Operando observation of NO reduction by CO on Ir(111) surface using NAP-XPS and mass spectrometry: Dominant reaction pathway to N2 formation under near realistic conditions

Kohei Ueda, Masaaki Yoshida, Kazuhisa Isegawa, Naoki Shirahata, Kenta Amemiya, Kazuhiko Mase, Bongjin Simon Mun, Hiroshi Kondoh

Research output: Contribution to journalArticle

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Abstract

The nitric oxide (NO) reduction by carbon monoxide (CO) on Ir(111) surfaces under near ambient pressure conditions was studied by a combination of near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) and mass spectrometry (MS), particularly paying attention to the dominant reaction pathway to formation of molecular nitrogen (N2). Under a relatively low CO pressure condition (50 mTorr NO + 10 mTorr CO), two reaction pathways to form N2 are clearly observed at different ignition temperatures (280 and 400 °C) and attributed to a reaction of NO adsorbed at atop site (NOatop) with atomic nitrogen (Nad) and associative desorption of Nad, respectively. Since the adsorption of NOatop is inhibited by CO adsorbed at atop site (COatop), the ignition of the NOatop + Nad reaction strongly depends on the coverage of COatop; the ignition temperature shifts to higher temperature as increasing CO pressure. In contrast, for the Nad + Nad reaction the ignition temperature keeps almost constant (∼400 °C). The online MS results indicate that the latter reaction is the dominant pathway to N2 formation and the former one less contributes to N2 formation with accompanying a small amount of nitrous oxide (N2O). No evidence for contribution of the isocyanate (NCO) species as an intermediate was observed in the operando NAP-XP spectra. (Graph Presented).

Original languageEnglish
Pages (from-to)1763-1769
Number of pages7
JournalJournal of Physical Chemistry C
Volume121
Issue number3
DOIs
Publication statusPublished - 2017 Jan 26

Fingerprint

Nitric oxide
Carbon Monoxide
nitric oxide
Carbon monoxide
carbon monoxide
Mass spectrometry
Nitric Oxide
mass spectroscopy
X ray photoelectron spectroscopy
photoelectron spectroscopy
Ignition
ignition temperature
x rays
Nitrogen
Isocyanates
Temperature
Nitrous Oxide
nitrogen
isocyanates
nitrous oxides

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

Cite this

Operando observation of NO reduction by CO on Ir(111) surface using NAP-XPS and mass spectrometry : Dominant reaction pathway to N2 formation under near realistic conditions. / Ueda, Kohei; Yoshida, Masaaki; Isegawa, Kazuhisa; Shirahata, Naoki; Amemiya, Kenta; Mase, Kazuhiko; Mun, Bongjin Simon; Kondoh, Hiroshi.

In: Journal of Physical Chemistry C, Vol. 121, No. 3, 26.01.2017, p. 1763-1769.

Research output: Contribution to journalArticle

Ueda, Kohei ; Yoshida, Masaaki ; Isegawa, Kazuhisa ; Shirahata, Naoki ; Amemiya, Kenta ; Mase, Kazuhiko ; Mun, Bongjin Simon ; Kondoh, Hiroshi. / Operando observation of NO reduction by CO on Ir(111) surface using NAP-XPS and mass spectrometry : Dominant reaction pathway to N2 formation under near realistic conditions. In: Journal of Physical Chemistry C. 2017 ; Vol. 121, No. 3. pp. 1763-1769.
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abstract = "The nitric oxide (NO) reduction by carbon monoxide (CO) on Ir(111) surfaces under near ambient pressure conditions was studied by a combination of near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) and mass spectrometry (MS), particularly paying attention to the dominant reaction pathway to formation of molecular nitrogen (N2). Under a relatively low CO pressure condition (50 mTorr NO + 10 mTorr CO), two reaction pathways to form N2 are clearly observed at different ignition temperatures (280 and 400 °C) and attributed to a reaction of NO adsorbed at atop site (NOatop) with atomic nitrogen (Nad) and associative desorption of Nad, respectively. Since the adsorption of NOatop is inhibited by CO adsorbed at atop site (COatop), the ignition of the NOatop + Nad reaction strongly depends on the coverage of COatop; the ignition temperature shifts to higher temperature as increasing CO pressure. In contrast, for the Nad + Nad reaction the ignition temperature keeps almost constant (∼400 °C). The online MS results indicate that the latter reaction is the dominant pathway to N2 formation and the former one less contributes to N2 formation with accompanying a small amount of nitrous oxide (N2O). No evidence for contribution of the isocyanate (NCO) species as an intermediate was observed in the operando NAP-XP spectra. (Graph Presented).",
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AU - Shirahata, Naoki

AU - Amemiya, Kenta

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AU - Mun, Bongjin Simon

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AB - The nitric oxide (NO) reduction by carbon monoxide (CO) on Ir(111) surfaces under near ambient pressure conditions was studied by a combination of near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) and mass spectrometry (MS), particularly paying attention to the dominant reaction pathway to formation of molecular nitrogen (N2). Under a relatively low CO pressure condition (50 mTorr NO + 10 mTorr CO), two reaction pathways to form N2 are clearly observed at different ignition temperatures (280 and 400 °C) and attributed to a reaction of NO adsorbed at atop site (NOatop) with atomic nitrogen (Nad) and associative desorption of Nad, respectively. Since the adsorption of NOatop is inhibited by CO adsorbed at atop site (COatop), the ignition of the NOatop + Nad reaction strongly depends on the coverage of COatop; the ignition temperature shifts to higher temperature as increasing CO pressure. In contrast, for the Nad + Nad reaction the ignition temperature keeps almost constant (∼400 °C). The online MS results indicate that the latter reaction is the dominant pathway to N2 formation and the former one less contributes to N2 formation with accompanying a small amount of nitrous oxide (N2O). No evidence for contribution of the isocyanate (NCO) species as an intermediate was observed in the operando NAP-XP spectra. (Graph Presented).

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