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Title: Vanadia-titania aerogels: I. Preparation, morphological properties, and activity for the selective catalytic reduction of NO by NH{sub 3}

Abstract

Highly dispersed vanadia-titania aerogels with high surface area have been synthesized by a two-stage sol-gel process with ensuing high-temperature supercritical drying. A titania gel was prepared by the addition of an acidic hydrolysant to tetrabutoxy-titanium(IV) in methanolic solution. The vanadium alkoxide precursor was added after redispersing the titania gel. The influences of different preparation conditions on the morphological and chemical properties of the aerogels were studied. The aerogels were characterized by means of nitrogen physisorption, X-ray diffraction, transmission electron microscopy, and thermal analysis (thermogravity, differential thermal analysis) coupled with mass spectroscopy. The meso- to macroporous vanadia-titania aerogels possess a BET surface area of 140 to 220 m{sup 2} g{sup -1} after calcination up to 673 K and contain well-developed anatase crystallites of ca. 10 nm mean size. Crystalline V{sub 2}O{sub 5} was detected only for samples calcined at 723 K. All other aerogel catalysts, calcined at lower temperature, showed no indication for long-range ordered vanadia domains. The catalytic properties of the aerogels were tested for the selective catalytic reduction of NO by NH{sub 3}. An increase in the vanadia loading from 5 to 30 wt% V{sub 2}O{sub 5} resulted in a marked increase in overall as well as specific activity,more » whereas the apparent activation energy decreased from 66 to 55 kJ mol{sup -1}. An increase in the calcination temperature from 573 to 673 K led to a significant rise in the activity of the vanadia-titania aerogel catalyst. The aerogel with 30 wt% V{sub 2}O{sub 5} showed a reaction rate referred to the vanadium content (turnover frequency) that is similar to that of multiply grafted well-dispersed vanadia/titania catalysts. Among all catalysts presented in this work, this aerogel exhibited the highest reaction rate per gram of catalyst. 47 refs., 13 figs., 4 tabs.« less

Authors:
; ;  [1]
  1. Swiss Federal Institute of Technology, Zuerich (Switzerland); and others
Publication Date:
OSTI Identifier:
98928
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 149; Journal Issue: 2; Other Information: PBD: Oct 1994
Country of Publication:
United States
Language:
English
Subject:
40 CHEMISTRY; 33 ADVANCED PROPULSION SYSTEMS; 20 FOSSIL-FUELED POWER PLANTS; VANADIUM OXIDES; STRUCTURAL CHEMICAL ANALYSIS; CATALYTIC EFFECTS; TITANIUM OXIDES; NITRIC OXIDE; SELECTIVE CATALYTIC REDUCTION; ACTIVATION ENERGY; CALCINATION; THERMAL ANALYSIS; MASS SPECTROSCOPY; TRANSMISSION ELECTRON MICROSCOPY; CHEMICAL PREPARATION; TEMPERATURE DEPENDENCE; TEMPERATURE RANGE 0400-1000 K

Citation Formats

Schneider, M, Maciejewski, M, and Tschudin, S. Vanadia-titania aerogels: I. Preparation, morphological properties, and activity for the selective catalytic reduction of NO by NH{sub 3}. United States: N. p., 1994. Web. doi:10.1006/jcat.1994.1301.
Schneider, M, Maciejewski, M, & Tschudin, S. Vanadia-titania aerogels: I. Preparation, morphological properties, and activity for the selective catalytic reduction of NO by NH{sub 3}. United States. https://doi.org/10.1006/jcat.1994.1301
Schneider, M, Maciejewski, M, and Tschudin, S. 1994. "Vanadia-titania aerogels: I. Preparation, morphological properties, and activity for the selective catalytic reduction of NO by NH{sub 3}". United States. https://doi.org/10.1006/jcat.1994.1301.
@article{osti_98928,
title = {Vanadia-titania aerogels: I. Preparation, morphological properties, and activity for the selective catalytic reduction of NO by NH{sub 3}},
author = {Schneider, M and Maciejewski, M and Tschudin, S},
abstractNote = {Highly dispersed vanadia-titania aerogels with high surface area have been synthesized by a two-stage sol-gel process with ensuing high-temperature supercritical drying. A titania gel was prepared by the addition of an acidic hydrolysant to tetrabutoxy-titanium(IV) in methanolic solution. The vanadium alkoxide precursor was added after redispersing the titania gel. The influences of different preparation conditions on the morphological and chemical properties of the aerogels were studied. The aerogels were characterized by means of nitrogen physisorption, X-ray diffraction, transmission electron microscopy, and thermal analysis (thermogravity, differential thermal analysis) coupled with mass spectroscopy. The meso- to macroporous vanadia-titania aerogels possess a BET surface area of 140 to 220 m{sup 2} g{sup -1} after calcination up to 673 K and contain well-developed anatase crystallites of ca. 10 nm mean size. Crystalline V{sub 2}O{sub 5} was detected only for samples calcined at 723 K. All other aerogel catalysts, calcined at lower temperature, showed no indication for long-range ordered vanadia domains. The catalytic properties of the aerogels were tested for the selective catalytic reduction of NO by NH{sub 3}. An increase in the vanadia loading from 5 to 30 wt% V{sub 2}O{sub 5} resulted in a marked increase in overall as well as specific activity, whereas the apparent activation energy decreased from 66 to 55 kJ mol{sup -1}. An increase in the calcination temperature from 573 to 673 K led to a significant rise in the activity of the vanadia-titania aerogel catalyst. The aerogel with 30 wt% V{sub 2}O{sub 5} showed a reaction rate referred to the vanadium content (turnover frequency) that is similar to that of multiply grafted well-dispersed vanadia/titania catalysts. Among all catalysts presented in this work, this aerogel exhibited the highest reaction rate per gram of catalyst. 47 refs., 13 figs., 4 tabs.},
doi = {10.1006/jcat.1994.1301},
url = {https://www.osti.gov/biblio/98928}, journal = {Journal of Catalysis},
number = 2,
volume = 149,
place = {United States},
year = {Sat Oct 01 00:00:00 EDT 1994},
month = {Sat Oct 01 00:00:00 EDT 1994}
}