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1.
  • Alvi, Sajid, 1987, et al. (författare)
  • Entropy Stabilized Medium High Entropy Alloy Anodes for Lithium-Ion Batteries
  • 2024
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 7:5
  • Tidskriftsartikel (refereegranskat)abstract
    • One often proposed route to improved energy density for lithium-ion batteries is to use alloy anodes, such as silicon, able to store large amounts of lithium. Mechanical instability caused by the large expansion and contraction associated with (de)lithiation, and hence bad cyclability, has, however, so far hindered progress. As proof-of-concept of a remedy, we here present BiSbSe1.5Te1.5, a medium high-entropy alloy with improved cycling stability for conversion-alloying (de)lithiation reactions. We attain five to twenty times more stable cycles than previously reported for comparable metal-Se and -Te-based anodes, with a very good reversible capacity (464 mAh g−1) for up to 110 cycles- and this without using any carbonaceous materials to create a composite. Altogether, this highlights how alloy engineering and increased entropy materials can stabilize conversion-alloying electrodes.
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2.
  • Björklund, Erik, et al. (författare)
  • Sulfolane-Based Ethylene Carbonate-Free Electrolytes for LiNi0.6Mn0.2Co0.2O2-Li4Ti5O12 Batteries
  • 2020
  • Ingår i: Batteries & Supercaps. - : Wiley. - 2566-6223. ; 3:2, s. 201-207
  • Tidskriftsartikel (refereegranskat)abstract
    • Most electrolytes in today's lithium-ion batteries contain a large proportion of ethylene carbonate (EC) mixed with other alkyl carbonate-based solvents. EC has, however, been shown to be unstable at the high potentials at which several novel cathode materials are electrochemically active. Here, different mixtures of sulfolane and DMC are investigated in this context. The electrochemical stability is explored in addition to galvanostatic cycling of LiNi0.6Mn0.2Co0.2O2-Li4Ti5O12 (NMC-LTO) cells. The measurement of the ionic conductivity showed that mixing 25 % sulfolane into DMC improved the electrolyte properties as compared to pure DMC, making the conductivity similar to EC:DEC electrolytes and therefore fully functional. Moreover, the addition of sulfolane slightly enhanced the capacity retention, likely caused by formation of thinner and more stable surface layers on the LTO electrodes as determined by X-ray photoelectron spectroscopy (XPS). The cycling performance is especially improved for sulfolane-based electrolytes during cycling at sub-zero temperatures.
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3.
  • Bouchal, Roza, 1990, et al. (författare)
  • Monitoring Polysulfide Solubility and Diffusion in Fluorinated Ether-Based Electrolytes by Operando Raman Spectroscopy
  • 2020
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 3:5, s. 397-401
  • Tidskriftsartikel (refereegranskat)abstract
    • Polysulfide (PS) solubility is a key property of Li-S battery electrolytes for the conversion reaction(s) at the electrolyte-electrode interface. When PSs shuttle between the composite C/S cathode and the lithium metal anode, however, this leads to a continuous loss of active material and thus rapid capacity fading. In order to restrict the shuttle effect, fluorinated ethers have recently been proposed as a remedy; by only sparsely dissolving PSs they physically block the diffusion. We show here how the diffusion of PSs in fluorinated ethers, as monitored by operando Raman spectroscopy, is selective and that only short-chain PS (S42-) are soluble and diffuse. This fundamental observation can be used to further leverage the practical performance of Li-S batteries by novel electrolyte design.
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4.
  • Buckel, Alexander, et al. (författare)
  • Importance of First Cycle Conditions on the Electrochemical Performance of Hard Carbon and Prussian White Based Sodium-Ion Batteries Using Fire Resistant, Fluorine-Free Electrolyte
  • 2024
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 7:2
  • Tidskriftsartikel (refereegranskat)abstract
    • Electrolytes based on sodium bis(oxolato)borate (NaBOB) in organophosphates (trimethyl phosphate and triethyl phosphate (TEP)) have shown promise in sodium-ion batteries when compared to conventional electrolytes in that they are fire resistant, fluorine-free and are of lower toxicity. However, these electrolytes tend to exhibit low initial Coulombic efficiency and high overpotentials. We have here demonstrated that NaBOB in TEP can be used in cells with near-commercial capacity loadings. Furthermore, we have shown that formation cycle conditions have a significant positive effect on the cell performance in these higher mass loading cells, and that modification of the formation cycle conditions can be used to increase the capacity retention, lower the overpotentials, and as such increase the rate capability. The viability of optimized formation protocols was also demonstrated in scaled up prototype cells. Formation cycling: In this article we present a solution to the poor cyclability of non-flammable sodium bis(oxolato)borate (NaBOB) in triethyl phosphate (TEP) electrolyte. By developing a formation cycle specific to this NaBOB in TEP electrolyte, we are able to cycle a 4.5 Ah full cell with high mass loading electrodes to beyond 900 cycles before reaching 80 % state of health.image
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5.
  • Castelli, Ivano E., et al. (författare)
  • Data Management Plans : the Importance of Data Management in the BIG-MAP Project
  • 2021
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 4:12, s. 1803-1812
  • Tidskriftsartikel (refereegranskat)abstract
    • Open access to research data is increasingly important for accelerating research. Grant authorities therefore request detailed plans for how data is managed in the projects they finance. We have recently developed such a plan for the EU H2020 BIG-MAP project-a cross-disciplinary project targeting disruptive battery-material discoveries. Essential for reaching the goal is extensive sharing of research data across scales, disciplines and stakeholders, not limited to BIG-MAP and the European BATTERY 2030+ initiative but within the entire battery community. The key challenges faced in developing the data management plan for such a large and complex project were to generate an overview of the enormous amount of data that will be produced, to build an understanding of the data flow within the project and to agree on a roadmap for making all data FAIR (findable, accessible, interoperable, reusable). This paper describes the process we followed and how we structured the plan.
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6.
  • Celeste, Arcangelo, et al. (författare)
  • Enhancement of Functional Properties of Liquid Electrolytes for Lithium-Ion Batteries by Addition of Pyrrolidinium-Based Ionic Liquids with Long Alkyl-Chains
  • 2020
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 3:10, s. 1059-1068
  • 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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7.
  • Chien, Yu-Chuan, 1990-, et al. (författare)
  • Impact of Compression on the Electrochemical Performance of the Sulfur/Carbon Composite Electrode in Lithium-Sulfur Batteries
  • 2022
  • Ingår i: Batteries & Supercaps. - : Wiley-VCH Verlagsgesellschaft. - 2566-6223. ; 5:7
  • Tidskriftsartikel (refereegranskat)abstract
    • While lithium-sulfur batteries theoretically have both high gravimetric specific energy and volumetric energy density, only its specific energy has been experimentally demonstrated to surpass that of the state-of-the-art lithium-ion systems at cell level. One major reason for the unrealized energy density is the low capacity density of the highly porous sulfur/carbon composite as the positive electrode. In this work, mechanical compression at elevated temperature is demonstrated to be an effective method to increase the capacity density of the electrode by at least 90 % and moreover extends its cycle life. Distinct impacts of compression on the resistance profiles of electrodes with different thickness are investigated by tortuosity factors derived from both electrochemical impedance spectroscopy, X-ray computed tomography and kinetic analysis based on operando X-ray diffraction. The results highlights the importance of a homogeneous electrode structure highlight lithium-sulfur system.
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8.
  • Clarke-Hannaford, Jonathan, et al. (författare)
  • The (In-)Stability of the Ionic Liquids [(TMEDA)BH2][TFSI] and -[FSI] on the Li(001) Surface
  • 2021
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 4:7, s. 1126-1134
  • Tidskriftsartikel (refereegranskat)abstract
    • Electrolytes that can enable the use of a Li metal anode at a vast 3860 mAh/g, in place of currently used graphite anodes (372 mAh/g), are required for the advancement of next-generation rechargeable Li batteries. Both quaternary ammonium and boronium (trimethylamine)(dimethylethylamine)dihydroborate [NNBH2](+) cation-based ionic liquids (ILs) show high electrochemical stability windows and thermal stability for use in Li batteries. Cyclization of the former cation shows improved electrolyte stability compared to the open-chain counterpart. However, it is not known whether this is the case for the cyclic derivative of [NNBH2](+), N,N,N',N'-tetramethylethylenediamine)dihydroborate [(TMEDA)BH2](+). Here, the details of the initial stages of solid-electrolyte interphase (SEI) layer formation on a lithium metal surface, Li(001), for the [(TMEDA)BH2](+) based ILs are revealed using density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations. These indicate that [(TMEDA)BH2](+) remains intact, displaying a similarly weak interaction with the Li metal surface as the open-chain analogue. The chemical stability shown by the boronium cation indicates spontaneous and unwanted side reactions with the Li anode are unlikely to occur, which could help to facilitate long-term cycling stability of the battery. Altogether, the findings suggest the [(TMEDA)BH2](+) ILs, like their [NNBH2](+) IL counterparts, are viable candidates for rechargeable Li metal batteries.
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9.
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10.
  • Edstrom, K., et al. (författare)
  • The NordBatt Conferences: The Journey so Far and the Future Ahead
  • 2023
  • Ingår i: Batteries and Supercaps. - 2566-6223. ; 6:11
  • Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
    • All great things have humble beginnings. In 2013 when NordBatt started, we had no lithium-ion battery manufacturing in the Nordic countries and we had rather few EVs on the roads, although things were clearly starting to move – Tesla Model S in fact topped the monthly new car sales of Norway in September that very year. Yet, even if the field was advancing and lively, relatively few Nordic research groups were doing any kind of battery R&D. Now, in 2023, almost everything is different; batteries and “electrify everything” are seen, not only by us, as the next industrial revolution – it is a topic gathering considerably many more actors in academia as well as in the whole ecosystem of batteries.
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11.
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12.
  • Fretz, Samuel Joseph, 1987, et al. (författare)
  • Amine- and Amide-Functionalized Mesoporous Carbons: A Strategy for Improving Sulfur/Host Interactions in Li-S Batteries
  • 2020
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 3:8, s. 757-765
  • Tidskriftsartikel (refereegranskat)abstract
    • Lithium-sulfur (Li-S) batteries are of great interest due to their potentially high energy density, but the low electronic conductivity of both the sulfur (S-8) cathode active material and the final discharge product lithium sulfide (Li2S) require the use of a conductive host. Usually made of relatively hydrophobic carbon, such hosts are typically ill-suited to retain polar discharge products such as the intermediate lithium polysulfides (LiPs) and the final Li2S. Herein, we propose a route to increase the sulfur utilization by functionalizing the surface of ordered mesoporous carbon CMK3 with polar groups. These derivatized CMK3 materials are made using a simple two-step procedure of bromomethylation and subsequent nucleophilic substitution with amine or amide nucleophiles. We demonstrate that, compared to the unfunctionalized control, these modified CMK3 surfaces have considerably larger binding energies with LiPs and Li2S, which are proposed to aid the electrochemical conversion between S-8 and Li2S by keeping the LiPs species in close proximity to the carbon surface during Li-S battery cycling. As a result, the functionalized cathodes exhibit significantly improved specific capacities relative to their unmodified precursor.
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13.
  • Gebert, Florian, et al. (författare)
  • Interfacial Decomposition Behaviour of Triethyl Phosphate‐Based Electrolytes for Lithium‐Ion Batteries
  • 2024
  • Ingår i: Batteries & Supercaps. - 2566-6223.
  • Tidskriftsartikel (refereegranskat)abstract
    • Triethyl phosphate (TEP) is a cheap, environmentally benign, and non‐flammable electrolyte solvent, whose implementation in lithium‐ion batteries is held back by its co‐intercalation into graphite anodes, resulting in exfoliation of the graphite structure. In this work, the electrode‐electrolyte interface behaviour of electrolytes containing up to 100% TEP was investigated and correlated to electrochemical performance. High capacity and stable cycling are maintained with up to 30% TEP in carbonate ester‐based electrolytes, but above this threshold the reversibility of Li+ intercalation into graphite drops sharply to almost zero. This represents a potential route to improved battery safety, while TEP can also improve safety indirectly by enabling the use of lithium bis(oxalato borate), a fluorine‐free salt with limited solubility in traditional electrolytes. To understand the poor performance at TEP concentrations of >30%, its solvation behaviour and interfacial reaction chemistry were studied. Nuclear magnetic resonance spectroscopy data confirms changes in the Li+ solvation shell above 30% TEP, while operando gas analysis indicates extensive gas evolution from TEP decomposition at the electrode above the threshold concentration, which is almost entirely absent below it. X‐ray photoelectron spectroscopy depth profiling of electrodes demonstrates poor passivation by the solid electrolyte interphase above 30% TEP and significant graphite exfoliation.
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14.
  • Gustafsson, Olof, et al. (författare)
  • Design and Operation of an Operando Synchrotron Diffraction Cell Enabling Fast Cycling of Battery Materials
  • 2021
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 4:10, s. 1599-1604
  • Tidskriftsartikel (refereegranskat)abstract
    • Operation of a battery typically involves dynamic and non-equilibrium processes, making real time operando techniques crucial for understanding their nature. Operando X-ray diffraction is an important technique for investigating metastable intermediates and non-equilibrium phase transitions in crystalline electrode materials. Currently employed experimental setups often apply a disruptive approach to cell design, whereby the integrity of standard electrochemical cells is compromised to facilitate collection of high-quality diffraction data. Here, we present a non-disruptive approach to adapting the use of a standard pouch cell that enables fast and long-term cell cycling. Suitability of the setup is demonstrated on the well-studied cathode material LiNi0.5Mn1.5O4. While exhibiting comparable electrochemical behavior to a standard pouch cell up to a current rate of 8 C (∼6.6 mA cm−2), phase transitions could be monitored accurately. Thus, the cell provides a new alternative to investigating non-equilibrium transitions and long-term aging effects in battery materials.
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15.
  • Hall, Charles Aram, et al. (författare)
  • Revisiting Amides as Cosolvents for Flame Resistant Sodium Bis(oxalato)borate in Triethyl Phosphate Electrolyte
  • 2024
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 7:1
  • Tidskriftsartikel (refereegranskat)abstract
    • In selecting electrolytes for Na-ion batteries, simply importing the analogue of common lithium-ion battery electrolytes to sodium-ion batteries does not address safety concerns like toxicity and flammability. Electrolytes based on sodium bis(oxalato)borate (NaBOB) in organophosphates like triethyl phosphate (TEP) largely alleviate these specific safety concerns. However, it may be beneficial to obtain solutions with higher ionic conductivities than NaBOB in TEP, and compare the performance in Na-ion batteries with high mass loading electrodes. Here, we have shown that N,N-dimethyl formamide (DMF), N,N-dimethyl acetamide (DMAc), and N-methyl pyrrolidone (NMP) cosolvents almost double the ionic conductivity (from similar to 3.5 mS/cm to similar to 7 mS/cm) without sacrificing the flame-retarding properties of the base NaBOB in TEP electrolyte. The physical properties of these cosolvent electrolyte mixtures are investigated, along with the electrochemical performance of these electrolytes full-cells based on hard carbon anodes and Prussian white cathodes with near-commercial areal capacity (similar to 2 mAh/cm(2)).
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16.
  • Hernández, Guiomar, et al. (författare)
  • Fluorine-Free Electrolytes for Lithium and Sodium Batteries
  • 2022
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 5:6
  • Forskningsöversikt (refereegranskat)abstract
    • Fluorinated components in the form of salts, solvents and/or additives are a staple of electrolytes for high-performance Li- and Na-ion batteries, but this comes at a cost. Issues like potential toxicity, corrosivity and environmental concerns have sparked interest in fluorine-free alternatives. Of course, these electrolytes should be able to deliver performance that is on par with the electrolytes being in use today in commercial batteries. This begs the question: Are we there yet? This review outlines why fluorine is regarded as an essential component in battery electrolytes, along with the numerous problems it causes and possible strategies to eliminate it from Li- and Na-ion battery electrolytes. The examples provided demonstrate the possibilities of creating fully fluorine-free electrolytes with similar performance as their fluorinated counterparts, but also that there is still a lot of room for improvement, not least in terms of optimizing the fluorine-free systems independently of their fluorinated predecessors.
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17.
  • Jankowski, Piotr, 1990, et al. (författare)
  • Designing High-Performant Lithium Battery Electrolytes by Utilizing Two Natures of Li+ Coordination: LiTDI/LiTFSI in Tetraglyme
  • 2021
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 4:4, s. 205-213
  • Tidskriftsartikel (refereegranskat)abstract
    • Highly concentrated electrolytes (HCEs) based on glymes, such as tetraglyme (G4), are currently the focus of much battery research, primarily due to their unique properties - especially with respect to ion transport and electrochemical stability. While the LiTFSI-G4 and LiTDI-G4 systems both have been studied extensively, we here design their hybrid electrolytes to answer; will the resulting properties be averages/superpositions or will there be synergies created? We find the latter to be true and demonstrate that the most performant electrolytes are obtained by introducing a minor amount of LiTDI to an LiTFSI based electrolyte, which promotes the disproportionation and formation of "free" cations and at the same to avoid large aggregates - shown comprehensively both experimentally and by different modelling approaches and analyses combined. This electrolyte composition strategy can be generalized to other salts and solvents and thus a route towards a flora of novel battery electrolytes is here suggested.
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18.
  • Jankowski, Piotr, 1990, et al. (författare)
  • Prospects for Improved Magnesocene-Based Magnesium Battery Electrolytes
  • 2021
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 4:8, s. 1335-1343
  • Tidskriftsartikel (refereegranskat)abstract
    • Magnesium batteries are currently attracting a lot of interest as a next generation battery technology. One critical issue is to find a suitable electrolyte and herein we explore an electrolyte based on magnesocene (MgCp2) in tetrahydrofuran (THF), aiming for low-voltage Mg batteries, with respect to: Mg plating characteristics, electrochemical stability windows, electrolyte speciation, and electrolyte decomposition reactions; both experimentally and computationally. Overall, the electrolyte does not seem to decompose on a Mg metal anode and most likely reduced solvation of Mg2+ by the Cp- anion is important and species such as MgCp2THF2 may play an important role for Mg plating with small overpotential. The oxidation limit is largely determined by the Cp- anion and density functional theory predicted oxidation reactions point to polymerized end-products to be possible. Furthermore, in silico substitution studies enable us to establish the prospects of some Cp- anion derivatives to further improve the oxidative stability, but still the Mg2+ solvation must be monitored for ease of reduction and Mg plating.
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19.
  • Jeschke, Steffen, 1986, et al. (författare)
  • Supervised Machine Learning-Based Classification of Li-S Battery Electrolytes
  • 2021
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 4:7, s. 1156-1162
  • Tidskriftsartikel (refereegranskat)abstract
    • Machine learning (ML) approaches have the potential to create a paradigm shift in science, especially for multi-variable problems at different levels. Modern battery R&D is an area intrinsically dependent on proper understanding of many different molecular level phenomena and processes alongside evaluation of application level performance: energy, power, efficiency, life-length, etc. One very promising battery technology is Li-S batteries, but the polysulfide solubility in the electrolyte must be managed. Today, many different electrolyte compositions and concepts are evaluated, but often in a more or less trial-and-error fashion. Herein, we show how supervised ML can be applied to accurately classify different Li-S battery electrolytes a priori based on predicting polysulfide solubility. The developed framework is a combined density functional theory (DFT) and statistical mechanics (COSMO-RS) based quantitative structure-property relationship (QSPR) model which easily can be extended to other battery technologies and electrolyte properties.
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20.
  • Johansson, Isabell L., et al. (författare)
  • Mechanically Stable UV-Crosslinked Polyester-Polycarbonate Solid Polymer Electrolyte for High-Temperature Batteries
  • 2020
  • Ingår i: Batteries & Supercaps. - : WILEY-V C H VERLAG GMBH. - 2566-6223. ; 3:6, s. 527-533
  • Tidskriftsartikel (refereegranskat)abstract
    • Due to the mechanism with which solid polymer electrolytes use to conduct ions, these materials are generally more suitable for high-temperature applications where the ionic conductivity is sufficient and where liquid electrolytes show insufficient stability. To enable high-temperature cycling of polymer electrolytes, the mechanical stability has to be improved. Herein, we report successful long-term cycling of a solid polyester-polycarbonate - poly(epsilon-caprolactone-co-trimethylene carbonate) (poly(CL-co-TMC)) - electrolyte cross-linked through the addition of multifunctional acrylates and the use of UV-irradiation, allowing stable cycling of cells for more than 100 cycles at 80 degrees C, with good rate capabilities (0.2 mA cm(-2)) and Coulombic efficiencies exceeding 99 %. Both the mechanical properties and the ionic conductivity of the mechanically stabilized poly(CL-co-TMC) were investigated and optimized to reduce the frequency dependence of the moduli while still achieving an acceptable ionic conductivity at elevated temperature. These results indicate that the poly(CL-co-TMC) system can straight-forwardly be modified to allow for higher-temperature applications.
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21.
  • Johansson, Patrik, 1969, et al. (författare)
  • Ten Ways to Fool the Masses When Presenting Battery Research
  • 2021
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 4:12, s. 1785 -1788
  • Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
    • As scientists within the field of battery research we may often find it quite difficult to match and trust the promises given in press releases and high-profile papers. Even though there are real breakthroughs, where the results indeed are as impressive as they are marketed to be, we may as often find the reporting of "revolutionary" results to omit critical aspects of the methods and materials used. The absolute majority of researchers do not actively pursue to present their science in any untrue fashion, but poor (ethical) judgement could affect anyone working long hours in a gloomy lab at dusk and at the same time feel being pressed for publications and citations. Here, we outline ten ways to make your results appear more attractive and ground-breaking than they actually are, especially to laypeople that might not appreciate the full range of difficulties associated with battery research. Consider it a light-hearted entry with respect to scientific quality in methodology and dissemination, that might assist you in looking for nebulous reporting practices in your own and your peers' work, but please do not consider it a guide, but a humorous contrast to the real publishing guidelines recently launched
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22.
  • Karlsmo, Martin, 1995, et al. (författare)
  • Sustainability and Technical Performance of An All-Organic Aqueous Sodium-Ion Hybrid Supercapacitor
  • 2022
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 5
  • Tidskriftsartikel (refereegranskat)abstract
    • Development of all-organic aqueous energy storage devices (ESDs) is a promising pathway towards meeting the needs of technically medium/low-demanding electrical applications. Such ESDs should favour low cost, low environmental impact, and safety, and thereby complement more expensive, high voltage, and energy/power dense ESDs such as lithium-ion batteries. Herein, we set out to assemble all-organic aqueous Na-ion hybrid supercapacitors, exclusively using commercial materials, with the aim to provide a truly sustainable and lowcost ESD. Overall, the created ESD delivers adequate technical performance in terms of capacity retention, Coulombic efficiency, energy efficiency, and energy/power density. Finally, we apply a straight-forward and qualitative biodegradability method to the ESD.
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23.
  • Klein, Antoine, 1998, et al. (författare)
  • Identifying the Role of Electrolyte Additives for Lithium Plating on Graphite Electrode by Operando X-ray Tomography
  • 2024
  • Ingår i: Batteries and Supercaps. - 2566-6223. ; 49:12, s. 5060-5083
  • Tidskriftsartikel (refereegranskat)abstract
    • The plating of lithium metal on the graphite electrode is a major degradation mechanism in lithium-ion batteries (LIBs). It brings a significant risk of internal shortcircuit by penetration of dendritic lithium through the separator, leading to short cycle life and safety issues. Understanding how and when plating occurs is crucial for the development of mitigation strategies, e. g. tuning the electrolyte composition. Here we present an operando X-ray tomographic microscopy (XTM) study to directly monitor the plating of lithium metal in a lithium/graphite cell. XTM enables a non-destructive and quantitative characterization at operando conditions of lithium deposition on a graphite electrode at relevant conditions. In this work it allows us to probe the role of the electrolyte additives vinylene carbonate (VC) and lithium bis(fluorosulfonyl)imide (LiFSI) in the standard LIB electrolyte LP57 (base electrolyte without additives). The additives show overall better performances in terms of delayed onset of lithium plating which is important for the utilisation of the full capacity of graphite intercallaiton. We show that there is a transition during lithiation of the dominating mechanism, once lithium plating is initiated this rapidly becomes dominating and hinders further intercalation. For the base electrolyte a homogeneous and dense morphology of plated lithium is found, whereas a more dendritic morphology is observed in the presence of additives. During delithiation, there is a rapid stripping of some of the plated lithium followed by deintercalation. In addition, our work provides a general methodology to track the morphology of plated lithium, which is crucial for fundamental research about battery safety.
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24.
  • Kumar, Tanuj, et al. (författare)
  • Photo-generated Charge Trapping in Phase Segregated Halide Perovskites : A Comprehensive Approach towards Efficient Photo-Rechargeable Ion Capacitors
  • 2023
  • Ingår i: Batteries & Supercaps. - : Wiley-VCH Verlagsgesellschaft. - 2566-6223. ; 6:10
  • Tidskriftsartikel (refereegranskat)abstract
    • The right balance between photo-absorption and electronic-ionic conductivity is needed for photo-rechargeable bifunctional devices for off-grid energy applications. Recently halide perovskites have been utilized for photo-rechargeable supercapacitors, but the mechanism of photo-capacitance enhancement is not known. Herein, we have fabricated mixed halide perovskites-based photo-rechargeable supercapacitors in two ways and examined the energy harvesting and storage capabilities of these devices. The porous electrode prepared from the mixed halide perovskites (CH3NH3PbBr2I) shows photo-capacitance enhancement up to 15 F/g, while the electrode prepared from the blend of CH3NH3PbBr3 and CH3NH3PbI3 (2 : 1 by molar ratio) shows the photo-capacitance diminution up to 12 F/g. Despite higher specific capacitance (~38 F/g in dark) in blend perovskites due to increased ion diffusion, the photo-generated charge trapping at nanoscale phase segregation is responsible for the diminution in photo-capacitance of these bifunctional devices, while a uniform mixing of halide ions in mixed halide perovskites nanocrystals leads to increased photo-capacitance.
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25.
  • Lee, Ming-Tao, et al. (författare)
  • The Surface Chemistry of Thin Lithium-Metal Electrodes in Lithium-Sulfur Cells
  • 2020
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 3:12, s. 1370-1376
  • Tidskriftsartikel (refereegranskat)abstract
    • In this work, we explore the surface chemistry of Li metal electrodes used in Li-S batteries when employing a very thin (30 mu m) lithium metal foil. The foil thickness is instrumental for achieving a balanced cell with optimal energy density, but previous work has largely neglected how the change to thinner anodes will influence the critical surface phenomena in the cell. X-ray photoelectron spectroscopy (XPS) was used as the main characterisation tool to follow the evolution of the solid electrolyte interphase (SEI) layer on the Li electrode, complemented by scanning electron microscopy. Based on the XPS analyses, the premature capacity fading observed for the cell with thin Li metal electrode could be ascribed to changes in the composition of the surface layer on the Li electrode, due to that the resulting rougher surface more rapidly consume the LiNO(3)electrolyte additive. This highlights that mitigating the degradation mechanisms at the Li metal surface is of large importance when the Li electrode is scaled down for better cell balancing in Li-S cells.
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26.
  • Lee, Tian Khoon, et al. (författare)
  • Polyester-ZrO2 Nanocomposite Electrolytes with High Li Transference Numbers for Ambient Temperature All-Solid-State Lithium Batteries
  • 2021
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 4:4, s. 653-662
  • Tidskriftsartikel (refereegranskat)abstract
    • Polyester- and polycarbonate-based polymer electrolytes have attracted great interest after displaying promising functionality for solid-state Li batteries. In this present work, poly(epsilon-caprolactone-co-trimethylene carbonate) electrolytes are further developed by the inclusion of ZrO2 particles, prepared by an in situ sol-gel method. SEM micrographs show that the ZrO2 particles are uniform and 30-50 nm in size. Contrary to many studies on filler-polymer electrolytes, the changes in ionic conductivity are less significant upon addition of zirconia filler to the polymer electrolyte, but remain at similar to 10(-5) S cm(-1) at room temperature. This can be explained by the amorphous nature of the polymer. Instead, high lithium transference numbers (0.83-0.87) were obtained. Plating/stripping tests with Li metal electrodes show long-term cycling performance for >1000 cycles at 0.2 mA cm(-2). Promising solid-state lithium battery cycling results at ambient temperature using the material are also shown.
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27.
  • Li, Gui, et al. (författare)
  • In operando study of microsupercapacitors with gel electrolytes using nano-beam synchrotron X-ray diffraction
  • 2024
  • Ingår i: Batteries & Supercaps. - : Wiley-VCH Verlagsgesellschaft. - 2566-6223. ; 7:8
  • Tidskriftsartikel (refereegranskat)abstract
    • Synchrotron radiation X-ray diffraction (XRD) with nanoscale beam size was used here for in situ and in operando study of micro-supercapacitors (MSC) with gel electrolyte and MXene Ti3C2Tx electrodes. The electrode structure was characterized as a function of applied voltage and distance from the gap separating electrodes using microscopic cells with cylindrical shape designed for transmission mode XRD. The devices with gel electrolytes based on H2SO4 (with H2O/PVA and DMSO/PVA) showed stable performance with no changes in MXene structure under voltage swaps between positive and negative values. Experiments with KI-based electrolytes demonstrated changes of MXene structure correlated with decrease of energy storage parameters under conditions of increased operation voltage starting from 0.8 V. The optimal performance of the MSCs was observed when the MXene structure remained unchanged upon switching the applied voltage polarity. The changes of inter-layer distance of MXene upon swap of applied voltage correlate with decrease of device performance and are undesirable for stable operation of MSC's. We also tested feasibility of X-ray fluorescence (XRF) for characterization of electrolyte ion migration in MSCs using 2D element mapping. Irreversible sorption of iodine by MXene was found using XRF mapping of charged electrodes using standard in-plane MSC device and KI electrolyte.
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28.
  • Lindberg, Simon, 1985, et al. (författare)
  • Electrochemical Behaviour of Nb-Doped Anatase TiO2 Microbeads in an Ionic Liquid Electrolyte
  • 2020
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 3:11, s. 1233-1238
  • Tidskriftsartikel (refereegranskat)abstract
    • TiO(2)is a promising material for high-power battery and supercapacitor applications. However, in general TiO(2)suffers from an initial irreversible capacity that limits its use in different applications. A combination of a microbead morphology, Nb-doping, and the use of an ionic liquid electrolyte is shown to significantly decrease the irreversible capacity loss. A change in the electrochemical response in the first cycles indicates formation of a solid-electrolyte interphase (SEI) or a modification of the structure of the surface layer of the TiO2/Nb microbeads, which apparently stabilises the performance. The change in the response is manifested in an increased charge transfer resistance and the presence of two charge transfer contributions. During prolonged cycling the TiO2/Nb electrode shows an excellent stability over 5000 cycles. Ex situ analysis after cycling shows that the overall microbead morphology is intact and that there are no changes in the crystal structure. However, a decrease in the intensity of the XRD pattern can point to a decrease in size of the nanocrystals building up the microbeads or the formation of amorphous phases.
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29.
  • Martin, Pierre-Alexandre, 1991, et al. (författare)
  • (Localized) Highly Concentrated Electrolytes for Calcium Batteries
  • 2023
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 6:5
  • Tidskriftsartikel (refereegranskat)abstract
    • The concept of non-aqueous highly concentrated electrolytes (HCEs) for modern rechargeable batteries has recently evolved further by also adding a non-coordinating solvent, i. e., a diluent, to create localized HCEs (LHCEs). LHCEs rely on a charge carrier design similar to that of HCEs in synergy with tailored macroscopic properties, especially reduced viscosity. LHCEs have now been extensively investigated for monovalent Li+ and Na+ based batteries, but here we investigate both HCEs and LHCEs for divalent Ca2+ conducting systems. Here we systematically map both molecular and macroscopic features as function of composition of Ca(TFSI)2 (calcium bis(trifluoromethane)sulfonimide) in PC (propylene carbonate) based HCEs as well as the corresponding LHCEs created using TTE (1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether) as diluent. Some unique HCE properties arise already at ca. 2.00 m, which is at a lower salt concentration than for monovalent systems, and in addition the local structure of the HCE can be maintained even within a nominal 0.45 m LHCE (starting from a 3.26 m parent HCE). The combined observations made at molecular and macro levels pave the way for further optimization of important physico-chemical properties, proper design of electrochemical investigations, and eventually a better understanding of how to best improve the desolvation kinetics at e. g., the electrolyte/electrode interfaces of a Ca metal anode.
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30.
  • Mathew, Alma, et al. (författare)
  • Understanding the Capacity Fade in Polyacrylonitrile Binder-based LiNi0.5Mn1.5O4 Cells
  • 2022
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 5:12
  • Tidskriftsartikel (refereegranskat)abstract
    • Abstract Binders are electrochemically inactive components that have a crucial impact in battery ageing although being present in only small amounts, typically 1?3?% w/w in commercial products. The electrochemical performance of a battery can be tailored via these inactive materials by optimizing the electrode integrity and surface chemistry. Polyacrylonitrile (PAN) for LiNi0.5Mn1.5O4 (LNMO) half-cells is here investigated as a binder material to enable a stable electrode-electrolyte interface. Despite being previously described in literature as an oxidatively stable polymer, it is shown that PAN degrades and develops resistive layers within the LNMO cathode. We demonstrate continuous internal resistance increase in LNMO-based cells during battery operation using intermittent current interruption (ICI) technique. Through a combination of on-line electrochemical mass spectrometry (OEMS) and X-ray photoelectron spectroscopy (XPS) characterization techniques, the degradation products can be identified as solid on the LNMO electrode surface, and no excessive gas formation seen. The increased resistance and parasitic processes are correlated to side-reactions of the PAN, possibly intramolecular cyclization, which can be identified as the main cause of the comparatively fast capacity fade.
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31.
  • Mishukova, Viktoriia, et al. (författare)
  • Microsupercapacitors Working at 250 °C
  • 2023
  • Ingår i: Batteries & Supercaps. - : Wiley-VCH Verlagsgesellschaft. - 2566-6223.
  • Tidskriftsartikel (refereegranskat)abstract
    • The raised demand for portable electronics in high-temperature environments (>150 °C) stimulates the search for solutions to release the temperature constraints of power supply. All-solid-state microsupercapacitors (MSCs) are envisioned as promising on-chip power supply components, but at present, nearly none of them can work at temperature over 200 °C, mainly restricted by the electrolytes which possess either low thermal stability or incompatible fabrication process with on-chip integration. In this work, we have developed a novel process to fabricate highly thermally stable ionic liquid/ceramic composite electrolytes for on-chip integrated MSCs. Remarkably, the electrolytes enable MSCs with graphene-based electrodes to operate at temperatures as high as 250 °C with a high areal capacitance (~72 mF cm−2 at 5 mV s−1) and good cycling stability (70 % capacitance retention after 1000 cycles at 1.4 mA cm−2).
  •  
32.
  • Mogensen, Ronnie, et al. (författare)
  • An Attempt to Formulate Non-Carbonate Electrolytes for Sodium-Ion Batteries
  • 2021
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 4:5, s. 791-814
  • Tidskriftsartikel (refereegranskat)abstract
    • Non-aqueous carbonate solvents have been the main choice for the development of lithium-ion batteries, and similarly most research on sodium-ion batteries have been performed using carbonate-based solvents. However, the differences between sodium and lithium batteries – in term chemistry/electrochemistry properties as well as electrode materials used – open up opportunities to have a new look at solvents that have attracted little attention as electrolyte solvent. This work investigates properties of a wide range of different solvent classes in the context of sodium-ion battery electrolytes and compares them to the performance of propylene carbonate. The thirteen solvents studied here include one or several members of glymes, carbonates, lactones, esters, pyrrolidones, sulfones, and alkyl phosphates. Out of those, five outperforming solvents of γ-butyrolactone (GBL), γ-valerolactone (GVL), N-methyl-2-pyrrolidone (NMP), propylene carbonate (PC), and trimethyl phosphate (TMP) were further investigated using additives of ethylene sulfite (ES), vinylene carbonate (VC), fluoroethylene carbonate (FEC), prop-1-ene-1,3-sultone (PES), sulfolane (TMS), tris(trimethylsilyl) phosphite (TTSPI), and sodium bis(oxalato)borate (NaBOB). The solvents TMS and tetraethylene glycol dimethyl ether (TEGDME) were tested in 1 : 1 mixtures by volume with the co-solvents; NMP, dimethoxyethane (DME), and TMP. All electrolytes used NaPF6 as the salt. Primary evaluation relied on electrochemical cycling of full-cell sodium-ion batteries consisting of Prussian white cathodes and hard-carbon anodes. Galvanostatic cycling was performed using both two- and three-electrode cells, in addition, cyclic and linear sweep voltammetry was used to further evaluate the electrolyte formulations. Moreover, the resistance was measured on the anode and cathode, using Intermittent current interruption (ICI) technique.
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33.
  • Navarro Suárez, Adriana, 1983, et al. (författare)
  • A Silatrane:Molecule-Based Crystal Composite Solid-State Electrolyte for All-Solid-State Lithium Batteries
  • 2019
  • Ingår i: Batteries and Supercaps. - : Wiley. - 2566-6223. ; 2:11, s. 956-962
  • Tidskriftsartikel (refereegranskat)abstract
    • All-solid-state batteries (ASSBs) are promoted as a promising option towards higher energies and power densities as well as drastically reduced safety risks as compared to conventional lithium-ion batteries (LIBs). Herein, a composite solid-state electrolyte (SSE) based on two crystalline materials with two distinctly different ion conduction mechanisms, percolation and ion hopping, is reported. By combining a silatrane (SA; here ethoxysilatrane) with a molecule-based crystal (MBC; here LiTFSI-TMEDA) the resulting SA : MBC 2 : 1 crystalline composite shows an appreciable ion conductivity of 10(-5) S cm(-1) at room temperature, and low apparent activation energy, 836 K, for the ion transport. Studies of the overall and local structure show that in the composite the Li+ and TFSI ions are dissociated, and this seems to be mediated by the SA part of the matrix. As a proof-of-concept, an ASSB based on this SSE can operate at 50 degrees C providing up to 105 mAh g(-1) during 20 cycles.
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34.
  • Palluzzi, Matteo, et al. (författare)
  • Ionic Liquids as Cathode Additives for High Voltage Lithium Batteries
  • 2024
  • Ingår i: Batteries and Supercaps. - 2566-6223. ; 7:7
  • Tidskriftsartikel (refereegranskat)abstract
    • Two oxalatoborate ionic liquids (ILs), which are commonly utilized as electrolyte additives that form a protective layer on the cathode surface, are investigated for the first time as electrode additives. Cathodes based on LiNi0.5Mn1.5O4 (LNMO) containing 3 wt % ILs, i. e., “IL-enriched cathodes”, exhibit capacity values above 120 mAh/g with high Coulombic efficiencies throughout cycling over 200 times. A cathode without ILs also exhibits a capacity of 119 mAh/g but its Coulombic efficiency becomes low and unstable after 109 cycles. In addition, when 0.3 M ILs are added to conventional carbonate-based electrolytes, the battery cycle life improves but there is a reduction in the capacity probably due to low ionic conductivity of the electrolyte mixtures. Post-mortem analyses of electrodes retrieved from cycled cells highlight less electrolyte decomposition and less cathode corrosion, enabled by using the IL as the additive in LNMO, which are confirmed by a particle shape with smooth surface identical to the fresh cathode. The study demonstrates that oxalatoborate ILs can be used as the electrode additive, and this provides a new concept for cathode formulations for high performance batteries with a small amount of ILs.
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35.
  • Qin, Leiqiang, 1987-, et al. (författare)
  • Flexible Solid-State Asymmetric Supercapacitors with Enhanced Performance Enabled by Free-Standing MXene-Biopolymer Nanocomposites and Hierarchical Graphene-RuOx Paper Electrodes
  • 2020
  • Ingår i: Batteries & Supercaps. - : WILEY-V C H VERLAG GMBH. - 2566-6223. ; 3:7, s. 604-610
  • Tidskriftsartikel (refereegranskat)abstract
    • Two-dimensional (2D) transition metal carbides and carbonitrides, called MXenes, with metallic conductivity and hydrophilic surfaces, show great promise as electrode materials for supercapacitors. A major drawback of 2D nanomaterials is the re-stacking of the nanosheets, which prevents full utilization of surface area and blocks the access of the electrolyte. In this study, a free-standing nanocomposite paper electrode is realized by combining Mo1.33C MXene and positively charged biopolymer lignin (the second most abundant biopolymer in nature, L-DEA). The self-assembled layered architecture with alternating polymer and MXene flakes increases the interlayer space to promote ion transport, and with combining charge storage capability of the lignin derivative and MXene in an interpenetrating MXene/L-DEA nanocomposite, which offers an impressive capacitance of 503.7 F g(-1). Moreover, we demonstrate flexible solid-state asymmetric supercapacitors (ASCs) using Mo1.33C@L-DEA as the negative electrode and electrochemically exfoliated graphene with ruthenium oxide (EG@RuOx) as the positive electrode. This asymmetric device operates at a voltage window of 1.35 V, which is about two times wider than that of a symmetric Mo1.33C@L-DEA based supercapacitor. Finally, the ASCs can deliver an energy density of 51.9 Wh kg(-1) at a power density of 338.5 W kg(-1), with 86 % capacitance retention after 10000 charge-discharge cycles.
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36.
  • Salian, Girish D., et al. (författare)
  • Understanding the electrochemical and interfacial behaviour of sulfolane-based electrolytes in LiNi0.5Mn1.5O4-graphite full-cells
  • 2023
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; n/a:n/a
  • Tidskriftsartikel (refereegranskat)abstract
    • An ethylene carbonate-free electrolyte composed of 1 M lithium bis(fluorosulfonyl) imide (LiFSI) in sulfolane (SL) is studied here for LiNi0.5Mn1.5O4-graphite full-cells. An important focus on the evaluation of the anodic stability of the SL electrolyte and the passivation layers formed on LNMO and graphite is being analysed along with intermittent current interruption (ICI) technique to observe the resistance while cycling. The results show that the sulfolane electrolyte shows more degradation at higher potentials unlike previous reports which suggested higher oxidative stability. However, the passivation layers formed due to this electrolyte degradation prevents further degradation. The resistance measurements show that major resistance arises from the cathode. The pressure evolution during the formation cycles suggests that there is lower gas evolution with sulfolane electrolyte than in the conventional electrolyte. The study opens a new outlook on the sulfolane based electrolyte especially regarding its oxidative/anodic stability.
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37.
  • Shao, Yunqi, et al. (författare)
  • Modelling Bulk Electrolytes and Electrolyte Interfaces with Atomistic Machine Learning
  • 2021
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 4:4, s. 585-595
  • Forskningsöversikt (refereegranskat)abstract
    • Batteries and supercapacitors are electrochemical energy storage systems which involve multiple time-scales and length-scales. In terms of the electrolyte which serves as the ionic conductor, a molecular-level understanding of the corresponding transport phenomena, electrochemical (thermal) stability and interfacial properties is crucial for optimizing the device performance and achieving safety requirements. To this end, atomistic machine learning is a promising technology for bridging microscopic models and macroscopic phenomena. Here, we provide a timely snapshot of recent advances in this area. This includes technical considerations that are particularly relevant for modelling electrolytes as well as specific examples of both bulk electrolytes and associated interfaces. A perspective on methodological challenges and new applications is also discussed.
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38.
  • Slim, Zaher, 1992, et al. (författare)
  • Hydride-Enhanced Plating and Stripping of Aluminum from Triflate-based Organic Electrolytes**
  • 2023
  • Ingår i: Batteries and Supercaps. - 2566-6223. ; 6:9
  • Tidskriftsartikel (refereegranskat)abstract
    • In the quest for developing rechargeable aluminum (Al) batteries, reversible Al plating in the absence of active-halide components is considered an immense challenge. For this reason, the choice of electrolyte has been primarily limited to the highly corrosive chloroaluminate systems based on aluminum trichloride (AlCl3). In this work, we demonstrate reversible room-temperature Al plating from an active-halide-free (AHF) organic electrolyte based on aluminum trifluoromethanesulfonate (Al(OTF)3) and lithium aluminum hydride (LiAlH4) in tetrahydrofuran (THF), as well as its AlCl3 counterpart. From insights obtained by Density Functional Theory (DFT) and Fourier-Transform Infrared (FTIR) spectroscopy, ionic speciation in the electrolyte is explored, and mechanisms for the underlying electrochemical processes in the trifluoromethanesulfonate (OTF−)-based electrolytes are proposed. Al plating and stripping were confirmed by optical microscopy, scanning electron microscopy (SEM) and X-ray diffraction (XRD). Characterizing the Al deposits from either the OTF−- or the chloride (Cl−)-based electrolytes via depth-profile X-ray Photoelectron Spectroscopy (XPS) analyses, we find that these deposits consist of metallic Al, aluminum oxide (Al2O3), and either aluminum trifluoride (AlF3) or aluminum chloride (AlxCly) contaminants arising from a reaction with the electrolyte components which occurs during the plating process.
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39.
  • Sångeland, Christofer, et al. (författare)
  • Decomposition of Carbonate-Based Electrolytes : Differences and Peculiarities for Liquids vs. Polymers Observed Using Operando Gas Analysis
  • 2021
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 4:5, s. 785-790
  • Tidskriftsartikel (refereegranskat)abstract
    • Direct tracking of solid polymer electrolyte (SPE) decomposition in comparison to a liquid analogue was accomplished by monitoring the evolution of volatile species using online electrochemical mass spectrometry (OEMS). Reduction of a poly(trimethylene carbonate)-based SPE was dominated by CO2 formation. Detection of CO2 and an absence of CO confirms a preferred reduction degradation pathway involving C−O bond cleavage at the carbonyl carbon, in correlation with earlier suggestions. In contrast, the alkyl carbonate-based liquid electrolyte exhibited extensive ethylene formation. Trace quantities of H2 evolution ascribed to water impurities were also observed in both systems. During oxidation, the SPE and liquid electrolyte exhibited CO2, CO and SO2 evolution synonymous with electrolyte solvent and salt degradation, albeit at different potentials. Overall, gas evolution rates and redox currents were lower in the SPE system. OEMS revealed significant gas formation independent of current response, as such highlighting the limitations of the voltammetry technique commonly used today to assess electrochemical stability.
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40.
  • Tavano, Ruben, 1997, et al. (författare)
  • Influence of carbonisation temperatures on multifunctional properties of carbon fibres for structural battery applications
  • 2024
  • Ingår i: Batteries and Supercaps. - 2566-6223. ; 7
  • Tidskriftsartikel (refereegranskat)abstract
    • Carbon fibres are multifunctional materials considered for the realisation of structural battery electrodes. Processing conditions affect the carbonaceous microstructure of carbon fibres. The microstructure dictates the fibre's mechanical properties, i.e. modulus and strength, as well as its electrochemical capacity. Here, carbon fibre processing conditions are investigated to identify the effect of carbonisation temperature on carbon fibre multifunctionality. Different thermal conditions during carbonisation are considered, while keeping the precursor material, applied tension, and oxidation temperature constant. The carbonaceous microstructure of fibres is investigated via wide-angle x-ray scattering (WAXS) and transmission electron microscopy (TEM) analyses to determine the effect of the carbonisation temperature. Mechanical and electrochemical tests are performed to characterise carbon fibre multifunctionality with respect to mechanical and electrochemical performance. A moderate trade-off between mechanical and electrochemical performance is demonstrated, where the elastic modulus and strength decrease and the electrochemical capacity increase with reduced carbonisation temperature. Here, for the studied temperature interval, the elastic modulus and strength is found to drop up to 7% with a 15% increase in capacity. Thus, fibres customised for targeted multifunctionality within a limited design space can be realised by careful selection of the processing conditions in conventional carbon fibre manufacture.
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41.
  • Timhagen, Johanna, 1993, et al. (författare)
  • Local Structure and Entropic Stabilization of Ca-Based Molten Salt Electrolytes
  • 2024
  • Ingår i: Batteries and Supercaps. - 2566-6223. ; In Press
  • Tidskriftsartikel (refereegranskat)abstract
    • Here molten salt electrolytes (MSEs) and specifically their physico-chemical properties as a function of composition are reported on, with a special emphasis on the compositional entropy and targeting calcium battery application. By using MSEs, several problematic issues associated with organic electrolytes, such as the blocking of Ca2+ transfer at the electrode/electrolyte interfaces and electrolyte flammability, are avoided. Ca(FSI)2 salt in combination with the analogous Li-, Na-, and KFSI salts are used in equimolar compositions to first create several ternary MSEs, melting at (ca.) 60–75 °C, a melting temperature which is further reduced to (ca.) 55 °C for the unique quaternary MSE. This is ascribed to an increased entropy of mixing, which also contributes to an improved stability (re−)crystallization, as shown by Raman spectroscopy. Furthermore, molecular dynamics simulations of the quaternary MSE alongside density functional theory calculations targeting the ion-ion interactions are used to elucidate the local structure in more detail, demonstrating that both the ionic radii and valence influence the coordination and solvation of the cations. These MSEs are stepping-stones towards completely solvent-free, semi-solid, and ideally room-temperature Ca-conducting electrolytes.
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42.
  • Wu, Liang-Ting, et al. (författare)
  • Prediction of SEI Formation in All-Solid-State Batteries : Computational Insights from PCL-based Polymer Electrolyte Decomposition on Lithium-Metal
  • 2022
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 5:9
  • Tidskriftsartikel (refereegranskat)abstract
    • Identifying the solid electrolyte interphase (SEI) components in all-solid-state lithium batteries (ASSLBs) is essential when developing strategies for improving this battery technology. However, a comprehensive understanding of the interfacial stability and decomposition reactions of solid polymer electrolyte with lithium metal anode remains a challenge, not least outside the dominating poly(ethylene oxide)-based materials. Here, we report the reactivity of an electrolyte system composed of a polyester (poly-epsilon-caprolactone, PCL) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt on Li (100) surface, and the subsequent SEI formation, using ab initio molecular dynamics (AIMD) simulations. The step-by-step electrolyte decomposition on the anode surface is monitored, and the resultant major SEI components are analyzed by Bader charges to correlate with X-ray photoelectron (XPS) signal. The presence of PCL at the Li surface promotes a rapid initial reduction of LiTFSI salt via cleavage of S-N and C-S bonds, and its complete dissociation and formation of major SEI components such as LiF, Li2O, Li2S, and C-containing species. Furthermore, a computational analysis of relevant XPS spectra is performed to support the degradation compounds.
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43.
  • Wu, Quan, et al. (författare)
  • Electro-Chemo-Mechanical Failure Mechanisms of Solid-State Electrolytes
  • 2023
  • Ingår i: Batteries and Supercaps. - 2566-6223. ; 6:11
  • Forskningsöversikt (refereegranskat)abstract
    • Solid-state lithium-metal batteries (SSLMBs) are considered as the next-generation energy storage systems due to their high theoretical energy density and safety. However, the practical deployment of SSLMBs has been impeded by the failure of solid-state electrolytes (SSEs) which is indicated by the increased impedance, elevated polarization, and capacity degradation. The failure is commonly a result of lithium (Li) dendrite growth and propagation, inactive Li generation, unstable interface formation, void and pore formation, and crack infiltration. The failure processes can be divided into electric failure, (electro)chemical failure, and mechanical failure based on the different mechanisms. The systematical understanding of SSEs failure is crucial for the development of SSEs. Therefore, this review comprehensively summarizes the details of the three SSEs failure to provide new insights for future studies, shedding light on the design of SSLMBs with high energy density, safety, and cycling stability. Failure mechanisms: This review provides a comprehensive summary of the coupled electro-chemo-mechanical failure mechanisms of solid-state electrolytes. The electric failure results from the short circuits caused by growth and propagation of Li dendrites and the capacity loss because of inactive Li formation. The formation of kinetics/thermal unstable interphase accounts for the (electro)chemical failure. Cracks infiltration and voids/pores formation lead to mechanical failure.
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44.
  • Xie, Tian, et al. (författare)
  • Rational Regulation of Cu-Co Thiospinel Hierarchical Microsphere to Enhance the Supercapacitive Properties
  • 2023
  • Ingår i: Batteries & Supercaps. - : Wiley-VCH Verlagsgesellschaft. - 2566-6223. ; 6:12
  • Tidskriftsartikel (refereegranskat)abstract
    • Micro-structure of the electrodes play significant role in regulating the supercapacitive properties. Herein, three-dimensional hierarchical heterostructures (3DHHs) CuCo2S4 microspheres with regulated micro-structure is constructed via a simple one-step method. The 3DHHs CuCo2S4 microspheres experience two-dimensional (2D) lamellar interpenetration structure→two-dimensional (2D) lamellar interpenetration structure with nanoparticles embedded on the 2D lamellar→nanoparticles assembled lamellar interpenetration structure by simply tuning the reaction time. Typically, the transition state exhibits much higher specific surface area, which is conducive to electrochemical reaction by providing adequate electrochemical interfaces. As supercapacitor electrode, the 3DHHs CuCo2S4-10 exhibits an excellent capacitance of 1060 F g−1 at 1 A g−1, and even superior capacity retention of 86.7 % at 5 A g−1 after 13000 cycles. Noteworthy, asymmetric supercapacitor assembles by 3DHHs CuCo2S4-10 and active carbon can achieve high energy density of 56.3 Wh kg−1 at 750 W kg−1, which holds more than 150 % capacitance retention over 5000 cycles. This work provides simply micro-structure regulation in materials synthesis, which has significant potential in renewable energy applications.
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45.
  • Yang, Li, et al. (författare)
  • A Highly Reversible Aqueous Ammonium-Ion Battery based on alpha-MoO3/Ti3C2Tz Anodes and (NH4)(x)MnO2/CNTs Cathodes
  • 2023
  • Ingår i: Batteries & Supercaps. - : WILEY-V C H VERLAG GMBH. - 2566-6223. ; 6
  • Tidskriftsartikel (refereegranskat)abstract
    • Aqueous ammonium-ion batteries (AAIBs) are appealing due to their relatively low cost and good rate performance. In general, AAIBs are environmentally friendlier than their non-aqueous counterparts. However, it is still a challenge to achieve highly reversible AAIBs with decent voltages and energy/power densities. Herein, we report on a full-cell configuration using alpha-MoO3/Ti3C2Tz films as anodes, and (NH4)(x)MnO2/CNTs films as cathodes in a 1 M ammonium acetate (NH4Ac) electrolyte. At 2 V, the operating cell voltage, OCV, is one of the highest reported for AAIBs. A maximum energy density of similar to 32 Wh kg(-1) (similar to 54 Wh L-1) at 0.2 A g(-1) and a maximum power density of similar to 10 kW kg(-1) (similar to 17 kW L-1) at 10 A g(-1) are attained. When the full cells are cycled 2,000 times at 1 A g(-1) they retain similar to 73 % of their initial capacity. When cycling at 10 A g(-1), similar to 96 % of capacity is retained after 43,500 cycles. After 10 h, self-discharge reduces the OCV to similar to 72 % of its original value. This work provides a roadmap for developing high performance AAIBs with high voltages and high energy/power densities. Before this is possible it is imperative that the self-discharge rate be substantially reduced.
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46.
  • Zhang, Leiting, et al. (författare)
  • Reactivity of TiS2 Anode towards Electrolytes in Aqueous Li‐ion Batteries
  • 2022
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 5:12
  • Tidskriftsartikel (refereegranskat)abstract
    • Aqueous rechargeable batteries are appealing alternatives for large-scale energy storage. Reversible cycling of high-energy aqueous batteries has been showcased using highly concentrated aqueous electrolytes, which lead to a significantly suppressed water activity and formation of a stable solid-electrolyte interphase (SEI). However, the high salt concentration inevitably raises the cost and compromises the environmental sustainability. Herein, we use layered TiS2 as a model anode to explore the feasibility of cycling aqueous cells in dilute electrolytes. By coupling three-electrode cycling data with online electrochemical mass spectrometry measurements, we depict the potential-dependent gas evolution from the cell in the absence of a stable SEI. We offer a comprehensive mechanistic understanding of the complex interfacial chemistry in dilute electrolytes, taking into account material reactivity and interfacial compatibility. Design strategies and research directions of layered-type electrodes for sustainable aqueous batteries with dilute electrolytes are recommended, based on the scientific discovery presented in this work.
  •  
47.
  • Zheng, Wei, et al. (författare)
  • MXene//MnO2 Asymmetric Supercapacitors with High Voltages and High Energy Densities
  • 2022
  • Ingår i: Batteries & Supercaps. - : Wiley-V C H Verlag GMBH. - 2566-6223. ; 5:10
  • Tidskriftsartikel (refereegranskat)abstract
    • Aqueous asymmetric supercapacitors (AASCs) can have high voltages and high energy densities. However, the rational design of AASCs with proper negative and positive electrodes remains a challenge. Herein, we report on an AASC using Mo1.33CTz MXene films as the negative electrode, and tetramethylammonium cation intercalated birnessite (TMA(+)-MnO2) films as the positive electrode in a 21 mol kg(-1) lithium bis(trifluoromethanesulphonyl)imide (LiTFSI) electrolyte. Benefiting from a high, stable voltage of 2.5 V, an energy density of 86.5 Wh L-1 at 2 mV s(-1) and a power density of 10.3 kW L-1 at 1 Vs(-1) were achieved. The cells also exhibit excellent cycling stability (>98% after 1,0000 cycles at 100 mV s(-1)) and a 51.1 % voltage retention after 10 h. This good performance is attributed to the high stable potential window and high volumetric capacitances of both Mo1.33CTz and TMA(+)-MnO2 electrodes in highly concentrated electrolytes. This work provides a roadmap for developing high performance AASCs with high voltages and high energy/power densities, with relatively slow self-discharge rates.
  •  
48.
  • Østli, Elise R. R., et al. (författare)
  • Stabilizing the Cathode Interphase of LNMO using an Ionic-liquid based Electrolyte
  • 2023
  • Ingår i: Batteries & Supercaps. - : John Wiley & Sons. - 2566-6223. ; 6:7
  • Tidskriftsartikel (refereegranskat)abstract
    • The ionic liquid (IL)-based electrolyte comprising 1.2 M lithium bis(fluorosulfonyl)imide (LiFSI) in N-propyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide (PYR13FSI) (ILE) has been evaluated as a suitable system for the high-voltage cathode material LiNi0.5-xMn1.5+xO4 (LNMO) when cycled vs. graphite anodes. The oxidative stability of the ILE was evaluated by linear sweep voltammetry (LSV) and synthetic charge-discharge profile voltammetry (SCPV) and was found to exceed that of state-of-the-art 1 M LiPF6 in 1 : 1 ethylene carbonate (EC) : diethylcarbonate (DEC) (LP40). Improved cycling performance both at 20 degrees C and 45 degrees C was found for LNMO||graphite full cells with the IL electrolyte. X-ray photoelectron spectroscopy (XPS) analysis showed that robust and predominantly inorganic surface layers were formed on the LNMO cathode using the ILE, which stabilized the electrode. Although the high viscosity of the ILE limits the rate performance at 20 degrees C, this ILE is a promising alternative electrolyte for use in lithium-ion batteries (LiBs) with high-voltage cathodes such as LNMO, especially for use at elevated temperatures.
  •  
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