Multidimensional Effects on Dissociation of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>on Ru(0001)

Dı́az, Cristina; Vincent, Jonathan; Krishnamohan, G. P.; Olsen, Roar A.; Kroes, Geert–Jan; Honkala, Karoliina; Nørskov, Jens K.

doi:10.1103/physrevlett.96.096102

Cited by 94 publications

(81 citation statements)

References 28 publications

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“…1, we find Θ vib (R) ≈ 1.6 for R in the range 0.0005-0.1. [31] This value is smaller than the Θ vib (R) ≈ 2.5 that can be estimated from experiments, [27] but both results are significantly larger than 1. There are a number of possible explanations for the rather large difference in efficacy found by theory and experiments: On the theoretical side it is possible that the PES calculated by DFT is not close enough to the actual PES governing the dynamics of the system.…”

Section: A 6d Dynamics and The Vibrational Efficacymentioning

confidence: 66%

“…3 in Ref. 31). Thus, since the minimum barrier is a very narrow bottleneck towards dissociation, and since the high barrier requires a high collision energy for the molecule to cross it which in turn makes it difficult for it to be steered [53,54] by the potential forces towards the lowest barrier configuration, only a molecule arriving at the surface with the right orientation and in the right position will cross the barrier.…”

Section: A 6d Dynamics and The Vibrational Efficacymentioning

confidence: 91%

“…The cutoff energy for the plane wave basis was set to 350 eV and to sample the Brillouin zone 18 Chadi-Cohen [39] kpoints were used. Extensive testing of all computational parameters at a number of selected configurations shows that the molecule-surface interaction energies are converged within 0.1 eV [30,31], a typical error bar for these type of DFT calculations. [40][41][42] B. Quasi-classical dynamics Classical dynamics is a very powerful tool for the kind of study we have carried out here.…”

Section: A the Dft Calculations And The Pes Representationmentioning

confidence: 99%

“…Detailed accounts of our six-dimensional (6D) PES for N 2 /Ru(0001) has been published elsewhere, [30,31] thus only a brief summary of the main characteristics is provided here.…”

Section: A the Dft Calculations And The Pes Representationmentioning

confidence: 99%

“…30 and 31, these theoretical results reproduce the surprisingly low dissociation probabilities [27,[50][51][52] found in the experiments. The results can be understood based on the very special characteristics of the N 2 /Ru(0001) PES: [28,30,31,51] The minimum barrier is very high, around 2.3 eV, and the PES displays high anisotropy and corrugation, i.e., small changes in the orientation and/or the position of the molecule gives rise to large changes in the potential energy (see Fig. 3 in Ref.…”

Section: A 6d Dynamics and The Vibrational Efficacymentioning

confidence: 99%

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A note on the vibrational efficacy in molecule-surface reactions

Dı́az¹,

Olsen²

2009

The Journal of Chemical Physics

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The effectiveness of vibrational energy in promoting dissociation of molecules colliding with surfaces can be measured through the so-called vibrational efficacy. It is by many thought to be a pure "energetic" measure and therefore believed to be limited from below by zero (in the case that there is no increase in dissociation probability upon vibrational excitation) and from above by one (in the case that all of the vibrational excitation energy is used to promote reaction).However, the quantity vibrational efficacy is clearly linked to the detailed dynamics of the system, and straightforward considerations lead to the conclusion that it is not limited either from below or above. Here we discuss these considerations together with a quasi-classical dynamics study of a molecule-surface system, N 2 /Ru(0001), for which a vibrational efficacy bigger than one has been found both experimentally and theoretically. We show that an analysis of the vibrational efficacy only in terms of energy transfer from vibration to translation can be too simple to describe the behavior of systems for which the potential energy surfaces present (high) reaction barriers, potential corrugation and anisotropy, and curved reaction paths.

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Section: A 6d Dynamics and The Vibrational Efficacymentioning

confidence: 66%

Section: A 6d Dynamics and The Vibrational Efficacymentioning

confidence: 91%

Section: A the Dft Calculations And The Pes Representationmentioning

confidence: 99%

“…Detailed accounts of our six-dimensional (6D) PES for N 2 /Ru(0001) has been published elsewhere, [30,31] thus only a brief summary of the main characteristics is provided here.…”

Section: A the Dft Calculations And The Pes Representationmentioning

confidence: 99%

Section: A 6d Dynamics and The Vibrational Efficacymentioning

confidence: 99%

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A note on the vibrational efficacy in molecule-surface reactions

Dı́az¹,

Olsen²

2009

The Journal of Chemical Physics

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References

2009

Multidimensional Quantum Dynamics

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Active Site Implantation for Ni(OH)₂ Nanowire Network Achieves Superior Hybrid Seawater Electrolysis at 1 A cm⁻² with Record‐Low Cell Voltage

Qian

et al. 2023

Adv Funct Materials

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Direct seawater electrolysis provides a grand blueprint for green hydrogen (H2) technology, while the high energy consumption has severely hindered its industrialization. Herein, a promising active site implantation strategy is reported for Ni(OH)2 nanowire network electrode on nickel foam substrate by Ru doping (denoted as RuNi(OH)2 NW2/NF), which can act as a dual‐function catalyst for hydrazine oxidation and hydrogen evolution, achieving an ultralow working potential of 114.6 mV to reach 1000 mA cm−2 and a small overpotential of 30 mV at 10 mA cm−2, respectively. Importantly, using the two‐electrode hydrazine oxidation assisted seawater electrolysis, it can drive a large current density of 500 mA cm−2 at 0.736 V with over 200 h stability. To demonstrate the practicability, a home‐made flow electrolyzer is constructed, which can realize the industry‐level rate of 1 A cm−2 with a record‐low voltage of 1.051 V. Theoretical calculations reveal that the Ru doping activates Ni(OH)2 by upgrading d‐band centers, which raises anti‐bonding energy states and thus strengthens the interaction between adsorbates and catalysts. This study not only provides a novel rationale for catalyst design, but also proposes a feasible strategy for direct alkaline seawater splitting toward sustainable, yet energy‐saving H2 production.

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Multidimensional Effects on Dissociation ofN2on Ru(0001)

Cited by 94 publications

References 28 publications

A note on the vibrational efficacy in molecule-surface reactions

A note on the vibrational efficacy in molecule-surface reactions

References

Active Site Implantation for Ni(OH)₂ Nanowire Network Achieves Superior Hybrid Seawater Electrolysis at 1 A cm⁻² with Record‐Low Cell Voltage

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Multidimensional Effects on Dissociation ofN2on Ru(0001)

Cited by 94 publications

References 28 publications

A note on the vibrational efficacy in molecule-surface reactions

A note on the vibrational efficacy in molecule-surface reactions

References

Active Site Implantation for Ni(OH)2 Nanowire Network Achieves Superior Hybrid Seawater Electrolysis at 1 A cm−2 with Record‐Low Cell Voltage

Contact Info

Product

Resources

About

Active Site Implantation for Ni(OH)₂ Nanowire Network Achieves Superior Hybrid Seawater Electrolysis at 1 A cm⁻² with Record‐Low Cell Voltage