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Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis

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Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis. / Sharma, Rajesh O.; Rantala, Tapio T.; Hoggan, Philip E.

In: International Journal of Quantum Chemistry, Vol. 120, No. 11, e26198, 05.06.2020.

Research output: Contribution to journalArticleScientificpeer-review

Harvard

Sharma, RO, Rantala, TT & Hoggan, PE 2020, 'Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis', International Journal of Quantum Chemistry, vol. 120, no. 11, e26198. https://doi.org/10.1002/qua.26198

APA

Sharma, R. O., Rantala, T. T., & Hoggan, P. E. (2020). Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis. International Journal of Quantum Chemistry, 120(11), [e26198]. https://doi.org/10.1002/qua.26198

Vancouver

Author

Sharma, Rajesh O. ; Rantala, Tapio T. ; Hoggan, Philip E. / Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis. In: International Journal of Quantum Chemistry. 2020 ; Vol. 120, No. 11.

Bibtex - Download

@article{ebdcde7e17314a279cd81434e2c96477,
title = "Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis",
abstract = "This rapid communication gives the salient points and results of the theoretical investigation of a chemical reaction for efficient selective hydrogen production. The clean fuel produced is a sustainable energy source. Accurate methods based on quantum theory are used because the changing electronic structure is a probe that monitors reactions. The reaction between water and carbon monoxide is used industrially with metal catalysts, usually platinum. There is a considerable economic and environmental challenge underpinning this fundamental investigation where bond dissociation plays an essential role. A bond dissociation process is often the limiting step of reaction rates for industrial catalysis. Most mainstream quantum approaches fail to a greater or lesser degree in the description of this process. The present work advocates a promising alternative: the initial analysis of statistical data generated by the Quantum Monte Carlo (QMC) method demonstrated very stringent statistical accuracy for essential information on hydrogen production via the water-gas shift reaction with platinum catalyst. The transition state structure is obtained from QMC force constants and illustrated here. It corresponds to water OH-stretch concerted with Pt-H bond formation, whilst the OH oxygen atom begins to interact with the CO carbon. The present QMC evaluation of the corresponding activation barrier is low: 17.0 ± 0.2 kcal/mol. It is close to the experimental apparent activation energy of 17.05 kcal/mol. This method is applicable to a wide range of similar systems.",
keywords = "heterogeneous catalysis, low activation barrier, metal surface, quantum Monte Carlo calculation",
author = "Sharma, {Rajesh O.} and Rantala, {Tapio T.} and Hoggan, {Philip E.}",
year = "2020",
month = "6",
day = "5",
doi = "10.1002/qua.26198",
language = "English",
volume = "120",
journal = "International Journal of Quantum Chemistry",
issn = "0020-7608",
publisher = "Wiley",
number = "11",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis

AU - Sharma, Rajesh O.

AU - Rantala, Tapio T.

AU - Hoggan, Philip E.

PY - 2020/6/5

Y1 - 2020/6/5

N2 - This rapid communication gives the salient points and results of the theoretical investigation of a chemical reaction for efficient selective hydrogen production. The clean fuel produced is a sustainable energy source. Accurate methods based on quantum theory are used because the changing electronic structure is a probe that monitors reactions. The reaction between water and carbon monoxide is used industrially with metal catalysts, usually platinum. There is a considerable economic and environmental challenge underpinning this fundamental investigation where bond dissociation plays an essential role. A bond dissociation process is often the limiting step of reaction rates for industrial catalysis. Most mainstream quantum approaches fail to a greater or lesser degree in the description of this process. The present work advocates a promising alternative: the initial analysis of statistical data generated by the Quantum Monte Carlo (QMC) method demonstrated very stringent statistical accuracy for essential information on hydrogen production via the water-gas shift reaction with platinum catalyst. The transition state structure is obtained from QMC force constants and illustrated here. It corresponds to water OH-stretch concerted with Pt-H bond formation, whilst the OH oxygen atom begins to interact with the CO carbon. The present QMC evaluation of the corresponding activation barrier is low: 17.0 ± 0.2 kcal/mol. It is close to the experimental apparent activation energy of 17.05 kcal/mol. This method is applicable to a wide range of similar systems.

AB - This rapid communication gives the salient points and results of the theoretical investigation of a chemical reaction for efficient selective hydrogen production. The clean fuel produced is a sustainable energy source. Accurate methods based on quantum theory are used because the changing electronic structure is a probe that monitors reactions. The reaction between water and carbon monoxide is used industrially with metal catalysts, usually platinum. There is a considerable economic and environmental challenge underpinning this fundamental investigation where bond dissociation plays an essential role. A bond dissociation process is often the limiting step of reaction rates for industrial catalysis. Most mainstream quantum approaches fail to a greater or lesser degree in the description of this process. The present work advocates a promising alternative: the initial analysis of statistical data generated by the Quantum Monte Carlo (QMC) method demonstrated very stringent statistical accuracy for essential information on hydrogen production via the water-gas shift reaction with platinum catalyst. The transition state structure is obtained from QMC force constants and illustrated here. It corresponds to water OH-stretch concerted with Pt-H bond formation, whilst the OH oxygen atom begins to interact with the CO carbon. The present QMC evaluation of the corresponding activation barrier is low: 17.0 ± 0.2 kcal/mol. It is close to the experimental apparent activation energy of 17.05 kcal/mol. This method is applicable to a wide range of similar systems.

KW - heterogeneous catalysis

KW - low activation barrier

KW - metal surface

KW - quantum Monte Carlo calculation

U2 - 10.1002/qua.26198

DO - 10.1002/qua.26198

M3 - Article

VL - 120

JO - International Journal of Quantum Chemistry

JF - International Journal of Quantum Chemistry

SN - 0020-7608

IS - 11

M1 - e26198

ER -