DFT Insights into Comparative Hydrogen Adsorption and Hydrogen Spillover Mechanisms of Pt<sub>4</sub>/Graphene and Pt<sub>4</sub>/Anatase (101) Surfaces



Sihag, Amita, Xie, Zong-Lun, Ho, Viet Thang, Kuo, Chin-Lung, Tseng, Fan-Gang, Dyer, Matthew Stephen ORCID: 0000-0002-4923-3003 and Chen, Hsin-Yi Tiffany
(2019) DFT Insights into Comparative Hydrogen Adsorption and Hydrogen Spillover Mechanisms of Pt<sub>4</sub>/Graphene and Pt<sub>4</sub>/Anatase (101) Surfaces. JOURNAL OF PHYSICAL CHEMISTRY C, 123 (42). pp. 25618-25627.

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Abstract

A comparative study of the hydrogen spillover phenomenon on pristine graphene and anatase (101)-supported Pt4 catalysts has been carried out by using density functional theory with Hubbard correction (DFT + U) and dispersion correction (Grimme-D3). The adsorption of the H2 molecule causes no dissociation on graphene but dissociation with nearly zero adsorption energy on anatase (101). This emphasizes the need for a metal catalyst for H2 dissociation to aid the stronger chemisorption of hydrogen atoms or protons on the substrate. The metal-support interaction is different for both substrates as Pt4 shows p-type doping for graphene and n-type doping for anatase (101) surfaces with binding energies of-2.16 and-5.82 eV, respectively. The differing nature of H2 adsorption and metal-support interactions lead to different hydrogen spillover phenomena for the two supports. Hydrogen spillover is unlikely to occur on Pt4/graphene even at high hydrogen coverage (24H atoms per Pt4) but has a tendency to take place on anatase (101) at medium hydrogen coverage (10H atoms per Pt4) from the perspectives of both thermodynamics and kinetics.

Item Type: Article
Uncontrolled Keywords: 7 Affordable and Clean Energy
Depositing User: Symplectic Admin
Date Deposited: 22 Oct 2020 08:24
Last Modified: 15 Mar 2024 06:21
DOI: 10.1021/acs.jpcc.9b04419
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URI: https://livrepository.liverpool.ac.uk/id/eprint/3104808