The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase

Yang, Guoju; Akhade, Sneha A.; Chen, Xi; Liu, Yue; Lee, Mal‐Soon; Glezakou, Vassiliki‐Alexandra; Rousseau, Roger; Lercher, Johannes A.

doi:10.1002/ange.201813958

Title: The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase

Journal Article · 29 January 2019 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.201813958 · OSTI ID:1492741

Yang, Guoju ^[1];

^[2]; Chen, Xi ^[3];

^[3];

^[2];

^[4]

Department of Chemistry and Catalysis Research Center Technische Universität München Lichtenbergstrasse 4 85747 Garching Germany, College of Chemistry and International Center of Future Science Jilin University Qianjin Str. 2699 130012 Changchun P. R. China
Institute for Integrated Catalysis Pacific Northwest National Laboratory P.O. Box 999 Richland WA 99352 USA
Department of Chemistry and Catalysis Research Center Technische Universität München Lichtenbergstrasse 4 85747 Garching Germany
Department of Chemistry and Catalysis Research Center Technische Universität München Lichtenbergstrasse 4 85747 Garching Germany, Institute for Integrated Catalysis Pacific Northwest National Laboratory P.O. Box 999 Richland WA 99352 USA

Abstract The thermodynamic state of H ₂ adsorbed on Pt in the aqueous phase was determined by kinetic analysis of H ₂ reacting with D ₂ O to HDO, HD, and D ₂ , and by DFT‐based ab initio molecular dynamics simulations of H ₂ adsorption on Pt(111), Pt(110), and Pt nanoparticles. Dissociative adsorption of H ₂ on Pt is significantly weakened in the aqueous phase compared to adsorption at gas–solid interfaces. Water destabilizes the adsorbed H atoms, decreasing the heat of adsorption by 19–22 kJ while inducing an additional entropy loss of 50–70 J K ⁻¹ . Upon dissociative adsorption of H ₂ , the average distance of water from the Pt surface increases and the liquid adopts a structure that is more ordered than before close to the Pt surface, which limits the translation mobility of the adsorbed H atoms. The presence of hydrated hydronium ions next to the Pt surface further lowers the H−Pt bond strength.

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Sponsoring Organization:: USDOE

OSTI ID:: 1492741

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 11 Vol. 131; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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