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Mechanism of the reaction of nitric oxide, ammonia, and oxygen over vanadia catalysts. 2. Isotopic transient studies with oxygen-18 and nitrogen-15

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j100311a016· OSTI ID:5353173

The mechanism of nitric oxide reduction with ammonia to form N/sub 2/, H/sub 2/O and N/sub 2/O both in the presence and in the absence of O/sub 2/ over the following series of catalysts, unsupported V/sub 2/O/sub 5/, V/sub 2/O/sub 5/ on TiO/sub 2/, V/sub 2/O/sub 5/ on SiO/sub 2//Al/sub 2/O/sub 3/, and V/sub 2/O/sub 5/ on Al/sub 2/O/sub 3/, has been investigated with the aid of labeled O/sub 2/ and labeled NH/sub 3/ at 400/sup 0/C. The behavior of ammonia was studied both in the presence and in the absence of O/sub 2/. The presence of labeled O/sub 2/ gives extra information about the product distribution and the reaction mechanism. Evidence is given that ammonia does not react with O/sub 2/ or O from any source during the reaction, but that nitrogen and nitrous oxide were produced by a reaction involving all three species, NO, NH/sub 3/, and/or O/sub 2/. Nitrous oxide and water are both formed at two different sites of the catalyst. A series of transient tracing studies were performed in a plug-flow reactor using /sup 15/NH/sub 3/ and /sup 18/O/sub 2/. Both /sup 15/NN and /sup 15/NNO were produced on the unsupported V/sub 2/O/sub 5/, V/sub 2/O/sub 5/ on TiO/sub 2/, V/sub 2/O/sub 5/ on SiO/sub 2//Al/sub 2/O/sub 3/, and V/sub 2/O/sub 5/ on Al/sub 2/O/sub 3/ with very high selectivities. The mechanism of the reaction of NO, NH/sub 3/, and O/sub 2/, proposed in a previous paper, is further evaluated on the basis of this new experimental evidence.

Research Organization:
Arnhem Institutions of the Dutch Electricity Utilities (Netherlands)
OSTI ID:
5353173
Journal Information:
J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 91:27; ISSN JPCHA
Country of Publication:
United States
Language:
English

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