Conversion of CO2and C2H6to propanoic acid on an iridium-modified graphene oxide surface: Quantum-chemical investigation

Chih Chun Chen, Chen Hao Yeh, Chun Chih Chang, Jia-Jen Ho

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

Using density-functional theory, we performed calculations on a single-atom catalyst (SAC) comprising an iridium atom on a modi fied graphene oxide (Ir1-GO) surface to investigate the conversion of CO2 and C2H6 molecules to propanoic acid. The great catalytic activity of this surface is due to the strong adsorption of C2H6 and CO2 (-0.92 and -0.56 eV adsorption energies, respectively). First, C2H6 is dehydrogenated at an oxide site of the surface to form C2H5 + OH with a barrier of height 0.63 eV; the adsorbed CO2 then reacts with ethyl to form C2H5COO or COOC2H5 with barriers of 0.95 and 1.70 eV, respectively. Less likely, the adsorbed CO2 might be hydrogenated by hydroxyl to form HCOO or COOH, with energy barriers of 1.34 and 1.49 eV, respectively. We predict that the most likely path for the conversion of the adsorbed CO2 and ethane molecules on the Ir1-graphene oxide surface would involve the formation of propanoic acid (C2H5COOH). To understand the interaction between adsorbates and surfaces, we calculated and analyzed the local densities of states (LDOS) and the electron localization function (ELF).

Original languageEnglish
Pages (from-to)1539-1546
Number of pages8
JournalIndustrial and Engineering Chemistry Research
Volume54
Issue number5
DOIs
Publication statusPublished - 2015 Jan 1

Fingerprint

Iridium
Graphite
Oxides
Graphene
Acids
Adsorption
Atoms
Molecules
Ethane
Energy barriers
Adsorbates
Hydroxyl Radical
Density functional theory
Catalyst activity
propionic acid
Catalysts
Electrons

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Chemistry(all)
  • Industrial and Manufacturing Engineering

Cite this

Conversion of CO2and C2H6to propanoic acid on an iridium-modified graphene oxide surface : Quantum-chemical investigation. / Chen, Chih Chun; Yeh, Chen Hao; Chang, Chun Chih; Ho, Jia-Jen.

In: Industrial and Engineering Chemistry Research, Vol. 54, No. 5, 01.01.2015, p. 1539-1546.

Research output: Contribution to journalArticle

@article{a5c4886a8412462a852c07705024c6df,
title = "Conversion of CO2and C2H6to propanoic acid on an iridium-modified graphene oxide surface: Quantum-chemical investigation",
abstract = "Using density-functional theory, we performed calculations on a single-atom catalyst (SAC) comprising an iridium atom on a modi fied graphene oxide (Ir1-GO) surface to investigate the conversion of CO2 and C2H6 molecules to propanoic acid. The great catalytic activity of this surface is due to the strong adsorption of C2H6 and CO2 (-0.92 and -0.56 eV adsorption energies, respectively). First, C2H6 is dehydrogenated at an oxide site of the surface to form C2H5 + OH with a barrier of height 0.63 eV; the adsorbed CO2 then reacts with ethyl to form C2H5COO or COOC2H5 with barriers of 0.95 and 1.70 eV, respectively. Less likely, the adsorbed CO2 might be hydrogenated by hydroxyl to form HCOO or COOH, with energy barriers of 1.34 and 1.49 eV, respectively. We predict that the most likely path for the conversion of the adsorbed CO2 and ethane molecules on the Ir1-graphene oxide surface would involve the formation of propanoic acid (C2H5COOH). To understand the interaction between adsorbates and surfaces, we calculated and analyzed the local densities of states (LDOS) and the electron localization function (ELF).",
author = "Chen, {Chih Chun} and Yeh, {Chen Hao} and Chang, {Chun Chih} and Jia-Jen Ho",
year = "2015",
month = "1",
day = "1",
doi = "10.1021/ie503982t",
language = "English",
volume = "54",
pages = "1539--1546",
journal = "Industrial & Engineering Chemistry Research",
issn = "0888-5885",
publisher = "American Chemical Society",
number = "5",

}

TY - JOUR

T1 - Conversion of CO2and C2H6to propanoic acid on an iridium-modified graphene oxide surface

T2 - Quantum-chemical investigation

AU - Chen, Chih Chun

AU - Yeh, Chen Hao

AU - Chang, Chun Chih

AU - Ho, Jia-Jen

PY - 2015/1/1

Y1 - 2015/1/1

N2 - Using density-functional theory, we performed calculations on a single-atom catalyst (SAC) comprising an iridium atom on a modi fied graphene oxide (Ir1-GO) surface to investigate the conversion of CO2 and C2H6 molecules to propanoic acid. The great catalytic activity of this surface is due to the strong adsorption of C2H6 and CO2 (-0.92 and -0.56 eV adsorption energies, respectively). First, C2H6 is dehydrogenated at an oxide site of the surface to form C2H5 + OH with a barrier of height 0.63 eV; the adsorbed CO2 then reacts with ethyl to form C2H5COO or COOC2H5 with barriers of 0.95 and 1.70 eV, respectively. Less likely, the adsorbed CO2 might be hydrogenated by hydroxyl to form HCOO or COOH, with energy barriers of 1.34 and 1.49 eV, respectively. We predict that the most likely path for the conversion of the adsorbed CO2 and ethane molecules on the Ir1-graphene oxide surface would involve the formation of propanoic acid (C2H5COOH). To understand the interaction between adsorbates and surfaces, we calculated and analyzed the local densities of states (LDOS) and the electron localization function (ELF).

AB - Using density-functional theory, we performed calculations on a single-atom catalyst (SAC) comprising an iridium atom on a modi fied graphene oxide (Ir1-GO) surface to investigate the conversion of CO2 and C2H6 molecules to propanoic acid. The great catalytic activity of this surface is due to the strong adsorption of C2H6 and CO2 (-0.92 and -0.56 eV adsorption energies, respectively). First, C2H6 is dehydrogenated at an oxide site of the surface to form C2H5 + OH with a barrier of height 0.63 eV; the adsorbed CO2 then reacts with ethyl to form C2H5COO or COOC2H5 with barriers of 0.95 and 1.70 eV, respectively. Less likely, the adsorbed CO2 might be hydrogenated by hydroxyl to form HCOO or COOH, with energy barriers of 1.34 and 1.49 eV, respectively. We predict that the most likely path for the conversion of the adsorbed CO2 and ethane molecules on the Ir1-graphene oxide surface would involve the formation of propanoic acid (C2H5COOH). To understand the interaction between adsorbates and surfaces, we calculated and analyzed the local densities of states (LDOS) and the electron localization function (ELF).

UR - http://www.scopus.com/inward/record.url?scp=84922976074&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84922976074&partnerID=8YFLogxK

U2 - 10.1021/ie503982t

DO - 10.1021/ie503982t

M3 - Article

AN - SCOPUS:84922976074

VL - 54

SP - 1539

EP - 1546

JO - Industrial & Engineering Chemistry Research

JF - Industrial & Engineering Chemistry Research

SN - 0888-5885

IS - 5

ER -