The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase

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

Research output: Contribution to journalArticle

Abstract

The thermodynamic state of H2 adsorbed on Pt in the aqueous phase was determined by kinetic analysis of H2 reacting with D2O to HDO, HD, and D2, and by DFT-based ab initio molecular dynamics simulations of H2 adsorption on Pt(111), Pt(110), and Pt nanoparticles. Dissociative adsorption of H2 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 mol-1 H2 while inducing an additional entropy loss of 50–70 Jmol-1 H2K−1. Upon dissociative adsorption of H2, 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.

Original languageEnglish
JournalAngewandte Chemie - International Edition
DOIs
Publication statusPublished - Jan 1 2019

Fingerprint

Platinum
Hydrogen
Adsorption
Atoms
Water
Discrete Fourier transforms
Molecular dynamics
Entropy
Thermodynamics
Nanoparticles
Kinetics
Computer simulation
Ions
Liquids

Keywords

  • adsorption
  • hydrogen
  • hydrogen binding energy
  • platinum
  • water phase

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Yang, G., Akhade, S. A., Chen, X., Liu, Y., Lee, M. S., Glezakou, V. A., ... Lercher, J. A. (2019). The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase. Angewandte Chemie - International Edition. https://doi.org/10.1002/anie.201813958

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.

In: Angewandte Chemie - International Edition, 01.01.2019.

Research output: Contribution to journalArticle

Yang, Guoju ; Akhade, Sneha A. ; Chen, Xi ; Liu, Yue ; Lee, Mal Soon ; Glezakou, Vassiliki Alexandra ; Rousseau, Roger ; Lercher, Johannes A. / The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase. In: Angewandte Chemie - International Edition. 2019.
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