The reduction of 15N14NO by CO and by H2 over Rh/SiO2: a test of a mechanistic proposal

Noel W. Cant; Dean C. Chambers; Irene O. Y. Liu

doi:10.1016/j.jcat.2010.11.005

The reduction of ¹⁵N¹⁴NO by CO and by H₂ over Rh/SiO₂: a test of a mechanistic proposal

Noel W. Cant
, Dean C. Chambers
, Irene O. Y. Liu

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

12 Citations (Scopus)

Abstract

A literature proposal that the reduction of nitrous oxide by carbon monoxide over rhodium catalysts proceeds by cleavage of the NN bond has been tested through the use of ¹⁵N¹⁴NO as the reactant. The results disprove the suggestion in that ¹⁴N¹⁵N is the dominant product at temperatures from 336 °C to 356 °C with nitrous oxide conversions from 26% to >99%. Little, if any, ¹⁴N ₂ and ¹⁵N₂ is formed, in contrast with the 25% of each expected for the model. Results for the corresponding reaction of ¹⁵N¹⁴NO with H₂ are even more clear-cut in demonstrating the absence of NN bond cleavage. The activity of the Rh/SiO ₂ used here for the N₂O/CO system fell within the rather wide of values reported in the literature for other Rh catalysts. However, activity for the reduction of N₂O by H₂ was approximately five times higher than the only previous result in the literature, that for a Rh/Al₂O₃ catalyst.

Original language	English
Pages (from-to)	162-166
Number of pages	5
Journal	Journal of Catalysis
Volume	278
Issue number	1
DOIs	https://doi.org/10.1016/j.jcat.2010.11.005
Publication status	Published - 14 Feb 2011

Keywords

NNO reduction mechanism
NO + H reaction
Rh/SiO NO + CO reaction

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10.1016/j.jcat.2010.11.005

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title = "The reduction of 15N14NO by CO and by H2 over Rh/SiO2: a test of a mechanistic proposal",

abstract = "A literature proposal that the reduction of nitrous oxide by carbon monoxide over rhodium catalysts proceeds by cleavage of the NN bond has been tested through the use of 15N14NO as the reactant. The results disprove the suggestion in that 14N15N is the dominant product at temperatures from 336 °C to 356 °C with nitrous oxide conversions from 26\% to >99\%. Little, if any, 14N 2 and 15N2 is formed, in contrast with the 25\% of each expected for the model. Results for the corresponding reaction of 15N14NO with H2 are even more clear-cut in demonstrating the absence of NN bond cleavage. The activity of the Rh/SiO 2 used here for the N2O/CO system fell within the rather wide of values reported in the literature for other Rh catalysts. However, activity for the reduction of N2O by H2 was approximately five times higher than the only previous result in the literature, that for a Rh/Al2O3 catalyst.",

keywords = "NNO reduction mechanism, NO + H reaction, Rh/SiO NO + CO reaction",

author = "Cant, \{Noel W.\} and Chambers, \{Dean C.\} and Liu, \{Irene O. Y.\}",

year = "2011",

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doi = "10.1016/j.jcat.2010.11.005",

language = "English",

volume = "278",

pages = "162--166",

journal = "Journal of Catalysis",

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T1 - The reduction of 15N14NO by CO and by H2 over Rh/SiO2

T2 - a test of a mechanistic proposal

AU - Cant, Noel W.

AU - Chambers, Dean C.

AU - Liu, Irene O. Y.

PY - 2011/2/14

Y1 - 2011/2/14

N2 - A literature proposal that the reduction of nitrous oxide by carbon monoxide over rhodium catalysts proceeds by cleavage of the NN bond has been tested through the use of 15N14NO as the reactant. The results disprove the suggestion in that 14N15N is the dominant product at temperatures from 336 °C to 356 °C with nitrous oxide conversions from 26% to >99%. Little, if any, 14N 2 and 15N2 is formed, in contrast with the 25% of each expected for the model. Results for the corresponding reaction of 15N14NO with H2 are even more clear-cut in demonstrating the absence of NN bond cleavage. The activity of the Rh/SiO 2 used here for the N2O/CO system fell within the rather wide of values reported in the literature for other Rh catalysts. However, activity for the reduction of N2O by H2 was approximately five times higher than the only previous result in the literature, that for a Rh/Al2O3 catalyst.

AB - A literature proposal that the reduction of nitrous oxide by carbon monoxide over rhodium catalysts proceeds by cleavage of the NN bond has been tested through the use of 15N14NO as the reactant. The results disprove the suggestion in that 14N15N is the dominant product at temperatures from 336 °C to 356 °C with nitrous oxide conversions from 26% to >99%. Little, if any, 14N 2 and 15N2 is formed, in contrast with the 25% of each expected for the model. Results for the corresponding reaction of 15N14NO with H2 are even more clear-cut in demonstrating the absence of NN bond cleavage. The activity of the Rh/SiO 2 used here for the N2O/CO system fell within the rather wide of values reported in the literature for other Rh catalysts. However, activity for the reduction of N2O by H2 was approximately five times higher than the only previous result in the literature, that for a Rh/Al2O3 catalyst.

KW - NNO reduction mechanism

KW - NO + H reaction

KW - Rh/SiO NO + CO reaction

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DO - 10.1016/j.jcat.2010.11.005

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AN - SCOPUS:79551505062

SN - 0021-9517

VL - 278

SP - 162

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JF - Journal of Catalysis

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ER -

The reduction of ¹⁵N¹⁴NO by CO and by H₂ over Rh/SiO₂: a test of a mechanistic proposal

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Keywords

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