Interfacial Phenomena in Electrocatalysis: 51 (Modern Aspects of Electrochemistry)

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Mathias, D. Baker, J. Zhang, Y. Liu, and W. Meier and. Eigenberger , Transport parameters for the modelling of water transport in ionomer membranes for PEM-fuel cells , Electrochimica Acta , vol. Murphy, D. Hitchens, and. Manko , High power density proton-exchange membrane fuel cells , Journal of Power Sources , vol.

Meland and S. Kjelstrup , Three steps in the anode reaction of the polymer electrolyte membrane fuel cell. Meland, S. Kjelstrup, and D.

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In other words, Pt-OH becomes available for reaction not only within its nominal reversible adsorption and desorption peak limits in regular mineral acid or base aqueous solutions, but depending on the reactant concentration, affinity, and its actual reaction rate, along a broad and extendable potential range. Roznyatovskii Aqueous electrochemistry of binuclear copper complex with Robson-type ligand: dissolved versus surface-immobilized reactant J. This is claimed to be the first and only volume to cover interfacial electrochemistry, as opposed to other facets of interfacial science. Antipov, M. Author s : Wolfgang E.

Bedeaux , Rate limiting proton hydration in the anode of the polymer electrolyte membrane fuel cell , Journal of Membrane Science , vol. Maranzana, T. Chupin et al. Mauritz and. Makharia, D. Mathias, and. Mainka, J. Maranzana, S. Dillet, O. Maranzana, J. Moyne, S. Power Sources , issue. Maillard, F. Martin, J. Gloaguen, and. Particle-size effect on the tolerance to methanol competition , Electrochimica Acta , vol. Nam and.

Nakamura, H. Nishikawa, T. Aoki, and Y. Ogami , The diffusion overpotential increase and appearance of overlapping arcs on the Nyquist plots in the low humidity temperature test conditions of polymer electrolyte fuel cell , Journal of Power Sources , vol. Nyikos and. Pajkossy , Fractal dimension and fractional power frequency-dependent impedance of blocking electrodes , Electrochimica Acta , vol. O-'hayre, S. Lee, F. Cha, and. Prinz , A sharp peak in the performance of sputtered platinum fuel cells at ultra-low platinum loading , J. Mark, B. Orazem, and. Tribollet , An integrated approach to electrochemical impedance spectroscopy , Electrochim.

Okada, Y. Xie, and. Tanabe , Theory of water management at the anode side of polymer electrolyte fuel cell membranes , Journal of Electroanalytical Chemistry , vol. Sousa, and. Mendes , Segmented polymer electrolyte membrane fuel cells??? A review , Renewable and Sustainable Energy Reviews , vol. Parthasarathy, C. Martin, S. Srinivasan, V. Paganin, C. Oliveira et al. Parthasarathy, S. Passalacqua, F. Squadrito, A. Lufrano, L. Pw04a, C. Pasaogullari, and. Wang , Two-phase transport and the role of microporous layer in polymer electrolyte fuel cells , Electrochim.

Pw04b, C. Qk02a, A. Qi, and. Qk02b, A. Andreazza, A. Brault, F. Caillard, C. Charles et al.

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Buy Interfacial Phenomena in Electrocatalysis (Modern Aspects of Topics in Number 51 include: Series: Modern Aspects of Electrochemistry (Book 51). Modern Aspects of Electrochemistry. Free Preview cover. © Interfacial Phenomena in Electrocatalysis. Editors: Vayenas Topics in Number 51 include: .

Rai90 and. Raistrick , Impedance studies of porous electrodes , Electrochim. Randles , Kinetics of rapid electrode reactions. Discussion of the Faraday Society , Ramousse, O. Deseure, S. Lottin, D. Didierjean, and. Didierjean, D.

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Lottin, and. Reu08 and. Rowe and. Li , Mathematical modeling of proton exchange membrane fuel cells , Journal of Power Sources , vol. Ramousse, S. Roy and. Roy, B. Tribollet, A. Rubatat, G. Rollet et al. Rodat, F. Sailler, P. Druart, Y. Thivel, P. Bultel et al. Rub03, M. Rubatat, A. Rubio, R. Urquia, S. Kuhn et al. John, R. Slattery, and. Bird , Calculation of the diffusion coefficient of dilute gases and of the self-diffusion coefficient of dense gases , AIChE J , vol. Schneider, A. Bayer, G. Wokaun, and. Sch03 and. Song, W. Lee , Optimal composition of polymer electrolyte fuel cell electrodes determined by the AC impedance method , Journal of Power Sources , vol.

Silva, A. Francesco, and. Pozio , Tangential and normal conductivities of Nafion?? Siegel, D. Ellis, M. Von, and. Sone, D.

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Ekdunge, and. Schneider, D. Freunberger, A. Kramer, G. Wokaun et al.

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Stamenkovic, B. Fowler, G. Mun, P. Wang et al. Saminathan, V. Kamavaram, A. Veedu, and. Kannan , Preparation and evaluation of electrodeposited platinum nanoparticles on in situ carbon nanotubes grown carbon paper for proton exchange membrane fuel cells , International Journal of Hydrogen Energy , vol. Stamenkovic and. Markovic , Oxygen reduction on platinum bimetallic alloy catalysts , Handbook of Fuel Cells -Fundamentals, Technology and Applications , p.

Saleh, M. Okajima, F. Hayase, T. Kitamura, and. Spk05a, B. Sun, K. Peppley, and. Karan , An improved two-dimensional agglomerate cathode model to study the influence of catalyst layer structural parameters , Electrochim. Spk05b, B. Springer and. Sauer, B. Sanders, T. Fricke, K. Saibuathong, K. Saejeng, M. Pruksathorn, N. Hunsom et al. Sepa, A. Vojnovic, and. Damjanovic , Reaction intermediates as a controlling factor in the kinetics and mechanism of oxygen reduction at platinum electrodes , Electrochimica Acta , vol.

Springer, S. Wilson, and. Seidenberger, T. Wilhelm, W. Schmitt, J. Lehnert et al. Zawodzinski, and. Springer, M. Zawodzinski, S. Tricoli, M. Carretta, and. Ticianelli, A. Derouin, S. Redondo, and. Thomas, S. Maranzana, O. Didierjean, J. This book presents a complete overview of the powerful but often misused technique of Electrochemical Impedance Spectroscopy EIS. The book presents a systematic and complete overview of EIS. The book carefully describes EIS and its application in studies of electrocatalytic reactions and other electrochemical processes of practical interest.

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Antolini, K. Ozoemena, J. Zagal, P. Zelenay, J. Dodelet, Z. Chen, L. Dai, K. Ota, N. Alonso-Vante, J. Feliu, P. Strasser, S. Ball, J. Zhang, P. Balbuena, R. Atanasoski, W. Recent intensive research efforts have led to the development of less expensive and more abundant electrocatalysts for fuel cells. This book aims to summarize recent advances of electrocatalysis in oxygen reduction and alcohol oxidation, with a particular focus on low- and non-Pt electrocatalysts. The book is divided into two parts containing 24 chapters total.

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Electrochemistry The Basics, with Examples. This book provides a balanced coverage of the thermodynamic and kinetic processes at the heart of electrochemical reactions and electrochemical systems. While the first half gives an overview of the fundamental concepts appropriate to undergraduate students, the second half gives an in depth account of electrochemical systems suitable to experienced scientists and course lecturers. The concepts are clearly explained and well illustrated.

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The book consists of 11 chapters covering the most critical aspects of the science and technology of nanomaterial electrodes for application in advanced lithium-ion batteries. The chapters include nanostructured anode materials based on Si, Ge, Sn, and other metals and metal oxides together with cathode materials of olivine, the hexagonal and spinel crystal structures. From the chemistry aspect, graphene is the extrapolated extreme of condensed polycyclic hydrocarbon molecules to infinite size.

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Electrochemical Dictionary, 2nd edition Editors: A. Bard, G. Inzelt, F. This second edition of the highly successful dictionary offers more than new or revised terms. A distinguished panel of electrochemists provides up-to-date, broad and authoritative coverage of terms most used in electrochemistry and energy research as well as related fields, including relevant areas of physics and engineering. Each entry supplies a clear and precise explanation of the term and provides references to the most useful reviews, books and original papers to enable readers to pursue a deeper understanding if so desired.

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Almost figures and illustrations elaborate the textual definitions. Polymer electrolyte membrane and direct methanol fuel cell technology Volume 1: Fundamentals and performance of low temperature fuel cells Volume 2: In-situ characterisation techniques for low-temperature fuel cells. Author s : Christoph Hartnig, Christina Roth eds. PEMFCs and DMFCs represent promising low-temperature electrochemical power generation technologies that operate on hydrogen and methanol, respectively. Volume 1 covers the fundamental science and engineering of these types of fuel cell, while volume 2 is dedicated to sophisticated in-situ characterisation methods.

Author s : Keith B. Oldham, Jan C. Myland and Alan M. The book treats electrochemistry as a science in its own right, albeit firmly based on foundations provided by Chemistry, Physics and Mathematics. Early chapters discuss the electrical and chemical properties of materials from which electrochemical cells are constructed. The behavior of such cells is addressed in later chapters, with emphasis on the electrodes and the reactions that occur on their surfaces.

The role of transport to and from electrodes is a topic that commands attention , because it crucially determines cell efficiency. Final chapters deal with voltammetry, the methodology used to investigate electrode behavior. Self-Organization in Electrochemical Systems. I: General Principles of Self-Organization. Temporal Instabilities. The two-volume monograph which discusses both the theory and experimental manifestations of self-organization periodic and chaotic oscillations, multistability in electrochemical systems.

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Topics examined in this volume include: single event electrochemistry, nanoparticle electrocatalysis, bipolar electrochemistry in the nanosciences, nanocarbon electrochemistry, electrochemistry within template nanosystems and electrochemistry within liquid nanosystems. The volume is a key reference in the field of electrochemistry, allowing the reader to become acquainted with the latest research and opinion. Purchasers of the print edition can register for free access to the electronic version. This book presents problems and worked examples for a wide range of theoretical and experimental subjects in the field of voltammetry.

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Electrochemical Synthesis of Nanomaterials in Ionic Liquids. Nanomaterials in Electrochemical Devices. The modern demand of distributed diagnostics imposes new challenges to the world of electrochemistry. In particular, low cost, easy to use, light, miniaturized, point-of-care, implantable VLSI systems need to be designed and developed. The schematization of the spectral broadening as a function of the applied potential, when a PD is present in the electrolyte, for a gold electrode in a 0.

In this experimental system, water and pyrazine molecules experience different electric potentials as function of its z -position within the PD 45 distance normal to the electrode surface, see Fig. The intensity-normalized N 1 s and O 1 s core-level peaks are shown in Fig. The N 1 s raw spectra possess two different identifiable components: the low BE feature centred at From these data, we can observe that the Py ESF and the adsorbed hydroxyls do not shift in BE with the applied potential, meaning that the corresponding species are electrically connected to the grounded gold WE see the energy diagram reported in Supplementary Fig.

The observed spectral broadening and BE shifts for the components within the liquid phase that is, within the EDL constitute the essential results of this work. The error bars were determined via repeated measurements of the FWHM of a given core level, propagated with the experimental spectral resolution see Methods section. Although the linear trend of the BEs as a function of the applied potential inherently carries information about the PD within the EDL, the peak FWHM trend allows an easier and direct comparison with the double-layer capacitance trend derived from electrochemical investigations , as shown in Fig.

In this manner, the core-level peak FWHM represents the direct link between spectroscopy and electrochemistry. The PZC, defined as the observed potential at which no net charge is present on the electrode surface and no PD is present in the EDL can be determined both electrochemically Fig. The trend of the double-layer capacitance reported in Fig. This agreement reflects the linkage between the double-layer capacitance and the trend of the peak FWHM values, thus establishing a clear correlation between an electrochemical property of the EDL and a pure spectroscopic feature.

It is noteworthy to report that the findings discussed above are valid also in case of a pyrazine free electrolyte, since the direct probing of EDL can be performed, as reported in Fig. More details are provided in Supplementary Fig. Additionally, we observed that the FWHM trends as a function of the applied potential implicitly carries the functional dependency fingerprint of the PD Fig.

The step and linear PD models were selected to test the fit to our data as well as our ability to distinguish the shape of the EDL structure, and thus do not represent a modern theory for the EDL structure. This approach provides the ability to objectively evaluate the agreement between the data and models for all applied potentials and electrolyte concentrations that is, EDL thicknesses, d EDL. As well documented by Fig. Due to the exponential decay of the photoelectron intensity, the spectral components localized at the IHP do not significantly contribute to the summation over all the initial states.

Future experimental and instrumental modifications are being planned to help improve this limitation. Moreover, the utilization of the SW-APXPS approach to provide a higher degree of spatial resolution near the electrode surface will be explored 42 , 47 , in particular towards the study of surface adsorbates, ion-specific adsorptions and charge transfers at the IHP, and their interplay in the faradaic processes occurring at the electrified interface. To get more insights into the EDL structure as a function of the electrolyte concentration, we have modulated the EDL thickness d EDL by gradually increasing the electrolyte concentration, passing from 0.

The N 1 s , O 1 s and Au 4 f data for each investigated electrolyte concentration are reported in Supplementary Fig. Further details are also reported in Supplementary Note 3. By using the aforementioned linear fitting procedure applied to the experimental FWHM trends as a function of the applied potential, we have determined the PZC values and described the evolution of the exponential potential profile directly from the spectroscopy data shown in Fig.

However, with the current signal-to-noise ratio, the definitive discrimination between an exponential and a linear shape for the PD is challenging to achieve. Potential of zero charge PZC determination and comparison between the experimental and simulated spectral full-width at half-maximum FWHM trends, as function of the applied potentials E and for an aqueous electrolyte containing 1. Future improvements of the experimental set-up will enhance spectral resolution and signal-to-noise ratio, which will improve our ability to discern the fine features of the PD functional dependency carried by the core-level spectral broadening.

The simulations of the PD profiles, similarly to what has been experimentally performed, have been generated as a function of the applied potential for different electrolyte concentrations that is, for different EDL thicknesses. The comparison between the experimental and simulated FWHM provides the ability to directly access and visualize the PD within the EDL that leads to the observed spectral broadening.

The resulting simulated exponential potential profiles are reported in Fig. This possibility paves the way toward a new type of EDL and its inherent properties such as the PD investigations under real electrochemical and photoelectrochemical reactions. Finally, for KOH concentrations higher than those shown in Fig. This result is consistent with a thinner EDL that can be expected from an increased ionic strength of the supporting electrolyte.

There is not enough signal from the molecules in the EDL to be resolved from the total O 1 s and N 1 s photoelectron intensity. Therefore, there is a concentration limit for this technique to discern the electrical potential profile within the EDL. The schematization reported in Supplementary Fig.

However, future experimental and instrumental modifications previously mentioned that is, SW-APXPS will allow us to overcome these current limitations 42 , The method has general applicability and is not restricted to one specific class of solids or liquids. We have shown that the FWHM trend of the core-level peaks of electrolyte as a function of the applied potential is strongly correlated to the double-layer capacitance trend. We have also demonstrated that the PZC obtained from spectroscopy is in line with the electrochemically-derived values, providing a synergistic correlation between electrochemistry and photoelectron spectroscopy.

Exploiting the element-specificity and potential-sensitivity of photoelectron spectroscopy, we have directly probed the PD within the EDL by studying the broadening of the core-level photoelectron spectra of the elements belonging to the liquid phase, as a function of the applied potential. Furthermore, by using numerical simulations, we have shown that our method provides the ability to identify the functional dependency that describes the PD within the double layer, providing a spectroscopic support for the current electrified interface theories.

A schematic representation of our combined experimental and simulation-based approach is reported in Supplementary Fig. The coupling between our APXPS performed under polarization conditions with the use of a solvent- or an independent probe-related core level, sets a paradigm for probing the properties of the EDL under realistic conditions.

The current results may open the door for studying the EDL dynamics in more complicated systems, such as redox reactions at photoactive semiconductor interfaces and in non-aqueous electrolytes, to name a few see Supplementary Note 1. The knowledge gained from this method may thus impact a wide range of scientific fields, including electrochemical conversion and storage of energy, environmental sciences and biology 14 , 15 , Beamline 9. The measurements were taken using a photon energy of 4.

During the fitting procedure, the Shirley background was optimized as well, together with the spectral components, increasing in this manner the precision and reliability of the fitting procedure 49 , 50 , In this work, we have used the FWHM for the quantification of the spectral broadening. The chemicals here employed were high purity reagents and they were used as received without further operations.

The working and counter electrodes Au and Pt polycrystalline foils respectively, Aldrich were polished to a mirror finish with silicon carbide papers of decreasing grain size Struers, grit: 2, and 4, Once the three electrodes were mounted on the manipulator 39 Supplementary Fig. The cleaning procedure was stopped after reaching the OCP of the cell from the cathodic side that is, after HER, to start the EDL probing on a cleaned metal surface Before its introduction into the experimental chamber, the electrolyte KOH 0.

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The first two models were considered to test the ability of distinguishing between different PD functional dependencies. The core algorithm was developed in Igor C-oriented language. An example of the performed simulations is reported in Supplementary Fig. Simulated N 1 s or O 1 s photoelectron peaks have been generated by using the envelope function-derived method 52 , by summing the different spectral contributions within the diffuse layer each one shifted according to the potential profile and in the bulk electrolyte rigidly shifted because of the shift of the liquid phase with the applied potential, see energy diagram reported in Supplementary Fig.

Then, by performing the summation over all the shifted N 1 s or O 1 s spectral components with a coefficient determined by the exponential dumping of the photoelectron intensity Beer—Lambert law , it is possible to finally obtain a simulated spectrum that can be compared with the experimental data.

The envelope function S BE at the base of the calculation, describing the final convolution of the simulated photoelectron peak as reported in equation The measurement was performed studying a thick drop of solution hanging from the WE, to rule out interfacial contribution and obtain the O 1 s and N 1 s photoelectron peaks exclusively from water and solvated pyrazine molecules in the bulk electrolyte, respectively.

The spectral components within the bulk electrolyte are instead fully shifted by the applied potential E. The two integers i and j vary over the PD within the EDL and the bulk region of the electrolyte layer B , respectively. The simulations were conducted probing both the EDL and the bulk electrolyte every 0.

The algorithm developed for the calculation of the simulated spectra as described by equation 1 is characterized by a good stability also for a significant number n of total elements in the summation; the complexity class of the algorithm belongs to O n. The D i,j coefficients that damps the intensity of the single summation elements are calculated according to the Beer—Lambert law equation 2. The data that support the findings of this study are available from the corresponding author upon request.

How to cite this article: Favaro, M. Zaera, F. Devanathan, M. The structure of the electrical double layer at the metal—solution interface. Delahay, P. Double layer studies. Grahame, D. The electrical double layer and the theory of electrocapillarity. Parsons, R. Electrical double layer: recent experimental and theoretical developments. Bard, A.