Piezoelectric Response to Surface Stress Change of a Palladium Electrode in Sulfate Aqueous Solutions

Seo, Masahiro; Aomi, Masaki

doi:10.1149/1.2069344

Cited by 31 publications

(13 citation statements)

References 9 publications

(24 reference statements)

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“…In particular, there are some relevant issues in the literature that require additional research [30]: (i) the first product formed during oxidation was considered by several authors to be Pd(OHads) [34,38,39,48,63,70], while other authors suggested the formation of Pd(II)-oxide/hydroxide species such as PdO [30,71] or Pd(OH)2 [31]; (ii) the potential for the formation of an oxide monolayer (generally reported to occur around 1.45-1.5 VRHE) is unclear, as is (iii) the onset potential for the formation of higher oxidation species (i.e Pd(IV)-oxide, thicker β Pd(IV)-oxide in the OER region);…”

Section: Discussionmentioning

confidence: 99%

Palladium electrodissolution from model surfaces and nanoparticles

Pizzutilo

Geiger

Freakley

et al. 2017

Electrochimica Acta

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Palladium (Pd) is considered as a possible candidate as catalyst for proton exchange membrane fuel cells (PEMFCs) due to its high activity and affordable price compared to platinum (Pt). However, the stability of Pd is known to be limited, yet still not fully understood. In this work, Pd dissolution is studied in acidic media using an online inductively coupled plasma mass spectrometry (ICP-MS) in combination with an electrochemical scanning flow cell (SFC). Crucial parameters influencing dissolution like potential scan rate, upper potential limit (UPL) and electrolyte composition are studied on a bulk polycrystalline Pd (poly -Pd). Furthermore, a comparison with a supported high -surface area catalyst is carried out for its potential use in industrial applications. For this aim, a carbon supported Pd nanocatalyst (Pd/C) is synthesized and its performance is compared with that of bulk poly -Pd. Our results evidence that the transient dissolution is promoted by three main contributions (one anodic and two cathodic). At potentials below 1.5 VRHE the anodic dissolution is the dominating mechanism, whereas at higher potentials the cathodic mechanisms prevail. On the basis of the obtained results, a model is thereafter proposed to explain the transient Pd dissolution.(C) 2017 Elsevier Ltd. All rights reserved

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Section: Discussionmentioning

confidence: 99%

Palladium electrodissolution from model surfaces and nanoparticles

Pizzutilo

Geiger

Freakley

et al. 2017

Electrochimica Acta

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“…The hydrogen absorption region has also been a topic of considerable interest and has been examined by several in situ techniques such as voltammetry, ,, electrochemical quartz crystal nanogravimetry, − piezoelectric response, and wafer curvature. − For the most part, the wafer curvature measurements have provided fundamental data on the hydride such as hydrogen diffusivity , and stress state. , Moreover, the curvature response of microcantilevers has also been exploited in the development of hydrogen sensors for the gas phase. − …”

Section: Introductionmentioning

confidence: 99%

In Situ Stress and Nanogravimetric Measurements During Hydrogen Adsorption/Absorption on Pd Overlayers Deposited onto (111)-Textured Au

Stafford

Bertocci

2009

J. Phys. Chem. C

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The stress induced by electrochemical hydrogen adsorption and absorption in very thin palladium layers electrodeposited onto (111)-textured gold has been examined in 0.1 M H2SO4 by the cantilever curvature method and by comparing resonant frequency changes on AT- and BT-cut quartz crystals. A compressive surface stress change of about −0.25 N m−1 is measured in the hydrogen adsorption region. Compressive stress for hydrogen adsorption is not expected from charge distribution models for adsorbate-induced surface stress but is consistent with first-principles calculations in the literature as well as experimental data for H adsorbed on Pt(111). Cantilever measurements in the hydrogen absorption region are consistent with a maximum atomic H/Pd loading of 0.63 and give a compressive stress-thickness change of −0.45 N m−1 per monolayer of Pd, corresponding to a biaxial stress change of −2.0 GPa. A somewhat lower value of −0.80 GPa for a H/Pd loading of 0.68 was obtained from EQNB data using the double crystal technique. These stress values fall well within the range of experimental values reported in the literature for β-hydride generated both electrochemically and from the gas phase.

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“…33 This method is somewhat similar to those that have utilized a piezoelectric ceramic element to quantify the piezo-response of electrodes to voltage stimulation. [34][35][36] The aim of DSA is to study the dynamics of any particular stress-generating process and link the stress to specific electrochemical and surface phenomena.Surface stress, f, is the reversible work per unit area required to elastically stretch a surface 37 and is defined by the Shuttleworth equation, 38 which in its scalar form iswhere γ is the surface free energy; i.e., the reversible work per unit area involved in forming a surface, and ε is the elastic strain. Unlike the established quadratic relationship that exists between the surface free energy and the charge density, 39 the relationship between the surface stress and the charge density cannot be derived directly from thermodynamic equations.…”

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confidence: 99%

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Dynamic Stress Analysis Applied to (111)-Textured Pt in HClO₄Electrolyte

Lafouresse

Bertocci

Stafford

2013

J. Electrochem. Soc.

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Dynamic stress analysis (DSA) was performed on Pt cantilever electrodes immersed in 0.1 mol/L HClO 4 electrolyte. DSA combines elements of electrochemical impedance spectroscopy (EIS) and cantilever curvature. In this paper DSA is used to determine the relationship between surface stress f and charge density q for (111)-textured Pt as a function of steady state potential. The parameter of merit is the stress-charge coefficient, ξ, a complex number, which is obtained from the product of the electrochemical impedance Z e and the stress admittance Y s . The magnitude and sign of ξ r , the real component of ξ, quantifies how the surface responds to changes in charge density. Three regions of stress-charge behavior have been identified at potentials bound by hydrogen adsorption and platinum oxide formation. In the hydrogen adsorption region, stress and charge are in phase, resulting in a positive value of ξ r . In the double layer region the surface stress and the charge density are 180 • out of phase, yielding a negative value of ξ r . The actual potential at which this phase angle transition occurs may vary by as much as 0.3 V, depending on electrode history. At more positive potential ξ r remains negative in the early oxide region, where the reversible adsorption of O occurs. Only at more positive potential, where place exchange between Pt and O occurs and the surface layer of PtO becomes fully formed, does ξ r transition back to a positive value. The experimental methods described in this work provide a means to probe the dynamic behavior of surface stress.The electrochemical community often uses in situ wafer curvature and cantilever bending techniques to examine stress development during electrochemical processing. For example, these techniques have been used to examine and quantify surface stress induced by surface charge (electrocapillarity) 1-4 and adsorption processes 5-8 as well as growth stress associated with underpotential deposition (UPD) 1,9-20 and electrodeposition. 21-32 In many cases the electrochemistry involves multiple processes that occur either simultaneously or in rapid succession so that a steady state stress measurement will simply reflect the influence of the dominant process in the time-scale of the experiment. Electrochemical impedance spectroscopy (EIS) is often used to separate processes with different characteristic time constants. A sinusoidal voltage (typically of the order of a few mV) is applied to an electrochemical system and the current response is measured. The frequency of the applied voltage is varied so that different processes can be singled out at specific frequencies. Dynamic stress analysis (DSA) is analogous to EIS, however in addition to the current, the cantilever's curvature is also measured as a function of frequency. 33 This method is somewhat similar to those that have utilized a piezoelectric ceramic element to quantify the piezo-response of electrodes to voltage stimulation. [34][35][36] The aim of DSA is to study the dynamics of any particular stress-generating...

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Piezoelectric Response to Surface Stress Change of a Palladium Electrode in Sulfate Aqueous Solutions

Cited by 31 publications

References 9 publications

Palladium electrodissolution from model surfaces and nanoparticles

Palladium electrodissolution from model surfaces and nanoparticles

In Situ Stress and Nanogravimetric Measurements During Hydrogen Adsorption/Absorption on Pd Overlayers Deposited onto (111)-Textured Au

Dynamic Stress Analysis Applied to (111)-Textured Pt in HClO₄Electrolyte

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Piezoelectric Response to Surface Stress Change of a Palladium Electrode in Sulfate Aqueous Solutions

Cited by 31 publications

References 9 publications

Palladium electrodissolution from model surfaces and nanoparticles

Palladium electrodissolution from model surfaces and nanoparticles

In Situ Stress and Nanogravimetric Measurements During Hydrogen Adsorption/Absorption on Pd Overlayers Deposited onto (111)-Textured Au

Dynamic Stress Analysis Applied to (111)-Textured Pt in HClO4Electrolyte

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Product

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Dynamic Stress Analysis Applied to (111)-Textured Pt in HClO₄Electrolyte