Temperature- and pressure-dependent adsorption configuration of NO molecules on Rh(111) surface: A theoretical study

Takahiro Hirai; Masaki Okoshi; Atsushi Ishikawa; Hiromi Nakai

doi:10.1016/j.susc.2019.04.004

Temperature- and pressure-dependent adsorption configuration of NO molecules on Rh(111) surface: A theoretical study

Takahiro Hirai, Masaki Okoshi, Atsushi Ishikawa, Hiromi Nakai^*

^*Corresponding author for this work

School of Advanced Science and Engineering

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

4 Citations (Scopus)

Abstract

Understanding the behavior of NO molecules on Rh metal surfaces is necessary for gaining fundamental knowledge about catalytic chemistry and surface science. The present theoretical study details the configuration of NO molecules adsorbed on Rh(111) surface on the basis of density functional theory (DFT) calculations. The impact of coverage dependences on the adsorption/desorption energies is examined systematically: multiple configurations of NO adsorption structures are investigated with NO surface coverage from 0.06 to 0.75. A phase diagram for the various NO configurations with temperature and pressure is obtained by considering the adsorption equilibrium. Adsorption energies of NO molecules generally decrease with increasing surface coverage, reflecting the repulsive interactions between the adsorbed NO molecules. Microkinetic simulations for temperature-programmed desorption (TPD) spectra are performed. Simulated TPD spectra on the basis of the surface coverage-dependent desorption energies are in reasonable agreement with the experimental results.

Original language	English
Pages (from-to)	58-62
Number of pages	5
Journal	Surface Science
Volume	686
DOIs	https://doi.org/10.1016/j.susc.2019.04.004
Publication status	Published - 2019 Aug

Keywords

Adsorption equilibrium
DFT (density functional theory)
NO (nitric oxide)
Phase diagram
Rh (rhodium)
TPD (temperature-programmed desorption)

ASJC Scopus subject areas

Condensed Matter Physics
Surfaces and Interfaces
Surfaces, Coatings and Films
Materials Chemistry

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10.1016/j.susc.2019.04.004

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title = "Temperature- and pressure-dependent adsorption configuration of NO molecules on Rh(111) surface: A theoretical study",

abstract = "Understanding the behavior of NO molecules on Rh metal surfaces is necessary for gaining fundamental knowledge about catalytic chemistry and surface science. The present theoretical study details the configuration of NO molecules adsorbed on Rh(111) surface on the basis of density functional theory (DFT) calculations. The impact of coverage dependences on the adsorption/desorption energies is examined systematically: multiple configurations of NO adsorption structures are investigated with NO surface coverage from 0.06 to 0.75. A phase diagram for the various NO configurations with temperature and pressure is obtained by considering the adsorption equilibrium. Adsorption energies of NO molecules generally decrease with increasing surface coverage, reflecting the repulsive interactions between the adsorbed NO molecules. Microkinetic simulations for temperature-programmed desorption (TPD) spectra are performed. Simulated TPD spectra on the basis of the surface coverage-dependent desorption energies are in reasonable agreement with the experimental results.",

keywords = "Adsorption equilibrium, DFT (density functional theory), NO (nitric oxide), Phase diagram, Rh (rhodium), TPD (temperature-programmed desorption)",

author = "Takahiro Hirai and Masaki Okoshi and Atsushi Ishikawa and Hiromi Nakai",

note = "Funding Information: Some of the present calculations were performed at the Research Center for Computational Science (RCCS), Okazaki Research Facilities, National Institutes of Natural Sciences (NINS), and the Institute for Solid State Physics (ISSP), the University of Tokyo. This study was supported in part by the “Elements Strategy Initiative for Catalysts & Batteries (ESICB)” project supported by the Ministry of Education, Culture, Sports, Science, and Technology (MEXT), Japan. Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",

year = "2019",

month = aug,

doi = "10.1016/j.susc.2019.04.004",

language = "English",

volume = "686",

pages = "58--62",

journal = "Surface Science",

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T2 - A theoretical study

AU - Hirai, Takahiro

AU - Okoshi, Masaki

AU - Ishikawa, Atsushi

AU - Nakai, Hiromi

N1 - Funding Information: Some of the present calculations were performed at the Research Center for Computational Science (RCCS), Okazaki Research Facilities, National Institutes of Natural Sciences (NINS), and the Institute for Solid State Physics (ISSP), the University of Tokyo. This study was supported in part by the “Elements Strategy Initiative for Catalysts & Batteries (ESICB)” project supported by the Ministry of Education, Culture, Sports, Science, and Technology (MEXT), Japan. Publisher Copyright: © 2019 Elsevier B.V.

PY - 2019/8

Y1 - 2019/8

N2 - Understanding the behavior of NO molecules on Rh metal surfaces is necessary for gaining fundamental knowledge about catalytic chemistry and surface science. The present theoretical study details the configuration of NO molecules adsorbed on Rh(111) surface on the basis of density functional theory (DFT) calculations. The impact of coverage dependences on the adsorption/desorption energies is examined systematically: multiple configurations of NO adsorption structures are investigated with NO surface coverage from 0.06 to 0.75. A phase diagram for the various NO configurations with temperature and pressure is obtained by considering the adsorption equilibrium. Adsorption energies of NO molecules generally decrease with increasing surface coverage, reflecting the repulsive interactions between the adsorbed NO molecules. Microkinetic simulations for temperature-programmed desorption (TPD) spectra are performed. Simulated TPD spectra on the basis of the surface coverage-dependent desorption energies are in reasonable agreement with the experimental results.

AB - Understanding the behavior of NO molecules on Rh metal surfaces is necessary for gaining fundamental knowledge about catalytic chemistry and surface science. The present theoretical study details the configuration of NO molecules adsorbed on Rh(111) surface on the basis of density functional theory (DFT) calculations. The impact of coverage dependences on the adsorption/desorption energies is examined systematically: multiple configurations of NO adsorption structures are investigated with NO surface coverage from 0.06 to 0.75. A phase diagram for the various NO configurations with temperature and pressure is obtained by considering the adsorption equilibrium. Adsorption energies of NO molecules generally decrease with increasing surface coverage, reflecting the repulsive interactions between the adsorbed NO molecules. Microkinetic simulations for temperature-programmed desorption (TPD) spectra are performed. Simulated TPD spectra on the basis of the surface coverage-dependent desorption energies are in reasonable agreement with the experimental results.

KW - Adsorption equilibrium

KW - DFT (density functional theory)

KW - NO (nitric oxide)

KW - Phase diagram

KW - Rh (rhodium)

KW - TPD (temperature-programmed desorption)

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JO - Surface Science

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ER -

Temperature- and pressure-dependent adsorption configuration of NO molecules on Rh(111) surface: A theoretical study

Abstract

Keywords

ASJC Scopus subject areas

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