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Title: Synthesizing alcohols and ketones by photoinduced catalytic partial oxidation of hydrocarbons in TiO{sub 2} film reactors prepared by three different methods

Abstract

The partial oxidation of cyclohexane to cyclohexanol and cyclohexanone on UV-irradiated titanium dioxide films in the presence of molecular oxygen at low temperatures and atmospheric pressure was studied. Three different coating methodologies (dip coating using titanium isopropoxide and commercially available titanium dioxide particles, sol-gel process, and flame aerosol process) were used to deposit the titanium dioxide films, and their effectiveness in partial oxidation of cyclohexane was compared. Conversions of the cyclohexane in the gas-phase reactor averaged between 1.1 and 8.7% per pass (8-s contact time) for the different film reactors. No detectable amount of carbon dioxide was generated. The selectivity for ketone formation ranged from 59 to 91%. The films produced by the flame aerosol method resulted in the highest yield per mass of catalyst used and showed no coking and deactivation for a total run time of approximately 10 h (2 cycles). The films were characterized by XRD, SEM, and TEM to establish the phase compositions, morphologies, and primary particle sizes, respectively. The flame aerosol coating resulted in the formation of high surface area aggregates consisting of nanometer-sized primary particles with high density (minimal internal porosity), whereas dip coating resulted in the formation of bulk crystallites that were moremore » susceptible to coking and deactivation. The flame-aerosol-deposited titania particles had more surface sites per unit mass for photooxidation and minimal intraparticle diffusion limitations.« less

Authors:
;  [1]; ;  [2]
  1. USEPA National Risk Management Research Lab., Cincinnati, OH (United States)
  2. Univ. of Cincinnati, OH (United States)
Publication Date:
OSTI Identifier:
697166
Resource Type:
Journal Article
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 38; Journal Issue: 9; Other Information: PBD: Sep 1999
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 10 SYNTHETIC FUELS; CYCLOHEXANE; PARTIAL OXIDATION PROCESSES; PHOTOLYSIS; TITANIUM OXIDES; CATALYTIC EFFECTS; CYCLOHEXANOL; CYCLOHEXANONE; SYNTHESIS; CHEMICAL REACTORS

Citation Formats

Sahle-Demessie, E., Gonzalez, M., Wang, Z.M., and Biswas, P. Synthesizing alcohols and ketones by photoinduced catalytic partial oxidation of hydrocarbons in TiO{sub 2} film reactors prepared by three different methods. United States: N. p., 1999. Web. doi:10.1021/ie990054l.
Sahle-Demessie, E., Gonzalez, M., Wang, Z.M., & Biswas, P. Synthesizing alcohols and ketones by photoinduced catalytic partial oxidation of hydrocarbons in TiO{sub 2} film reactors prepared by three different methods. United States. doi:10.1021/ie990054l.
Sahle-Demessie, E., Gonzalez, M., Wang, Z.M., and Biswas, P. Wed . "Synthesizing alcohols and ketones by photoinduced catalytic partial oxidation of hydrocarbons in TiO{sub 2} film reactors prepared by three different methods". United States. doi:10.1021/ie990054l.
@article{osti_697166,
title = {Synthesizing alcohols and ketones by photoinduced catalytic partial oxidation of hydrocarbons in TiO{sub 2} film reactors prepared by three different methods},
author = {Sahle-Demessie, E. and Gonzalez, M. and Wang, Z.M. and Biswas, P.},
abstractNote = {The partial oxidation of cyclohexane to cyclohexanol and cyclohexanone on UV-irradiated titanium dioxide films in the presence of molecular oxygen at low temperatures and atmospheric pressure was studied. Three different coating methodologies (dip coating using titanium isopropoxide and commercially available titanium dioxide particles, sol-gel process, and flame aerosol process) were used to deposit the titanium dioxide films, and their effectiveness in partial oxidation of cyclohexane was compared. Conversions of the cyclohexane in the gas-phase reactor averaged between 1.1 and 8.7% per pass (8-s contact time) for the different film reactors. No detectable amount of carbon dioxide was generated. The selectivity for ketone formation ranged from 59 to 91%. The films produced by the flame aerosol method resulted in the highest yield per mass of catalyst used and showed no coking and deactivation for a total run time of approximately 10 h (2 cycles). The films were characterized by XRD, SEM, and TEM to establish the phase compositions, morphologies, and primary particle sizes, respectively. The flame aerosol coating resulted in the formation of high surface area aggregates consisting of nanometer-sized primary particles with high density (minimal internal porosity), whereas dip coating resulted in the formation of bulk crystallites that were more susceptible to coking and deactivation. The flame-aerosol-deposited titania particles had more surface sites per unit mass for photooxidation and minimal intraparticle diffusion limitations.},
doi = {10.1021/ie990054l},
journal = {Industrial and Engineering Chemistry Research},
number = 9,
volume = 38,
place = {United States},
year = {1999},
month = {9}
}