Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis
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Details
| Original language | English |
|---|---|
| Article number | e26198 |
| Journal | International Journal of Quantum Chemistry |
| Volume | 120 |
| Issue number | 11 |
| DOIs | |
| Publication status | Published - 5 Jun 2020 |
| Publication type | A1 Journal article-refereed |
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.
ASJC Scopus subject areas
Keywords
- heterogeneous catalysis, low activation barrier, metal surface, quantum Monte Carlo calculation