Through online mass spectrometry it is demonstrated that steady-state
production of syngas (CO and H2) can be attained within 5 s after
admitting large alkanes (i-octane, n-octane, n-decane, or n-hexadecane)
and air into a short-contact-time reactor by using an automotive
fuel injector and initially preheating the Rh-coated catalyst above
the respective catalytic autoignition temperature for each fuel.
Minimum catalytic autoignition temperatures on Rh were ~260 degC
for n-octane and 240 degC for i-octane and n-decane. In contrast,
catalytic autoignition of n-hexadecane indirectly occurred at temperatures
(>220 degC) lower than those of the other fuels investigated because
of exothermic homogeneous chemistry that preheated the catalyst (30-60
degC) to a temperature (~280 degC) sufficient for surface lightoff.Additionally,
the ignition kinetics for the large alkanes were determined and compared
with those of methane. The step controlling surface ignition possessed
an apparent activation energy of ~78 kJ/mol that was not significantly
different between fuels (p > 0.05). However, a significant difference
was found between the ignition preexponential for methane, O(104
s-1), and the other large alkanes, O(106 -1). The dominant energetic
step for large alkane surface ignition is hypothesized to be oxygen
desorption at saturation coverage as has been suggested for methane.
%0 Journal Article
%1 Williams2006
%A Williams, Kenneth A.
%A Schmidt, Lanny D.
%D 2006
%J Applied Catalysis A: General
%K Alkanes Catalysis Lightoff Liquid Partial Reaction Rhodium Start-up Surface Transient catalyst experiments fuels ignition kinetics oxidation
%P 30-45
%T Catalytic autoignition of higher alkane partial oxidation on Rh-coated
foams
%U http://www.sciencedirect.com/science/article/B6TF5-4HKCYVG-8/2/3a26157d307167f1dc47303425e93b8e
%V 299
%X Through online mass spectrometry it is demonstrated that steady-state
production of syngas (CO and H2) can be attained within 5 s after
admitting large alkanes (i-octane, n-octane, n-decane, or n-hexadecane)
and air into a short-contact-time reactor by using an automotive
fuel injector and initially preheating the Rh-coated catalyst above
the respective catalytic autoignition temperature for each fuel.
Minimum catalytic autoignition temperatures on Rh were ~260 degC
for n-octane and 240 degC for i-octane and n-decane. In contrast,
catalytic autoignition of n-hexadecane indirectly occurred at temperatures
(>220 degC) lower than those of the other fuels investigated because
of exothermic homogeneous chemistry that preheated the catalyst (30-60
degC) to a temperature (~280 degC) sufficient for surface lightoff.Additionally,
the ignition kinetics for the large alkanes were determined and compared
with those of methane. The step controlling surface ignition possessed
an apparent activation energy of ~78 kJ/mol that was not significantly
different between fuels (p > 0.05). However, a significant difference
was found between the ignition preexponential for methane, O(104
s-1), and the other large alkanes, O(106 -1). The dominant energetic
step for large alkane surface ignition is hypothesized to be oxygen
desorption at saturation coverage as has been suggested for methane.
@article{Williams2006,
abstract = {Through online mass spectrometry it is demonstrated that steady-state
production of syngas (CO and H2) can be attained within 5 s after
admitting large alkanes (i-octane, n-octane, n-decane, or n-hexadecane)
and air into a short-contact-time reactor by using an automotive
fuel injector and initially preheating the Rh-coated catalyst above
the respective catalytic autoignition temperature for each fuel.
Minimum catalytic autoignition temperatures on Rh were ~260 [deg]C
for n-octane and 240 [deg]C for i-octane and n-decane. In contrast,
catalytic autoignition of n-hexadecane indirectly occurred at temperatures
(>220 [deg]C) lower than those of the other fuels investigated because
of exothermic homogeneous chemistry that preheated the catalyst (30-60
[deg]C) to a temperature (~280 [deg]C) sufficient for surface lightoff.Additionally,
the ignition kinetics for the large alkanes were determined and compared
with those of methane. The step controlling surface ignition possessed
an apparent activation energy of ~78 kJ/mol that was not significantly
different between fuels (p > 0.05). However, a significant difference
was found between the ignition preexponential for methane, O(104
s-1), and the other large alkanes, O(106 -1). The dominant energetic
step for large alkane surface ignition is hypothesized to be oxygen
desorption at saturation coverage as has been suggested for methane.},
added-at = {2007-11-22T09:11:49.000+0100},
author = {Williams, Kenneth A. and Schmidt, Lanny D.},
biburl = {https://www.bibsonomy.org/bibtex/2f099b54e2287efffcf2690b9903d765f/tboehme},
endnotereftype = {Journal Article},
interhash = {88f5cc4d03a2246672bae59df2ffcf87},
intrahash = {f099b54e2287efffcf2690b9903d765f},
journal = {Applied Catalysis A: General},
keywords = {Alkanes Catalysis Lightoff Liquid Partial Reaction Rhodium Start-up Surface Transient catalyst experiments fuels ignition kinetics oxidation},
pages = {30-45},
shorttitle = {Catalytic autoignition of higher alkane partial oxidation on Rh-coated
foams},
timestamp = {2007-11-22T09:12:09.000+0100},
title = {Catalytic autoignition of higher alkane partial oxidation on Rh-coated
foams},
url = {http://www.sciencedirect.com/science/article/B6TF5-4HKCYVG-8/2/3a26157d307167f1dc47303425e93b8e },
volume = 299,
year = 2006
}