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  • 11
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    Evaluating the Thermodynamics of Electrochemical Ammonia Oxidation for Hydrogen Production
    The Electrochemical Society ; 2014
    In:  ECS Meeting Abstracts Vol. MA2014-01, No. 14 ( 2014-04-01), p. 655-655
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2014-01, No. 14 ( 2014-04-01), p. 655-655
    Abstract: Objective Electrolysis of ammonia on platinum electrodes is a viable technology for wastewater remediation and hydrogen production[1]. Ammonia is oxidized at the anode, in the presence of hydroxide ions, and water is reduced at the cathode. The only products generated are nitrogen and hydrogen. While the anodic reaction is limited by slow kinetics and catalyst deactivation[2], improvements have been made using bimetallic catalysts[3,4] , especially at low concentrations of ammonia. This improved activity by empirical observation indicated a need for more fundamental analysis through a surface chemistry approach to the electrochemical reaction. This analysis will aid in designing improved catalysts and catalytic compositions. The use of density functional theory for characterizing chemical reactions, especially at the catalyst surface, has yielded valuable insight into the thermodynamics and kinetics of the reactions[5] and this method will be applied for this study. Methodology Density Functional Theory as applied in Gaussian 09[6] was used to generate the electronic and thermodynamic properties of the reactants, products and intermediates of ammonia electro-oxidation. Unrestricted spin calculations (due to unpaired electrons) were performed using the hybrid B3LYP functional[7] while the basis sets used were LANL2DZ[8-11] for platinum atoms and 6-311++G** for nitrogen, oxygen, and hydrogen atoms[12,13] . Using the computational hydrogen electrode[14], the effect of an applied potential was evaluated. Results The aforementioned species present during ammonia electro-oxidation are of the form: NH x (x = 0 – 3), OH y (y = 1 & 2) and N 2 H z (z = 0 – 4) when ammonia electrolysis occurs on platinum below the potential for oxide formation. The adsorption of these species has been previously investigated and characterized using the method above[15,16]. The following trend for adsorption was predicted: N 2 〈 H 2 O 〈 NH 3 〈 N 2 H 2 〈 N 2 H 4 〈 N 2 H 〈 N 2 H 3 〈 OH 〈 NH 2 〈 NH 〈 N . However, these calculations have not accounted for the effect of an applied potential, pH or the solvent environment. Using the method of Norskov et al. ,[14] the effect of these pertubations, which are essential to electrochemical reactions, have been investigated. These results will be presented at the meeting. References [1] F. Vitse, M. Cooper, and G. G. Botte, Journal of Power Sources 142, 18 (2005). [2] H. Gerischer and A. Mauerer, Journal of Electroanalytical Chemistry 25, 421 (1970). [3] E. P. Bonnin, E. J. Biddinger, and G. G. Botte, Journal of Power Sources 182(2008). [4] B. K. Boggs and G. G. Botte, Electrochimica Acta 55(2010). [5] J. Norskov, T. Bligaard, J. Rossmeisl, and C. Christensen, Nature Chemistry 1, 37 (2009). [6] M. J. Frisch et al., Gaussian 09, Revision B.01, Gaussian, Inc., 2009. [7] A. D. Becke, Journal of Chemical Physics 98, 5648 (1993). [8] T. H. Dunning, Journal of Chemical Physics 90, 1007 (1989). [9] P. J. Hay and W. R. Wadt, Journal of Chemical Physics 82, 299 (1985). [10] P. J. Hay and W. R. Wadt, Journal of Chemical Physics 82, 270 (1985). [11] W. R. Wadt and P. J. Hay, Journal of Chemical Physics 82, 284 (1985). [12] G. S. Chandler and A. D. McLean, Journal of Chemical Physics 71, 2175 (1979). [13] A. D. McLean and G. S. Chandler, Journal of Chemical Physics 72, 5639 (1980). [14] J. Norskov, J. Rossmeisl, A. Logadottir, L. Lindqvist, J. Kitchin, T. Bligaard, and H. Jonsson, Journal of Physical Chemistry B 108, 17886 (2004). [15] D. A. Daramola and G. G. Botte, Computational and Theoretical Chemistry 989, 7 (2012). [16] D. A. Daramola and G. G. Botte, Journal of Colloid and Interface Science 402, 204 (2013).
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2014-01/14/655
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    Publisher: The Electrochemical Society
    Publication Date: 2014
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  • 12
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    Instrument for Measuring Local Ionic Conductivity of Porous Electrodes
    The Electrochemical Society ; 2019
    In:  ECS Meeting Abstracts Vol. MA2019-02, No. 5 ( 2019-09-01), p. 255-255
    Details
    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
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2019-02/5/255
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    Publisher: The Electrochemical Society
    Publication Date: 2019
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  • 13
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    Theoretical Investigations of Electrochemical CO 2 Reduction
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-02, No. 45 ( 2017-09-01), p. 2008-2008
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    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
    URL: Article
    DOI: 10.1149/MA2017-02/45/2008
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    Publisher: The Electrochemical Society
    Publication Date: 2017
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  • 14
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    Single-Ion-Conducting Glass-Polymer Hybrid Electrolytes for Lithium Batteries
    The Electrochemical Society ; 2016
    In:  ECS Meeting Abstracts Vol. MA2016-01, No. 1 ( 2016-04-01), p. 127-127
    Details
    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
    URL: Article
    DOI: 10.1149/MA2016-01/1/127
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    Publisher: The Electrochemical Society
    Publication Date: 2016
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  • 15
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    Effects of Non-Uniform Temperature Distribution on Degradation of Lithium-Ion Cells
    The Electrochemical Society ; 2018
    In:  ECS Meeting Abstracts Vol. MA2018-01, No. 3 ( 2018-04-13), p. 364-364
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2018-01, No. 3 ( 2018-04-13), p. 364-364
    Abstract: Lithium-ion cells degrade much faster at temperatures higher than 25 °C mainly due to accelerated solid-electrolyte interface (SEI) growth in anode and degeneration of cathode [1, 2]. It is also known that temperature distributions in lithium-ion cells are not uniform [3] due to very low thermal conductivity of battery materials. The non-uniform temperature distributions could cause non-uniform degradation, thus exacerbating the thermal degradation problem, especially for large-format lithium-ion cells during high power operation. The effects of non-uniform temperature distributions on degradation of lithium-ion cells will be investigated and progress will be presented. References [1] C.Y. Wang, G. Zhang, S. Ge, T. Xu, Y. Ji, X.G. Yang, Y. Leng. Lithium-ion battery structure that self-heats at low temperatures, Nature , 529(7587) (2016) 515-518. [2] T. Waldmann, M. Wilka, M. Kasper, M. Fleischhammer, M. Wohlfahrt-Mehrens. Temperature dependent ageing mechanisms in lithium-ion batteries – A post-mortem study, Journal of Power Sources, 262 (2014) 129-135. [3] G. Zhang, L. Cao, S. Ge, C.Y. Wang, C.E. Shaffer, C.D. Rahn. In situ measurement of radial temperature distributions in cylindrical Li-ion cells, Journal of The Electrochemical Society , 161(10) (2014) A1499-A1507.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2018-01/3/364
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    Publisher: The Electrochemical Society
    Publication Date: 2018
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  • 16
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    Electrochemical Growth and OER Catalytic Activityof Ultrathin Epitaxial Cobalt Oxide Films
    The Electrochemical Society ; 2020
    In:  ECS Meeting Abstracts Vol. MA2020-01, No. 19 ( 2020-05-01), p. 1187-1187
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2020-01, No. 19 ( 2020-05-01), p. 1187-1187
    Abstract: Iron-group oxides are among the best earth abundant catalysts for the oxygen evolution reaction (OER) in alkaline and neutral electrolytes [ 1 ],[ 2 ]. Such oxides have been prepared with an amorphous or a crystalline structure, using thermal salt decomposition [ 3 ], autoclave synthesis [ 4 ], photochemical reactions [ 5 ], sol-gel synthesis [ 6 ], metal electrodeposition and subsequent oxidation, [ 7 ] and direct oxide electrodeposition [ 1 ], [ 8 ]. This work focuses on well-defined epitaxial CoOx [ 9 ] electrocatalysts grown by direct electrodeposition on Au(111) according to an approach similar to that introduced by Switzer [ 8 ]. The growth modes of catalysts and the mechanisms of deposition will be discussed based on electrochemical characterizations, XRD characterizations and microscopic observations. In particular to explain that CoOOH may be obtained at a potential of +1V/RHE by oxidation of a Co(II) complex diluted in an alkaline solution while thermodynamics predicts that Co 3 O 4 should be formed. The electrochemical properties in pre-OER and within OER will be discussed as a function of the surface structure and morphology of layers. In particular to show that the large pseudocapacitance measured at the electrode is not related to its ECSA but to electrical charging within the bulk of the electrode. [1] M. W. Kanan and D. G. Nocera, Science 321 , 1072 (2008). [2] C. C. L. McCrory, S. Jung, I. M. Ferrer et al., Journal of the American Chemical Society 137 , 4347 (2015). [3] C. Pirovano and S. Trasatti, Journal of Electroanalytical Chemistry and Interfacial Electrochemistry 180 , 171 (1984). [4] D. Yuming, H. Kun, Y. Lin et al., Nanotechnology 18 , 435602 (2007). [5] S. R. Alvarado, Y. Guo, T. P. A. Ruberu et al., The Journal of Physical Chemistry C 116 , 10382 (2012). [6] A. Bergmann, E. Martinez-Moreno, D. Teschner et al., Nature Communications 6 , 8625 (2015). [7] M. W. Louie and A. T. Bell, Journal of the American Chemical Society 135 , 12329 (2013). [8] J. A. Koza, Z. He, A. S. Miller et al., Chem. Mat. 24 , 3567 (2012). [9] F. Reikowski, F. Maroun, I. Pacheco et al., ACS Catalysis 9 , 3811 (2019).
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2020-01191187mtgabs
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    Publisher: The Electrochemical Society
    Publication Date: 2020
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  • 17
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    Metal-Air Batteries
    The Electrochemical Society ; 2016
    In:  ECS Meeting Abstracts Vol. MA2016-03, No. 1 ( 2016-06-10), p. 18-18
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2016-03, No. 1 ( 2016-06-10), p. 18-18
    Abstract: Li-ion and related battery technologies will be important for years to come. However, society needs energy storage that exceeds that 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 alternative is the Li-air (O 2 ) battery, Fig. 1; 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 oxygen redox processes at the positive electrode within the battery. [6-15] As a result of these fundamental studies it is generally accepted that a solution growth mechanism for Li 2 O 2 will be required to achieve high rates and capacities, avoiding the formation of passivating Li 2 O 2 films on the electrode surface.  Recent results exploring the electrochemical mechanism of O 2 reduction to form Li 2 O 2 at the positive electrode have identified new strategies to achieve this by exploiting the effect of the electrolyte solution. Moving to a solution phase discharge mechanism highlights the requirement for charge mediation between the electroactive species and the electrode, thus using solid Li 2 O 2 simply as a storage material for lithium ions and electrons. The implications of this will be discussed 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.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2016-03/1/18
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    Publisher: The Electrochemical Society
    Publication Date: 2016
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  • 18
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    Incorporation of Conductive Internal Additives within Electrocuring Adhesives
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-01, No. 20 ( 2017-04-15), p. 1083-1083
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    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2017-01, No. 20 ( 2017-04-15), p. 1083-1083
    Abstract: Low-voltage activated adhesives have recently been invented, aka ‘voltaglue’, leading to electrochemically mediated adhesive curing (electrocuring)[1]. Consisting of new and established adhesive crosslinking groups, formulations incorporate dendrimers that have a preference of intermolecular crosslinking while allowing flexible incorporation of functional groups. Upon voltage activation, specific functional groups are activated and covalently bond to a variety of surfaces, but this is highly dependent on bulk conductivity. To tailor the adhesive properties and adhesion strength, internal additives have been explored towards increasing conductivity and ultimately the ‘voltaglue’ crosslinking efficiency. Flexible electrocuring is sought to achieve a range of material properties, from viscous gels to hard set matrices. Ferrocene, a well-known redox active compound with reversible one-electron redox behaviour[2], is often incorporated in polymers/dendrimers due to its reversible nature and conductive aspects [3] . By integrating the ferrocene internal additive into dendrimer formulations combined with the electrically activated crosslinking additives we are able to mediate the electrocuring properties to a limited degree. In this work we present the synthesis of PAMAM-g-ferrocene-g-diazirine, an electrocuring adhesive that is able to adhere to a range of substrates, with adhesive strengths at the kPa scale. Real time electrorheology measurements chemistry evaluate the range of material properties available and demonstrate the synergistic performance ferrocene internal additives impart on the ‘voltaglue’ adhesives.     References   [1] J. Ping, F. Gao, J.L. Chen, R.D. Webster, T.W.J. Steele, Adhesive curing through low-voltage activation, Nature Communications 6 (2015). [2] M.E. N.P.R.A. Silva, A.J.L. Pombeiro, J.J.R. Fraústo da Silva, R. Herrmann, N. Deus, R. E.Bozak, Redox potential and substituent effects in ferrocene derivatives: II, Journal of Organometallic Chemistry 480 (1994). [3] R. Gracia, D. Mecerreyes, Polymers with redox properties: materials for batteries, biosensors and more, Polymer Chemistry 4 (2013). [4] C.M. Elson, M.T.H. Liu, C. Mailer, Electron-spin-resonance studies of diazirine anion radicals, Journal of the Chemical Society, Chemical Communications 7 (1986).
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2017-01/20/1083
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    Publication Date: 2017
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  • 19
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    Elucidating the Pre-Oxygen Evolution Surface Chemistry on Ruthenium Dioxide Surfaces
    The Electrochemical Society ; 2017
    In:  ECS Meeting Abstracts Vol. MA2017-02, No. 47 ( 2017-09-01), p. 2061-2061
    Details
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2017-02, No. 47 ( 2017-09-01), p. 2061-2061
    Abstract: The unique interaction between water and rutile Ruthenium Dioxide (RuO 2 ) affords high pseudocapacitance and catalytic activities for a number of reactions such as the oxygen evolution reaction (OER) 1,2,3 . While the low energy, RuO 2 (110) and (100) surfaces have been studied as model systems for gas phase catalysis and ultra high vacuum surface science studies 4,5 , the nature of adsorbed species in aqueous solutions remains to be understood. In this work, we examine the structural and chemical changes occurring on oriented RuO 2 single crystal surfaces as a function of potential, in acidic electrolyte, using in situ  synchrotron-based surface X-ray diffraction (crystal truncation rod) measurements. We find that the positions of the surface Ru and O atoms are largely unchanged from 0.5 V to 1.5 V versus the reversible hydrogen electrode (RHE) scale while adsorbed water molecules on the co-ordinatively unsaturated site (CUS) are deprotonated gradually with increasing potential. At oxygen evolution potentials, we observe the formation of an –OO like group on the co-ordinatively unsaturated site, which is the probable precursor of the evolved oxygen. In order to validate experimentally observed changes in the nature of adsorbed oxygen, we use density functional theory to compute surface Pourbaix diagrams that show the most stable surface termination at any given potential. The experimental and computational results are in strong agreement and provide an atomistic understanding of the surface structural changes associated with the redox transitions prior to oxygen evolution and its implications on the oxygen evolution pathway on RuO 2 . References [1] Trasatti S. Electrochimica Acta. 1984;29(11):1503-1512. [2] Lee Y, Suntivich J, May KJ, Perry EE, Shao-Horn Y. The Journal of Physical Chemistry Letters. 2012;3(3):399-404. [3] Stoerzinger KA, Qiao L, Biegalski MD, Shao-Horn Y. The Journal of Physical Chemistry Letters. 2014;5:1636-1641. [4] Over H. Chemical Reviews. 2012;112(6):3356-3426. [5] Sun Q, Reuter K, Scheffler M. Physical Review B. 2003;67(20):205424.
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    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2017-02/47/2061
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  • 20
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    (Invited) High-Throughput Nanoscale Resolved Electrochemistry to Study Electrochemical Nucleation, Growth and Dissolution
    The Electrochemical Society ; 2022
    In:  ECS Meeting Abstracts Vol. MA2022-01, No. 23 ( 2022-07-07), p. 1148-1148
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    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2022-01, No. 23 ( 2022-07-07), p. 1148-1148
    Abstract: Electrochemical nucleation and growth (EN & G) is the cornerstone for many (nano)material growth routes and the main factor limiting battery durability. At the same time electrochemical dissolution (ED) is the main cause of material degradation in exposed environments (corrosion) or energy conversion and storage devices. The in-depth experimental assessment of both processes is very challenging. The reasons are the random nature of initiation events (nucleation), the heterogeneity of surfaces and the (very) fast kinetics of these processes across several length scales. For all that, our current understanding of the mechanisms involved is inaccurate and incomplete [1]. During the last years, we have developed an approach based on using carbon-coated TEM grids as electrodes to combine ex-situ atomic-scale TEM characterization with electron tomography and macroscale electrochemical measurements [2,3]. This approach has brought valuable evidence of non-classical growth pathways such as growth mediated by nanocluster aggregation. Yet, it does not capture the influence of the heterogeneous nature of the surface where EN & G proceeds, nor the dynamics before, during and after nucleation [4,5]. In this contribution, we present our recent work in which we combine high-throughput nanoscale resolved electrochemistry by Scanning Electrochemical Cell Microscopy (SECCM), with ex-situ and in-situ high resolution characterization, including electrochemical transmission electron microscopy (EC-TEM), to study the electrochemical nucleation, growth, and dissolution of metal (Cu, Au, Ag and Pt) nanoparticles (NPs) [6,7]. The spatially resolved electrochemical characterization enables a one-to-one correlation between the electrochemical data and the local surface properties, which can be evaluated by different surface analytical tools. Moreover, the confinement of the electrochemical cell to the SECCM meniscus enables us to resolve a diversity of events during the electrochemical dissolution of electrodeposited NPs. EC-TEM experiments advocate that the nature of these events corresponds to the dissolution of individual NPs spanning a wide range of time [6]. The combination of SECCM and EC-TEM opens up new opportunities for the rational design of functional nanostructured materials by electrodeposition, and for the evaluation of their durability under electrochemical polarization. The ability to study these taking into account the heterogeneous nature of the supports and the differences within nanomaterial ensembles is essential for applications in electrochemical conversion and storage. References: [1] Ustarroz, J. Current Opinion in Electrochemistry . 19 (2020) 144–152. [2] Ustarroz, J et al. Journal of the American Chemical Society (2013), 135, 11550–11561. [3] Ustarroz, J et al. The Journal of Physical Chemistry C (2012), 116, 2322–2329. [4] Hussein H. E. M. et al., ACS Nano . 12, 7388–7396 (2018). [5] Harniman R. L. et al., Nat. Commun. 8, 971 (2017). [6] Bernal, M. et al. In revision (2022). [7] Torres, D. et al. To be submitted (2022).
    Type of Medium: Online Resource
    ISSN: 2151-2043
    URL: Article
    DOI: 10.1149/MA2022-01231148mtgabs
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2022
    detail.hit.zdb_id: 2438749-6
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