Combined experimental and density functional theory (DFT) studies on the catalyst design for the oxidative coupling of methane

Seoyeon Lim, Jae Wook Choi, Dong Jin Suh, Kwang Ho Song, Hyung Chul Ham, Jeong Myeong Ha

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Catalytic descriptors were studied to design optimum catalysts for the oxidative coupling of methane (OCM) by combining density functional theory (DFT) calculations and actual reaction experiments. SrTiO3 perovskite catalysts, selected for OCM, were modified using metal dopants, and their electronic structures were calculated using the DFT method. The CH3 adsorption energy Eads(CH3) and the oxygen vacancy formation energy Ef(vac) exhibited volcano-type correlations with the C2+ selectivity and O2-consumption for the formation of COx, respectively. The optimum catalytic activity, represented by the C2+ selectivity, was obtained for Eads(CH3) = −2.0 to −1.5 eV, indicating that overly strong adsorption of methyl radicals (or easily dissociated C[sbnd]H bonds of methane) and relatively insufficient oxygen supplementation to the catalyst surface improve deep oxidation to CO and CO2. Praseodymium (Pr)- and neodymium (Nd)-doped SrTiO3 catalysts confirm the DFT-predicted optimum electronic structure of the OCM catalysts.

Original languageEnglish
Pages (from-to)478-492
Number of pages15
JournalJournal of Catalysis
Volume375
DOIs
Publication statusPublished - 2019 Jul 1

Fingerprint

Methane
Density functional theory
methane
density functional theory
catalysts
Catalysts
Electronic structure
Praseodymium
selectivity
electronic structure
Neodymium
Adsorption
Volcanoes
adsorption
praseodymium
Catalyst selectivity
neodymium
oxygen
energy of formation
Oxygen vacancies

Keywords

  • Density functional theory
  • Methyl radical adsorption
  • Oxidative coupling of methane
  • Perovskite

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

Combined experimental and density functional theory (DFT) studies on the catalyst design for the oxidative coupling of methane. / Lim, Seoyeon; Choi, Jae Wook; Suh, Dong Jin; Song, Kwang Ho; Ham, Hyung Chul; Ha, Jeong Myeong.

In: Journal of Catalysis, Vol. 375, 01.07.2019, p. 478-492.

Research output: Contribution to journalArticle

Lim, Seoyeon ; Choi, Jae Wook ; Suh, Dong Jin ; Song, Kwang Ho ; Ham, Hyung Chul ; Ha, Jeong Myeong. / Combined experimental and density functional theory (DFT) studies on the catalyst design for the oxidative coupling of methane. In: Journal of Catalysis. 2019 ; Vol. 375. pp. 478-492.
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AU - Ha, Jeong Myeong

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