Isothermal Reduction of IrO2 (110) Films by Methane Investigated Using In Situ X-ray Photoelectron Spectroscopy

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Isothermal Reduction of IrO2 (110) Films by Methane Investigated Using In Situ X-ray Photoelectron Spectroscopy

Martin, Rachel (author): Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA.,University of Florida

Kim, Minkyu (author): Yeungnam Univ, Sch Chem Engn, Gyongsan 38541, South Korea.,Yeungnam University

Lee, Christopher J. (author): Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA.,University of Florida

Mehar, Vikram (author): Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA.,University of Florida

Albertin, Stefano (author): Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH

Hejral, Uta (author): Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH

Merte, Lindsay R. (author): Malmö University,Malmö universitet,Institutionen för materialvetenskap och tillämpad matematik (MTM)

Asthagiri, Aravind (author): Ohio State Univ, William G Lowrie Chem & Biomol Engn, Columbus, OH 43210 USA.,Ohio State University

Weaver, Jason F. (author): Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA.,University of Florida

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Univ Florida, Dept Chem Engn, Gainesville, FL 32611 USA University of Florida (creator_code:org_t)

2021-04-09
2021
English.
In: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 11:9, s. 5004-5016

Related links:: http://dx.doi.org/10...; show more...; https://urn.kb.se/re...; https://doi.org/10.1...; https://lup.lub.lu.s...; show less...

Journal article (peer-reviewed)

Abstract Subject headings

Continuous exposure to methane causes IrO2 (110) films on Ir(100) to undergo extensive reduction at temperatures from 500 to 650 K. Measurements using in situ X-ray photoelectron spectroscopy (XPS) confirm that CH4 oxidation on IrO2 (110) converts so-called bridging oxygen atoms (O-br) at the surface to HObr groups while concurrently removing oxygen from the oxide film. Reduction of the IrO2 (110) film by methane is mildly activated as evidenced by an increase in the initial reduction rate as the temperature is increased from 500 to 650 K. The XPS results show that subsurface oxygen efficiently replaces O-br atoms at the IrO2 (110) surface during CH4 oxidation, even after the reduction of multiple layers of the oxide film, and that metallic Ir gradually forms at the surface as well. The isothermal rate of IrO2 (110) reduction by methane decreases continuously as metallic Ir replaces surface IrO2 (110) domains, demonstrating that IrO2 (110) is the active phase for CH4 oxidation under the conditions studied. A key finding is that the replacement of O-br atoms with oxygen from the subsurface is efficient enough to preserve IrO2 (110) domains at the surface and enable CH4 to reduce the similar to 10-layer IrO2 (110) films nearly to completion. In agreement with these observations, density functional theory calculations predict that oxygen atoms in the subsurface layer can replace O-br atoms at rates that are comparable to or higher than the rates at which O-br atoms are abstracted during CH4 oxidation. The efficacy with which oxygen in the bulk reservoir replenishes surface oxygen atoms has implications for understanding and modeling catalytic oxidation processes promoted by IrO2 (110).

Subject headings

TEKNIK OCH TEKNOLOGIER -- Materialteknik (hsv//swe)
ENGINEERING AND TECHNOLOGY -- Materials Engineering (hsv//eng)
NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP -- Kemi -- Oorganisk kemi (hsv//swe)
NATURAL SCIENCES -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)

Keyword

ambient-pressure X-ray photoelectron spectroscopy
methane activation
metal oxide
alkane
methane oxidation
iridium
IrO2
DFT
alkane
ambient-pressure X-ray photoelectron spectroscopy
DFT
iridium
IrO
metal oxide
methane activation
methane oxidation

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By the author/editor: Martin, Rachel; Kim, Minkyu; Lee, Christopher ...; Mehar, Vikram; Albertin, Stefan ...; Hejral, Uta; show more...; Merte, Lindsay R ...; Asthagiri, Aravi ...; Weaver, Jason F.; show less...

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ENGINEERING AND TECHNOLOGY: ENGINEERING AND ...; and Materials Engine ...

NATURAL SCIENCES: NATURAL SCIENCES; and Chemical Science ...; and Physical Chemist ...

NATURAL SCIENCES: NATURAL SCIENCES; and Chemical Science ...; and Inorganic Chemis ...

Articles in the publication: ACS Catalysis

By the university: Malmö University; Lund University

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