| 1. |
- Agostini, Marco, 1987, et al.
(author)
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Designing a Safe Electrolyte Enabling Long‐Life Li/S Batteries
- 2019
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In: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 12:18, s. 4176-4184
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Journal article (peer-reviewed)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. |
- Brige, Amandine, et al.
(author)
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A comparative study of hydroxyethylcellulose-based solid polymer electrolytes for solid state Zn batteries
- 2023
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In: NANO SELECT. - : Wiley. - 2688-4011. ; 4:1, s. 102-111
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Journal article (peer-reviewed)abstract
- Rechargeable zinc metal batteries are greener and safer alternative to lithium batteries, but they suffer from poor reversibility due to growth of zinc dendrites and water splitting reactions of aqueous electrolytes. One strategy to overcome these drawbacks is replacing aqueous electrolyte with solid polymer electrolyte (SPE). In this work, we examine the possibility of fabricating solid electrolyte from a bio-based polymer, hydroxyethylcellulose (HEC), with the aim to further increase the sustainability of zinc batteries. Various types of zinc salts, drying procedures and the salt concentrations are investigated for their impact on the ionic conductivity, structure, and phase behavior of as-prepared polymer electrolytes. It is found that HEC has a good film-forming ability compared with commonly used poly(ethylene oxide) but its low salt-dissociation capability leads to an ionic conductivity of 10(-6) S cm(-1) even at the elevated temperature of 110 degrees C, hindering the possibility of solely utilizing HEC as matrix of solid electrolyte. Our results suggest that introducing a new polymer with higher salt-dissociation capability or lower glass transition temperature into the HEC matrix can be a reliable way to build solid polymer electrolytes with sufficient ionic conductivity and good mechanical property for future zinc batteries.
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| 3. |
- Calcagno, Giulio, 1990, et al.
(author)
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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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In: Energies. - : MDPI AG. - 1996-1073 .- 1996-1073. ; 13:19
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Journal article (peer-reviewed)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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| 4. |
- 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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| 5. |
- Lee, Suyeong, et al.
(author)
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High-Energy and Long-Lifespan Potassium–Sulfur Batteries Enabled by Concentrated Electrolyte
- 2022
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In: Advanced Functional Materials. - : Wiley. - 1616-3028 .- 1616-301X. ; 32:46
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Journal article (peer-reviewed)abstract
- Potassium–sulfur (K–S) batteries are emerging as low-cost and high-capacity energy-storage technology. However, conventional K–S batteries suffer from two critical issues that have not yet been successfully resolved: the dissolution of potassium polysulfides (KPS) into the liquid electrolyte and the formation of K dendrites on the K metal anode, which lead to inadequate cycling efficiencies with a low reversible capacity. Herein, a high-capacity and long cycle-life K–S battery consisting of a highly concentrated electrolyte (HCE) (4.34 mol kg−1 potassium bis(fluorosulfonyl)imide in a 1,2-Dimethoxyethane) and a sulfurized polyacrylonitrile (SPAN) cathode is presented The application of a HCE efficiently suppresses the dendritic growth of K, as evidenced by operando optical imaging and phase field modeling, owing to the reduced K-ion depletion on the electrode surface and a uniform Faradaic current density over the K metal anode surface. Additionally, because S is covalently bonded to the C backbone of PAN in the SPAN structure, the SPAN cathode inhibits the dissolution of KPS. These features generate synergy that the proposed K–S battery can provide a practical areal capacity of 2.5 mAh cm−2 and unprecedented lifetimes with high Coulombic efficiencies over 700 cycles.
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| 6. |
- Lee, Suyeong, et al.
(author)
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Recent developments and future challenges in designing rechargeable potassium-sulfur and potassium-selenium batteries
- 2020
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In: Energies. - : MDPI AG. - 1996-1073 .- 1996-1073. ; 13:11
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Journal article (peer-reviewed)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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| 7. |
- Liu, Qiao, et al.
(author)
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Enhanced ionic conductivity and interface stability of hybrid solid-state polymer electrolyte for rechargeable lithium metal batteries
- 2019
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In: Energy Storage Materials. - : Elsevier BV. - 2405-8297. ; 23, s. 105-111
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Journal article (peer-reviewed)abstract
- Compared to conventional organic liquid electrolyte, solid-state polymer electrolytes are extensively considered as an alternative candidate for next generation high-energy batteries because of their high safety, non-leakage and electrochemical stability with the metallic lithium (Li) anode. However, solid-state polymer electrolytes generally show low ionic conductivity and high interfacial impedance to electrodes. Here we report a hybrid solid-state electrolyte, presenting an ultra-high ionic conductivity of 3.27 mS cm −1 at room temperature, a wide electrochemical stability window of 4.9 V, and non-flammability. This electrolyte consists of a polymer blend matrix (polyethylene oxide and poly (vinylidene fluoride-co-hexafluoropropylene)), Li + conductive ceramic filler (Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 ) and a solvate ionic liquid (LiFSI in tetra ethylene glycol dimethyl ether, 1:1 in molar ratio) as plasticizer. The introduction of the solvate ionic liquid to the solid-state electrolyte not only improves its ionic conductivity but also remarkably enhances the stability of the interface with Li anode. When applied in Li metal batteries, a Li|Li symmetric cell can operate stably over 800 h with a minimal polarization of 25 mV and a full Li|LiFePO 4 cell delivers a high specific capacity of 158 mAh g −1 after 100 cycles at room temperature.
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| 8. |
- Liu, Yangyang, et al.
(author)
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Electro-Chemo-Mechanical Modeling of Artificial Solid Electrolyte Interphase to Enable Uniform Electrodeposition of Lithium Metal Anodes
- 2022
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In: Advanced Energy Materials. - : Wiley. - 1614-6840 .- 1614-6832. ; 12:9
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Journal article (peer-reviewed)abstract
- Nonuniform electrodeposition of lithium during charging processes is the key issue hindering development of rechargeable Li metal batteries. This deposition process is largely controlled by the solid electrolyte interphase (SEI) on the metal surface and the design of artificial SEIs is an essential pathway to regulate electrodeposition of Li. In this work, an electro-chemo-mechanical model is built and implemented in a phase-field modelling to understand the correlation between the physical properties of artificial SEIs and deposition of Li. The results show that improving ionic conductivity of the SEI above a critical level can mitigate stress concentration and preferred deposition of Li. In addition, the mechanical strength of the SEI is found to also mitigate non-uniform deposition and influence electrochemical kinetics, with a Young's modulus around 4.0 GPa being a threshold value for even deposition of Li. By comparison of the results to experimental results for artificial SEIs it is clear that the most important direction for future work is to improve the ionic conductivity without compromising mechanical strength. In addition, the findings and methodology presented here not only provide detailed guidelines for design of artificial SEI on Li-metal anodes but also pave the way to explore strategies for regulating deposition of other metal anodes.
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| 9. |
- Liu, Yangyang, et al.
(author)
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Insight into the Critical Role of Exchange Current Density on Electrodeposition Behavior of Lithium Metal
- 2021
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In: Advanced Science. - : Wiley. - 2198-3844 .- 2198-3844. ; 8:5
-
Journal article (peer-reviewed)abstract
- Due to an ultrahigh theoretical specific capacity of 3860 mAh g−1, lithium (Li) is regarded as the ultimate anode for high-energy-density batteries. However, the practical application of Li metal anode is hindered by safety concerns and low Coulombic efficiency both of which are resulted fromunavoidable dendrite growth during electrodeposition. This study focuses on a critical parameter for electrodeposition, the exchange current density, which has attracted only little attention in research on Li metal batteries. A phase-field model is presented to show the effect of exchange current density on electrodeposition behavior of Li. The results show that a uniform distribution of cathodic current density, hence uniform electrodeposition, on electrode is obtained with lower exchange current density. Furthermore, it is demonstrated that lower exchange current density contributes to form a larger critical radius of nucleation in the initial electrocrystallization that results in a dense deposition of Li, which is a foundation for improved Coulombic efficiency and dendrite-free morphology. The findings not only pave the way to practical rechargeable Li metal batteries but can also be translated to the design of stable metal anodes, e.g., for sodium (Na), magnesium (Mg), and zinc (Zn) batteries.
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| 10. |
- Liu, Yangyang, et al.
(author)
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Promoted rate and cycling capability of Li–S batteries enabled by targeted selection of co-solvent for the electrolyte
- 2020
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In: Energy Storage Materials. - : Elsevier BV. - 2405-8297. ; 25, s. 131-136
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Journal article (peer-reviewed)abstract
- Lithium sulfur (Li–S) batteries are considered as promising candidates for high-energy-density battery systems owing to the high theoretical capacity of sulfur (1675 mAh g−1) and low cost of raw materials. However, their practical application is hampered by low rate capability and rapid degradation of capacity, arising from the passivation of the cathode by lithium sulfides (Li2S2/Li2S) deposited during discharge and low interfacial stability of the Li anode. Herein, we report on a comprehensive strategy to select co-solvent to the electrolyte to regulate the deposition of lithium sulfides during charge-discharge process. We show that addition of a co-solvent with high solubility, and strong interaction with Li2S to a conventional electrolyte effectively mitigates the formation of a passivating layer on the sulfur cathode and dramatically improves the interfacial stability of the Li anode. We demonstrate that Sulfolane (SL) has these properties and that a Li–S cell with an electrolyte containing 6 vol% SL exhibits outstanding cyclic performance (0.083% decay per cycle) and rate capability (capacity density of 765 mAh g−1 at rate of 1.0C). Thus, we provide a facile strategy for the selection of co-solvent for improved performance of Li–S batteries, realizing their practical application for high-energy-density battery systems.
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