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  • 1.
    Bergfelt, Andreas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Hernández, Guiomar
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lacey, Matthew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Bowden, Tim Melander
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    A Mechanical Robust yet highly Conductive Diblock Copolymer-based Solid Polymer Electrolyte for Room Temperature Structural Battery Applications2020In: ACS Applied Polymer Materials, ISSN 2637-6105, Vol. 2, no 2, p. 939-948Article in journal (Refereed)
    Abstract [en]

    In this paper we present a solid polymer electrolyte (SPE) that uniquely combines ionic conductivity and mechanical robustness. This is achieved with a diblock copolymer poly(benzyl methacrylate)-poly(ε-caprolactone-r-trimethylene carbonate). The SPE with 16.7 wt% lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) showed the highest ionic conductivity (9.1×10−6 S cm−1 at 30 °C) and apparent transference number (T+) of 0.64 ± 0.04. Due to the employment of the benzyl methacrylate hard-block, this SPE is mechanically robust with a storage modulus (E') of 0.2 GPa below 40 °C, similar to polystyrene, thus making it a suitable material also for load-bearing constructions. The cell Li|SPE|LiFePO4 is able to cycle reliably at 30 °C for over 300 cycles. The promising mechanical properties, desired for compatibility with Li-metal, together with the fact that BCT is a highly reliable electrolyte material makes this SPE an excellent candidate for next-generation all-solid-state batteries.

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  • 2.
    Bergfelt, Andreas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lacey, Matthew
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Guiomar, Hernández
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Mechanically Robust and Highly Conductive Di-Block Copolymers as Solid Polymer Electrolytes for Room Temperature Li-ion Batteries2018Conference paper (Other academic)
    Abstract [en]

    Alternative solid polymer electrolytes (SPEs) hosts to the archetype poly(ethylene oxide) are gaining attention thanks to their appealing properties, such as higher cation transport number, thermal stability and electrochemical stability [1]. In addition, high mechanical stability is required in order to integrate easy-to-use materials into flexible or ‘structural’ batteries [2, 3].

     In this work, a solid polymer electrolyte (SPE) featuring high ionic conductivity and mechanical robustness at room temperature is presented. The SPE consists of a di-block copolymer, poly(benzyl methacrylate)-poly(ε-caprolactone-r-trimethylene carbonate) (BCT), mixed with different loadings of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The highest ionic conductivity achieved for these SPEs was found with 16.7 wt% LiTFSI loading (BCT17), reaching 9.1 x 10-6 S cm-1 at 30 °C. The limited current fraction (F+) for the BCT17 electrolyte was calculated to be 0.64 with the Bruce-Vincent method. Furthermore, dynamic mechanical analysis showed a storage modulus (E’) of 0.2 GPa below 40 °C and 1 MPa above 50 °C. These results indicate that BCT with LiTFSI is a competitive electrolyte, combining high ionic conductivity and modulus at ambient temperatures.

     LiFePO4|BCT17|Li half-cells showed good cycling performance at 60 °C. At 30 °C, where the SPE possessed significantly higher modulus, decent cell performance could still be achieved after several optimization steps. These included incorporating a SPE as binder, and infiltration cast the SPE on the electrode to maximize the contact between both components, thereby improving the interfacial contact and decreasing the cell resistance and overpotential when cycling the battery device.

     References

    [1] J. Mindemark, M.J. Lacey, T. Bowden, D. Brandell. Prog Polym Sci, (2018). DOI: 10.1016/j.progpolymsci.2017.12.004.

    [2] J.F. Snyder, R.H. Carter, E.D. Wetzel. Chem Mater, 19 (2007) 3793-801.

    [3] W.S. Young, W.F. Kuan, Thomas H. Epps. J Polym Sci, Part B: Polym Phys, 52 (2014) 1-16.

  • 3.
    Bergfelt, Andreas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Rubatat, Laurent
    Univ Pau & Pays Adour, CNRS, Inst Sci Analyt & Physicochim Environm & Mat, UMR5254, F-64000 Pau, France.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    d8-poly(methyl methacrylate)-poly[(oligo ethylene glycol) methyl ether methacrylate] tri-block-copolymer electrolytes: Morphology, conductivity and battery performance2017In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 131, p. 234-242Article in journal (Refereed)
    Abstract [en]

    A series of deuterated tri-block copolymers with the general structure d(8)-PMMA-POEGMA-d(8)-PMMA, with variation in d(8)-PMMA chain length, were synthesized using sequential controlled radical polymerization (ATRP). Solid polymer electrolytes (SPEs) were produced by blending tri-block copolymers and lithium bis(trifluoro methylsulfonate) (LiTFSI). Small-angle neutron scattering (SANS) was used to study the bulk morphology of the deuterated tri-block copolymer electrolyte series at 25 degrees C, 60 degrees C and 95 degrees C. The lack of a second T-g in DSC analysis together with modelling with the random phase approximation model (RPA) confirmed that the electrolytes are in the mixed state, with negative Flory-Huggins interaction parameters. AC impedance spectroscopy was used to study the ionic conductivity of the SPE series in the temperature interval 30 degrees C-90 degrees C, and a battery device was constructed to evaluate a 25 wt% d(8)-PMMA electrolyte. The Li | SPE | LiFePO4 cell cycled at 60 degrees C, giving a discharge capacity of 120 mAh g(-1), while cyclic voltammetry showed that the SPE was stable at 60 degrees C.

  • 4.
    Brant, William
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Colbin, Simon
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Ojwang, Dickson O.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Schmid, Siegbert
    Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia.
    Häggstrom, Lennart
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Ericsson, Tore
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Jaworski, Aleksander
    Stockholm Univ, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden.
    Pell, Andrew J.
    Stockholm Univ, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Selective Control of Composition in Prussian White for Enhanced Material Properties2019In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 31, no 18, p. 7203-7211Article in journal (Refereed)
    Abstract [en]

    Sodium-ion batteries based on Prussian blue analogues (PBAs) are ideal for large-scale energy storage applications due to the ability to meet the huge volumes and low costs required. For Na2-xFe[Fe(CN)(6)](1-y)center dot zH(2)O, realizing its commercial potential means fine control of the concentration of sodium, Fe(CN)(6) vacancies, and water content. To date, there is a huge variation in the literature of composition leading to variable electrochemical performance. In this work, we break down the synthesis of PBAs into three steps for controlling the sodium, vacancy, and water content via an inexpensive, scalable synthesis method. We produce rhombohedral Prussian white Na1.88(5)Fe[Fe-(CN)(6)]center dot 0.18(9)H2O with an initial capacity of 158 mAh/g retaining 90% capacity after 50 cycles. Subsequent characterization revealed that the increased polarization on the 3 V plateau is coincident with a phase transition and reduced utilization of the high-spin Fe(III)/Fe(II) redox couple. This reveals a clear target for subsequent improvements of the material to boost long-term cycling stability. These results will be of great interest for the myriad of applications of PBAs, such as catalysis, magnetism, electrochromics, and gas sorption.

  • 5.
    Colbin, Simon
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Faculty of Science and Technology. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Faculty of Science and Technology. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Buckel, Alexander
    Uppsala University, Disciplinary Domain of Science and Technology, Faculty of Science and Technology. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Wang, Yong‐Lei
    Department of Materials and Environmental Chemistry Arrhenius Laboratory Stockholm University Stockholm SE‐10691 Sweden.
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Faculty of Science and Technology. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Kullgren, Jolla
    Uppsala University, Disciplinary Domain of Science and Technology, Faculty of Science and Technology. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Faculty of Science and Technology. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    A Halogen‐Free and Flame‐Retardant Sodium Electrolyte Compatible with Hard Carbon Anodes2021In: Advanced Materials Interfaces, ISSN 2196-7350, Vol. 8, no 23, article id 2101135Article in journal (Refereed)
    Abstract [en]

    For sodium-ion batteries, two pressing issues concerning electrolytes are flammability and compatibility with hard carbon anode materials. Non-flammable electrolytes that are sufficiently stable against hard carbon have—to the authors’ knowledge—previously only been obtained by either the use of high salt concentrations or additives. Herein, the authors present a simple, fluorine-free, and flame-retardant electrolyte which is compatible with hard carbon: 0.38 m sodium bis(oxalato)borate (NaBOB) in triethyl phosphate (TEP). A variety of techniques are employed to characterize the physical properties of the electrolyte, and to evaluate the electrochemical performance in full-cell sodium-ion batteries. The results reveal that the conductivity is sufficient for battery operation, no significant self-discharge occurs, and a satisfactory passivation is enabled by the electrolyte. In fact, a mean discharge capacity of 107 ± 4 mAh g−1 is achieved at the 1005th cycle, using Prussian white cathodes and hard carbon anodes. Hence, the studied electrolyte is a promising candidate for use in sodium-ion batteries.

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  • 6.
    Gond, Ritambhara
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    van Ekeren, Wessel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Non-flammable liquid electrolytes for safe batteries2021In: Materials Horizons, ISSN 2051-6347, E-ISSN 2051-6355, Vol. 8, no 11, p. 2913-2928Article in journal (Refereed)
    Abstract [en]

    With continual increments in energy density gradually boosting the performance of rechargeable alkali metal ion (e.g. Li+, Na+, K+) batteries, their safe operation is of growing importance and needs to be considered during their development. This is essential, given the high-profile incidents involving battery fires as portrayed by the media. Such hazardous events result from exothermic chemical reactions occurring between the flammable electrolyte and the electrode material under abusive operating conditions. Some classes of non-flammable organic liquid electrolytes have shown potential towards safer batteries with minimal detrimental effect on cycling and, in some cases, even enhanced performance. This article reviews the state-of-the-art in non-flammable liquid electrolytes for Li-, Na- and K-ion batteries. It provides the reader with an overview of carbonate, ether and phosphate-based organic electrolytes, co-solvated electrolytes and electrolytes with flame-retardant additives as well as highly concentrated and locally highly concentrated electrolytes, ionic liquids and inorganic electrolytes. Furthermore, the functionality and purpose of the components present in typical non-flammable mixtures are discussed. Moreover, many non-flammable liquid electrolytes are shown to offer improved cycling stability and rate capability compared to conventional flammable liquid electrolytes.

  • 7.
    Hedman, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Björefors, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Fiber Optic Sensor for Detection of Sodium Plating in Sodium-ion BatteriesManuscript (preprint) (Other academic)
    Abstract [en]

    Optical fiber sensors integrated into sodium-ion batteries could provide a battery management system (BMS) with information to identify early warning signs of plating, preventing catastrophic failure and maintaining safe operation during fast charging. This work shows the possibility to directly detect plating of sodium metal in electrochemical cells by means of operando fiber optic evanescent wave (FOEW) spectroscopy. The results include measurements with FOEW sensors on bare copper substrates as well as on hard carbon anodes during operation in both half- and full-cell configurations. Full-cells using hard carbon anodes and Prussian white cathodes with high areal capacities (>1.5 mAh cm−2) and integrated FOEW sensors are shown to cycle well in pouch cells. The results also include measurements to demonstrate plating on hard carbon during sodiation at different rates.

  • 8.
    Hedman, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Björefors, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Fiber Optic Sensors for Detection of Sodium Plating in Sodium-Ion Batteries2022In: ACS Applied Energy Materials, E-ISSN 2574-0962, Vol. 5, no 5, p. 6219-6227Article in journal (Refereed)
    Abstract [en]

    Optical fiber sensors integrated into sodium-ion batteries could provide a battery management system (BMS) with information to identify early warning signs of plating, preventing catastrophic failure and maintaining safe operation during fast charging. This work shows the possibility of directly detecting plating of sodium metal in electrochemical cells by means of operando fiber optic evanescent wave (FOEW) spectroscopy. The results include measurements with FOEW sensors on bare copper substrates as well as on hard carbon anodes during operation in both half- and full-cell configurations. Full cells using hard carbon anodes and Prussian white cathodes with high areal capacities (>1.5 mAh cm(-2)) and integrated FOEW sensors are shown to cycle well in pouch cells. The results also include measurements to demonstrate plating on hard carbon during sodiation at different rates.

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  • 9.
    Hedman, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Björefors, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Fiber Optical Detection of Lithium Plating at Graphite Anodes2023In: Advanced Materials Interfaces, ISSN 2196-7350, Vol. 10, no 3, article id 2201665Article in journal (Refereed)
    Abstract [en]

    Avoiding the plating of metallic lithium on the graphite anode in lithium-ion batteries, potentially leading to aging and the formation of dendrites is critical for long term and safe operation of the cells. In this contribution, in operando detection of lithium plating via a fiber optical sensor placed at the surface of a graphite electrode is demonstrated. The detection is based on the modulation of light at the sensing region, which is in direct contact with the graphite particles. This is first demonstrated by the intentional deposition of lithium on a copper electrode, followed by experiments with graphite electrodes in pouch cells where plating is initiated both as a result of over-lithiation and excessive cycling rates. The plating resulted in a significant loss of light from the fiber, and the findings correlated well with previous experiments on the detection of sodium plating. The modulated light is also found to correlate well with the graphite staging via changes in the optical properties of the graphite during slow (de)intercalation of lithium ions. In a practical application, the fiber optical sensor may provide a battery management system (BMS) with input to optimize the charging procedure or to warn for cell failure.

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  • 10.
    Hernández, Guiomar
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Fluorine-Free Electrolytes for Lithium and Sodium Batteries2022In: Batteries & Supercaps, E-ISSN 2566-6223, Vol. 5, no 6, article id e202100373Article, review/survey (Refereed)
    Abstract [en]

    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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  • 11.
    Källquist, Ida
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Condensed Matter Physics of Energy Materials.
    Le Ruyet, Ronan
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Liu, Haidong
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lee, Ming-Tao
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Advances in studying interfacial reactions in rechargeable batteries by photoelectron spectroscopy2022In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 10, no 37, p. 19466-19505Article, review/survey (Refereed)
    Abstract [en]

    Many of the challenges faced in the development of lithium-ion batteries (LIBs) and next-generation technologies stem from the (electro)chemical interactions between the electrolyte and electrodes during operation. It is at the electrode-electrolyte interfaces where ageing mechanisms can originate through, for example, the build-up of electrolyte decomposition products or the dissolution of metal ions. In pursuit of understanding these processes, X-ray photoelectron spectroscopy (XPS) has become one of the most important and powerful techniques in a large collection of available tools. As a highly surface-sensitive technique, it is often thought to be the most relevant in characterising the interfacial reactions that occur inside modern rechargeable batteries. This review tells the story of how XPS is employed in day-to-day battery research, as well as highlighting some of the most recent innovative in situ and operando methodologies developed to probe battery materials in ever greater detail. A large focus is placed not only on LIBs, but also on next-generation materials and future technologies, including sodium- and potassium-ion, multivalent, and solid-state batteries. The capabilities, limitations and practical considerations of XPS, particularly in relation to the investigation of battery materials, are discussed, and expectations for its use and development in the future are assessed.

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  • 12.
    Li, Zhenguang
    et al.
    Tokyo Univ Agr & Technol, Grad Sch Bioapplicat & Syst Engn, 2-24-16 Naka Cho, Koganei, Tokyo 1848588, Japan.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Uppsala Univ, Dept Chem, Angstrom Lab, SE-75121 Uppsala, Sweden.
    Tominaga, Yoichi
    Tokyo Univ Agr & Technol, Grad Sch Bioapplicat & Syst Engn, 2-24-16 Naka Cho, Koganei, Tokyo 1848588, Japan.
    Ion-Conductive and Thermal Properties of a Synergistic Poly(ethylene carbonate)/Poly(trimethylene carbonate) Blend Electrolyte2018In: Macromolecular rapid communications, ISSN 1022-1336, E-ISSN 1521-3927, Vol. 39, no 14, article id 1800146Article in journal (Refereed)
    Abstract [en]

    Electrolytes comprising poly(ethylene carbonate) (PEC)/poly(trimethylene carbonate) (PTM C) with lithium bis(trifluoromethane sulfonyl)imide (LiTFSI) are prepared by a simple solvent casting method. Although PEC and PTMC have similar chemical structures, they are immiscible and two glass transitions are present in the differential scanning calorimetry (DSC) measurements. Interestingly, these two polymers change to miscible blends with the addition of LiTFSI, and the ionic conductivity increases with increasing lithium salt concentration. The optimum composition of the blend electrolyte is achieved at PEC6PTMC4, with a conductivity as high as 10(-6) S cm(-1) at 50 degrees C. This value is greater than that for single PEC- and PTMC-based electrolytes. Moreover, the thermal stability of the blend-based electrolytes is improved as compared to PEC-based electrolytes. It is clear that the interaction between C=O groups and Li+ gives rise to a compatible amorphous phase of PEC and PTMC.

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  • 13.
    Ma, Le Anh
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Solid electrolyte interphase in Na-ion batteries2020In: Na-ion batteries / [ed] Laure Monconduit & Laurence Croguennec, Hoboken: John Wiley & Sons, 2020, p. 243-264Chapter in book (Refereed)
  • 14.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Smith, Michael J.
    Univ Minho, Ctr Quim, P-4710057 Braga, Portugal..
    Silva, Maria Manuela
    Univ Minho, Ctr Quim, P-4710057 Braga, Portugal..
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Polycarbonates as alternative electrolyte host materials for solid-state sodium batteries2017In: Electrochemistry communications, ISSN 1388-2481, E-ISSN 1873-1902, Vol. 77, p. 58-61Article in journal (Refereed)
    Abstract [en]

    This paper describes the first implementation of the aliphatic polycarbonate PTMC- that has previously been successfully applied to lithium polymer batteries- as a non-polyether host matrix in solid-state sodium batteries. Despite higher glass transition temperatures of PTMC-NaTFSI and PTMC-NaClO4 electrolytes than their Li-containing counterparts, the ionic conductivities were found to be similar to the equivalent Li salt electrolytes. Finally, the functionality of PTMC-NaTESI was demonstrated through cycling of Na/Prussian blue half-cells displaying high discharge capacities and limited polarization at C/10 and 60 degrees C.

  • 15.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Realization of Sodium-ion Batteries: From Electrode to Electrolyte Materials2020Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Batteries are among the most important technologies required to enable the world to move beyond fossil fuels towards a more efficient and environmentally friendly society based on electricity from renewable sources. Unfortunately, the rapidly increasing number and size of batteries that the world needs in order to perform this paradigm shift is putting enormous strain on the supply of traditional raw materials for batteries, such as lithium and cobalt. Batteries built using only earth abundant elements could guarantee that the supply of energy storage will be available to everyone at reasonable prices. Sodium-ion batteries are among the most popular candidates to achieve battery systems that can provide performance close to or on par with lithium-ion batteries at a lower cost and environmental impact. Although the sodium-ion and lithium-ion batteries share many properties, there is a lot of research required before sodium-ion batteries can compete with the highly optimised lithium-ion batteries. This work explores the stability of the solid electrolyte interphase (SEI) formed on the anode in sodium-ion batteries through means of electrochemical measurements and x-ray photoelectron spectroscopy (XPS) analysis. The fundamental properties in regards to solubility and electrochemical stability of the surface layer on model anodes as well as on anode materials like hard carbon and tin-phosphide is discussed. The synthesis and electrochemical performance of Prussian white comprising of all earth abundant elements for use as a low-cost and high-performance cathode material is demonstrated. The work also includes several investigations of alternative solvents and salts for electrolytes that have been analysed in conjunction with sodium-ion cells based on hard carbon and Prussian white. The electrolytes studied possess a wide spectrum of different opportunities such as high ionic conductivity, non-flammability, fluorine-free composition and improved low and high-temperature performance.

    List of papers
    1. Solubility of the Solid Electrolyte Interphase (SEI) in Sodium Ion Batteries
    Open this publication in new window or tab >>Solubility of the Solid Electrolyte Interphase (SEI) in Sodium Ion Batteries
    2016 (English)In: ACS Energy Letters, E-ISSN 2380-8195, Vol. 1, no 6, p. 1173-1178Article in journal, Letter (Refereed) Published
    Abstract [en]

    It is often stated that formation of a functional solid electrolyte interphase (SEI) in sodium ion batteries is hampered by the higher solubility of SEI components such as sodium salts in comparison to the lithium analogues. In order to investigate these phenomena, SEI formation and functionality, as well as cell self-discharge, are studied for the sodium ion system with comparative experiments on the equivalent lithium ion system. By conducting a set of experiments on carbonaceous anodes, the impact of SEI dissolution is tested. The results show that the SEI layer in sodium ion cells is inferior to that in lithium ion counterparts with regards to self-discharge; sodium cells show a loss in capacity at a dramatic rate as compared to the lithium counterparts when they are stored at sodiated and lithiated states, respectively, for a long time with no external applied current or potential. Also, synchrotron-based hard X-ray photoelectron spectroscopy measurements indicate that the major factor leading to increased self-discharge is dissolution of significant parts of the sodium-based SEI. Furthermore, the influence of fluoroethylene carbonate (FEC) electrolyte additive on self-discharge is tested as part of the work.

    Place, publisher, year, edition, pages
    American Chemical Society (ACS), 2016
    Keywords
    batteries, sodium, interphase, self-discharge
    National Category
    Inorganic Chemistry Physical Chemistry
    Research subject
    Chemistry with specialization in Inorganic Chemistry; Chemistry with specialization in Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-307681 (URN)10.1021/acsenergylett.6b00491 (DOI)000390086400016 ()
    Funder
    Swedish Energy Agency, 40468-1
    Available from: 2016-11-19 Created: 2016-11-19 Last updated: 2020-12-15Bibliographically approved
    2. Evolution of the solid electrolyte interphase on tin phosphide anodes in sodium ion batteries probed by hard x-ray photoelectron spectroscopy
    Open this publication in new window or tab >>Evolution of the solid electrolyte interphase on tin phosphide anodes in sodium ion batteries probed by hard x-ray photoelectron spectroscopy
    Show others...
    2017 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 245, p. 696-704Article in journal (Refereed) Published
    Abstract [en]

    In this work the high capacity anode material Sn4P3 for sodium ion batteries is investigated by electrochemical cycling and synchrotron-based hard x-ray photoelectron spectroscopy (HAXPES) in order to elucidate the solid electrolyte interphase (SEI) properties during the first 1.5 cycles. The electrochemical properties of tin phosphide (Sn4P3) when used as an anode material are first established in half cells versus metallic sodium in a 1 M NaFSI in EC: DEC electrolyte including 5 vol% FEC as SEI forming additive. The data from these experiments are then used to select the parameters for the samples to be analysed by HAXPES. A concise series of five cycled samples, as well as a soaked and pristine sample, were measured at different states of sodiation after the initial sodiation and after the following full cycle of sodiation and desodiation. Our results indicate that the SEI is not fully stable, as both significant thickness and composition changes are detected during cell cycling. (C) 2017 Elsevier Ltd. All rights reserved.

    Place, publisher, year, edition, pages
    PERGAMON-ELSEVIER SCIENCE LTD, 2017
    Keywords
    Solid electrolyte interphase, Sn4P3, Na-ion battery, photoelectron spectroscopy, alloying
    National Category
    Chemical Sciences
    Identifiers
    urn:nbn:se:uu:diva-334039 (URN)10.1016/j.electacta.2017.05.173 (DOI)000406762700077 ()
    Available from: 2017-11-21 Created: 2017-11-21 Last updated: 2020-04-22Bibliographically approved
    3. Capacity fading mechanism of tin phosphide anodes in sodium-ion batteries
    Open this publication in new window or tab >>Capacity fading mechanism of tin phosphide anodes in sodium-ion batteries
    2018 (English)In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 47, no 31, p. 10752-10758Article in journal (Refereed) Published
    Abstract [en]

    Tin phosphide (Sn4P3) is here investigated as an anode material in half-cell, symmetrical, and full-cell sodium-ion batteries. Results from the half-cells using two different electrolyte salts of sodium bis(fluorosulfonyl)imide (NaFSI) or sodium hexafluorophosphate (NaPF6) show that NaFSI provides improved capacity retention but results from symmetrical cells disclose no advantage for either salt. The impact of high and low desodiation cut-off potentials is studied and the results show a drastic increase in capacity retention when using the desodiation cut-off potential of 1.2 V as compared to 2.5 V. This effect is clear for both NaFSI and NaPF6 salts in a 1:1 binary mixture of ethylene carbonate and diethylene carbonate with 10 vol% fluoroethylene carbonate. Hard X-ray photoelectron spectroscopy (HAXPES) results revealed that the thickness of the solid electrolyte interphase (SEI) changed during cycling and that SEI was stripped from tin particles when tin phosphide was charged to 2.5 V with NaPF6 based electrolyte.

    National Category
    Inorganic Chemistry
    Identifiers
    urn:nbn:se:uu:diva-363107 (URN)10.1039/c8dt01068d (DOI)000441151700048 ()29978157 (PubMedID)
    Funder
    StandUp
    Available from: 2018-10-16 Created: 2018-10-16 Last updated: 2020-04-22Bibliographically approved
    4. Selective Control of Composition in Prussian White for Enhanced Material Properties
    Open this publication in new window or tab >>Selective Control of Composition in Prussian White for Enhanced Material Properties
    Show others...
    2019 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 31, no 18, p. 7203-7211Article in journal (Refereed) Published
    Abstract [en]

    Sodium-ion batteries based on Prussian blue analogues (PBAs) are ideal for large-scale energy storage applications due to the ability to meet the huge volumes and low costs required. For Na2-xFe[Fe(CN)(6)](1-y)center dot zH(2)O, realizing its commercial potential means fine control of the concentration of sodium, Fe(CN)(6) vacancies, and water content. To date, there is a huge variation in the literature of composition leading to variable electrochemical performance. In this work, we break down the synthesis of PBAs into three steps for controlling the sodium, vacancy, and water content via an inexpensive, scalable synthesis method. We produce rhombohedral Prussian white Na1.88(5)Fe[Fe-(CN)(6)]center dot 0.18(9)H2O with an initial capacity of 158 mAh/g retaining 90% capacity after 50 cycles. Subsequent characterization revealed that the increased polarization on the 3 V plateau is coincident with a phase transition and reduced utilization of the high-spin Fe(III)/Fe(II) redox couple. This reveals a clear target for subsequent improvements of the material to boost long-term cycling stability. These results will be of great interest for the myriad of applications of PBAs, such as catalysis, magnetism, electrochromics, and gas sorption.

    Place, publisher, year, edition, pages
    AMER CHEMICAL SOC, 2019
    National Category
    Materials Chemistry Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-395840 (URN)10.1021/acs.chemmater.9b01494 (DOI)000487859200012 ()
    Funder
    StandUpSwedish Research Council, 2016-03441ÅForsk (Ångpanneföreningen's Foundation for Research and Development)
    Available from: 2019-10-25 Created: 2019-10-25 Last updated: 2022-01-29Bibliographically approved
    5. Non-carbonate solvents as electrolytes for sodium-ion batteries: candidate evaluation and resistance behavior of additives and co-solvents
    Open this publication in new window or tab >>Non-carbonate solvents as electrolytes for sodium-ion batteries: candidate evaluation and resistance behavior of additives and co-solvents
    (English)Manuscript (preprint) (Other academic)
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-409480 (URN)
    Available from: 2020-04-21 Created: 2020-04-21 Last updated: 2020-04-22
    6. Sodium bis(oxalato)borate (NaBOB) in trimethyl phosphate: a fire-extinguishing, fluorine-free, and low-cost electrolyte for fullcell sodium-ion batteries
    Open this publication in new window or tab >>Sodium bis(oxalato)borate (NaBOB) in trimethyl phosphate: a fire-extinguishing, fluorine-free, and low-cost electrolyte for fullcell sodium-ion batteries
    Show others...
    2020 (English)In: ACS Applied Energy Materials, E-ISSN 2574-0962, Vol. 3, no 5, p. 4974-4982Article in journal (Refereed) Published
    Abstract [en]

    Sodium-ion batteries based on all-naturally abundant elements, in which no cobalt, nickel, copper, and fluorine is used, can lead to a major breakthrough in making batteries more sustainable. Safety aspects-in particular, flammability of electrolytes-in the state-of-the-art battery technology is another important concern, especially for applications in which large numbers of cells are employed. Nonflammable battery electrolytes studied so far are based on highly fluorinated compounds or high salt concentrations, which suffer from high cost and toxicity. We here propose an electrolyte based on a single solvent and low-cost and fluorine-free salt at a lower range of "standard" concentrations. Our results show-for the first time-that sodium bis(oxalato)borate (NaBOB) is soluble in the nonflammable solvent trimethyl phosphate (TMP). This finding enables a nonflammable electrolyte with high ionic conductivity and promising electrochemical performance in full-cell sodium-ion batteries. An electrolyte of 0.5 M NaBOB in TMP provides an ionic conductivity of 5 mS cm(-1) at room temperature, which is comparable to the commonly used electrolytes based on sodium hexafluorophosphate (NaPF6) and organic carbonate solvents. The proposed electrolyte shows a Coulombic efficiency of above 80% in the first cycle, which increased to about 97% from the second cycle in sodium-ion battery full-cells consisting of a hard carbon anode and a Prussian white cathode. This work opens up opportunities to design safe electrolytes which can further be optimized with electrolyte additives such as vinylene carbonate for industrial applications.

    Place, publisher, year, edition, pages
    American Chemical Society (ACS), 2020
    Keywords
    electrolyte salt, non-flammable, fire-retardant, hardcarbon, full-cell, Na-ion battery, TMP, NaBOB
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-409478 (URN)10.1021/acsaem.0c00522 (DOI)000537656400100 ()
    Funder
    ÅForsk (Ångpanneföreningen's Foundation for Research and Development), 19-705Swedish Foundation for Strategic Research
    Available from: 2020-04-21 Created: 2020-04-21 Last updated: 2024-06-25Bibliographically approved
    7. A wide temperature, low-cost, fluorine-free battery electrolyte based on sodium bis(oxalato)borate
    Open this publication in new window or tab >>A wide temperature, low-cost, fluorine-free battery electrolyte based on sodium bis(oxalato)borate
    (English)Manuscript (preprint) (Other academic)
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-409479 (URN)
    Available from: 2020-04-21 Created: 2020-04-21 Last updated: 2020-04-22
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  • 16.
    Mogensen, Ronnie
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Solubility of the Solid Electrolyte Interphase (SEI) in Sodium Ion Batteries2016In: ACS Energy Letters, E-ISSN 2380-8195, Vol. 1, no 6, p. 1173-1178Article in journal (Refereed)
    Abstract [en]

    It is often stated that formation of a functional solid electrolyte interphase (SEI) in sodium ion batteries is hampered by the higher solubility of SEI components such as sodium salts in comparison to the lithium analogues. In order to investigate these phenomena, SEI formation and functionality, as well as cell self-discharge, are studied for the sodium ion system with comparative experiments on the equivalent lithium ion system. By conducting a set of experiments on carbonaceous anodes, the impact of SEI dissolution is tested. The results show that the SEI layer in sodium ion cells is inferior to that in lithium ion counterparts with regards to self-discharge; sodium cells show a loss in capacity at a dramatic rate as compared to the lithium counterparts when they are stored at sodiated and lithiated states, respectively, for a long time with no external applied current or potential. Also, synchrotron-based hard X-ray photoelectron spectroscopy measurements indicate that the major factor leading to increased self-discharge is dissolution of significant parts of the sodium-based SEI. Furthermore, the influence of fluoroethylene carbonate (FEC) electrolyte additive on self-discharge is tested as part of the work.

  • 17.
    Mogensen, Ronnie
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Buckel, Alexander
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Colbin, Simon
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    A Wide-Temperature-Range, Low-Cost, Fluorine-Free Battery Electrolyte Based On Sodium Bis(Oxalate)Borate2021In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 33, no 4, p. 1130-1139Article in journal (Refereed)
    Abstract [en]

    Common battery electrolytes comprise organic carbonate solvents and fluorinated salts based on hexafluorophosphate (PF6-) anions. However, these electrolytes suffer from high flammability, limited operating temperature window, and high cost. To address those issues, we here propose a fluorine-free electrolyte based on sodium bis(oxalate)borate (NaBOB). Although lithium bis(oxalate)borate (LiBOB) has previously been investigated for lithium-ion batteries, NaBOB was considered too insoluble in organic solvents to be used in practice. Here, we show that NaBOB can be dissolved in mixtures of N-methyl-2-pyrrolidone (NMP) and trimethyl phosphate (TMP) and in each sole solvent. NMP provides higher solubility of NaBOB with a concentration of almost 0.7 M, resulting in an ionic conductivity up to 8.83 mS cm(-1) at room temperature. The physical and electrochemical properties of electrolytes based on NaBOB salt dissolved in NMP and TMP solvents and their binary mixtures are here investigated. The results include the thermal behavior of the sole solvents and their mixtures, flammability tests, NaBOB solubility, and ionic conductivity measurements of the electrolyte mixtures. Full-cell sodium-ion batteries based on hard carbon anodes and Prussian white cathodes were evaluated at room temperature and 55 degrees C using the aforementioned electrolytes. The results show a much improved performance compared to conventional electrolytes of 1 M NaPF6 in carbonate solvents at high currents and elevated temperatures. The proposed electrolytes provide a high ionic conductivity at a wide temperature range from room temperature to -60 degrees C as NMP-TMP mixtures have low freezing points. The flammability tests indicate that NaBOB in NMP-TMP electrolytes are nonflammable when the electrolyte contains more than 30 vol % TMP.

    Download full text (pdf)
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  • 18.
    Mogensen, Ronnie
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Colbin, Simon
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Menon, Ashok Sreekumar
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Björklund, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sodium bis(oxalato)borate (NaBOB) in trimethyl phosphate: a fire-extinguishing, fluorine-free, and low-cost electrolyte for fullcell sodium-ion batteries2020In: ACS Applied Energy Materials, E-ISSN 2574-0962, Vol. 3, no 5, p. 4974-4982Article in journal (Refereed)
    Abstract [en]

    Sodium-ion batteries based on all-naturally abundant elements, in which no cobalt, nickel, copper, and fluorine is used, can lead to a major breakthrough in making batteries more sustainable. Safety aspects-in particular, flammability of electrolytes-in the state-of-the-art battery technology is another important concern, especially for applications in which large numbers of cells are employed. Nonflammable battery electrolytes studied so far are based on highly fluorinated compounds or high salt concentrations, which suffer from high cost and toxicity. We here propose an electrolyte based on a single solvent and low-cost and fluorine-free salt at a lower range of "standard" concentrations. Our results show-for the first time-that sodium bis(oxalato)borate (NaBOB) is soluble in the nonflammable solvent trimethyl phosphate (TMP). This finding enables a nonflammable electrolyte with high ionic conductivity and promising electrochemical performance in full-cell sodium-ion batteries. An electrolyte of 0.5 M NaBOB in TMP provides an ionic conductivity of 5 mS cm(-1) at room temperature, which is comparable to the commonly used electrolytes based on sodium hexafluorophosphate (NaPF6) and organic carbonate solvents. The proposed electrolyte shows a Coulombic efficiency of above 80% in the first cycle, which increased to about 97% from the second cycle in sodium-ion battery full-cells consisting of a hard carbon anode and a Prussian white cathode. This work opens up opportunities to design safe electrolytes which can further be optimized with electrolyte additives such as vinylene carbonate for industrial applications.

    Download full text (pdf)
    fulltext
  • 19.
    Mogensen, Ronnie
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Colbin, Simon
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    An Attempt to Formulate Non-Carbonate Electrolytes for Sodium-Ion Batteries2021In: Batteries & Supercaps, E-ISSN 2566-6223, Vol. 4, no 5, p. 791-814Article in journal (Refereed)
    Abstract [en]

    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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    fulltext
  • 20.
    Mogensen, Ronnie
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Maibach, Julia
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brant, William R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Evolution of the solid electrolyte interphase on tin phosphide anodes in sodium ion batteries probed by hard x-ray photoelectron spectroscopy2017In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 245, p. 696-704Article in journal (Refereed)
    Abstract [en]

    In this work the high capacity anode material Sn4P3 for sodium ion batteries is investigated by electrochemical cycling and synchrotron-based hard x-ray photoelectron spectroscopy (HAXPES) in order to elucidate the solid electrolyte interphase (SEI) properties during the first 1.5 cycles. The electrochemical properties of tin phosphide (Sn4P3) when used as an anode material are first established in half cells versus metallic sodium in a 1 M NaFSI in EC: DEC electrolyte including 5 vol% FEC as SEI forming additive. The data from these experiments are then used to select the parameters for the samples to be analysed by HAXPES. A concise series of five cycled samples, as well as a soaked and pristine sample, were measured at different states of sodiation after the initial sodiation and after the following full cycle of sodiation and desodiation. Our results indicate that the SEI is not fully stable, as both significant thickness and composition changes are detected during cell cycling. (C) 2017 Elsevier Ltd. All rights reserved.

  • 21.
    Mogensen, Ronnie
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Maibach, Julia
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Capacity fading mechanism of tin phosphide anodes in sodium-ion batteries2018In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 47, no 31, p. 10752-10758Article in journal (Refereed)
    Abstract [en]

    Tin phosphide (Sn4P3) is here investigated as an anode material in half-cell, symmetrical, and full-cell sodium-ion batteries. Results from the half-cells using two different electrolyte salts of sodium bis(fluorosulfonyl)imide (NaFSI) or sodium hexafluorophosphate (NaPF6) show that NaFSI provides improved capacity retention but results from symmetrical cells disclose no advantage for either salt. The impact of high and low desodiation cut-off potentials is studied and the results show a drastic increase in capacity retention when using the desodiation cut-off potential of 1.2 V as compared to 2.5 V. This effect is clear for both NaFSI and NaPF6 salts in a 1:1 binary mixture of ethylene carbonate and diethylene carbonate with 10 vol% fluoroethylene carbonate. Hard X-ray photoelectron spectroscopy (HAXPES) results revealed that the thickness of the solid electrolyte interphase (SEI) changed during cycling and that SEI was stripped from tin particles when tin phosphide was charged to 2.5 V with NaPF6 based electrolyte.

    Download full text (pdf)
    fulltext
  • 22.
    Ojwang, Dickson O.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Häggström, Lennart
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Physics. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Ericsson, Tore
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Physics. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brant, William
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Guest water hinders sodium-ion diffusion in low-defect Berlin green cathode material2022In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 51, no 38, p. 14712-14720Article in journal (Refereed)
    Abstract [en]

    Among Prussian blue analogues (PBAs), NaxFe[Fe(CN)(6)](1-y)center dot nH(2)O is a highly attractive cathode material for sodium-ion batteries due to its high theoretical capacity of similar to 170 mA h g(-1) and inexpensive raw materials. However, concerns remain over its long-term electrochemical performance and structural factors which impact sources of resistance in the material and subsequently rate performance. Refined control of the [Fe(CN)(6)] vacancies and water content could help in realizing its market potential. In this context, we have studied a low-defect Berlin green (BG) Na0.30(5)Fe[Fe(CN)(6)](0.94(2))center dot nH(2)O with varied water content corresponding to 10, 8, 6, and 2 wt%. The impact of water on the electrochemical properties of BG was systematically investigated. The electrodes were cycled within a narrow voltage window of 3.15-3.8 V vs. Na/Na+ to avoid undesired phase transitions and side reactions while preserving the cubic structure. We demonstrate that thermal dehydration leads to a significantly improved cycling stability of over 300 cycles at 15 mA g(-1) with coulombic efficiency of >99.9%. In particular, the electrode with the lowest water content exhibited the fastest Na+-ion insertion/extraction as evidenced by the larger CV peak currents during successive scans compared to hydrated samples. The results provide fundamental insight for designing PBAs as electrode materials with enhanced electrochemical performance in energy storage applications.

  • 23.
    Ojwang, Dickson O.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Svensson, Mikael
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Njel, Christian
    Karlsruhe Inst Technol KIT, Inst Appl Mat IAM, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany.;Karlsruhe Inst Technol KIT, Karlsruhe Nano Micro Facil KNMF, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Menon, Ashok S.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Ericsson, Tore
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Häggström, Lennart
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Maibach, Julia
    Karlsruhe Inst Technol KIT, Inst Appl Mat IAM, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany.;Karlsruhe Inst Technol KIT, Karlsruhe Nano Micro Facil KNMF, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany.
    Brant, William R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Moisture-Driven Degradation Pathways in Prussian White Cathode Material for Sodium-Ion Batteries2021In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 13, no 8, p. 10054-10063Article in journal (Refereed)
    Abstract [en]

    The high-theoretical-capacity (∼170 mAh/g) Prussian white (PW), NaxFe[Fe(CN)6]y·nH2O, is one of the most promising candidates for Na-ion batteries on the cusp of commercialization. However, it has limitations such as high variability of reported stable practical capacity and cycling stability. A key factor that has been identified to affect the performance of PW is water content in the structure. However, the impact of airborne moisture exposure on the electrochemical performance of PW and the chemical mechanisms leading to performance decay have not yet been explored. Herein, we for the first time systematically studied the influence of humidity on the structural and electrochemical properties of monoclinic hydrated (M-PW) and rhombohedral dehydrated (R-PW) Prussian white. It is identified that moisture-driven capacity fading proceeds via two steps, first by sodium from the bulk material reacting with moisture at the surface to form sodium hydroxide and partial oxidation of Fe2+ to Fe3+. The sodium hydroxide creates a basic environment at the surface of the PW particles, leading to decomposition to Na4[Fe(CN)6] and iron oxides. Although the first process leads to loss of capacity, which can be reversed, the second stage of degradation is irreversible. Over time, both processes lead to the formation of a passivating surface layer, which prevents both reversible and irreversible capacity losses. This study thus presents a significant step toward understanding the large performance variations presented in the literature for PW. From this study, strategies aimed at limiting moisture-driven degradation can be designed and their efficacy assessed.

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  • 24.
    Ostrander, John
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    High Voltage Redox-Meditated Flow Batteries with Prussian Blue Solid Booster2021In: Energies, E-ISSN 1996-1073, Vol. 14, no 22, p. 7498-7498Article in journal (Refereed)
    Abstract [en]

    This work presents Prussian blue solid boosters for use in high voltage redox-mediated flow batteries (RMFB) based on non-aqueous electrolytes. The system consisted of sodium iodide as a redox mediator in an acetonitrile catholyte containing solid Prussian blue powder. The combination enabled the solid booster utilization in the proposed systems to reach as high as 66 mAh g−1 for hydrated Prussian blue and 110 mAh g−1 for anhydrous rhombohedral Prussian blue in cells with an average potential of about 3 V (vs. Na+/Na). Though the boosted system suffers from capacity fading, it opens up possibilities to develop non-aqueous RMFB with low-cost materials. flow battery; Prussian blue; solid booster; redox-mediated; non-aqueous

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  • 25.
    Sångeland, Christofer
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Stable Cycling of Sodium Metal All-Solid-State Batteries with Polycarbonate-Based Polymer Electrolytes2019In: ACS APPLIED POLYMER MATERIALS, ISSN 2637-6105, Vol. 1, no 4, p. 825-832Article in journal (Refereed)
    Abstract [en]

    Solid polymer electrolytes based on high-molecular-weight poly(trimethylene carbonate) (PTMC) in combination with NaFSI salt were investigated for application in sodium batteries. The polycarbonate host material proved to be able to dissolve large amounts of salt, at least up to a carbonate:Na+ ratio of 1:1. Combined DSC, conductivity, and FTIR data indicated the formation of a percolating network of salt clusters along with the transition to a percolation-type ion transport mechanism at the highest salt concentrations. While the highest total ionic conductivities were seen at the highest salt concentrations (up to a remarkable 5 x 10(-5) S cm(-1) at 25 degrees C at a 1:1 carbonate:Na+ ratio), the most stable battery performance was seen at a more moderate salt loading of 5:1 carbonate:Na+, reaching >80 cycles at a stable capacity of similar to 90 mAh g(-1) at 60 degrees C in a sodium metal/Prussian blue cell. The results highlight the importance of the choice of salt and salt concentration on electrolyte performance as well as demonstrate the potential of utilizing polycarbonate-based electrolytes in sodium-based energy storage systems.

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  • 26.
    Tapia-Ruiz, Nuria
    et al.
    Univ Lancaster, Dept Chem, Lancaster LA1 4YB, England.;Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Armstrong, A. Robert
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ St Andrews, Eastchem Sch Chem, St Andrews KY16 9ST, Fife, Scotland..
    Alptekin, Hande
    Imperial Coll London, Dept Chem Engn, London SW7 2AZ, England..
    Amores, Marco A.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Sheffield, Dept Chem & Biol Engn, Sheffield S1 3JD, S Yorkshire, England..
    Au, Heather
    Imperial Coll London, Dept Chem Engn, London SW7 2AZ, England..
    Barker, Jerry
    Farad Ltd, Innovat Ctr, 217 Portobello, Sheffield S1 4DP, S Yorkshire, England..
    Boston, Rebecca
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Sheffield, Dept Mat Sci & Engn, Sheffield S1 3JD, S Yorkshire, England..
    Brant, William R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brittain, Jake M.
    Univ Oxford, Inorgan Chem Lab, Oxford OX1 3QR, England..
    Chen, Yue
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Lancaster, Dept Phys, Lancaster LA1 4YB, England..
    Chhowalla, Manish
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Cambridge, Dept Mat Sci & Met, Cambridge CB3 0FS, England..
    Choi, Yong-Seok
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England. UCL, Thomas Young Ctr, Gower St, London WC1E 6BT, England..
    Costa, Sara I. R.
    Univ Lancaster, Dept Chem, Lancaster LA1 4YB, England.;Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Crespo Ribadeneyra, Maria
    Imperial Coll London, Dept Chem Engn, London SW7 2AZ, England..
    Cussen, Serena A.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Sheffield, Dept Chem & Biol Engn, Sheffield S1 3JD, S Yorkshire, England.;Univ Sheffield, Dept Mat Sci & Engn, Sheffield S1 3JD, S Yorkshire, England..
    Cussen, Edmund J.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Sheffield, Dept Chem & Biol Engn, Sheffield S1 3JD, S Yorkshire, England.;Univ Sheffield, Dept Mat Sci & Engn, Sheffield S1 3JD, S Yorkshire, England..
    David, William I. F.
    ISIS Neutron and Muon Spallation Source, STFC Rutherford Appleton Laboratory, Harwell, Oxford OX11 0QX, United Kingdom;Inorganic Chemistry Laboratory, University of Oxford, Oxford OX1 3QR, United Kingdom.
    Desai, Aamod, V
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ St Andrews, Eastchem Sch Chem, St Andrews KY16 9ST, Fife, Scotland..
    Dickson, Stewart A. M.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ St Andrews, Sch Chem, St Andrews KY16 9ST, Fife, Scotland..
    Eweka, Emmanuel, I
    Amte Power Ltd, 153A Eastern Ave,Milton Pk, Oxford OX14 4SB, England..
    Forero-Saboya, Juan D.
    Inst Ciencia Mat Barcelona ICMAB CSIC, Campus UAB, Bellaterra 08193, Catalonia, Spain..
    Grey, Clare P.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England..
    Griffin, John M.
    Univ Lancaster, Dept Chem, Lancaster LA1 4YB, England.;Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Gross, Peter
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Hua, Xiao
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ St Andrews, Eastchem Sch Chem, St Andrews KY16 9ST, Fife, Scotland..
    Irvine, John T. S.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Johansson, Patrik
    Chalmers Univ Technol, Dept Phys, S-41296 Gothenburg, Sweden.;CNRS, Alistore ERI, FR 3104, 15 Rue Baudelocque, F-80039 Amiens, France..
    Jones, Martin O.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Sci & Technol Facil Council, North Star Ave, Swindon SN2 1SZ, Wilts, England..
    Karlsmo, Martin
    Chalmers Univ Technol, Dept Phys, S-41296 Gothenburg, Sweden..
    Kendrick, Emma
    Univ Birmingham, Sch Met & Mat, Birmingham BT15 2TT, W Midlands, England..
    Kim, Eunjeong
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ St Andrews, Eastchem Sch Chem, St Andrews KY16 9ST, Fife, Scotland..
    Kolosov, Oleg, V
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Lancaster, Dept Phys, Lancaster LA1 4YB, England..
    Li, Zhuangnan
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Mertens, Stijn F. L.
    Univ Lancaster, Dept Chem, Lancaster LA1 4YB, England.;Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Monconduit, Laure
    Univ Montpellier, CNRS, ICGM, Montpellier, France.;CNRS, RS2E, Amiens, France..
    Morris, Russell E.
    Univ St Andrews, Eastchem Sch Chem, St Andrews KY16 9ST, Fife, Scotland.;Charles Univ Prague, Dept Phys & Macromol Chem, Hlavova 8, Prague 12843, Czech Republic..
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Nikman, Shahin
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    O'Keefe, Christopher A.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England..
    Ould, Darren M. C.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England..
    Palgrave, R. G.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Poizot, Philippe
    Univ Nantes, CNRS, Inst Mat Jean Rouxel, IMN, F-44000 Nantes, France..
    Ponrouch, Alexandre
    Inst Ciencia Mat Barcelona ICMAB CSIC, Campus UAB, Bellaterra 08193, Catalonia, Spain..
    Renault, Steven
    Université de Nantes, CNRS, Institut des Matériaux Jean Rouxel, IMN, F-44000 Nantes, France.
    Reynolds, Emily M.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Sci & Technol Facil Council, North Star Ave, Swindon SN2 1SZ, Wilts, England..
    Rudola, Ashish
    Farad Ltd, Innovat Ctr, 217 Portobello, Sheffield S1 4DP, S Yorkshire, England..
    Sayers, Ruth
    Farad Ltd, Innovat Ctr, 217 Portobello, Sheffield S1 4DP, S Yorkshire, England..
    Scanlon, David O.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Diamond Light Source Ltd, Diamond House,Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England..
    Sen, S.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Seymour, Valerie R.
    Univ Lancaster, Dept Chem, Lancaster LA1 4YB, England.;Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Silvan, Begona
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Sougrati, Moulay Tahar
    Univ Montpellier, CNRS, ICGM, Montpellier, France.;CNRS, RS2E, Amiens, France..
    Stievano, Lorenzo
    CNRS, RS2E, Amiens, France..
    Stone, Grant S.
    Amte Power Ltd, Denchi House,Thurso Business Pk, Thurso KW14 7XW, Caithness, England..
    Thomas, Chris, I
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Sheffield, Dept Mat Sci & Engn, Sheffield S1 3JD, S Yorkshire, England..
    Titirici, Maria-Magdalena
    Imperial Coll London, Dept Chem Engn, London SW7 2AZ, England..
    Tong, Jincheng
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England..
    Wood, Thomas J.
    SIS Neutron and Muon Spallation Source, STFC Rutherford Appleton Laboratory, Harwell, Oxford OX11 0QX, United Kingdom.
    Wright, Dominic S.
    Quad One, Faraday Inst, Harwell Sci & Innovat Campus, Oxford OX11 0RA, England.;Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England..
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    2021 roadmap for sodium-ion batteries2021In: Journal of Physics: Energy, E-ISSN 2515-7655, Vol. 3, no 3, article id 031503Article in journal (Refereed)
    Abstract [en]

    Increasing concerns regarding the sustainability of lithium sources, due to their limited availability and consequent expected price increase, have raised awareness of the importance of developing alternative energy-storage candidates that can sustain the ever-growing energy demand. Furthermore, limitations on the availability of the transition metals used in the manufacturing of cathode materials, together with questionable mining practices, are driving development towards more sustainable elements. Given the uniformly high abundance and cost-effectiveness of sodium, as well as its very suitable redox potential (close to that of lithium), sodium-ion battery technology offers tremendous potential to be a counterpart to lithium-ion batteries (LIBs) in different application scenarios, such as stationary energy storage and low-cost vehicles. This potential is reflected by the major investments that are being made by industry in a wide variety of markets and in diverse material combinations. Despite the associated advantages of being a drop-in replacement for LIBs, there are remarkable differences in the physicochemical properties between sodium and lithium that give rise to different behaviours, for example, different coordination preferences in compounds, desolvation energies, or solubility of the solid-electrolyte interphase inorganic salt components. This demands a more detailed study of the underlying physical and chemical processes occurring in sodium-ion batteries and allows great scope for groundbreaking advances in the field, from lab-scale to scale-up. This roadmap provides an extensive review by experts in academia and industry of the current state of the art in 2021 and the different research directions and strategies currently underway to improve the performance of sodium-ion batteries. The aim is to provide an opinion with respect to the current challenges and opportunities, from the fundamental properties to the practical applications of this technology.

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  • 27.
    van Ekeren, Wessel
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Albuquerque, Marcelo
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Ek, Gustav
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brant, William R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Costa, Luciano T.
    Fluminense Fed Univ, Inst Chem, Phys Chem Dept, MolMod CS, Campus Valonguinho, BR-24020141 Niteroi, RJ, Brazil..
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    A comparative analysis of the influence of hydrofluoroethers as diluents on solvation structure and electrochemical performance in non-flammable electrolytes2023In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 11, no 8, p. 4111-4125Article in journal (Refereed)
    Abstract [en]

    To enhance battery safety, it is of utmost importance to develop non-flammable electrolytes. An emerging concept within this research field is the development of localized highly concentrated electrolytes (LHCEs). This type of liquid electrolyte relies on the concept of highly concentrated electrolytes (HCEs), but possesses lower viscosity, improved conductivity and reduced costs due to the addition of diluent solvents. In this work, two different hydrofluoroethers, i.e., bis(2,2,2-trifluoroethyl) ether (BTFE) and 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE), are studied as diluents in a phosphate-based non-flammable liquid electrolyte. These two solvents were added to a highly concentrated electrolyte of 3.0 M lithium bis(fluorosulfonyl)imide (LiFSI) in triethyl phosphate (TEP) whereby the salt concentration was diluted to 1.5 M. The solvation structures of the HCE and LHCE were studied by means of Raman spectroscopy and Nuclear Magnetic Resonance (NMR) spectroscopy, where the latter was shown to be essential to provide more detailed insights. By using molecular dynamics simulations, it was shown that a highly concentrated Li+-TEP solvation sheath is formed, which can be protected by the diluents TTE and BTFE. These simulations have also clarified the energetic interaction between the components in the LHCE, which supports the experimental results from the viscosity and the NMR measurements. By performing non-covalent interaction analysis (NCI) it was possible to show the main contributions of the observed chemical shifts, which indicated that TTE has a stronger effect on the solvation structure than BTFE. Moreover, the electrochemical performances of the electrolytes were evaluated in half-cells (Li|NMC622, Li|graphite), full-cells (NMC622|graphite) and Li metal cells (Li|Cu). Galvanostatic cycling has shown that the TTE based electrolyte performs better in full-cells and Li-metal cells, compared to the BTFE based electrolyte. Operando pressure measurements have indicated that no significant amount of gases is evolved in NMC622|graphite cells using the here presented LHCEs, while a cell with 1.0 M LiFSI in TEP displayed clear formation of gaseous products in the first cycles. The formation of gaseous products is accompanied by solvent co-intercalation, as shown by operando XRD, and quick cell failure. This work provides insights on understanding the solvation structure of LHCEs and highlights the relationship between electrochemical performance and pressure evolution.

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  • 28.
    Welch, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    van Ekeren, Wessel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Eriksson, Henrik
    LiFeSiZE AB, SE-754 50, Uppsala, 754 50, SWEDEN.
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Optimization of Sodium Bis(oxalato)borate (NaBOB) in Triethyl Phosphate (TEP) by Electrolyte Additives2022In: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 169, no 12, article id 120523Article in journal (Refereed)
    Abstract [en]

    The electrolyte solution of NaBOB in TEP is a low-cost, fluorine-free and flame-retardant electrolyte with ionic conductivity of 5 mS cm(-1), recently discovered to show promises for sodium-ion batteries. Here, the abilities of this electrolyte to effectively form a solid electrolyte interphase (SEI) was augmented with five common electrolyte additives of fluoroethylene carbonate (FEC), vinylene carbonate (VC), prop-1-ene-1,3-sultone (PES), 1,3,2-dioxathiolane 2,2-dioxide (DTD) and tris(trimethylsilyl)phosphite (TTSPi). Full-cells with electrodes of Prussian white and hard carbon and industrial mass loadings of >10 mg cm(-2) and electrolyte volumes of <5 ml g(-1) were used. X-ray photoelectron spectroscopy (XPS) and pressure analysis were also deployed to investigate parasitic reactions. Cells using electrolyte additives of PES, PES+DTD and PES+TTSPi (3 wt%) showed significantly increased performance in terms of capacity retention and initial Coulombic efficiency as compared to additive-free NaBOB-TEP. The best cell retained 80% discharge capacity (89 mAh g(-1)) after 450 cycles, which is also significantly better than reference cells using 1 M NaPF6 in EC:DEC electrolyte. This study sheds light on opportunities to optimize the NaBOB-TEP electrolyte for full-cell sodium-ion batteries in order to move from low-mass-loading lab-scale electrodes to high mass loading electrodes aiming for commercialization of sodium-ion batteries.

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  • 29.
    Younesi, Reza
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brant, William
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Larsson, Paul
    ALTRIS AB.
    A Cheap and Sustainable Cathode Material for Sodium Ion Batteries2017Conference paper (Other academic)
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