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Title: Acrylonitrile from propane on (VO)[sub 2]P[sub 2]O[sub 7] with preadsorbed ammonia 2. Study of the mechanism of ammonia adsorption and reaction with C[sub 3] hydrocarbons

Abstract

Infrared data on the time-on-stream changes of the adsorbed species on vanadyl pyrophosphate with preadsorbed ammonia during interaction with propane and oxygen are reported, together with an infrared and thermogravimetric analysis of the ammonia interaction with this catalyst and of the adsorbed species formed in ammonia and propylene coadsorption. Results indicate that (i) ammonia forms mainly ammonium ions at room temperature, but increasing the temperature of interaction up to 400[degrees]C results in a progressive increase in the amount of ammonia coordinated to surface Lewis acid sites; (ii) the amount of adsorbed ammonia at 400[degrees]C corresponds to about a 1:1 NH[sub 3]-to-P surface ratio, but is lower for higher reaction temperatures; (iii) in the presence of gaseous oxygen, the amount of coordinated ammonia decreases, with the probable formation of an amido (NH[sub 2]) species; (iv) propylene is coordinated as a [pi]-bonded complex with vanadium Lewis acid sites and, in the absence of gaseous oxygen, is slowly transformed to acrylonitrile through the intermediate formation of propylamine; and (v) propane does not form adsorbed intermediates in the absence of gaseous oxygen, but in the presence of gaseous oxygen, acrylate species are detected. It is suggested that two pathways of formation of acrylonitrile frommore » propane are present on vanadyl pyrophosphate, the first in anaerobic conditions involving the intermediate formation of propylamine and the second, when O[sub 2] is present, involving the reaction between surface acrylate species and chemisorbed ammonia species. The second pathway is much more rapid than the first. 23 refs., 7 figs.« less

Authors:
;  [1]
  1. Universita di Bologna (Italy)
Publication Date:
OSTI Identifier:
5713917
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis; (United States)
Additional Journal Information:
Journal Volume: 142:1; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 02 PETROLEUM; ACRYLONITRILE; CHEMICAL PREPARATION; AMMONIA; ADSORPTION; PYROPHOSPHATES; CATALYTIC EFFECTS; VANADIUM OXIDES; ABSORPTION SPECTROSCOPY; ANAEROBIC CONDITIONS; CARBON OXIDES; CATALYSTS; DEHYDROGENATION; HETEROGENEOUS CATALYSIS; LEWIS ACIDS; PROPANE; REACTION INTERMEDIATES; SORPTIVE PROPERTIES; THERMAL GRAVIMETRIC ANALYSIS; ALKANES; CARBON COMPOUNDS; CATALYSIS; CHALCOGENIDES; CHEMICAL ANALYSIS; CHEMICAL REACTIONS; GRAVIMETRIC ANALYSIS; HYDRIDES; HYDROCARBONS; HYDROGEN COMPOUNDS; INORGANIC ACIDS; NITRILES; NITROGEN COMPOUNDS; NITROGEN HYDRIDES; ORGANIC COMPOUNDS; ORGANIC NITROGEN COMPOUNDS; OXIDES; OXYGEN COMPOUNDS; PHOSPHORUS COMPOUNDS; QUANTITATIVE CHEMICAL ANALYSIS; SORPTION; SPECTROSCOPY; SURFACE PROPERTIES; SYNTHESIS; THERMAL ANALYSIS; TRANSITION ELEMENT COMPOUNDS; VANADIUM COMPOUNDS; 400201* - Chemical & Physicochemical Properties; 020400 - Petroleum- Processing

Citation Formats

Centi, G, and Perathoner, S. Acrylonitrile from propane on (VO)[sub 2]P[sub 2]O[sub 7] with preadsorbed ammonia 2. Study of the mechanism of ammonia adsorption and reaction with C[sub 3] hydrocarbons. United States: N. p., 1993. Web. doi:10.1006/jcat.1993.1191.
Centi, G, & Perathoner, S. Acrylonitrile from propane on (VO)[sub 2]P[sub 2]O[sub 7] with preadsorbed ammonia 2. Study of the mechanism of ammonia adsorption and reaction with C[sub 3] hydrocarbons. United States. https://doi.org/10.1006/jcat.1993.1191
Centi, G, and Perathoner, S. 1993. "Acrylonitrile from propane on (VO)[sub 2]P[sub 2]O[sub 7] with preadsorbed ammonia 2. Study of the mechanism of ammonia adsorption and reaction with C[sub 3] hydrocarbons". United States. https://doi.org/10.1006/jcat.1993.1191.
@article{osti_5713917,
title = {Acrylonitrile from propane on (VO)[sub 2]P[sub 2]O[sub 7] with preadsorbed ammonia 2. Study of the mechanism of ammonia adsorption and reaction with C[sub 3] hydrocarbons},
author = {Centi, G and Perathoner, S},
abstractNote = {Infrared data on the time-on-stream changes of the adsorbed species on vanadyl pyrophosphate with preadsorbed ammonia during interaction with propane and oxygen are reported, together with an infrared and thermogravimetric analysis of the ammonia interaction with this catalyst and of the adsorbed species formed in ammonia and propylene coadsorption. Results indicate that (i) ammonia forms mainly ammonium ions at room temperature, but increasing the temperature of interaction up to 400[degrees]C results in a progressive increase in the amount of ammonia coordinated to surface Lewis acid sites; (ii) the amount of adsorbed ammonia at 400[degrees]C corresponds to about a 1:1 NH[sub 3]-to-P surface ratio, but is lower for higher reaction temperatures; (iii) in the presence of gaseous oxygen, the amount of coordinated ammonia decreases, with the probable formation of an amido (NH[sub 2]) species; (iv) propylene is coordinated as a [pi]-bonded complex with vanadium Lewis acid sites and, in the absence of gaseous oxygen, is slowly transformed to acrylonitrile through the intermediate formation of propylamine; and (v) propane does not form adsorbed intermediates in the absence of gaseous oxygen, but in the presence of gaseous oxygen, acrylate species are detected. It is suggested that two pathways of formation of acrylonitrile from propane are present on vanadyl pyrophosphate, the first in anaerobic conditions involving the intermediate formation of propylamine and the second, when O[sub 2] is present, involving the reaction between surface acrylate species and chemisorbed ammonia species. The second pathway is much more rapid than the first. 23 refs., 7 figs.},
doi = {10.1006/jcat.1993.1191},
url = {https://www.osti.gov/biblio/5713917}, journal = {Journal of Catalysis; (United States)},
issn = {0021-9517},
number = ,
volume = 142:1,
place = {United States},
year = {Thu Jul 01 00:00:00 EDT 1993},
month = {Thu Jul 01 00:00:00 EDT 1993}
}