In situ FTIR Study of the Formation and Consumption Routes of Nitroorganic Complexes — Intermediates in Selective CatalyticvReduction of Nitrogen Oxides by Propene over Zirconia-Based Catalysts Full article
Conference |
Catalysis: Art to Science : an International Symposium in Honour of the Contribution of Julian Ross to the Advancement of Catalysis Science 03-03 Sep 2007 , Limerick |
||||||
---|---|---|---|---|---|---|---|
Journal |
Catalysis Today
ISSN: 0920-5861 , E-ISSN: 1873-4308 |
||||||
Output data | Year: 2009, Volume: 145, Number: 1-2, Pages: 152-162 Pages count : 11 DOI: 10.1016/j.cattod.2008.04.018 | ||||||
Tags | FTIRS, Intermediates, Isopropoxide, Mechanism, NOx propene SRC, Organic nitrocompounds, Spectrokinetic studies, Surface nitrate species, Zirconia, ZrPILC | ||||||
Authors |
|
||||||
Affiliations |
|
Funding (1)
1 | International Association for the Promotion of Co-operation with Scientists from the New Independent States of the Former Soviet Union | 97-11720 |
Abstract:
The results of this study show that the adsorption and catalytic properties of bulk ZrO2 and nanoscale ZrO2 pillars in pillared clay are significantly different. The NO + O2 interaction with the surface of bulk zirconia results in the formation of three types of surface nitrate complexes (bridging, bidentate and monodentate), while over ZrO2 pillars monodentate nitrates are not revealed.
The interaction of the propene–oxygen mixture with the surface of bulk zirconia leads to the formation of the acetate complexes only. Meanwhile, the main activation form of propene over ZrO2 pillars is the isopropoxide complex; the acetate complexes are observed only in small amounts at elevated temperatures. Complexes of three types are formed on the surface of Pt,Cu/ZrPILC after interaction with the propene–oxygen mixture flow: isopropoxide complexes, coordination-bound acetone, and acetates. Modification of ZrO2 pillars by Pt and Cu results in a significant change in the concentration and the temperature range of existence of C–H–O surface compounds.
The difference in the forms of reagents activation results in different structures of nitroorganic complexes. Over bulk zirconia the acetate and nitrate complexes form surface complexes with the structure similar to that of adsorbed nitromethane, monodentate nitrate being the most reactive species. Under reaction conditions at relatively low temperatures, over both modified and unmodified ZrO2 pillars, interaction of isopropoxide and nitrate complexes produces surface complexes structurally similar to adsorbed dinitropropane.
IR spectral kinetic studies revealed that the rates of surface nitrate and nitroorganic complexes transformation are in general close to each other and to the rate of catalytic reaction, significantly increasing due to Pt + Cu supporting on pillars. This demonstrates that these complexes are real intermediates of NOx HC–SCR over studied catalysts.
Cite:
Matyshak V.A.
, Sadykov V.A.
, Chernyshov K.A.
, Ross J.
In situ FTIR Study of the Formation and Consumption Routes of Nitroorganic Complexes — Intermediates in Selective CatalyticvReduction of Nitrogen Oxides by Propene over Zirconia-Based Catalysts
Catalysis Today. 2009. V.145. N1-2. P.152-162. DOI: 10.1016/j.cattod.2008.04.018 WOS Scopus РИНЦ
In situ FTIR Study of the Formation and Consumption Routes of Nitroorganic Complexes — Intermediates in Selective CatalyticvReduction of Nitrogen Oxides by Propene over Zirconia-Based Catalysts
Catalysis Today. 2009. V.145. N1-2. P.152-162. DOI: 10.1016/j.cattod.2008.04.018 WOS Scopus РИНЦ
Dates:
Published online: | Jun 4, 2008 |
Published print: | Jul 15, 2009 |
Identifiers:
Web of science | WOS:000267517500021 |
Scopus | 2-s2.0-66849101975 |
Elibrary | 13613673 |
Chemical Abstracts | 2009:663870 |
Chemical Abstracts (print) | 151:179891 |
OpenAlex | W1993840429 |