| 1. |
- 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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| 2. |
- 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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| 3. |
- 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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| 4. |
- 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
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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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| 5. |
- Xu, Xieyu, et al.
(author)
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Role of Li-Ion Depletion on Electrode Surface: Underlying Mechanism for Electrodeposition Behavior of Lithium Metal Anode
- 2020
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In: Advanced Energy Materials. - : Wiley. - 1614-6840 .- 1614-6832. ; 10:44
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Journal article (peer-reviewed)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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