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

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 inito molecular dynamic simulation 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 interface. Water destabilizes adsorbed H, decreasing the heat of adsorption by 19 – 22 kJ/mol(H₂), while inducing an additional entropy loss of 50 – 70 J/(mol(H₂)·K). Upon dissociative H₂ adsorption, the averaged distance of water from the Pt surface increases and it assumes a more ordered structure. In turn, the more ordered water layer limits the translation mobility of adsorbed H. In conclusion, the presence of hydrated hydronium ions next to Pt further reduces the H–Pt bond strength.

Authors:
 [1];  [2];  [1];  [1];  [2];  [2];  [2];  [1]
  1. Technische Univ. Munchen, Garching bei Munchen (Germany)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1487149
Alternate Identifier(s):
OSTI ID: 1492743
Report Number(s):
PNNL-SA-134839
Journal ID: ISSN 1433-7851
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 11; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; hydrogen; adsorption; water phase; platinum; hydrogen binding energy

Citation Formats

Yang, Guoju, Akhade, Sneha A., Chen, Xi, Liu, Yue, Lee, Mal -Soon, Glezakou, Vassiliki -Alexandra, Rousseau, Roger, and Lercher, Johannes A. Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase. United States: N. p., 2018. Web. doi:10.1002/anie.201813958.
Yang, Guoju, Akhade, Sneha A., Chen, Xi, Liu, Yue, Lee, Mal -Soon, Glezakou, Vassiliki -Alexandra, Rousseau, Roger, & Lercher, Johannes A. Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase. United States. doi:10.1002/anie.201813958.
Yang, Guoju, Akhade, Sneha A., Chen, Xi, Liu, Yue, Lee, Mal -Soon, Glezakou, Vassiliki -Alexandra, Rousseau, Roger, and Lercher, Johannes A. Mon . "Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase". United States. doi:10.1002/anie.201813958.
@article{osti_1487149,
title = {Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase},
author = {Yang, Guoju and Akhade, Sneha A. and Chen, Xi and Liu, Yue and Lee, Mal -Soon and Glezakou, Vassiliki -Alexandra and Rousseau, Roger and Lercher, Johannes A.},
abstractNote = {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 inito molecular dynamic simulation 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 interface. Water destabilizes adsorbed H, decreasing the heat of adsorption by 19 – 22 kJ/mol(H₂), while inducing an additional entropy loss of 50 – 70 J/(mol(H₂)·K). Upon dissociative H₂ adsorption, the averaged distance of water from the Pt surface increases and it assumes a more ordered structure. In turn, the more ordered water layer limits the translation mobility of adsorbed H. In conclusion, the presence of hydrated hydronium ions next to Pt further reduces the H–Pt bond strength.},
doi = {10.1002/anie.201813958},
journal = {Angewandte Chemie (International Edition)},
number = 11,
volume = 58,
place = {United States},
year = {2018},
month = {12}
}

Journal Article:
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Works referenced in this record:

Hydrogenolysis Goes Bio: From Carbohydrates and Sugar Alcohols to Platform Chemicals
journal, February 2012

  • Ruppert, Agnieszka M.; Weinberg, Kamil; Palkovits, Regina
  • Angewandte Chemie International Edition, Vol. 51, Issue 11, p. 2564-2601
  • DOI: 10.1002/anie.201105125

Just a Dream�or Future Reality?
journal, April 2009