Elucidation of the Electrochemical Activation of Water over Pd by First Principles

Filhol, Jean‐Sébastien; Neurock, Matthew

doi:10.1002/anie.200502540

Cited by 388 publications

(367 citation statements)

References 6 publications

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“…103 Carbon-supported Pd-rich pseudo-core-shell Pd-Pt (Pd@Pt/C) nanoparticles can be prepared by a galvanic replacement reaction, and analyzed using microstructural characterization techniques. 104 Core-shell Pd 70 @Pt 30 catalysts with a loading of 20.4 mg (total metals) per cm 2 showed a minimum two-fold enhancement in their ORR activity in 0.1 M HClO 4 , and presented some advantages in terms of cost and methanol tolerance.…”

Section: Effects Of the Synthetic Methodsmentioning

confidence: 99%

Nanostructured Pt-alloy electrocatalysts for PEM fuel cell oxygen reduction reaction

et al. 2010

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In this critical review, we present the current technological advances in proton exchange membrane (PEM) fuel cell catalysis, with a focus on strategies for developing nanostructured Pt-alloys as electrocatalysts for the oxygen reduction reaction (ORR). The achievements are reviewed and the major challenges, including high cost, insufficient activity and low stability, are addressed and discussed. The nanostructured Pt-alloy catalysts can be grouped into different clusters: (i) Pt-alloy nanoparticles, (ii) Pt-alloy nanotextures such as Pt-skins/monolayers on top of base metals, and (iii) branched or anisotropic elongated Pt or Pt-alloy nanostructures. Although some Pt-alloy catalysts with advanced nanostructures have shown remarkable activity levels, the dissolution of metals, including Pt and alloyed base metals, in a fuel cell operating environment could cause catalyst degradation, and still remains an issue. Another concern may be low retention of the nanostructure of the active catalyst during fuel cell operation. To facilitate further efforts in new catalyst development, several research directions are also proposed in this paper (130 references).

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Section: Effects Of the Synthetic Methodsmentioning

confidence: 99%

Nanostructured Pt-alloy electrocatalysts for PEM fuel cell oxygen reduction reaction

et al. 2010

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“…Several methods [5][6][7][8][9][10][11][12][13] have been proposed for correcting quantum chemical calculations to constant electrode potential. The most elegant solution would be to treat electrons in the grand canonical ensemble, that is, to allow the number of electrons to change during the electronic structure self-consistency loop, which is equivalent to connecting the system to a fictitious potentiostat.…”

Section: Introductionmentioning

confidence: 99%

Ab Initio Electrochemistry: Exploring the Hydrogen Evolution Reaction on Carbon Nanotubes

Holmberg

Laasonen

2015

J. Phys. Chem. C

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Density functional theory (DFT) was employed to investigate the hydrogen evolution reaction (HER) on pristine and nitrogen doped carbon nanotubes (CNTs) in acidic solution. As the reaction is an electrocatalytic surface reaction, an accurate description of HER requires performing simulations under constant electrode potential conditions. To this end, we examined HER at several electrode charges allowing us to determine grand canonical activation energies as a continuous function of electrode potential. By studying the elementary steps of HER -the Volmer, Tafel and Heyrovsky reactions -and by considering hydrogen coverage effects, we found that the Volmer-Heyrovsky mechanism is the predominant HER mechanism on CNTs with the Heyrovsky step being rate-determining. Our results indicated that CNTs are electrochemically active towards HER, which seen as a decrease in activation energies with growing electrode potential, but that the activity is lower than on platinum matching experimental data.Substitutional nitrogen doping did not improve HER activity, and further research is required to determine which nitrogen configurations contribute to the enhanced catalytic activity observed for experimental NCNTs.

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“…Recent work, however, indicates that such conventions are emerging. 1,2,[6][7][8] It has, for example, been shown that many of the conventions from heterogeneous catalysis and gas-phase reactions can be applied to electrochemistry. 2 This requires a reference to connect the gas-phase surface calculations to those under electrochemical control.…”

Section: Introductionmentioning

confidence: 99%

“…1,6,10 The work function is therefore related to the normal hydrogen electrode, similar to eq 1, via the following equation…”

Section: Introductionmentioning

confidence: 99%

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Calculated Phase Diagrams for the Electrochemical Oxidation and Reduction of Water over Pt(111)

Rossmeisl¹,

Nørskov²,

Taylor³

et al. 2006

J. Phys. Chem. B

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415

459

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Ab initio density functional theory is used to calculate the electrochemical phase diagram for the oxidation and reduction of water over the Pt(111) surface. Three different schemes proposed in the literature are used to calculate the potential-dependent free energy of hydrogen, water, hydroxyl, and oxygen species adsorbed to the surface. Despite the different foundations for the models and their different complexity, they can be directly related to one another through a systematic Taylor series expansion of the Nernst equation. The simplest model, which includes the potential only as a shift in the chemical potential of the electrons, accounts very well for the thermochemical features determining the phase-diagram.

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Elucidation of the Electrochemical Activation of Water over Pd by First Principles

Cited by 388 publications

References 6 publications

Nanostructured Pt-alloy electrocatalysts for PEM fuel cell oxygen reduction reaction

Nanostructured Pt-alloy electrocatalysts for PEM fuel cell oxygen reduction reaction

Ab Initio Electrochemistry: Exploring the Hydrogen Evolution Reaction on Carbon Nanotubes

Calculated Phase Diagrams for the Electrochemical Oxidation and Reduction of Water over Pt(111)

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