Dissolution of Platinum: Limits for the Deployment of Electrochemical Energy Conversion?

Topalov, Angel Angelov; Katsounaros, Ioannis; Auinger, Michael; Cherevko, Serhiy; Meier, J.; Klemm, Sebasian Oliver; Mayrhofer, Karl Johann Jakob

doi:10.1002/anie.201207256

Cited by 374 publications

(444 citation statements)

References 25 publications

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“…It should also be noted that corrosion mechanisms are highly dependent on the material. [39] The degradation of some materials may actually be accelerated by potential cycling (as shown by Mayrhofer and co-workers to be the case for Pt, by combining cyclic voltammetry with online ICP measurements [61] ). Consequently, to study the resistance to corrosion of such materials, potentiodynamic-rather than potentiostatic-tests would be necessary.…”

Section: à2mentioning

confidence: 99%

Benchmarking the Stability of Oxygen Evolution Reaction Catalysts: The Importance of Monitoring Mass Losses

et al. 2014

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Because of the rising need for energy storage, potentially facilitated by electrolyzers, improvements to the catalysis of the oxygen evolution reaction (OER) become increasingly relevant. Standardized protocols have been developed for determining critical figures of merit, such as the electrochemical surface area, mass activity and specific activity. Even so, when new and more active catalysts are reported, the catalyst stability tends to play a minor role. In this work, we monitor corrosion on RuO2 and MnOx by combining the electrochemical quartz crystal microbalance (EQCM) with inductively coupled plasma mass spectrometry (ICP–MS). We show that a meaningful estimation of the stability cannot be achieved based on purely electrochemical tests. On the catalysts tested, the anodic dissolution current was four orders of magnitude lower than the total current. We propose that even if long‐term testing cannot be replaced, a useful evaluation of the stability can be achieved with short‐term tests by using EQCM or ICP–MS.

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Section: à2mentioning

confidence: 99%

Benchmarking the Stability of Oxygen Evolution Reaction Catalysts: The Importance of Monitoring Mass Losses

et al. 2014

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“…The works of Topalov et al [10], Xing et al [21], as well as Rinaldo et al [22] revealed a staggering enhancement in Pt dissolution rate by a factor ∼2000 during voltage cycling in accelerated stress tests when the upper potential limit of the voltage cycle was increased above 1.2 V RHE . It was found consistently in these independent studies that the reduction of Pt oxide during the reduction part of the voltage cycle is responsible for the hugely increased rate of Pt dissolution.…”

Section: Introductionmentioning

confidence: 96%

“…However, it is known that typical operational conditions such as high temperature, high potential, low pH and, in particular, extensive potential cycling lead to unacceptable rates of Pt dissolution [10][11][12]. The kinetics of Pt dissolution in turn is correlated with loss of catalyst material, transformation of porous composite structure, decrease of active surface area, change in wettability of pore walls, decline of electrochemical performance, and ultimately the lifetime reduction of the device [13].…”

Section: Introductionmentioning

confidence: 99%

Atomistic Mechanism of Pt Extraction at Oxidized Surfaces: Insights from DFT

Eslamibidgoli

Eikerling

2016

Electrocatalysis

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In this article, we propose a novel mechanism for the atomic-level processes that lead to oxide formation and eventually Pt dissolution at an oxidized Pt(111) surface. The mechanism involves a Pt extraction step followed by the substitution of chemisorbed oxygen to the subsurface. The energy diagrams of these processes have been generated using density functional theory and were analyzed to determine the critical coverages of chemisorbed oxygen for the Pt extraction and O ads substitution steps. The Pt extraction process depends on two essential conditions: (1) the local coordination of a Pt surface atom by three chemisorbed oxygen atoms at nearestneighboring fcc adsorption sites; (2) the interaction of the buckled Pt atom with surface water molecules. Results are discussed in terms of surface charging effects caused by oxygen coverage, surface strain effects, as well the contribution from electronic interaction effects. The utility of the proposed mechanism for the understanding of Pt stability at bimetallic surfaces will be demonstrated by evaluating the energy diagram of a Cu ML /Pt(111) near-surface alloy.

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“…Thus a percentage change in activity is the same percentage change in surface area, as per the Tafel equation. Relationships which describe the reduction of the surface area (activity) and mass of a spherical particle over the course of an AST are a f = a bot − pa bot [1] and m r = m bot − m f [2] where n is the percent reduction, a bot is the spherical particle surface area at the beginning of the test, a f is the final spherical particle surface area, m bot is the spherical particle mass at the beginning of the test, m f is the final sphere mass (i.e. when the sphere surface area has decreased by p percent) and m r is the sphere mass reduction.…”

Section: F858mentioning

confidence: 99%

“…Topalov et al 1,2 showed that minute amounts (in the order of ng cm −2 ) of Pt are dissolved every time an electrode potential transient which has an upper potential limit > 1.0 V RHE causes the oxidation or reduction of Pt. Cherevko et al 3 and Ahluwalia et al 4 demonstrated that Pt is also unstable during normal fuel cell operational potentials (≤1.0 V), i.e.…”

mentioning

confidence: 99%

Screening Bifunctional Pt Based NSTF Catalysts for Durability with the Rotating Disk Electrode: The Effect of Ir and Ru

Crowtz

Dahn

2018

J. Electrochem. Soc.

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Various amounts of Ir (<20 μg cm −2 ) and Ru (up to 12 μg cm −2 ) on a consistent base Pt loading of 85 μg cm −2 , were sputter deposited on a nanostructured thin film catalyst support to mimic a hydrogen fuel cell's cathode catalyst. The nanostructured support was grown on glassy carbon disks designed for a rotating disk electrode, which was used to simulate what happens to a fuel cell cathode during repeated start-up, operation, and shut-down. The testing protocol subjected the catalyst to a minimum potential of 0.65 V RHE and a maximum between 1.53 and 1.8 V RHE . The upper potential was achieved with a galvanostatic hold which is an alternative way to simulate potential transients on the cathode caused by start-up and shut-down. Increasing Ir loading improved the durability of both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity. When combined with Ir, Ru provided no benefit to OER durability except at an Ir loading of 10 μg cm −2 . Ru addition (no Ir present) improved the ORR durability compared to pure Pt. ORR durability was not influenced by Ru addition to Ir-containing samples. In general, ORR durability showed no dependence on Ru loading for all the Ru containing samples and ORR activity was decreased by OER catalyst addition, though more so for Ir than Ru.

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Dissolution of Platinum: Limits for the Deployment of Electrochemical Energy Conversion?

Cited by 374 publications

References 25 publications

Benchmarking the Stability of Oxygen Evolution Reaction Catalysts: The Importance of Monitoring Mass Losses

Benchmarking the Stability of Oxygen Evolution Reaction Catalysts: The Importance of Monitoring Mass Losses

Atomistic Mechanism of Pt Extraction at Oxidized Surfaces: Insights from DFT

Screening Bifunctional Pt Based NSTF Catalysts for Durability with the Rotating Disk Electrode: The Effect of Ir and Ru

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