| 1. |
- Wang, Shangjie, et al.
(author)
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In situ polymerization design of a quasi-solid electrolyte enhanced by NMP additive for lithium metal batteries
- 2024
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In: Energy Storage Materials. - : Elsevier B.V.. - 2405-8289 .- 2405-8297. ; 69
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Journal article (peer-reviewed)abstract
- Solid polymer electrolytes (SPEs) are considered one promising candidate for lithium metal batteries due to their high flexibility, low cost, and roll-to-roll scalability. However, conventional SPEs prepared via ex situ methods are confronted with challenges such as poor contact and high resistance at the electrode|SPE interface, as well as low ionic conductivity at room temperature. In this study, we developed a quasi-solid electrolyte (QSE) using an in situ polymerization approach, employing butyl acrylate as the monomer and incorporating NMP as an additive. Spectroscopic investigations and DFT calculations revealed that NMP tends to form an overleaf-structured [Li(NMP)3][TFSI] complex with LiTFSI, promoting lithium salt dissociation. Owing to this advantage, the QSE exhibits high room-temperature ionic conductivity (6.94 × 10−4 S cm−1) and an extensive electrochemical stability window (5.01 V vs. Li+/Li). Furthermore, the in situ polymerization method facilitates full contact at the interface, enhancing the interfacial stability and reducing the interface resistance, thus resulting in stable cycling of Li|Built-in QSE|Li symmetric cell for 1100 h at 0.1 mA cm−2. The assembled LiFePO4|Built-in QSE|Li cell also demonstrates excellent rate and long-term cycling performance. Our findings offer valuable insights into the interaction between organic additives and lithium salts and present a novel strategy for the development of polymer electrolytes.
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| 2. |
- Ahmad Ishfaq, Hafiz, 1995, et al.
(author)
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Enhanced performance of lithium metal batteries via cyclic fluorinated ether based electrolytes
- 2024
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In: Energy Storage Materials. - 2405-8297. ; 69
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Journal article (peer-reviewed)abstract
- To address the challenges associated with applying high-voltage cathodes in lithium metal batteries (LMBs) there is a need for new electrolytes enabling stable interphases at both electrodes. Here we attack this by using a dioxolane-derived cyclic fluorinated ether, 2,2-bis(trifluoromethyl)-1,3-dioxolane (BTFD), as a fluorinated diluent to a 1,2-dimethoxyethane (DME) based electrolyte. The cells using the resulting BTFD-based electrolytes exhibit higher Coulombic efficiencies for lithium stripping and plating as compared to those using the non-fluorinated ether-based electrolyte. This originates from the reduced formation of ‘dead Li’ at the anode, as shown by using electrochemical impedance spectroscopy (EIS). In practice, the BTFD-based electrolytes are shown to improve the performance of Li||NMC cells, which is due to the formation of a predominantly inorganic cathode electrolyte interphase (CEI) that suppresses the cathode degradation during cycling. We used X-ray photoelectron spectroscopy (XPS) and scanning transmission electron microscopy (STEM) to characterize the CEIs’ overall composition and structure. To obtain more details on the CEI speciation, Raman and nuclear magnetic resonance (NMR) spectroscopies were employed, assisted by molecular level computations. Overall, we demonstrate how the very design of the electrolyte composition influences the performance of LMBs.
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| 3. |
- Brown, John, et al.
(author)
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Exploring the electrochemistry of PTCDI for aqueous lithium-ion batteries
- 2024
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In: Energy Storage Materials. - 2405-8297. ; 66:103218
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Journal article (peer-reviewed)abstract
- Aqueous lithium-ion batteries (ALIBs) hold promise of providing cost-effective and safe energy storage in the context of an increasingly environmentally aware narrative. Moreover, mitigating concerns surrounding the critical raw materials present in traditional LIBs reinforces the alignment with such ideals. Herein, we delve into the electrochemistry of perylene-3,4,9,10-tetracarboxylic acid diimide (PTCDI) and evaluate its potential as an organic anode active material for ALIBs. We find the all-organic anode to reversibly (de)intercalate Li+ with moderately concentrated aqueous electrolytes, although in a slightly different manner compared with organic solvents. Furthermore, the half-cell electrochemical performance in terms of capacity, capacity retention, rate performance, Coulombic efficiency, and self-discharge, is all indeed satisfactory, where proof-of-concept ALIBs using the high voltage lithium manganese oxide (LMO) exhibit >70 Wh kg−1(PTCDI+LMO) and an average voltage of ca. 1.5 V. These findings have the intention to further encourage organic redox-active material R&D with more dilute aqueous electrolytes, potentially paving the way towards a greener and more sustainable energy landscape.
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| 4. |
- Jiao, Xingxing, et al.
(author)
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Grain size and grain boundary strength: Dominative role in electro-chemo-mechanical failure of polycrystalline solid-state electrolytes
- 2024
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In: Energy Storage Materials. - 2405-8297. ; 65
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Journal article (peer-reviewed)abstract
- Solid-state batteries with lithium metal anode have been accepted extensively as the competitive option to fulfill the upping requirement for safe and efficient energy devices. Nevertheless, its wide-ranging application has been impeded by the failure of solid-state electrolyte (SSE) induced by development of lithium (Li) filament. Based on the nature of polycrystalline ceramic SSE with varying grain size and boundary strength, the constitutive equation coupled with electrochemical kinetics was applied to picture the propagation of damage and corresponding disintegration caused by the development of Li filament. Based on the results, we found that the stress generated along with the growth of Li filament spreads away via the opening and sliding of grain boundary. Thus, damage occurs along grain boundaries, of which propagation behavior and damage level are controlled by grain size. Especially, over-refinement and under-refinement of grains of SSE can cause flocculent damage with inordinate damage degree and accelerate the failure time of SSE, respectively. On the other hand, the failure time is powerfully prolongated through strengthening the grain boundary of SSE. Eventually, grain size of 0.2 μm and tensile strength of grain boundary of 0.8-time-of-grain are posted as the threshold to realize the postponed failure of NASICON-based SSE. Inspiringly, electro-chemo-mechanical model in this contribution is generally applicable to other type of ceramic SSE to reveal the failure process and provide the design guideline, fostering the improvement of solid-state batteries.
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| 5. |
- Kumar, Sonal, et al.
(author)
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A Bi-based artificial interphase to achieve ultra-long cycling life of Al-metal anode in non-aqueous electrolyte
- 2024
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In: Energy Storage Materials. - 2405-8297. ; 65
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Journal article (peer-reviewed)abstract
- Rechargeable aluminum-ion batteries (RAB) with Al-metal anode are regarded as cost-effective and environmentally sustainable energy storage systems. However, tapping the high volumetric capacity of the Al-anode has been a challenge because of the spontaneous and irreversible formation of the oxide layer on its surface that renders it electrochemically inactive. Though recently reported AlCl3-based electrolytes overcome this problem by breaking down this oxide layer, their highly corrosive nature hampers commercialization. Here, we investigate a novel approach to protect the Al-anode from severe oxidation by engineering an artificial protective interphase. A unique and less corrosive combination of Al(CF3SO3)3 salt and BiCl3 additive reacts with the Al-anode intrinsically to form an inorganic-rich protective bilayer. This layer is electronically insulating and significantly reduces the charge transfer resistance and surface activation energy at the anode, enabling plating/stripping at extremely low overpotential of <0.1 V that can be sustained for record-long cycling times of >4000 h.
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| 6. |
- Ortiz-Vitoriano, N., et al.
(author)
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Unlocking the role of electrolyte concentration for Na-O 2 batteries
- 2024
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In: Energy Storage Materials. - 2405-8297. ; 70
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Journal article (peer-reviewed)abstract
- Na-O2 batteries have attracted great interest in recent years mainly due to their high energy density, in theory having prospects to outperform the commercialized lithium-ion batteries. In the quest for optimization, a recently explored approach is to use highly concentrated electrolytes (HCEs). The knowledge of molecular level of solvation as function of electrolyte concentration and its impact on Na-O2 battery performance is, however, still very limited. In this work, experimental and computational methods are used to characterize the cation solvation and when the emergence of anions into the cation first solvation shell occurs, which affects the de-solvation process and formation of discharge products. Furthermore, the solid electrolyte interphase (SEI) formed using HCEs demonstrates presence of anion fragments, with poorer protection of the Na metal anode. Moreover, the use of HCEs is also linked to lowered capacity, possibly due to a decrease in the size of the cubic-shaped discharge products as the electrolyte concentration increases, causing clogging of the pores of the air cathode. Thus, increasing the electrolyte salt concentration seems to have a detrimental effect on the cyclability of Na-O2 batteries. Instead, electrolytes with a lower than conventional salt concentration show the best performance, which highlights the importance of carefully tuning the cation solvation alongside overall physico-chemical properties to enhance battery performance.
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| 7. |
- Park, Jimin, et al.
(author)
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Introduction of a nitrate anion with solubility mediator in a carbonate-based electrolyte for a stable potassium metal anode
- 2024
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In: Energy Storage Materials. - 2405-8297. ; 69
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Journal article (peer-reviewed)abstract
- In this study, sodium nitrate (NaNO3) dissolves in a carbonate electrolyte for K-metal batteries (KMBs) using a dimethylacetamide (DMA) solvent with a higher Gutmann donor number than that of NO3−. The K-metal anode in 0.02 M NaNO3 electrolyte exhibits enhanced stability due to the modified solid-electrolyte interphase (SEI) layer resulting from the preferential reduction of NaNO3. Reduced NaNO3 forms ionically conductive and mechanically robust compounds in the SEI layer. This compound plays a critical role in altering the morphology of electrodeposited K-metal from dendritic to spherical, reducing the barrier energy of nucleation potential for K-ions. These unique features make K-metal highly resistant to dendrite formation and aggressive electrolyte chemistry. Therefore, the K-metal anode in the proposed electrolyte containing 0.02 M NaNO3 additive ensures excellent cycle life with stable Coulombic efficiency in both symmetrical K/K half cells and full-cells coupled with a Prussian green FeFe(CN)6 cathode.
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| 8. |
- Wang, Kai, et al.
(author)
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Zinc anode based alkaline energy storage system: Recent progress and future perspectives of zinc–silver battery
- 2024
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In: Energy Storage Materials. - 2405-8297. ; 69
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Research review (peer-reviewed)abstract
- Rechargeable zinc-based batteries have come to the forefront of energy storage field with a surprising pace during last decade due to the advantageous safety, abundance and relatively low cost, making them important supplements of lithium-ion batteries. As a significant role in zinc-based batteries, zinc-silver battery owns the advantages of high specific energy density, stable working voltage, high charging efficiency, safety and environmental friendliness, and it has been widely used in military such as in aerospace, deep water manned and civil field such as energy supply for watch and hearing aid. However, it is still suffering from a few drawbacks such as unsatisfactory cycle life, low utilization of the cathode. This review introduces the basic principles of zinc-silver batteries and elaborates the battery configurations aiming to understand its working mechanisms as well as the related issues. Most importantly, the very recent research updates and the concerns have arisen in the development are summarized from conventional cell to flexible device and hybrid device. Finally, the challenges and perspectives of zinc-silver batteries are further prospected to give a broad idea to readers new in the area and trigger inspirations for motivated researchers to further widen the utilization of silver-zinc batteries.
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