Thermodynamic stability of Pd–Ru alloy nanoparticles: combination of density functional theory calculations, supervised learning, and Wang–Landau sampling

Koyama, Michihisa

doi:10.1039/d2cp01848a

Cited by 7 publications

(4 citation statements)

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“…In the Pd-or Ru-rich conditions, the alloy tends to be more stable. The results calculated by PFP in this work is in good agreement with previous work using DFT [21].…”

Section: Excess Energysupporting

confidence: 91%

“…The lowest is for Pd64Ru192 (about 1300K) and the highest is for Pd192Ru64 (3400 K). In the case of Pd128Ru128, the transition temperature is about 2400 K. Comparing these values with the results of previous work in which the total energy was calculated using supervised learning [21], it was found that the transition temperatures for the three compounds in this study are higher.…”

Section: Thermodynamic Propertiessupporting

confidence: 77%

“…In (b), (c), and (d), the specific heat calculated from each selectedDoS segment is compared to that calculated from full DoS. Full DoS data was taken from ref[21]. with some extrapolation to the high temperature range.…”

mentioning

confidence: 99%

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On the Thermodynamic Stability of Alloys: Combination of Neural Network Potential and Wang-Landau Sampling

KOYAMA

2022

J. Comput. Chem. Jpn.

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Thermodynamic properties and atomic configuration of PdRu alloy were investigated using Wang-Landau Monte Carlo method in combination with a newly-developed universal neural network potential. by using this new potential, excess energy of PdRu alloy was calculated. It is found that PdRu alloy in FCC lattice is unstable in the full range of alloy composition. This agrees with previous study based on density functional theory. The combined method was able to determine the configurational density of states, from which thermodynamic properties of the alloy were derived. It is found that when temperature increases, the excess free energy of the alloy is reduced, increasing the possibility of alloy mixing. Depending on the composition, transition peaks appear at finite temperatures where there are changes of preferable atomic arrangement due to the effect of temperature via the configurational entropy.In addition, the analyses on short-range order parameter and bond fraction show that PdRu alloy prefers to be in segregated form, where Pd and Ru are immiscible at low temperature, consistent with the experimental observations. The random mixing of Pd and Ru atoms in the form of solid-solution can occur at high temperature.

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“…In the Pd-or Ru-rich conditions, the alloy tends to be more stable. The results calculated by PFP in this work is in good agreement with previous work using DFT [21].…”

Section: Excess Energysupporting

confidence: 91%

Section: Thermodynamic Propertiessupporting

confidence: 77%

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On the Thermodynamic Stability of Alloys: Combination of Neural Network Potential and Wang-Landau Sampling

KOYAMA

2022

J. Comput. Chem. Jpn.

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“…Considering the small size and the interaction with the silica support, the trends in selectivity and thermal stability may be influenced by the nanosizing and support effects. To obtain the insights closer into the real HEI/SiO 2 catalyst, more sophisticated theoretical studies based on a supported nanoparticle model are preferred. − Although modeling and studying such a complex system are highly challenging, success in this approach will advance the chemistry of HEI-based catalysis.…”

Section: Resultsmentioning

confidence: 99%

High-Entropy Intermetallics Serve Ultrastable Single-Atom Pt for Propane Dehydrogenation

et al. 2022

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Propane dehydrogenation has been a promising propylene production process that can compensate for the increasing global demand for propylene. However, Pt-based catalysts with high stability at ≥600 °C have barely been reported because the catalysts typically result in short catalyst life owing to side reactions and coke formation. Herein, we report a new class of heterogeneous catalysts using high-entropy intermetallics (HEIs). Pt−Pt ensembles, which cause side reactions, are entirely diluted by the component inert metals in PtGe-type HEIs. The resultant HEI (PtCoCu) (GeGaSn)/Ca−SiO 2 exhibited an outstandingly high catalytic stability, even at 600 °C (k d −1 = τ = 4146 h = 173 d), and almost no deactivation of the catalyst was observed for 2 months for the first time. Detailed experimental studies and theoretical calculations demonstrated that the combination of the site-isolation and entropy effects upon multimetallization of PtGe drastically enhanced the desorption of propylene and the thermal stability, eventually suppressing the side reactions even at high reaction temperatures.

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Machine Learning-Based Approaches in Nanoparticle Catalysis

Huerta

Hisama

Koyama

2024

Comprehensive Computational Chemistry

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Thermodynamic stability of Pd–Ru alloy nanoparticles: combination of density functional theory calculations, supervised learning, and Wang–Landau sampling

Abstract: Solid-solution alloy nanoparticles (NPs) comprising Pd and Ru, which are immiscible in the bulk state, have been synthesised and show excellent catalytic performance. To date, most studies have evaluated the...

Cited by 7 publications

References 50 publications

On the Thermodynamic Stability of Alloys: Combination of Neural Network Potential and Wang-Landau Sampling

On the Thermodynamic Stability of Alloys: Combination of Neural Network Potential and Wang-Landau Sampling

High-Entropy Intermetallics Serve Ultrastable Single-Atom Pt for Propane Dehydrogenation

Machine Learning-Based Approaches in Nanoparticle Catalysis

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