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  • 1
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    (Invited) Calcium-Ion Cathode Materials
    The Electrochemical Society ; 2020
    In:  ECS Meeting Abstracts Vol. MA2020-02, No. 2 ( 2020-11-23), p. 222-222
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2020-02, No. 2 ( 2020-11-23), p. 222-222
    Abstract: Calcium-ion batteries (CIBs) could be an alternative to lithium-ion batteries (LIBs) for certain niche applications due to their theoretically high operating potentials and the high natural abundance of calcium. However, the development of CIBs has been limited by the lack of proper electrolytes and electrode materials due to the difficulties identifying Ca-ion insertion host materials. Previous efforts to develop CIB cathodes have been made mainly based on intercalation materials such as Prussian blue-based materials (1) , layered oxide materials (MoO 3 (2), V 2 O 5 (3), CaCo 2 O 4 (4-5), and layered phosphates (VOPO 4 ·2H 2 O) (6). In this discussion we will be reviewing the state of Ca-ion battery materials and delve into an analysis of several functional polyanionic materials that show promising properties and characteristics as CIB cathodes. The NASICON-type NaV 2 (PO 4 ) 3, derived from de-sodiation of Na 3 V 2 (PO 4 ) 3 , has been shown to reversibly intercalate Ca 2+ -ions (capacity 81 mA h g-1) above 3V (vs. Ca 2+ /Ca) with stable cycling performance. DFT calculations, XAS, XRD, and TEM studies were used to support the insertion of Ca-ions and give insights into the diffusion mechanism of the materials involved (7,8). The presentation will also provide insights into materials design aspects of CIB materials and note areas of need that would benefit the MV battery community. References: (1) Albert L. Lipson, Baofei Pan, Saul H. Lapidus, Chen Liao, John T. Vaughey,Brian J. Ingram “Odyssey of Rechargeable Ca-Ion Batteries: A New Energy Storage System”. Chem. Mat. 2015, 27 , 8442. (2) Marta Cabello, Francisco Nacimiento, Ricardo Alcántara, Pedro Lavela, Carlos Pérez Vicente,José L. Tirado “Applicability of Molybdite as an Electrode Material in Calcium Batteries: A Structural Study of Layer-type Ca x MoO 3 ” Chem. Mat ., 2018, 30, 5853−5861 (3) M. Bervas, L.C. Klein, G.G. Amatucci “Vanadium oxide–propylene carbonate composite as a host for theintercalation of polyvalent cations”. Solid State Ionics 2005 176, 2735–2747. (4) A. Ponrouch, M.R. Palacin “On the road toward calcium-based batteries” Current Opinion in Electrochemistry 2018 , 9 , 1-7. (5) Haesun Park, Yanjie Cui, Sanghyeon Kim, J. T. Vaughey, PeterZapol “Ca Cobaltites as Potential Cathode Materials for Rechargeable Ca-Ion Batteries: Theory and Experiment” J. Phys. Chem. C 2020, 124, 5902−5909 (6) J.J. Wang, S.S. Tan, F.Y. Xiong, R.H. Yu, P.H. Wu, L.M. Cui, Q.Y. An “VOPO4 2H(2)O as a new cathode material for rechargeable Ca-ion batteries” Chem Comm . 2020 56 3805. (7) M.L. Mao, T. Gao, T, S.Y., Hou, C.S. Wang “A critical review of cathodes for rechargeable Mg batteries” Chem Soc Reviews 2018 47 8804. (8) T.N. Chen, G.S. Gautam, W.X. Huang, G. Ceder, G “First-Principles Study of the Voltage Profile and Mobility of Mg Intercalation in a Chromium Oxide Spinel” Chem Mat 2018 30 152.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2020-022222mtgabs
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2020
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  • 2
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    Kinetics of Alloying and Deposition in Multivalent Battery Anodes Using Real-Time X-Ray Diffraction
    The Electrochemical Society ; 2016
    In:  ECS Meeting Abstracts Vol. MA2016-03, No. 2 ( 2016-06-10), p. 388-388
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2016-03, No. 2 ( 2016-06-10), p. 388-388
    Abstract: A multivalent successor to lithium ion batteries will likely incorporate a metal anode. However, many electrodeposition processes are prone to energy losses from side reactions and overpotentials for plating or stripping. To develop a link between the kinetics of crystal growth/dissolution with electrochemical data, we have followed electrodeposition of Mg and Zn with operando x-ray diffraction using a variety of electrolytes and current collectors. In some cases we find that alloying or passivation competes with metal deposition and can dramatically alter the morphology of the deposited metal, as seen by texture analysis of the diffraction.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2016-03/2/388
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    Publisher: The Electrochemical Society
    Publication Date: 2016
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  • 3
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    Cathode Coatings for Magnesium Ion Batteries
    The Electrochemical Society ; 2018
    In:  ECS Meeting Abstracts Vol. MA2018-01, No. 3 ( 2018-04-13), p. 260-260
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2018-01, No. 3 ( 2018-04-13), p. 260-260
    Abstract: Over the past 25 years, significant effort has gone into perfecting lithium ion battery chemistries, including materials coatings, electrolytes, and electrolyte additives to improve safety, capacity, and cyclability. [1,2] By comparison, the area of non-lithium-based batteries is far less explored due to the relative novelty of the technology. Magnesium ion batteries in particular are promising as a next-generation energy storage technology due to the forecasted lower costs. The best cathode materials to date have been metal sulfides and have been demonstrated to achieve high cycleability; however, their capacity and voltage are relatively low compared to state of the art Li ion batteries. One of the challenges in demonstrating high voltage MV-based systems is identifying a cathode capable of desolvating Mg 2+ at the cathode-electrolyte interface in order to allow Mg 2+ insertion. [3] Additionally, magnesium electrolytes can become quite complicated, with highly solvated ions, large anions, and a variety of both solvents and ion pairs (i.e. Mg x Cl x species). For most electrolyte/cathode pairs, the interaction between electrolyte and cathode surface is not well understood. In the case of the Chevrel Mo 6 S 8 cathode and APC electrolyte, Wan and Prendergast calculated that Mg-Cl species actually interact quite favorably with Mo 6 S 8 , which facilitates breaking the Mg-Cl bond and Mg 2+ insertion. [4] The cathode-electrolyte interface of magnesium cathode materials is what facilitates desolvation and Mg 2+ insertion. By modifying the surface of these cathodes, improvements in performance and lifetime of magnesium ion batteries could be achieved. Materials such as metal sulfides and metal nanoparticles have been demonstrated to interact with the solvated Mg complex and improve the insertion rates of Mg 2+ into a host lattice. As the Chevrel Mo 6 S 8 was calculated to favorably interact with magnesium electrolytes, it is possible that other transition metal sulfides will provide the same type of interactions and facilitate Mg 2+ insertion into cathode materials. Here we focus on Prussian blue type cathode materials, as they have a relatively high voltage and have demonstrated issues with reaching their full theoretical capacity due to desolvation and ion pairing issues. [5] Coatings of Ag­ 2 S and MnS were found to decrease the accessible capacity by about 40% (Figure 1), with similar behavior found in two different coating methods. As cathodes and electrolytes are highly particular in their interactions, coatings may also need to be tailored to the specific cathode/electrolyte system. Figure 1. Charge/discharge curves for Ni[Fe(CN) 6 ] with Mg(TFSI) 2 in propylene carbonate electrolyte, with Ag 2 S and MnS coatings. Cycled at 10 mA/g with a BP2000 carbon anode. References M. M. Thackeray, C. Wolverton and E. D. Isaacs, Energy & Environmental Science , 5 (2012). Z. Chen and J. R. Dahn, Electrochimica Acta, 49, 1079 (2004). P. Canepa, G. S. Gautam, D. C. Hannah, R. Malik, M. Lui, K. G. Gallagher, K. A. Persson, and G. Ceder, Chemical Reviews , 117, 4287 (2017). L. F. Wan, B. R. Perdue, C. A. Apblett and D. Prendergast, Chemistry of Materials , 27, 5932 (2015). A. L. Lipson, S.-D. Han, S. Kim, B. Pan, N. Sa, C. Liao, T. T. Fister, A. K. Burrell, J. T. Vaughey, and B. J. Ingram, Journal of Power Sources , 325, 646 (2016). Figure 1
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2018-01/3/260
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    Publisher: The Electrochemical Society
    Publication Date: 2018
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  • 4
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    Case Studies on Non-Aqueous Zn Ion Systems to Develop Multivalent Ion Batteries
    The Electrochemical Society ; 2016
    In:  ECS Meeting Abstracts Vol. MA2016-02, No. 5 ( 2016-09-01), p. 715-715
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2016-02, No. 5 ( 2016-09-01), p. 715-715
    Abstract: For applications involving transportation and the electricity grid, future energy storage systems will require high energy density, fast charge/discharge times, increased safety, and low cost compared to current Li-ion batteries. Non-aqueous multivalent metal (Mg, Zn, Ca, Al) based cells are a promising advanced energy storage technology due to their higher theoretical volumetric capacity, limited dendrite formation, and low cost. A major need for these systems is the development of compatible electrolytes for both electrodes that show reversible multivalent intercalation cathodes. 1,2 In the case of non-aqueous Mg or Ca ion systems the electrolyte compatibility issues (e.g., low Coulombic efficiency, a high overpotential, and corrosion) hold back the development of Mg or Ca metal batteries. 3 However, non-aqueous Zn 2+ ion chemistry in Zn metal cells with a reversible intercalation cathode is an exception among multivalent metals with a number of promising features including high volumetric capacity, 1 similar ionic radius compared with Li + and Mg 2+ ions, 4 relatively lower activation barrier energy for diffusion in cathode materials (e.g., FePO 4 , CoO 2 and V 2 O 5 ) 5 and highly-efficient reversible Zn deposition behavior on a Zn metal anode with wide electrochemical window. 3 Considering these advantages, a non-aqueous Zn system provides an opportunity to delve into the mechanisms in multivalent-ion cell chemistry and solve the present issues in multivalent cell design and prototyping. 3 In this study, the intercalation chemistry on a variety of cathodes materials (e.g., V 2 O 5 and Mn 2 O 4 ) and reversible deposition/dendritic growth issues on a Zn metal anode have been investigated in various non-aqueous Zn electrolytes. The electrochemical and transport properties―reversible Zn deposition behavior, Coulombic efficiency, anodic stability, ionic conductivity and diffusion coefficient―were characterized utilizing the experimental and computational analysis. Among various Zn metal cells, a hydrated Zn/nanostructured bilayered V 2 O 5 cell with an acetonitrile(AN)-Zn(TFSI) 2 electrolyte demonstrates good reversibility and stability for 120+ cycles with nearly 100% Coulombic efficiency and ~170 mAhg -1 of gravimetric capacity, albeit operating at a cell voltage of 0.7 V. 6 A low crystalline Zn/Nanostructured δ -MnO 2 cell with an AN-Zn(TFSI) 2 electrolyte also shows good reversibility (~100% Coulombic efficiency) and stability for 50+ cycles with ~100 mAhg -1 capacity and relatively higher operating voltage of 1.2 V. On the other hand, Zn dendrite growth studies on a Zn metal anode in non-aqueous Zn electrolytes have been performed under various conditions, including various current densities (0.1, 1.0, and 10 mA cm -2 ) and time (0.2 and 2.0 h cycle -1 ). The cycled Zn metal anodes were characterized using SEM-EDX and X-ray tomography to analyze morphological changes and dendritic growth in both selected regions and overall samples.   References J. Muldoon, C. B. Bucur and T. Gregory, Chem. Rev. 2014, 114 , 11683-11720. H. D. Yoo, I. Shterenberg, Y. Gofer, G. Gershinsky, N. Pour and D. Aurbach, Energy Environ. Sci. 2013, 6 , 2265-2279. S.-D. Han, N. N. Rajput, X. Qu, B. Pan, M. He, M. S. Ferrandon, C. Liao, K. A. Persson and A. K. Burrell, ACS Appl. Mater. Inter. 2016, 8 , 3021-3031. R. D. Shannon, Acta Cryst. 1976, A32 , 751-767. Z. Rong, R. Malik, P. Canepa, G. Gautam, M. Liu, A. Jain, K. Persson and G. Ceder, Chem. Mater. 2015, 27 , 6016-6021. P. Senguttuvan, S.-D. Han, S. Kim, A. L. Lipson, S. Tepavcevic, T. T. Fister, A. K. Burrell and C. S. Johnson, 2016, submitted.  
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2016-02/5/715
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    Publisher: The Electrochemical Society
    Publication Date: 2016
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  • 5
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    Ex Situ and Operando Characterization of Energy Storage Materials By Benchtop XAFS and XES
    The Electrochemical Society ; 2019
    In:  ECS Meeting Abstracts Vol. MA2019-01, No. 5 ( 2019-05-01), p. 534-534
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2019-01, No. 5 ( 2019-05-01), p. 534-534
    Abstract: Advanced x-ray spectroscopies permit the interrogation of a material’s local electronic structure in an element-specific manner. In particular, these techniques reveal the speciation and ligand environment of an electroactive element and can provide direct insight into the state-of-charge and state-of-health of a battery. Despite their utility, the scientific impact of advanced x-ray spectroscopies is necessarily constrained by the availability of instrumentation. For x-ray absorption fine structure (XAFS) and x-ray emission spectroscopy (XES), studies are traditionally performed at synchrotron x-ray facilities. These facilities frequently serve to push the forefront of science and, as a result, necessarily operate under an access model which excludes projects which require routine analytical characterization, rapid feedback, or regular access. Over the last four years, our group at the University of Washington has developed several families of laboratory-based instruments to expand the accessibility of advanced x-ray spectroscopies. For the study of transition metal chemistry, we have constructed two Rowland circle spectrometers based upon related designs. Both spectrometers provide energy resolutions comparable to that observed at a synchrotron endstation. Their designs are also highly efficient, allowing studies to be completed with commercial x-ray tube sources in time scales relevant for materials research programs. For many such studies, the instrumentation can generate satisfactory spectra in a matter of minutes, permitting operando studies of battery materials at charge rates in excess of 1C. From the standpoint of instrumentation, a brief review of the present designs is presented with emphasis on recent advances in extended-XAFS capabilities. Differences between the spectrometer designs and the advantages of each will also be highlighted. Regarding materials inquiry, a survey of the above instrument’s application to energy storage research is provided. This will include XAFS analyses of two systems of nanoparticle compounds which were engineered to be catalysts or pseudocapacitors. These results will facilitate a review of the information attainable from the underlying technique. The rich electronic structure of vanadyl phosphate cathode materials, as well a suite of vanadium oxides, is probed via valence-to-core XES (VTC-XES). Finally, operando x-ray absorption near-edge structure (XANES) results obtained from a pouch cell containing a nickel-rich NMC cathode at a variety of charge rates are presented.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2019-01/5/534
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    Publisher: The Electrochemical Society
    Publication Date: 2019
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  • 6
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    MgCr 2-X V x O 4 High Voltage Spinel Oxide Cathodes for Mg-Ion Batteries
    The Electrochemical Society ; 2019
    In:  ECS Meeting Abstracts Vol. MA2019-02, No. 6 ( 2019-09-01), p. 556-556
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2019-02, No. 6 ( 2019-09-01), p. 556-556
    Abstract: Theoretical and experimental evidences have revealed that Cr-spinel oxides fulfill the cationic mobility requirements of Mg-ion cathode with a suitable activation energy, while V-spinel oxides with lower redox potentials are moderate to the operating potentials of current candidates of non-aqueous high voltage electrolyte. By controlling structure, composition and complexity, a largely solid-solution MgCrVO 4 spinel was synthesized which unlike nanocomposites can bring together the advantages of each transition metal. The spinel was successfully prepared by a simple solid-state reaction with minor inactive Cr or V rich components which was confirmed via 25 Mg MAS NMR and high resolution X-ray diffraction analyses. A thermally stable Mg(TPFA) 2 /triglyme electrolyte was utilized for high temperature electrochemistry, lowering kinetic barriers at and across interfaces so as to observe reversible intercalation in the designed oxide. Multimodal characterization confirmed an apparent bulk demagnesiation from MgCrVO 4 with partial reversibility, by probing evolution of the local and long range structure as well as vanadium and chromium electronic states within the lattice. Characterization experiments also provided direct evidence of (de)intercalation reactions that occurred without any major competitive conversion reactions or insertion of protons into the lattice. These findings expand materials composition and complexity design opportunities for Mg-ion cathodes while highlighting the need to identify the origins of reversibility challenges due to but not limited to phase stability particularly for the charged states, barriers at the interface, electrolyte stability and desolvation phenomena.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2019-02/6/556
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    Publisher: The Electrochemical Society
    Publication Date: 2019
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  • 7
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    Benchtop, High-Resolution XAFS and Xes Spectrometers As Tools for Electrochemical Research
    The Electrochemical Society ; 2018
    In:  ECS Meeting Abstracts Vol. MA2018-01, No. 36 ( 2018-04-13), p. 2122-2122
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2018-01, No. 36 ( 2018-04-13), p. 2122-2122
    Abstract: Advanced x-ray spectroscopies allow the direct and element-specific interrogation of local electronic structure, yet their scientific impact is necessarily constrained by access limitations. This is particularly evident for x-ray absorption fine structure (XAFS) and x-ray emission spectroscopy (XES) techniques. Here, the technical capability afforded by a synchrotron x-ray facility allows researchers to answer basic or applied research questions and push the forefront of science. These national-lab scale sources often provide the only means to perform these techniques, consequently slowing progress on critical projects, and also largely excluding routine analytical characterization. Over the last four years, our group at the University of Washington has been developing several new families of lab-based instruments to expand the accessibility of advanced x-ray spectroscopies. [1-5] It is now possible to identify the electroactive element in a material and assess its oxidation state, spin state, and coordination chemistry – all with benchtop XAFS and XES. The feasibility of these studies is established by comparing performance of our benchtop instruments with various synchrotrons in the context of several electrochemical systems. From the standpoint of materials inquiry, we will present a variety of measurements of lithium ion batteries, valence-to-core XES results from a series of oxides, and preliminary efforts toward solution-phase measurements will be presented. The latter will be done with an eye toward future electrolyte analyses. William M. Holden, et al. “A Compact Dispersive Refocusing Rowland Circle X-ray Emission Spectrometer for Laboratory, Synchrotron and XFEL Applications”, Rev. Sci. Instrum 88 , 073904 (2017). [DOI: 10.1063/1.4994739] T. Seidler, et al., “A Laboratory-based Hard X-ray Monochromator for High-Resolution X-ray Emission Spectroscopy and X-ray Absorption Near Edge Structure Measurements,” Review of Scientific Instruments 85 , 113906 (2014). [DOI: 10.1063/1.4901599] T. Seidler, et al., “A Modern Laboratory XAFS Cookbook,” Journal of Physics: Conference Series 712 , 012015 (2016). [ http://iopscience.iop.org/article/10.1088/1742-6596/712/1/012015] R. Mortensen, et al., “Benchtop Nonresonant X-ray Emission Spectroscopy: Coming Soon to Laboratories and Beamlines Near You,” Journal of Physics: Conference Series 712 , 012036. (2016) [http://iopscience.iop.org/article/10.1088/1742-6596/712/1/012036] G.T. Seidler, “The Case for Analytical XAFS”, https://www.linkedin.com/pulse/case-benchtop-analytical-xafs-gerald-seidler
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2018-01/36/2122
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    Publisher: The Electrochemical Society
    Publication Date: 2018
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  • 8
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    Toward High Voltage Mg-Ion Battery Cathode Via a Solid-Solution Cr-Mn Spinel Oxide
    The Electrochemical Society ; 2020
    In:  ECS Meeting Abstracts Vol. MA2020-02, No. 2 ( 2020-11-23), p. 269-269
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2020-02, No. 2 ( 2020-11-23), p. 269-269
    Abstract: The capability of the tailored solid-solution spinel, MgCrMnO 4 , is evaluated by theoretical and experimental approaches. Lattice Mg 2+ in the designed oxide is electrochemically utilized at high potentials in a non-aqueous electrolyte. Complementary evidence supports bulk Mg 2+ (de)intercalation throughout the designed oxide frame where strong electrostatic interaction between Mg 2+ and O 2- exists. Mg/Mn antisite inversion in the spinel is lowered via post-annealing to further improve Mg +2 mobility. Spinel lattice is preserved upon removal of Mg 2+ without any phase transformations, denoting structural stability at the charged state at a high potential. In the remagnesiated state, insertion of Mg 2+ into interstitial sites in the spinel is detected possibly resulting in partial reversibility which needs to be addressed for structural stability. The observations constitute a first clear path to the development of a practical high voltage Mg-ion cathode using a spinel oxide.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2020-022269mtgabs
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    Publisher: The Electrochemical Society
    Publication Date: 2020
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  • 9
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    Study of the Zn Insertion into Nanostructured d-MnO2 in Non-Aqueous Metal Batteries Using in-Situ X-Ray Absorption Spectroscopy
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-02, No. 5 ( 2017-09-01), p. 506-506
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2017-02, No. 5 ( 2017-09-01), p. 506-506
    Abstract: Nonaqueous multivalent battery chemistries provide high theoretical volumetric capacity, limited dendrite formation, and wide electrochemical windows that are a promising alternative to traditional lithium-based energy storage materials. However, transport limitations and volume change have often restricted cathodes to nanophase materials. To better understand these structural changes, we have studied Zn intercalation in δ-MnO 2 cathodes using X-ray absorption spectroscopy during charge and discharge. When paired with a zinc metal anode and a AN-Zn(TFSI) 2 electrolyte, the MnO 2 cathode provides excellent reversibility (~100% Coulombic efficiency) and stability for 50+ cycles with ~100 mAhg -1 capacity with an operating voltage of 1.2 V vs. Zn/Zn 2+ . In situ x-ray absorption spectroscopy (XAS) provides element-specific characterization of both crystalline and amorphous phases and enables direct correlations between electrochemical performance and structural/redox changes associated with Mn and Zn species while cycling. By looking at the main edge of the Mn K-edge XANES spectra, the δ-MnO 2 samples show clear reversible changes in redox state upon Zn insertion and deinsertion which allows Mn absorption edge shifts systematically from left to the right while cycling. These redox changes can be correlated to the local structure at the Mn site using extended X-ray absorption fine structure (EXAFS). We find a substantial decrease in the first two coordination shells upon discharge and nearly complete recovery upon charge, which we attribute to Jahn-Teller distortions during reduction to Mn 3+ .
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2017-02/5/506
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    Publisher: The Electrochemical Society
    Publication Date: 2017
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  • 10
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    Case Studies on Nonaqueous Zn 2+ Ion Chemistry with a Reversible Intercalation Cathodes for the Development of Multivalent Metal Batteries
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-02, No. 5 ( 2017-09-01), p. 507-507
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2017-02, No. 5 ( 2017-09-01), p. 507-507
    Abstract: Recently, new energy storage chemistries based on nonaqueous electrolytes and multivalent metals (e.g., Mg, Zn, Ca and Al) have drawn the attention of the researchers as a promising advanced energy storage technology due to their higher theoretical volumetric capacity, limited dendrite formation and low cost. 1 A major developmental need for these systems is the identification of electrolytes compatible with both electrodes while showing reversible deposition/dissolution on an anode and multivalent intercalation into a cathode. 1,2 In the case of nonaqueous Mg or Ca ion-based systems, electrolyte compatibility issues (e.g., low Coulombic efficiency, a high overpotential and corrosion) have held back the development of Mg or Ca metal batteries. 3 However, the nonaqueous Zn 2+ ion chemistry utilized in a Zn metal cells with a reversible intercalation cathode is an exception with a number of promising features including highly-efficient reversible Zn deposition/dissolution on a Zn metal anode with a wide electrochemical window, 3 similar ionic radius compared with Li + and Mg 2+ ions, 4 relatively lower activation barrier energy for diffusion in cathode materials (e.g., FePO 4 , CoO 2 and V 2 O 5 ) 5 and high volumetric capacity. 1 Considering these advantages, a nonaqueous Zn system provides an opportunity to delve into the mechanisms in multivalent-ion cell chemistry and solve the present issues in multivalent cell design and prototyping. 3 In this study, the intercalation chemistry on a variety of cathodes materials (e.g., V 2 O 5 , Mn 2 O 4 and FePO 4 ) have been investigated in various nonaqueous Zn electrolytes. The electrochemical and transport properties of the electrolytes (e.g., reversible Zn deposition, anodic/cathodic stability, ionic conductivity and diffusion coefficient) were characterized utilizing the experimental and computational analysis. 3 Among various Zn metal cells, a Zn/nanostructured bilayered V 2 O 5 cell with a selected acetonitrile(AN)-Zn(TFSI) 2 electrolyte demonstrates good reversibility and stability for 120+ cycles with nearly 100% Coulombic efficiency and ~170 mAhg -1 of gravimetric capacity, albeit operating at a cell voltage of 0.7 V vs. Zn/Zn 2+ . 6 A Zn/nanostructured layered δ -MnO 2 cell with an AN-Zn(TFSI) 2 electrolyte also shows good reversibility (~100% Coulombic efficiency) and stability for 50+ cycles with ~100 mAhg -1 capacity with an operating voltage of 1.2 V vs. Zn/Zn 2+ . 7 By utilizing a combination of analytical tools, we address numerous factors affecting capacity fade, and issues associated with the second phase formation including Mn dissolution in Zn/ δ -MnO 2 cells that have been extensively cycled. 7 References 1. J. Muldoon, C. B. Bucur and T. Gregory, Chem. Rev. 2014, 114 , 11683-11720. 2. H. D. Yoo, I. Shterenberg, Y. Gofer, G. Gershinsky, N. Pour and D. Aurbach, Energy Environ. Sci. 2013, 6 , 2265-2279. 3. S.-D. Han, N. N. Rajput, X. Qu, B. Pan, M. He, M. S. Ferrandon, C. Liao, K. A. Persson and A. K. Burrell, ACS Appl. Mater. Inter. 2016, 8 , 3021-3031. 4. R. D. Shannon, Acta Cryst. 1976, A32 , 751-767. 5. Z. Rong, R. Malik, P. Canepa, G. Gautam, M. Liu, A. Jain, K. Persson and G. Ceder, Chem. Mater. 2015, 27 , 6016-6021. 6. P. Senguttuvan, S.-D. Han, S. Kim, A. L. Lipson, S. Tepavcevic, T. T. Fister, I. D. Bloom, A. K. Burrell and C. S. Johnson, Adv. Energy Mater. 2016, 6 , 1600826. 7. S.-D. Han, S. Kim, D. Li, V. Petkov, H. D. Yoo, P. J. Phillips, H. Wang, J. J. Kim, K. L. More, B. Key, R. F. Klie, J. Cabana, V. Stamenkovic, T. T. Fister, N. M. Markovic, A. K. Burrell, S. Tepavcevic, J. T. Vaughey, 2017, in revision.
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    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2017-02/5/507
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    Publisher: The Electrochemical Society
    Publication Date: 2017
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