| 1. |
- Agostini, Marco, 1987, et al.
(författare)
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Designing a Safe Electrolyte Enabling Long‐Life Li/S Batteries
- 2019
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 12:18, s. 4176-4184
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Tidskriftsartikel (refereegranskat)abstract
- Lithium–sulfur (Li/S) batteries suffer from “shuttle” reactions in which soluble polysulfide species continuously migrate to and from the Li metal anode. As a consequence, the loss of active material and reactions at the surface of Li limit the practical applications of Li/S batteries. LiNO3 has been proposed as an electrolyte additive to reduce the shuttle reactions by aiding the formation of a stable solid electrolyte interphase (SEI) at the Li metal, limiting polysulfide shuttling. However, LiNO3 is continuously consumed during cycling, especially at low current rates. Therefore, the Li/S battery cycle life is limited by the LiNO3 concentration in the electrolyte. In this work, an ionic liquid (IL) [N-methyl-(n-butyl)pyrrolidinium bis(trifluoromethylsulfonyl)imide] was used as an additive to enable longer cycle life of Li/S batteries. By tuning the IL concentration, an enhanced stability of the SEI and lower flammability of the solutions were demonstrated, that is, higher safety of the battery. The Li/S cell built with a high sulfur mass loading (4 mg cm−2) and containing the IL-based electrolyte demonstrated a stable capacity of 600 mAh g−1 for more than double the number of cycles of a cell containing LiNO3 additive.
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| 2. |
- Agostini, Marco, 1987, et al.
(författare)
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Rational Design of Low Cost and High Energy Lithium Batteries through Tailored Fluorine-free Electrolyte and Nanostructured S/C Composite
- 2018
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 11:17, s. 2981-2986
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Tidskriftsartikel (refereegranskat)abstract
- We report a new Li–S cell concept based on an optimized F-free catholyte solution and a high loading nanostructured C/S composite cathode. The Li2S8present in the electrolyte ensures both buffering against active material dissolution and Li+conduction. The high S loading is obtained by confining elemental S (≈80 %) in the pores of a highly ordered mesopores carbon (CMK3). With this concept we demonstrate stabilization of a high energy density and excellent cycling performance over 500 cycles. This Li–S cell has a specific capacity that reaches over 1000 mA h g−1, with an overall S loading of 3.6 mg cm−2and low electrolyte volume (i.e., 10 μL cm−2), resulting in a practical energy density of 365 Wh kg−1. The Li–S system proposed thus meets the requirements for large scale energy storage systems and is expected to be environmentally friendly and have lower cost compared with the commercial Li-ion battery thanks to the removal of both Co and F from the overall formulation.
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| 3. |
- Agostini, Marco, 1987, et al.
(författare)
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Stabilizing the Performance of High-Capacity Sulfur Composite Electrodes by a New Gel Polymer Electrolyte Configuration
- 2017
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 10:17, s. 3490-3496
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Tidskriftsartikel (refereegranskat)abstract
- Increased pollution and the resulting increase in global warming are drawing attention to boosting the use of renewable energy sources such as solar or wind. However, the production of energy from most renewable sources is intermittent and thus relies on the availability of electrical energy-storage systems with high capacity and at competitive cost. Lithium–sulfur batteries are among the most promising technologies in this respect due to a very high theoretical energy density (1675 mAh g?1) and that the active material, sulfur, is abundant and inexpensive. However, a so far limited practical energy density, life time, and the scaleup of materials and production processes prevent their introduction into commercial applications. In this work, we report on a simple strategy to address these issues by using a new gel polymer electrolyte (GPE) that enables stable performance close to the theoretical capacity of a low cost sulfur–carbon composite with high loading of active material, that is, 70 % sulfur. We show that the GPE prevents sulfur dissolution and reduces migration of polysulfide species to the anode. This functional mechanism of the GPE membranes is revealed by investigating both its morphology and the Li-anode/GPE interface at various states of discharge/charge using Raman spectroscopy.
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| 4. |
- Celeste, Arcangelo, et al.
(författare)
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Enhancement of Functional Properties of Liquid Electrolytes for Lithium-Ion Batteries by Addition of Pyrrolidinium-Based Ionic Liquids with Long Alkyl-Chains
- 2020
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Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 3:10, s. 1059-1068
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Tidskriftsartikel (refereegranskat)abstract
- Three ionic liquid belonging to the N-alkyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imides (Pyr(1),nTFSI with n=4,5,8) have been added as co-solvent to two commonly used electrolytes for Li-ion cells: (a) 1 M lithium hexafluorophosphate (LiPF6) in a mixture of ethylene carbonate (EC) and linear like dimethyl carbonate (DMC) in 1 : 1 v/v and (b) 1 M lithium bis-(trifluoromethanesulfonyl)imide (LiTFSI) in EC : DMC 1 : 1 v/v. These electrolyte formulations (classified as P and T series containing LiPF6 or LiTFSI salts, respectively) have been analyzed by comparing ionic conductivities, transport numbers, viscosities, electrochemical stability as well as vibrational properties. In the case of the Pyr(1,5)TFSI and Pyr(1,8)TFSI blended formulations, this is the first ever reported detailed study of their functional properties in Li-ion cells electrolytes. Overall, P-electrolytes demonstrate enhanced properties compared to the T-ones. Among the various P electrolytes those containing Pyr(1,4)TFSI and Pyr(1,5)TFSI limit the accumulation of irreversible capacity upon cycling with satisfactory performance in lithium cells.
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| 5. |
- Sadd, Matthew, 1994, et al.
(författare)
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Polysulfide Speciation and Migration in Catholyte Lithium−Sulfur Cells
- 2022
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Ingår i: ChemPhysChem. - : Wiley. - 1439-7641 .- 1439-4235. ; 23:4
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Tidskriftsartikel (refereegranskat)abstract
- Semi-liquid catholyte Lithium−Sulfur (Li−S) cells have shown to be a promising path to realize high energy density energy storage devices. In general, Li−S cells rely on the conversion of elemental sulfur to soluble polysulfide species. In the case of catholyte cells, the active material is added through polysulfide species dissolved in the electrolyte. Herein, we use operando Raman spectroscopy to track the speciation and migration of polysulfides in the catholyte to shed light on the processes taking place. Combined with ex-situ surface and electrochemical analysis we show that the migration of polysulfides is central in order to maximize the performance in terms of capacity (active material utilization) as well as interphase stability on the Li-metal anode during cycling. More specifically we show that using a catholyte where the polysulfides have the dual roles of active material and conducting species, e. g. no traditional Li-salt (such as LiTFSI) is present, results in a higher mobility and faster migration of polysulfides. We also reveal how the formation of long chain polysulfides in the catholyte is delayed during charge as a result of rapid formation and migration of shorter chain species, beneficial for reaching higher capacities. However, the depletion of ionic species during the last stage of charge, due to the conversion to and precipitation of elemental sulfur on the cathode support, results in polarization of the cell before full conversion can be achieved.
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