N+NO reaction on Rh(111) surfaces studied with fast near-edge X-ray absorption fine structure spectroscopy: Role of NO dimer as an extrinsic precursor

Ikuyo Nakai; Hiroshi Kondoh; Toru Shimada; Masanari Nagasaka; Reona Yokota; Kenta Amemiya; Hideo Orita; Toshiaki Ohta

doi:10.1021/jp0665933

N+NO reaction on Rh(111) surfaces studied with fast near-edge X-ray absorption fine structure spectroscopy: Role of NO dimer as an extrinsic precursor

Ikuyo Nakai, Hiroshi Kondoh, Toru Shimada, Masanari Nagasaka, Reona Yokota, Kenta Amemiya, Hideo Orita, Toshiaki Ohta

Research output: Contribution to journal › Article › peer-review

17 Citations (Scopus)

Abstract

We studied the mechanism of the N+NO reaction on Rh(111) surfaces by means of fast near-edge X-ray absorption fine structure spectroscopy. This reaction is important as a basis of NO_x reduction reactions on platinum-group metal surfaces. Atomic nitrogen layers on Rh(111) were titrated with NO at various temperatures. N₂O is exclusively formed and desorbs into the gas phase below 350 K. The consumption rate of atomic nitrogen exhibits strange temperature dependence between 100 and 350 K; the reaction proceeds slower with increasing temperature. Reaction kinetics analyses and isotope-controlled experiments have revealed that the surface N atoms do not react with chemisorbed NO molecules but with NO dimers weakly bound on top of the chemisorbed layer, which play a role as an extrinsic precursor. The present results may support the possibility that NO dimers participate in various NO-related synthetic, biochemical, and surface reactions as an intermediate.

Original language	English
Pages (from-to)	25578-25581
Number of pages	4
Journal	Journal of Physical Chemistry B
Volume	110
Issue number	51
DOIs	https://doi.org/10.1021/jp0665933
Publication status	Published - 2006 Dec 28
Externally published	Yes

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Surfaces, Coatings and Films
Materials Chemistry

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title = "N+NO reaction on Rh(111) surfaces studied with fast near-edge X-ray absorption fine structure spectroscopy: Role of NO dimer as an extrinsic precursor",

abstract = "We studied the mechanism of the N+NO reaction on Rh(111) surfaces by means of fast near-edge X-ray absorption fine structure spectroscopy. This reaction is important as a basis of NOx reduction reactions on platinum-group metal surfaces. Atomic nitrogen layers on Rh(111) were titrated with NO at various temperatures. N2O is exclusively formed and desorbs into the gas phase below 350 K. The consumption rate of atomic nitrogen exhibits strange temperature dependence between 100 and 350 K; the reaction proceeds slower with increasing temperature. Reaction kinetics analyses and isotope-controlled experiments have revealed that the surface N atoms do not react with chemisorbed NO molecules but with NO dimers weakly bound on top of the chemisorbed layer, which play a role as an extrinsic precursor. The present results may support the possibility that NO dimers participate in various NO-related synthetic, biochemical, and surface reactions as an intermediate.",

author = "Ikuyo Nakai and Hiroshi Kondoh and Toru Shimada and Masanari Nagasaka and Reona Yokota and Kenta Amemiya and Hideo Orita and Toshiaki Ohta",

year = "2006",

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T1 - N+NO reaction on Rh(111) surfaces studied with fast near-edge X-ray absorption fine structure spectroscopy

T2 - Role of NO dimer as an extrinsic precursor

AU - Nakai, Ikuyo

AU - Kondoh, Hiroshi

AU - Shimada, Toru

AU - Nagasaka, Masanari

AU - Yokota, Reona

AU - Amemiya, Kenta

AU - Orita, Hideo

AU - Ohta, Toshiaki

PY - 2006/12/28

Y1 - 2006/12/28

N2 - We studied the mechanism of the N+NO reaction on Rh(111) surfaces by means of fast near-edge X-ray absorption fine structure spectroscopy. This reaction is important as a basis of NOx reduction reactions on platinum-group metal surfaces. Atomic nitrogen layers on Rh(111) were titrated with NO at various temperatures. N2O is exclusively formed and desorbs into the gas phase below 350 K. The consumption rate of atomic nitrogen exhibits strange temperature dependence between 100 and 350 K; the reaction proceeds slower with increasing temperature. Reaction kinetics analyses and isotope-controlled experiments have revealed that the surface N atoms do not react with chemisorbed NO molecules but with NO dimers weakly bound on top of the chemisorbed layer, which play a role as an extrinsic precursor. The present results may support the possibility that NO dimers participate in various NO-related synthetic, biochemical, and surface reactions as an intermediate.

AB - We studied the mechanism of the N+NO reaction on Rh(111) surfaces by means of fast near-edge X-ray absorption fine structure spectroscopy. This reaction is important as a basis of NOx reduction reactions on platinum-group metal surfaces. Atomic nitrogen layers on Rh(111) were titrated with NO at various temperatures. N2O is exclusively formed and desorbs into the gas phase below 350 K. The consumption rate of atomic nitrogen exhibits strange temperature dependence between 100 and 350 K; the reaction proceeds slower with increasing temperature. Reaction kinetics analyses and isotope-controlled experiments have revealed that the surface N atoms do not react with chemisorbed NO molecules but with NO dimers weakly bound on top of the chemisorbed layer, which play a role as an extrinsic precursor. The present results may support the possibility that NO dimers participate in various NO-related synthetic, biochemical, and surface reactions as an intermediate.

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N+NO reaction on Rh(111) surfaces studied with fast near-edge X-ray absorption fine structure spectroscopy: Role of NO dimer as an extrinsic precursor

Abstract

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