aquilanti, Lorenzo Stievano, Maria Joseph Helen, Anji Reddy Munnangi, Maximilian Fichtner, Iztok Arčon, 2018, original scientific article

Abstract: Li-S batteries are promising energy storage technology for the future, however there two major problems remained which need to be solved before successful commercialization. Capacity fading due to polysulfide shuttle and corrosion of lithium metal are directly connected with the type and quantity of electrolyte used in the cells. Several recent works show dependence of the electrochemical behavior of Li-S batteries on type of the electrolyte. In this work we compare and discuss a discharge mechanism of sulfur conversion in three different electrolytes based on measurements with sulfur K-edge XAS. The sulfur conversion mechanism in the ether based electrolytes, the most studied type of solvents in the Li-S batteries, which are enabling high solubility of polysulfides are compared with the fluorinated ether based electrolytes with a reduced polysulfide solubility and in carbonate based electrolytes with the sulfur confined into a ultramicroporous carbon. In all three cases the sulfur reduction proceeds through polysulfide intermediate phases with a difference on the type polysulfides detected at different steps of discharge.
Found in: ključnih besedah
Summary of found: ...Li-S batteries, operando sulphur K-edge XANES, EXAFS, Li-polysulphides...
Keywords: Li-S batteries, operando sulphur K-edge XANES, EXAFS, Li-polysulphides
Published: 01.06.2018; Views: 1870; Downloads: 0
.pdf Fulltext (579,89 KB)

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