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  • The Electrochemical Society  (429)
  • 2015-2019  (429)
  • 1
    Online Resource
    Online Resource
    The Electrochemical Society ; 2019
    In:  ECS Meeting Abstracts Vol. MA2019-01, No. 27 ( 2019-05-01), p. 1322-1322
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2019-01, No. 27 ( 2019-05-01), p. 1322-1322
    Abstract: Nature Communications is an open access, multidisciplinary journal that is dedicated to publishing high-quality research from all areas of the natural sciences, including solid-state electronics and photonics. This presentation will include an overview of publishing in Nature Communications as well as other Nature journals. Recent publications on self-powered devices, triboelectric nanogenerators, energy harvesting, wearable devices, etc. will be highlighted.
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    ISSN: 2151-2043
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    Publisher: The Electrochemical Society
    Publication Date: 2019
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  • 2
    Online Resource
    Online Resource
    The Electrochemical Society ; 2018
    In:  ECS Meeting Abstracts Vol. MA2018-02, No. 5 ( 2018-07-23), p. 370-370
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2018-02, No. 5 ( 2018-07-23), p. 370-370
    Abstract: Interest in the rechargeable Li-O 2 battery is driven by its high theoretical specific energy (3500 Whkg -1 ). 1-2 However, a number of challenges face the realization of practical devices. 3-10 Overcoming these challenges requires an understanding of the reactions and processes in the cell, especially at the electrodes. Our focus has been on the reaction at the positive electrode: O 2 + 2e - + 2Li + = Li 2 O 2 This simple reaction belies the complexity of the problems during charge and discharge. Li 2 O 2 , is an insulating solid, if it grows on the electrode surface it can only do so to a thickness of approx. 6 to 7 nm. The resulting passivation leads to low rates and low capacities. 11 If Li 2 O 2 grows from solution, passivation is avoided, leading to high rates and capacities. 12 The solvent donor number is an important factor in controlling which pathway, surface film or solution growth, occurs. Low donor number ethers promote surface films while high donor numbers result in solution growth. Unfortunately, high donor number solvents are more susceptible to decomposition by the reactive O 2 - nucleophile (the intermediate in the O 2 /Li 2 O 2 reaction is LiO 2 ). 13 We show that using redox mediator molecules to shuttle electrons between the electrode surface and solution, Li 2 O 2 can be formed and decomposed in solution even in low donor number solvent like ethers. 14 As a result, rates and capacities of several mA and mAh cm -2 respectively are observed. The impact of the mediators on solvent and electrode stability will be discussed in the context of the mechanism of Li 2 O 2 formation and decomposition. Ultimately, the Li-O 2 cell must operate in air. The effect of H 2 O in the gas stream and hence in the electrolyte solution on the mechanism of O 2 /Li 2 O 2 and the effect on cell performance are important. The influence of H 2 O on the O 2 reduction mechanism will be considered. REFERENCES [1] D. Aurbach; B.D. McCloskey; L.F. Nazar; P.G. Bruce, Nature Energy 2016, 1 , 16128. [2] J.W. Choi; D. Aurbach, Nature Reviews Materials 2016, 1 , 16013. [3] N. Mahne; B. Schafzahl; C. Leypold; M. Leypold , et al. , Nature Energy 2017, 2 , 17036. [4] K.U. Schwenke; M. Metzger; T. Restle; M. Piana , et al. , Journal of The Electrochemical Society 2015, 162 (4), A573-A584. [5] D. Grübl; B. Bergner; D. Schröder; J. Janek , et al. , The Journal of Physical Chemistry C 2016, 120 (43), 24623-24636. [6] H.-D. Lim; B. Lee; Y. Zheng; J. Hong , et al. , Nature Energy 2016, 1 (6), 16066. [7] B.D. McCloskey; D. Addison, ACS Catalysis 2017, 7 (1), 772-778. [8] S. Ganapathy; J.R. Heringa; M.S. Anastasaki; B.D. Adams , et al. , The Journal of Physical Chemistry Letters 2016 . [9] A.I. Belova; D.G. Kwabi; L.V. Yashina; Y. Shao-Horn , et al. , The Journal of Physical Chemistry C 2017, 121 (3), 1569-1577. [10] D. Krishnamurthy; H.A. Hansen; V. Viswanathan, ACS Energy Letters 2016, 1 (1), 162-168. [11] V. Viswanathan; K.S. Thygesen; J.S. Hummelshoj; J.K. Norskov , et al. , Journal of Chemical Physics 2011, 135 (21), 214704. [12] L. Johnson; C. Li; Z. Liu; Y. Chen , et al. , Nature Chemistry 2014, 6 (12), 1091-1099. [13] A. Khetan; A. Luntz; V. Viswanathan, The Journal of Physical Chemistry Letters 2015, 6 (7), 1254-1259. [14] X. Gao; Y. Chen; L.R. Johnson; Z.P. Jovanov , et al. , Nature Energy 2017, 2 , 17118.
    Type of Medium: Online Resource
    ISSN: 2151-2043
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    Publisher: The Electrochemical Society
    Publication Date: 2018
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  • 3
    Online Resource
    Online Resource
    The Electrochemical Society ; 2015
    In:  ECS Meeting Abstracts Vol. MA2015-02, No. 3 ( 2015-07-07), p. 257-257
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2015-02, No. 3 ( 2015-07-07), p. 257-257
    Abstract: Li-ion and related battery technologies will be important for years to come. However, society needs energy storage that exceeds the capacity of Li-ion batteries. We must explore alternatives to Li-ion if we are to have any hope of meeting the long-term needs for energy storage. One such alternative is the Li-air (O 2 ) battery; its theoretical specific energy exceeds that of Li-ion, but many hurdles face its realization. 1-5 One spin-off of the recent interest in rechargeable Li-O 2 batteries, based on aprotic electrolytes is that it has highlighted the importance of understanding the fundamental electrochemistry at the positive electrode within the battery. 6-15 The challenges of obtaining efficient, reversible charge and discharge are well documented in the field.  Here, we describe how our recent studies into the electrochemical mechanism of O 2 reduction to form Li 2 O 2 at the positive electrode might allow us to design new strategies to overcome these limitations. 16 For example, exploiting the effect of solvent donor number, Fig. 1. We will describe our resent results using redox mediators 17 to facilitate the electrochemistry along with the implications of the results for the future of rechargeable Li-O 2 batteries. References (1) Bruce, P. G.; Freunberger, S. A.; Hardwick, L. J.; Tarascon, J.-M. Nature Materials 2012 , 11 , 19. (2) Lu, Y. C.; Gallant, B. M.; Kwabi, D. G.; Harding, J. R.; Mitchell, R. R.; Whittingham, M. S.; Shao-Horn, Y. Energy & Environmental Science 2013 , 6 , 750. (3) Black, R.; Adams, B.; Nazar, L. F. Advanced Energy Materials 2012 , 2 , 801. (4) Girishkumar, G.; McCloskey, B.; Luntz, A. C.; Swanson, S.; Wilcke, W. The Journal of Physical Chemistry Letters 2010 , 1 , 2193. (5) Li, F.; Zhang, T.; Zhou, H. Energy & Environmental Science 2013 , 6 , 1125. (6) Adams, B. D.; Radtke, C.; Black, R.; Trudeau, M. L.; Zaghib, K.; Nazar, L. F. Energy & Environmental Science 2013 , 6 , 1772. (7) Horstmann, B.; Gallant, B.; Mitchell, R.; Bessler, W. G.; Shao-Horn, Y.; Bazant, M. Z. The Journal of Physical Chemistry Letters 2013 , 4 , 4217. (8) Hummelshoj, J. S.; Luntz, A. C.; Norskov, J. K. The Journal of Chemical Physics 2013 , 138 , 034703. (9) McCloskey, B. D.; Scheffler, R.; Speidel, A.; Girishkumar, G.; Luntz, A. C. The Journal of Physical Chemistry C 2012 , 116 , 23897. (10) Mitchell, R. R.; Gallant, B. M.; Shao-Horn, Y.; Thompson, C. V. The Journal of Physical Chemistry Letters 2013 , 4 , 1060. (11) Trahan, M. J.; Mukerjee, S.; Plichta, E. J.; Hendrickson, M. A.; Abraham, K. M. Journal of The Electrochemical Society 2013 , 160 , A259. (12) Sharon, D.; Etacheri, V.; Garsuch, A.; Afri, M.; Frimer, A. A.; Aurbach, D. The Journal of Physical Chemistry Letters 2012 , 4 , 127. (13) Jung, H. G.; Kim, H. S.; Park, J. B.; Oh, I. H.; Hassoun, J.; Yoon, C. S.; Scrosati, B.; Sun, Y. K. Nano Letters 2012 , 12 , 4333. (14) Peng, Z.; Freunberger, S. A.; Hardwick, L. J.; Chen, Y.; Giordani, V.; Barde, F.; Novak, P.; Graham, D.; Tarascon, J. M.; Bruce, P. G. Angewandte Chemie International Edition 2011 , 50 , 6351. (15) Zhai, D.; Wang, H. H.; Yang, J.; Lau, K. C.; Li, K.; Amine, K.; Curtiss, L. A. Journal of the American Chemical Society 2013 , 135 , 15364. (16) Johnson, L.; Li, C. ; Liu, Z.; Chen, Y.; Freunberger, S. A.; Ashok, P.; Praveen, B.; Dholakia, K.; Tarascon, J-M.; Bruce, P. G. Nature Chemistry 2014 , 6 , 1091. (17) Chen, Y.; Freunberger, S. A.; Peng, Z.; Fontaine, O.; Bruce, P. G. Nature Chemistry 2013 , 5 , 489. Figure 1
    Type of Medium: Online Resource
    ISSN: 2151-2043
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    Publisher: The Electrochemical Society
    Publication Date: 2015
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  • 4
    Online Resource
    Online Resource
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-02, No. 5 ( 2017-09-01), p. 454-454
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2017-02, No. 5 ( 2017-09-01), p. 454-454
    Abstract: Li-ion and related battery technologies will be important for years to come. However, we must explore alternatives if we are to have any hope of meeting the long-term needs for energy storage. One such alternative is the metal-O 2 battery; the theoretical specific energy of typical aprotic metal-O 2 batteries exceeds that of Li-ion, but many obstacles hinder realization of this technology.[1-4] Overcoming these hurdles will require an understanding of the fundamental electrochemistry at the positive electrode within aprotic metal-air batteries.[5-12] Recently interest in the Na-O 2 battery has grown due to the relatively low polarization during cycling and the high rates.[13, 14] This is despite the lower specific energy of this battery chemistry.[15] A number of groups have shown promising results with this system.[16-18] An important area of contention is the nature of the discharge product, which, unlike the lithium system that forms Li 2 O 2 , may form the superoxide, peroxide or oxide. The discharge product in the metal-O 2  battery directly influences the specific capacity and ease of charge. Therefore, it is important to understand the mechanism such that this can be controlled. We have combined a range of electrochemical, spectroscopic and microscopy methods to investigate the mechanism of electrochemical O 2 reduction. The results of these studies will be presented, along with the implications for the future of rechargeable metal-O 2  batteries. References: 1. Bruce, P.G., et al., Li-O 2 and Li-S batteries with high energy storage. Nature Materials, 2012. 11 (1): p. 19-29. 2. Lu, Y.C., et al., Lithium-oxygen batteries: bridging mechanistic understanding and battery performance. Energy & Environmental Science, 2013. 6 (3): p. 750-768. 3. Girishkumar, G., et al., Lithium−air battery: promise and challenges. The Journal of Physical Chemistry Letters, 2010. 1 (14): p. 2193-2203. 4. Li, F., T. Zhang, and H. Zhou, Challenges of non-aqueous Li-O 2 batteries: electrolytes, catalysts, and anodes. Energy & Environmental Science, 2013. 6 (4): p. 1125-1141. 5. Adams, B.D., et al., Current density dependence of peroxide formation in the Li-O 2 battery and its effect on charge. Energy & Environmental Science, 2013. 6 (6): p. 1772-1778. 6. Horstmann, B., et al., Rate-Dependent Morphology of Li2O2 Growth in Li–O2 Batteries. The Journal of Physical Chemistry Letters, 2013. 4 (24): p. 4217-4222. 7. Hummelshoj, J.S., A.C. Luntz, and J.K. Norskov, Theoretical evidence for low kinetic overpotentials in Li-O2 electrochemistry. The Journal of Chemical Physics, 2013. 138 (3): p. 034703-12. 8. McCloskey, B.D., et al., On the mechanism of nonaqueous Li–O 2 electrochemistry on C and its kinetic overpotentials: Some implications for Li–air batteries. The Journal of Physical Chemistry C, 2012. 116 (45): p. 23897-23905. 9. Mitchell, R.R., et al., Mechanisms of Morphological Evolution of Li2O2 Particles During Electrochemical Growth. The Journal of Physical Chemistry Letters, 2013. 4 (7): p. 1060–1064. 10. Trahan, M.J., et al., Studies of Li-Air Cells Utilizing Dimethyl Sulfoxide-Based Electrolyte. Journal of The Electrochemical Society, 2013. 160 (2): p. A259-A267. 11. Jung, H.G., et al., A transmission electron microscopy study of the electrochemical process of lithium-oxygen cells. Nano Letters, 2012. 12 (8): p. 4333-5. 12. Zhai, D., et al., Disproportionation in li-o2 batteries based on a large surface area carbon cathode. Journal of the American Chemical Society, 2013. 135 (41): p. 15364-72. 13. Hartmann, P., et al., A rechargeable room-temperature sodium superoxide (NaO2) battery. Nature Materials, 2013. 12 (3): p. 228-232. 14. McCloskey, B.D., J.M. Garcia, and A.C. Luntz, Chemical and Electrochemical Differences in Nonaqueous Li-O-2 and Na-O-2 Batteries. Journal of Physical Chemistry Letters, 2014. 5 (7): p. 1230-1235. 15. Das, S.K., S. Lau, and L.A. Archer, Sodium-oxygen batteries: a new class of metal-air batteries. Journal of Materials Chemistry A, 2014. 2 (32): p. 12623-12629. 16. Hartmann, P., et al., Discharge and Charge Reaction Paths in Sodium–Oxygen Batteries: Does NaO2Form by Direct Electrochemical Growth or by Precipitation from Solution? The Journal of Physical Chemistry C, 2015. 119 (40): p. 22778-22786. 17. Xia, C., et al., The critical role of phase-transfer catalysis in aprotic sodium oxygen batteries. Nat Chem, 2015. 7 (6): p. 496-501. 18. Lutz, L., et al., High Capacity Na–O2 Batteries: Key Parameters for Solution-Mediated Discharge. The Journal of Physical Chemistry C, 2016. 120 (36): p. 20068-20076. Figure 1
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    ISSN: 2151-2043
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    Publisher: The Electrochemical Society
    Publication Date: 2017
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  • 5
    Online Resource
    Online Resource
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-02, No. 32 ( 2017-09-01), p. 1391-1391
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2017-02, No. 32 ( 2017-09-01), p. 1391-1391
    Abstract: Catalyst layers (CLs) in polymer-electrolyte fuel cells have garnered the attention of researchers due to their association with high local mass-transport resistance at low catalyst loadings [1, 2]. Nevertheless, the genesis and nature of CL resistance(s) is still under debate. CLs are only a few micrometers thick with complex geometry and heterogeneous phases making in-situ examination of CL transport processes extreme ly difficult. In this study, we probe the nature of CL resistances experimentally and theoretically. Using a hydrogen-pump limiting-current modality, we deconvolute the various gas-transport-related resistances without the impact of those associated with the oxygen-reduction reaction (e.g., water production) [3]. An analytical model to quantify the experimental measurements is developed to analyze the data and to elucidate limiting regimes. Our new results are in agreement with literature limiting-current measurements. Similar to previously reported studies [4], the model demonstrates that the transport of the reactant to the surface through the ionomer film tends to be the dominant resistance in CLs with a linear dependence on the inverse of Pt loading (i.e., roughness factor) [5] . Further, we study the dependence of this resistance on operational parameters including pressure, R H , temperature, gas molecular mass, and ionomer type. The garnered information exposes the controlling resistances, especially in comparison to ex-situ ionomer thin-film properties. Our efforts can be utilized to understand and develop mitigation strategies for local CL resistances. Acknowledgements We would like to thank helpful discussions and data provided by KC Neyerlin at NREL. This work was funded under the Fuel Cell Performance and Durability Consortium (FC PAD) funded by the Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, of the U. S. Department of Energy under contract number DE-AC02-05CH11231. References: A. Weber and A. Kusoglu, Journal of Material Chemistry A, 2,17207–17211 (2014). A. Kongkanand and M. F. Mathias, The Journal of Physical Chemistry Letters, 7, 1127 (2016). F. Spingler, A. Phillips, T. Schuler, M. Tucker and A. Weber, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.01.036 N. Nonoyama, S. Okazaki, A. Weber, Y. Ikogi and T. Yoshida, Journal of The Electrochemical Society, 158 (5), B416 (2011). T. Greszler, D. Caulk and P. Sinha, Journal of The Electrochemical Society, 159, F831 (2012).
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    ISSN: 2151-2043
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    Publisher: The Electrochemical Society
    Publication Date: 2017
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  • 6
    Online Resource
    Online Resource
    The Electrochemical Society ; 2016
    In:  ECS Meeting Abstracts Vol. MA2016-03, No. 2 ( 2016-06-10), p. 378-378
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2016-03, No. 2 ( 2016-06-10), p. 378-378
    Abstract: Li-ion and related battery technologies will be important for years to come. However, society needs energy storage that exceeds the capacity of Li-ion batteries. We must explore alternatives to Li-ion if we are to have any hope of meeting the long-term needs for energy storage. One such alternative is the Li-air (O 2 ) battery; its theoretical specific energy exceeds that of Li-ion, but many hurdles face its realization. [1-5] One spin-off of the recent interest in rechargeable Li-O 2 batteries, based on aprotic electrolytes is that it has highlighted the importance of understanding the fundamental electrochemistry at the positive electrode within the battery. [6-15] The challenges of obtaining efficient, reversible charge and discharge are well-documented in the field.  Here, we describe how our recent studies into the electrochemical mechanism of O 2 reduction to form Li 2 O 2 at the positive electrode might allow us to design new strategies to overcome these limitations; [16] For example, exploiting the effect of solvent donor number, Fig. 1. We will describe our resent results using redox mediators to facilitate the electrochemistry along with the implications of the results for the future of rechargeable Li-O 2  batteries. REFERENCES   [1]. Bruce, P. G.; Freunberger, S. A.; Hardwick, L. J.; Tarascon, J.-M. Nature Materials 2012 , 11 , 19. [2]. Lu, Y. C.; Gallant, B. M.; Kwabi, D. G.; Harding, J. R.; Mitchell, R. R.; Whittingham, M. S.; Shao-Horn, Y. Energy & Environmental Science 2013 , 6 , 750. [3]. Black, R.; Adams, B.; Nazar, L. F. Advanced Energy Materials 2012 , 2 , 801. [4]. Girishkumar, G.; McCloskey, B.; Luntz, A. C.; Swanson, S.; Wilcke, W. The Journal of Physical Chemistry Letters 2010 , 1 , 2193. [5]. Li, F.; Zhang, T.; Zhou, H. Energy & Environmental Science 2013 , 6 , 1125. [6]. Adams, B. D.; Radtke, C.; Black, R.; Trudeau, M. L.; Zaghib, K.; Nazar, L. F. Energy & Environmental Science 2013 , 6 , 1772. [7]. Horstmann, B.; Gallant, B.; Mitchell, R.; Bessler, W. G.; Shao-Horn, Y.; Bazant, M. Z. The Journal of Physical Chemistry Letters 2013 , 4 , 4217. [8]. Hummelshoj, J. S.; Luntz, A. C.; Norskov, J. K. The Journal of Chemical Physics 2013 , 138 , 034703. [9]. McCloskey, B. D.; Scheffler, R.; Speidel, A.; Girishkumar, G.; Luntz, A. C. The Journal of Physical Chemistry C 2012 , 116 , 23897. [10]. Mitchell, R. R.; Gallant, B. M.; Shao-Horn, Y.; Thompson, C. V. The Journal of Physical Chemistry Letters 2013 , 4 , 1060. [11]. Trahan, M. J.; Mukerjee, S.; Plichta, E. J.; Hendrickson, M. A.; Abraham, K. M. Journal of The Electrochemical Society 2013 , 160 , A259. [12]. Sharon, D.; Etacheri, V.; Garsuch, A.; Afri, M.; Frimer, A. A.; Aurbach, D. The Journal of Physical Chemistry Letters 2012 , 4 , 127. [13]. Jung, H. G.; Kim, H. S.; Park, J. B.; Oh, I. H.; Hassoun, J.; Yoon, C. S.; Scrosati, B.; Sun, Y. K. Nano Letters 2012 , 12 , 4333. [14]. Peng, Z.; Freunberger, S. A.; Hardwick, L. J.; Chen, Y.; Giordani, V.; Barde, F.; Novak, P.; Graham, D.; Tarascon, J. M.; Bruce, P. G. Angewandte Chemie International Edition 2011 , 50 , 6351. [15]. Zhai, D.; Wang, H. H.; Yang, J.; Lau, K. C.; Li, K.; Amine, K.; Curtiss, L. A. Journal of the American Chemical Society 2013 , 135 , 15364. [16]. Johnson, L.; Li, C. ; Liu, Z.; Chen, Y.; Freunberger, S. A.; Ashok, P.; Praveen, B.; Dholakia, K.; Tarascon, J-M.; Bruce, P. G. Nature Chemistry 2014 , 6 , 1091. Figure 1
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    ISSN: 2151-2043
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    Publisher: The Electrochemical Society
    Publication Date: 2016
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  • 7
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2016-01, No. 2 ( 2016-04-01), p. 302-302
    Abstract: Solid-state electrolytes (SSE’s) are crucial in realizing the potential of novel rechargeable batteries. All-solid-state batteries with inorganic solid electrolytes offer a number of advantages by improving safety, reliability, and cost [1]. Sulfide glasses are promising as a solid electrolyte due to their superionic ionic conductivity [3] . Na 3 PS 4 is a glass-ceramic that is precipitated from the sulfide glass matrix, exhibiting ionic conductivities of 10 -6 and 10 -4 S/cm for the tetragonal and cubic phases, respectively [4]. Here we provide a simple synthesis process for stabilizing the cubic phase, which also reduces the activation energy to 330 meV. We also investigate anion doping, which can further improve upon this result by increasing Na vacancies, via a composition curve of Cl-doping to determine optimal concentration of (1-x)Na 3 PS 4 -xNaCl, for 0 〉 x 〉 0.0625. Acknowledgements This work was supported by National Science Foundation under grant number ACI-1053575. References [1]      Kamaya, Noriaki et al. “A Lithium Superionic Conductor.” Nature Materials 10.9 (2011): 682–686. Web. [2]      Hayashi, Akitoshi et al. “Superionic Glass-Ceramic Electrolytes for Room-Temperature Rechargeable Sodium Batteries.” Nature Communications 3.May (2012): 856. Web.Tatsumisago, Masahiro, and Akitoshi Hayashi. “Sulfide Glass-Ceramic Electrolytes for All-Solid-State Lithium and Sodium Batteries.” International Journal of Applied Glass Science 10 (2014): 226–235. Web. [3]      Ribes, M., B. Barrau, and J.L Souquet. “Sulfide Glasses: Glass Forming Region, Structure and Ionic Conduction of Glasses in Na2S-XS2 (X=Si, Ge), Na2S-P2S5, and Li2SGeS2 Systems.” Journal of Non-Crystalline Solids 39 (1980): 271–276. Print. [4]      Hayashi, Akitoshi et al. “Superionic Glass-Ceramic Electrolytes for Room-Temperature Rechargeable Sodium Batteries.” Nature Communications 3.May (2012): 856. Web. Figure 1
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  • 8
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    Online Resource
    The Electrochemical Society ; 2019
    In:  ECS Meeting Abstracts Vol. MA2019-02, No. 5 ( 2019-09-01), p. 255-255
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2019-02, No. 5 ( 2019-09-01), p. 255-255
    Abstract: Due to the nature of how porous battery electrodes are fabricated, their microstructure is not uniform. For instance, there are variations in composition, effective electronic transport, and effective ionic transport. Such heterogeneity has been associated with several battery application issues. For example, variability in transport of ions can lead to a tendency for localized plating of lithium on anodes during fast charging [1-2]. Studying the heterogeneity of electrodes is a growing research topic. Our research group has previously developed a micro-four-line probe that successfully measured the variation of electronic conductivity of electrodes [3]. Another method to study the microstructure of electrodes is by means of SEM and X-ray tomography, and the variation of tortuosity (effective ionic resistance) in electrodes was computed by analyzing the tomographic data of microstructure [4] . We report here on a new technique to measure the local ionic resistance on a sub-mm length scale. A probe was made to detect the local transport of ions through a small aperture. The probe is scanned across the surface of a porous thin-film electrode in order to create maps of tortuosity or MacMullin number. The measurement was performed using electrochemical impedance spectroscopy, and an associated model is needed to invert the experimental results. [1] Harris et al., The Journal of Physical Chemistry C 117, 6481 (2013). [2] Vogel et al., Electrochimica Acta 297, 820 (2019). [3] Lanterman et al., Journal of the Electrochemical Society 162, A2145 (2015). [4] Kehrwald et al. Journal of The Electrochemical Society 158, A1393 (2011). Figure 1
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  • 9
    Online Resource
    Online Resource
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-02, No. 45 ( 2017-09-01), p. 2008-2008
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2017-02, No. 45 ( 2017-09-01), p. 2008-2008
    Abstract: The electrochemical reduction of CO 2 has the potential to store energy from intermittent renewable sources and to produce carbon-neutral fuels and chemicals[1]. In recent years, theoretical studies of CO 2 reduction have usually applied the computational hydrogen electrode model, which allows for the determination of the energies of reaction intermediates without explicitly treating the potential and the ions in solution[2]. This thermochemical approach has been shown to correlate well with experimental onset potentials [3, 4] and applied to computational screening of new catalysts [5, 6]. However, an understanding of charge transfer barriers, kinetics, selectivity, and pH effects all require explicit consideration of solvent and charge. In this talk, I will discuss new developments in the explicit treatment of the electrochemical interface, which is based on a simple capacitor model that uses the interfacial charge to obtain barriers at constant potential [7, 8] . I will then discuss the application of such a scheme to CO 2 reduction: the determination of reaction pathways on transition metals field and solvation effects[9, 10], the resultant kinetics, and the implications for catalyst design. 1. Whipple, D.T. and P.J.A. Kenis, Prospects of CO2 Utilization via Direct Heterogeneous Electrochemical Reduction. The Journal of Physical Chemistry Letters, 2010. 1 (24): p. 3451-3458. 2. Nørskov, J.K., et al., Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode. J. Phys. Chem. B, 2004. 108 (46): p. 17886--17892. 3. Shi, C., et al., Chan, K., Yoo, J., Nørskov, J.K.  Trends in electrochemical CO2 reduction activity for open and close-packed metal surfaces. Physical Chemistry Chemical Physics, 2014. 16 (10): p. 4720-4727. 4. Kuhl, K.P., et al., Electrocatalytic Conversion of Carbon Dioxide to Methane and Methanol on Transition Metal Surfaces. Journal of the American Chemical Society, 2014. 5. Chan, K., et al., Molybdenum Sulfides and Selenides as Possible Electrocatalysts for CO2 Reduction. ChemCatChem, 2014. 6 (7): p. 1899-1905. 6. Asadi, M., et al., Robust carbon dioxide reduction on molybdenum disulphide edges. Nature communications, 2014. 5 . 7. Chan, K. and J.K. Nørskov, Electrochemical Barriers Made Simple. J. Phys. Chem. Lett., 2015: p. 2663--2668. 8. Chan, K. and J.K. Nørskov, Potential Dependence of Electrochemical Barriers from ab Initio Calculations. The Journal of Physical Chemistry Letters, 2016: p. 1686-1690. 9. Montoya, J.H., et al., Theoretical Insights into a CO Dimerization Mechanism in CO2 Electroreduction. The journal of physical chemistry letters, 2015. 6 (11): p. 2032--2037. 10. Chen, L.D., Urushihara, M., Chan, K., Nørskov, J.K.  Electric Field Effects in Electrochemical CO2 Reduction. ACS Catalysis, 2016. 11. Liu, X., Xiao, J., Peng, H., Hong, X., Chan, K., Nørskov, J.K.  Understanding trends in CO2 reduction on transition metals.  Nature Communications, 2017.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2017
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    Online Resource
    The Electrochemical Society ; 2016
    In:  ECS Meeting Abstracts Vol. MA2016-01, No. 1 ( 2016-04-01), p. 127-127
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2016-01, No. 1 ( 2016-04-01), p. 127-127
    Abstract: Electrolytes used in lithium-ion batteries that power personal electronic devices and electric vehicles comprise lithium salts dissolved in flammable organic liquids. Catastrophic battery failure often begins with the electrolyte decomposition and combustion. Mixtures of liquids and salts have additional limitations. The passage of current results in an accumulation of salt in the vicinity of one electrode and depletion close to the other electrode, because only the cation participates in the electrochemical reactions. These effects are minimized in the case of single-ion-conducting-solid electrolytes due to the absent of concentration polarization and the limited solubility and slow diffusion (1). Therefore, non-flammable single-ion-conducting solid electrolytes have the potential to dramatically improve safety and performance of lithium batteries (2,3). Solid electrolytes such as inorganic sulfide glasses (Li 2 S–P 2 S 5 ) are single-ion-conductors with high shear moduli (18-25 GPa) and high ionic conductivity (over 10 −4 S/cm) at room temperature (4,5). However, these materials, on their own, cannot serve as efficient electrolytes as they cannot adhere to moving boundaries of the active particles in the battery electrode as they are charged and discharged. In this study, we describe hybrid single-ion-conducting electrolytes based on inorganic sulfide glasses and perfluoropolyether polymers for lithium batteries. Herein, it is demonstrated that hybrid electrolytes provide a compelling alternative to the traditional glass, ceramic, or polymer battery electrolytes. These electrolytes present high transference numbers, unprecedented ionic conductivities at room temperature, excellent electrochemical stability, and limit the dissolution of lithium polysulfides. The results in this work represent a significant step toward addressing the challenges of enabling the next generation cathodes such as lithium nickel manganese cobalt oxide and sulfur. _______________________ [1] J.M. Tarascon, M. Armand, Nature , 414 ( 2001 ) 359-367. [2] R. Bouchet, et al., Nature Materials , 12 ( 2013 ) 452-457. [3] N. Kamaya, et al., Nature Materials , 10 ( 2011 ) 682-686. [4] Z. Liu, et al., Journal of the American Chemical Society , 135 ( 2013 ) 975-978. [5] A. Sakuda, A. Hayashi, Y. Takigawa, K. Higashi, M. Tatsumisago, Journal of the Ceramic Society of Japan , 121 ( 2013 ) 946-949.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2016
    detail.hit.zdb_id: 2438749-6
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