The study of electrochemical palladium behavior using the quartz crystal microbalance

Grdeń, M.; Kotowski, Jakub; Czerwiński, A.

doi:10.1007/s100080050204

Cited by 64 publications

(32 citation statements)

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“…Nevertheless, this approach is probably the most imprecise out of these three, since the definition of an integration baseline free of pseudo-capacitive contributions is highly ambiguous, and the stoichiometry of these (hydr)oxides changes with the potential. While several works [36][37][38][39] …”

Section: −2mentioning

confidence: 99%

Bulk-Palladium and Palladium-on-Gold Electrocatalysts for the Oxidation of Hydrogen in Alkaline Electrolyte

Henning

Herranz

Gasteiger

2014

J. Electrochem. Soc.

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The commercial feasibility of alkaline-exchange membrane fuel cells and electrolyzers passes by the development of hydrogen oxidation and evolution reaction (HOR/HER) catalysts featuring an activity and/or cost advantage over platinum, which remains the most active metal for these processes. Among these alternatives, Pd appears as a promising candidate, since its price is typically 2-3 fold lower than that of Pt. With this motivation, the first section of this study displays our attempts at quantifying the kinetic parameters of the HOR/HER on bulk Pd in 0.1 M NaOH, which were prevented by the simultaneous absorption of hydrogen into bulk palladium. We succeeded at circumventing this issue by depositing Pd-adlayers on a polycrystalline Au-substrate by galvanic displacement of underpotentially-deposited Cu or by electrochemical plating of Pd 2+ . The resulting surfaces appear to consist of three-dimensional Pd-structures of an unknown thickness that we believe to scale with the palladium coverage, θ Pd/Au . This last parameter is inversely proportional to the HOR/HER-activity of the Pd-on-Au surfaces, in agreement with numerous theoretical and experimental studies in acid media that correlate this effect to the tensile strain induced by the Au-substrate on the Pd-lattice. Proton-exchange membrane fuel cells (PEMFCs) fueled with hydrogen stored at 700 bar can attain energy densities in excess of 200 Wh · kg −1 (on a PEMFC system basis), making them excellent candidates for the propulsion of environmentally-benign, full range (≥ 300 miles) vehicles.1 However, the actual commercialization of PEMFC powered cars has been deterred by the lack of a hydrogen infrastructure and the high cost of the PEMFC. In this last respect, a significant fraction of the system's price is related to the costly platinum-based catalysts needed to catalyze the oxidation of hydrogen and the reduction of oxygen taking place at the FC anode and cathode, respectively.1-3 The kinetics of the oxygen reduction reaction (ORR) on Pt 4 are ≈7 orders of magnitude slower than those of the hydrogen oxidation reaction (HOR), 5 in agreement with the HOR 5 -and ORR 4 -exchange-current density (i 0 ) values of 4 ± 2 · 10 +2 mA · cmPt estimated by Neyerlin and coworkers (at 80• C and 100 kPa H 2 /air partial pressure). As such, the Pt-loading at the PEMFC's cathode (≈0.2-0.4 mg Pt · cm −2 ) is well above the ≤ 0.05 mg Pt · cm −2 required for the anodic HOR, and thus much research is being devoted to the development of more active and/or less expensive ORR catalysts.6-10 These include alloys of Pt with non-noble metals like Ni, Co or Cu (as well as their de-alloyed derivatives), and catalysts consisting of non-noble metal nanoparticles covered by one or a few monolayers of Pt (i.e., the so-called "core-shell" catalysts).Alternatively, operating a fuel cell in alkaline environment allows for the use a wider variety of potentially inexpensive, noblemetal free ORR-catalysts. Among these, certain materials based on Fe-, Co-and/or Cu-N 4 chelates (or equivalent no...

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Section: −2mentioning

confidence: 99%

Bulk-Palladium and Palladium-on-Gold Electrocatalysts for the Oxidation of Hydrogen in Alkaline Electrolyte

Henning

Herranz

Gasteiger

2014

J. Electrochem. Soc.

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“…In general, the EQCM response can be determined by several factors [16][17][18] but in the case of hydrogen electrosorption the most important are two of them: (i) electrode mass changes (i.e. changes in the amount of electrosorbed hydrogen) and (ii) stresses in crystal lattice induced by hydrogen absorption [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15]19,20]. Therefore, the following equation is valid [6,14,15]:…”

Section: Introductionmentioning

confidence: 99%

“…In the literature, there are numerous reports devoted to the application of the electrochemical quartz crystal microbalance (EQCM) in the investigation of hydrogen absorption in Pd [1][2][3][4][5][6][7][8][9][10][11][12] and some of its alloys [13][14][15].…”

Section: Introductionmentioning

confidence: 99%

Electrochemical quartz crystal microbalance study on hydrogen absorption and desorption into/from palladium and palladium–noble metal alloys

Łukaszewski

Czerwiński

2006

Journal of Electroanalytical Chemistry

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“…Voltammetric experiments suggest that oxidation of Pd@PdO nanoparticle in aqueous alkaline electrolyte could proceed via formation of Pd(OH) x adsorbed species further evolving to Pd oxides and/or Pd 2+ ions in solution [51], similarly to the growth of porous PdO films on Pd electrodes [52]. Solid state electrochemistry of nanoheterogeneous deposits of Pd nanoparticles covered by PdO shell on graphite electrodes in contact with aqueous permits a direct estimation of the thickness of the PdO shell and the size of the palladium core by using electrochemical data alone [51].…”

Section: Molecule-type Behaviormentioning

confidence: 99%

“…Cyclic voltammetric experiments on QD dispersions [52] and adsorbed on electrode surfaces [53] have been used for determining energy band gaps, the relationship between optical and electrochemical band gaps being expressed by Eq. 5.…”

Section: Molecule-type Behaviormentioning

confidence: 99%

Electrochemistry of Metal Nanoparticles and Quantum Dots

Doménech‐Carbó

Galian

Aguilera‐Sigalat

et al. 2014

Handbook of Nanoparticles

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Metal nanoparticles, with a wide range of applications in catalysis and sensing, have structural and electronic properties that differ from those of their bulk macroscopic counterparts. Electrochemical techniques are of particular interest in the study of metal nanoparticles because electrons may undergo quantum confinement effects which are reflected in their electrochemical behavior, resulting, ultimately, in three distinguishable voltammetric regimes: bulk continuum, quantized double-layer charging, and molecule-like. Similarly, semiconductor nanoparticles (quantum dots, QDs) are receiving considerable attention due to their high fluorescence, which makes them of interest for biological and medical applications, among others. The semiconductor bulk materials possess defect states that originate from impurities, divacancies, or surface reactions as a result of their synthesis. Voltammetric features provide information on bandgap energy, the position of conduction and valence band edges, and the position of defect sites as well as on the interaction with the capping ligand. This chapter is devoted to provide a critical view of the current state of the art in the electrochemistry of such systems.

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The study of electrochemical palladium behavior using the quartz crystal microbalance

Cited by 64 publications

References 0 publications

Bulk-Palladium and Palladium-on-Gold Electrocatalysts for the Oxidation of Hydrogen in Alkaline Electrolyte

Bulk-Palladium and Palladium-on-Gold Electrocatalysts for the Oxidation of Hydrogen in Alkaline Electrolyte

Electrochemical quartz crystal microbalance study on hydrogen absorption and desorption into/from palladium and palladium–noble metal alloys

Electrochemistry of Metal Nanoparticles and Quantum Dots

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