Abstract
NO reduction by CO on Rh(111) was investigated by near-ambient pressure X-ray photoelectron spectroscopy, mass spectrometry, and kinetic analysis. Under exposure to NO + CO mixed gases and with heating the surface from room temperature to 450 °C, NO dissociation and NO reduction reaction start simultaneously independent of gas pressure ratio of NO/CO, which indicates that NO dissociation triggers this reaction. From kinetic analyses based on observed adsorbate coverages under reaction conditions, the following two points are suggested: (i) NOhollow is a reactive species for N2 and N2O formation via N + NO reaction. (ii) At low temperatures, the N + NO reaction is dominant for N2 production, whereas above around 400 °C, the N + N reaction becomes dominant, which leads to an increase in N2 selectivity at the higher temperatures. Compared with the NO + CO reaction on Ir(111) surfaces, which exhibits a high N2 selectivity, the adsorption site of reactive NO and the availability of vacant surface sites could be key factors for the lower N2 selectivity for Rh(111).
| Original language | English |
|---|---|
| Pages (from-to) | 11663-11670 |
| Number of pages | 8 |
| Journal | ACS Catalysis |
| DOIs | |
| Publication status | Accepted/In press - 2018 Jan 1 |
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Keywords
- kinetics
- NAP-XPS
- NO reduction
- operando observation
- reaction mechanism
- Rh
ASJC Scopus subject areas
- Catalysis
- Chemistry(all)
Cite this
Operando NAP-XPS Observation and Kinetics Analysis of NO Reduction over Rh(111) Surface : Characterization of Active Surface and Reactive Species. / Ueda, Kohei; Isegawa, Kazuhisa; Amemiya, Kenta; Mase, Kazuhiko; Kondoh, Hiroshi.
In: ACS Catalysis, 01.01.2018, p. 11663-11670.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Operando NAP-XPS Observation and Kinetics Analysis of NO Reduction over Rh(111) Surface
T2 - Characterization of Active Surface and Reactive Species
AU - Ueda, Kohei
AU - Isegawa, Kazuhisa
AU - Amemiya, Kenta
AU - Mase, Kazuhiko
AU - Kondoh, Hiroshi
PY - 2018/1/1
Y1 - 2018/1/1
N2 - NO reduction by CO on Rh(111) was investigated by near-ambient pressure X-ray photoelectron spectroscopy, mass spectrometry, and kinetic analysis. Under exposure to NO + CO mixed gases and with heating the surface from room temperature to 450 °C, NO dissociation and NO reduction reaction start simultaneously independent of gas pressure ratio of NO/CO, which indicates that NO dissociation triggers this reaction. From kinetic analyses based on observed adsorbate coverages under reaction conditions, the following two points are suggested: (i) NOhollow is a reactive species for N2 and N2O formation via N + NO reaction. (ii) At low temperatures, the N + NO reaction is dominant for N2 production, whereas above around 400 °C, the N + N reaction becomes dominant, which leads to an increase in N2 selectivity at the higher temperatures. Compared with the NO + CO reaction on Ir(111) surfaces, which exhibits a high N2 selectivity, the adsorption site of reactive NO and the availability of vacant surface sites could be key factors for the lower N2 selectivity for Rh(111).
AB - NO reduction by CO on Rh(111) was investigated by near-ambient pressure X-ray photoelectron spectroscopy, mass spectrometry, and kinetic analysis. Under exposure to NO + CO mixed gases and with heating the surface from room temperature to 450 °C, NO dissociation and NO reduction reaction start simultaneously independent of gas pressure ratio of NO/CO, which indicates that NO dissociation triggers this reaction. From kinetic analyses based on observed adsorbate coverages under reaction conditions, the following two points are suggested: (i) NOhollow is a reactive species for N2 and N2O formation via N + NO reaction. (ii) At low temperatures, the N + NO reaction is dominant for N2 production, whereas above around 400 °C, the N + N reaction becomes dominant, which leads to an increase in N2 selectivity at the higher temperatures. Compared with the NO + CO reaction on Ir(111) surfaces, which exhibits a high N2 selectivity, the adsorption site of reactive NO and the availability of vacant surface sites could be key factors for the lower N2 selectivity for Rh(111).
KW - kinetics
KW - NAP-XPS
KW - NO reduction
KW - operando observation
KW - reaction mechanism
KW - Rh
UR - http://www.scopus.com/inward/record.url?scp=85056500829&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85056500829&partnerID=8YFLogxK
U2 - 10.1021/acscatal.8b03180
DO - 10.1021/acscatal.8b03180
M3 - Article
AN - SCOPUS:85056500829
SP - 11663
EP - 11670
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
ER -