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

doi:10.1002/anie.201813958

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

Chair of Chemical Technology II

Technical University of Munich
Jilin University
Pacific Northwest National Laboratory

Research output: Contribution to journal › Article › peer-review

88 Scopus citations

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 (Formula presented.) while inducing an additional entropy loss of 50–70 J (Formula presented.) K⁻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 language	English
Pages (from-to)	3527-3532
Number of pages	6
Journal	Angewandte Chemie - International Edition
Volume	58
Issue number	11
DOIs	https://doi.org/10.1002/anie.201813958
State	Published - 11 Mar 2019

Keywords

adsorption
hydrogen
hydrogen binding energy
platinum
water phase

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10.1002/anie.201813958

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title = "The 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 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{\textendash}solid interfaces. Water destabilizes the adsorbed H atoms, decreasing the heat of adsorption by 19{\textendash}22 kJ (Formula presented.) while inducing an additional entropy loss of 50{\textendash}70 J (Formula presented.) K−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.",

keywords = "adsorption, hydrogen, hydrogen binding energy, platinum, water phase",

author = "Guoju Yang and Akhade, \{Sneha A.\} and Xi Chen and Yue Liu and Lee, \{Mal Soon\} and Glezakou, \{Vassiliki Alexandra\} and Roger Rousseau and Lercher, \{Johannes A.\}",

note = "Publisher Copyright: {\textcopyright} 2019 Wiley-VCH Verlag GmbH \& Co. KGaA, Weinheim",

year = "2019",

month = mar,

day = "11",

doi = "10.1002/anie.201813958",

language = "English",

volume = "58",

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journal = "Angewandte Chemie - International Edition",

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TY - JOUR

T1 - The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase

AU - Yang, Guoju

AU - Akhade, Sneha A.

AU - Chen, Xi

AU - Liu, Yue

AU - Lee, Mal Soon

AU - Glezakou, Vassiliki Alexandra

AU - Rousseau, Roger

AU - Lercher, Johannes A.

PY - 2019/3/11

Y1 - 2019/3/11

N2 - 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 (Formula presented.) while inducing an additional entropy loss of 50–70 J (Formula presented.) K−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.

AB - 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 (Formula presented.) while inducing an additional entropy loss of 50–70 J (Formula presented.) K−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.

KW - adsorption

KW - hydrogen

KW - hydrogen binding energy

KW - platinum

KW - water phase

UR - https://www.scopus.com/pages/publications/85060807109

U2 - 10.1002/anie.201813958

DO - 10.1002/anie.201813958

M3 - Article

C2 - 30556940

AN - SCOPUS:85060807109

SN - 1433-7851

VL - 58

SP - 3527

EP - 3532

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 11

ER -

The Nature of Hydrogen Adsorption on Platinum in the Aqueous Phase

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