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author:

Gu, Kaixuan (Gu, Kaixuan.) [1] | Lin, Sen (Lin, Sen.) [2] (Scholars:林森)

Indexed by:

EI Scopus SCIE

Abstract:

Hydrogen spillover, involving the surface migration of dissociated hydrogen atoms from active metal sites to the relatively inert catalyst support, plays a crucial role in hydrogen-involved catalytic processes. However, a comprehensive understanding of how H atoms are driven to spill over from active sites onto the catalyst support is still lacking. Here, we examine the atomic-scale perspective of the H spillover process on a Pt/Cu(111) single atom alloy surface using machine-learning accelerated molecular dynamics calculations based on density functional theory. Our results show that when an impinging H2 dissociates at an active Pt site, the Pt atom undergoes deactivation due to the dissociated hydrogen atoms that attach to it. Interestingly, collisions between H2 and sticking H atoms facilitate H spillover onto the host Cu, leading to the reactivation of the Pt atom and the realization of a continuous H spillover process. This work underscores the importance of the interaction between gas molecules and adsorbates as a driving force in elucidating chemical processes under a gaseous atmosphere, which has so far been underappreciated in thermodynamic studies. Collisions between H2 and adsorbed H atoms at the Pt site play a pivotal role in promoting hydrogen spillover, underscoring the importance of the interaction between gas molecules and adsorbates in elucidating chemical processes under a gas atmosphere.image

Keyword:

Gas-Phase Reactions H Spillover Hydrogen Molecular Dynamics Potential Energy Surface

Community:

  • [ 1 ] [Gu, Kaixuan]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350002, Peoples R China
  • [ 2 ] [Lin, Sen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350002, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

ISSN: 1433-7851

Year: 2023

Issue: 47

Volume: 62

1 6 . 1

JCR@2023

1 6 . 1 0 0

JCR@2023

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 1

SCOPUS Cited Count: 2

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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