Ind. Eng. Chem. Res.

1996, 35, 99-105 99

Effect of Reaction Pressure on Octane Number and Reformate and

Hydrogen Yields in Catalytic Reforming

Kjell Moljord,* Hilde Gunn Hellenes, Anne Hoff, and Ingunn Tanem
SINTEF Applied Chemistry, N-7034 Trondheim, Norway

Knut Grande
Statoil Research Centre, N-7004 Trondheim, Norway

Anders Holmen
Department Industrial Chemistry, NTH, The University of Trondheim, N-7034 Trondheim, Norway

The effect of reaction pressure in catalytic reforming was studied in a pilot reactor with a
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commercial Pt-Re/Al2O3 reforming catalyst and a hydrotreated naphtha from a North Sea crude.
Reformate and hydrogen yields, research octane numbers (RON), and reformate composition at
reactor pressures in the range of 12-25 bar were measured as a function of temperature in the
range of 95-105 RON. Reformate and hydrogen yields increased as the pressure was reduced.
This effect was more pronounced at high severity and in the high-pressure range. For the lower
reaction pressures the hydrogen yields increased with increasing severity, but for the higher
pressures the hydrogen yields started to decline above certain severities. RON was linearly
dependent on the concentration of aromatics in the reformate, although the selectivity toward
aromatics depended on both pressure and temperature. Less hydrodealkylation of C8 and heavier
aromatics to benzene and toluene resulted in a shift toward xylenes and heavier aromatic
components when pressure was lowered. Variations in the degree of paraffin isomerization did
not influence RON significantly at those severities.

Introduction to increase the hydrotreating capacity in the refineries.

Catalytic reforming is an important process for con-
version of low-octane naphthas into high-octane motor
fuels. In a modern refinery catalytic reforming is also
an important source of hydrogen for a number of
processes. Naphtha consists of a mixture of hydrocar-
bons having 6-10 carbon atoms, and the low-octane
components should be converted to components with
better octane rating, mainly aromatics and i-paraffins,
in the same boiling range. However, even with modern
advanced catalysts those transformations are accom-
panied by a significant loss of reformate and hydrogen
yields, as a portion of the feed is converted to fuel gas
(C1 + C2) and LPG (C3 + C4).
Recent legislation requires a reduction in emissions
of volatile and toxic components in gasoline sold in
certain areas in the US. This affects hydrocarbons with
high-octane quality, specifically n-butane, light olefins,
and aromatics (Unzelman, 1990). As reformate is a
major source of aromatics in gasoline, reduced reformer
severity can be seen as one way to reduce the amount
of aromatics in gasoline. The addition of oxygenates
such as methyl tert-butyl ether (MTBE) to gasoline does
have beneficial effects on CO emissions (Davis, 1992),
and the octane contribution from those additives will
allow refiners to reduce reformer severity.
The general phaseout of lead in gasoline has led to
increased catalytic reformer severity which has been
accompanied by a significant loss of reformate yield and
cycle length. However, the additional hydrogen gener-
ated by increased reformer severity has been utilized
* Author to whom correspondence should be addressed.
e-mail address: kjell.moljord@kjemi.sintef.no. Fax: +47 73
596995.
0888-5885/96/2635-0099$12.00/0
As new legislation on diesel and fuel oil sulfur content
is introduced, the demand for hydrogen will increase
further. The refineries will thus face a severe problem
with hydrogen supply if reformer severity is reduced as
a consequence of gasoline reformulation. In order to
maintain the hydrogen production when reducing re-
former severity, refiners might be considering changes
in reformer operating conditions. It is known (Bourn-
onville and Franck, 1988) that both hydrogen and
reformate yields increase as the reformer pressure is
lowered, but at the expense of increased catalyst deac-
tivation and shorter cycle lengths. With reduced re-
former severity there might be room, however, for some
reduction of reaction pressure without loss of cycle
length.
The present work was carried out to examine the
effect of reformer pressure on the yields of reformate
and hydrogen, as well as on the detailed reformate
composition. In particular, emphasis is put on how the
reformate composition changes with the reaction condi-
tions, as this kind of information is relevant to gasoline
reformulation.
The study was carried out in relatively small isother-
mal reactors without recycle, originally constructed for
testing and comparison of different catalysts and feed-
stocks with respect to catalyst activity, selectivity, and
stability. As discussed by Sie and Blauwhoff (1991), this
is a type of equipment which will allow discrimination
between reforming catalysts and can be used to deter-
mine the effect of changes in operating variables as well.
Exact predictions of the performance of a commercial
reformer unit consisting of 3-4 adiabatic reactors will
need additional modeling of the kinetics and the actual
reactor configuration.
© 1996 American Chemical Society
100 Ind. Eng. Chem. Res., Vol. 35, No. 1, 1996
Figure 1. Flow diagram for each reactor of the pilot reactor unit (MFC ) mass flow controller; PC ) pressure controller).
Experimental Section
Reactor Unit. A schematic flow diagram of the
reactor unit is given in Figure 1. The unit consists of
three once-through isothermal reactors in parallel,
designed for simultaneous testing of different catalysts
(or feedstocks). The three reactors are operated inde-
pendently, which means that a set of three different
experimental conditions can be investigated at the same
time. The reactors are heated in three separate baths
of circulating molten salt, assuring very high rates of
heat transfer and good temperature control as reported
by Van Trimpont et al. (1988). Each reactor tube has
an internal diameter of 19 mm and an available length
of approximately 750 mm and is equipped with a central
tube for a moveable thermocouple, leaving about 190
cm3 of reactor volume.
The catalyst bed was diluted by a low-surface, chloride-
free alumina with the same particle shape and size
(1/16 in. extrudates) as the catalyst itself. The degree of
dilution was varied in three different zones of each
reactor, with the highest dilution at the reactor inlet,
in order to minimize the temperature drop caused by
the rapid, endothermic naphthene dehydrogenation. The
temperature drop at the reactor inlet, measured with
the axial thermocouple, was less than 5 °C.
The reactor effluent was analyzed by on-line GC
analysis prior to condensation. Each reactor line was
equipped with a HP 5890 GC with a flame ionization
detector (FID), interfaced with a PC for data handling
and storage. The method of analysis, based on HP’s
PONA analysis, included all important hydrocarbons up
to C11. Heavier components than this were only present
in trace amounts and were not analyzed. Research
octane numbers (RON) were calculated from GC analy-
sis based on an adapted version of the method presented
by Anderson et al. (1972). The hydrogen yield was
calculated from GC analysis as the hydrogen balance
over the reactor.
The critical operating variables (temperatures and
pressures) were monitored continuously by an in-house-
programmed PC which would shut the unit down
automatically if certain safety limits were exceeded.
Test Procedures. The tests were performed with
35 g of catalyst in each reactor, and the catalyst was
oxychlorinated, reduced, and sulfided in the reactors
prior to testing. Oxychlorination was carried out in
order to ensure uniform chloride content as well as a
highly dispersed metal function on the catalyst. Oxy-
chlorination was carried out in flowing air with a given
ratio of H2O and HCl at 500 °C, before “rejuvenation”
of the metal function in dry air. The catalyst was then
reduced in H2 at 10 bar, with temperature ramping of
+20 °C/h from 400 to 480 °C and kept at 480 °C for 2 h.
Finally the catalyst was presulfided with 0.08% H2S in
H2 at 425 °C until breakthrough of H2S. After flushing
with pure H2, naphtha was introduced at 400 °C, and
the reactor temperature was slowly raised to 480 °C.
The tests were carried out at WHSV ) 2.03, a molar
ratio H2/hydrocarbon ) 4.34, and pressures of 12, 16,
20, and 25 bar. For each pressure level the reaction
was examined at three different temperatures, 480, 495,
and 510 °C, and each temperature was kept constant
for 30-50 h. Prior to this the catalyst was “lined out”
at either 16 or 25 bar at 480 °C for about 125 h to
stabilize the fresh catalyst.
By carrying out a number of repeated runs, the
standard deviations for reformate and hydrogen yields
were determined as 0.25 and 0.02 wt %, respectively,
and 0.25 units for RON. In order to achieve this, a
detailed calibration of the GC systems had to be carried
out, and the reactor thermocouples, the hydrogen mass
flow controllers, and naphtha feed pumps were thor-
oughly calibrated between each test run.
Catalyst and Feed. The tests were carried out with
a commercial, balanced Pt-Re (0.3 wt % Pt and 0.3 wt
% Re) reforming catalyst, supplied, and used in the form

Table 1. Naphtha Composition (wt %) As Determined by
GC Analysis
paraffins cyclopentanes cyclohexanes aromatics total
C5 0.2 3.2 4.9 1.4 0.2
C6 6.3 5.1 8.7 6.4 15.8
C7 11.2 6.2 1.5 8.3 31.4
C8 14.2 1.2 6.8 2.7 30.2
C9 8.0 0.1 0.4 18.7
C10 3.2 3.7
C11 0.1 0.1
total 43.2 15.7 22.0 19.2 100.1
of 1/16 in. extrudates. A hydrotreated, straight-run
naphtha from a North Sea crude was used as feedstock
in the test program. The compostion as determined by
GC analysis is given in Table 1. The hydrotreated
naphtha contained less than 0.5 ppm sulfur. The
naphtha was dried over a 4-Å molecular sieve and stored
under an inert gas (Ar) prior to use. Using Karl-
Fischer analysis, the water content of dried naphtha
was measured to 5-8 wt ppm. In order to compensate
the effect of the remaining water on the chloride content
of the catalyst, 0.8 wt ppm chloride as 1,1,2-trichloro-
ethane was added to the naphtha. The chloride content
of the catalyst at different positions in the reactor was
determined after each test run, to check the water/
chloride balance during testing.
H2 (99.995%, Norsk Hydro), supplied from gas cylin-
ders, was passed over a deoxo catalyst (BASF R3-11)
at 70 °C and a 4-Å molelular sieve to remove traces of
oxygen and water. The deoxo catalyst as well as the
molecular sieve were regenerated before each test run.
Results and Discussion
The conversion and selectivity in catalytic reforming
are functions of thermodynamic and kinetic factors for
the great number of reactions taking place. The desired
reactions are the following (Gates et al., 1979):
(a) Dehydrocyclization of paraffins into aromatics.
(b) Isomerization of alkylcyclopentanes into cyclohex-
anes.
(c) Dehydrogenation of cyclohexanes into aromatics.
(d) Isomerization of linear paraffins into isoparaffins.
The dehydrocyclization and dehydrogenation reac-
tions are desired also because they produce hydrogen.
Both reactions are favored by low reaction pressure and
high temperature.
The most important side reactions are as follows:
(a) Hydrocracking of naphthenes and paraffins.
(b) Hydrodealkylation of aromatics.
(c) Alkylation and transalkylation of aromatics.
(d) Coke formation.
Hydrocracking and hydrodealkylation are mostly
undesired reactions because they lower the reformate
and hydrogen yields, while coke formation deactivates
the catalyst and reduces the cycle length, i.e., the time
between catalyst regeneration. Indirectly, coke forma-
tion also influences the reformate and hydrogen yields
because the loss in catalyst activity is normally com-
pensated for by higher reaction temperatures which
favor hydrocracking reactions (Little, 1985).
Octane Number and Reformate Yield. While the
dehydrogenation of cyclohexanes to aromatics is selec-
tive and nearly complete, the reactions involving paraf-
fins and alkylcyclopentanes are the most critical ones
for obtaining good reformate yield during high-severity
reforming (Hughes et al., 1988). High octane numbers
Ind. Eng. Chem. Res., Vol. 35, No. 1, 1996 101
Figure 2. RON as a function of the total concentration of
aromatics in the reformate at different reaction conditions (dif-
ferent temperatures and pressures).
can only be achieved through extensive paraffin dehy-
drocyclization, as the octane number obtained from
dehydrogenation of naphthenes and from isomerization
of paraffins is well below the desired values (Sterba and
Haensel, 1976). Paraffin dehydrocyclization is relatively
slow and comparable to paraffin hydrocracking under
normal reformer conditions (Sterba and Haensel, 1976).
However, under high-severity reforming paraffin dehy-
drocyclization to aromatics can approach thermody-
namic equilibrium values. Furthermore, hydrocracking
of paraffins contributes to the high octane numbers by
concentrating the aromatics in the reformate.
RON depends highly on the concentration of aromat-
ics in the reformate. As shown in Figure 2, there is a
linear correlation between RON and the total concen-
tration of aromatics in the reformate, regardless of
reaction pressure and temperature. For a given feed-
stock, variations in the yields of other components
(paraffinic or naphthenic) are therefore of minor impor-
tance for the research octane number at high-severity
reforming. RON is primarily a function of the yield of
aromatics and the yield of reformate (C5+), as those two
values combined define the concentration of aromatics
in the reformate. As RON is so closely linked to the
concentration of aromatics in the reformate, changing
the operating variables will not influence the content
of aromatics in the reformate at a given RON.
A simple model for calculation of RON directly from
the aromatics concentration has been proposed by
McCoy (1975). Based on a linear relationship between
the octane number and the concentration of aromatics,
RON can be expressed as:
RON ) A × (% aromatics) + B
The values obtained by linear regression were A )
0.4822 and B ) 64.976 with a correlation coefficient r
) 0.9970 over the whole severity range of 95-105 RON.
However, it has been demonstrated that this method
is not universal, as the coefficients A and B depend on
the feedstock (Petroff et al., 1988). Various models
based on a linear octane contribution of different
components determined by gas chromatography have
been proposed (Jenkins et al., 1968; Walsh and Mor-
timer, 1971; Anderson et al., 1972; Dorbon et al., 1990).
RON values calculated from GC analysis by an adapted
version of the method presented by Anderson et al.
(1972) corresponded to test engine RON values for the
debutanized reformate samples (25 samples) with a
standard deviation of 0.55 RON units, which is close to
the accuracy of the engine measurements.
102 Ind. Eng. Chem. Res., Vol. 35, No. 1, 1996
Figure 3. RON (a) and reformate yield (b) as a function of
reaction temperature at different reaction pressures.
In parts a and b of Figure 3, RON and the reformate
yield are shown as a function of temperature at 12, 16,
20, and 25 bar pressure. Both RON and reformate yield
are favored by low pressure. As a consequence, a lower
temperature is needed to obtain a given RON at a lower
reaction pressure, and the reformate yield increases as
a direct result of low pressure as well as of low
temperature. The effect of pressure on reformate yield
increases with the temperature, while the effect of
pressure on RON is almost temperature-independent.
For a given severity in the range of 99-102 RON, the
temperature can be lowered by 8-9 °C when going from
25 to 20 bar and by 4-5 °C when going from 16 to 12
bar (Figure 3a). As can be seen from Figure 3b, a
temperature reduction of 9.0 °C gives a yield benefit of
2.7 wt % at 20 bar, in addition to a yield increase of 1.5
wt % when reducing the pressure from 25 to 20 bar at
constant temperature (498.0 °C, corresponding to 99.0
RON at 25 bar). The yield benefit when reducing the
pressure from 16 to 12 bar at a constant temperature
(484.3 °C, corresponding to 99.0 RON at 16 bar) is 1.0
wt %, while a temperature reduction of 4.7 °C at 12 bar
gives an additional 1.0 wt % yield benefit. At 102 RON
the gain in reformate yield by reducing the pressure is
even greater than at 99 RON. This is a result of the
steeper decline in reformate yield with temperature at
high pressure (Figure 3b), so that the difference in yield
increases with the severity.
The incremental values, calculated as weight percent
reformate yield increase per bar reduction in pressure,
are given as a function of RON in Figure 4. The benefit
in weight percent reformate yield per bar is higher in
the high-pressure range than in the lower, regardless
of severity. Furthermore, the yield benefit per bar
increases substantially with increased severity.
Aromatic Components. The aromatics did account
for 62-82 wt % of the reformate, depending on the
reaction conditions. Toluene was by far the single
dominating component, accounting for 23-31 wt % of
Figure 4. Increase in the yield of reformate per bar pressure
reduction in the intervals of 20-25 and 12-16 bar.
the reformate, while benzene accounted for 7-12 wt %.
In Figure 5 the yields of the most important aromatics
are shown as a function of temperature at pressures
between 12 and 25 bar.
The yields of benzene and toluene respond to changes
in the temperature in a similar way: As expected the
yields increase with increasing temperature because
dehydrocyclization and dehydrogenation reactions are
favoured by high temperature. Furthermore, benzene
and toluene formation is favored by lower pressure. On
the contrary, the yield of ethylbenzene is reduced with
increasing temperature, probably as an effect of more
side-chain hydrodealkylation. This reaction is favored
by high pressure and gives benzene and ethane as
products (Van Broekhoven et al., 1990). The xylenes
are less susceptible to high-severity hydrodealkylation
than ethylbenzene, and both p- and m-xylene increase
with increased temperature for all reaction pressures
except at 25 bar, where the yields level off. The yield
of o-xylene, however, reaches a maximum at 495 °C and
decreases at higher temperatures. p-Xylene differs from
the two other xylenes by a much lower pressure depen-
dency. The heavier aromatics, lumped as C9+, diminish
with increasing temperature for all the pressures stud-
ied but are more pronounced the higher the pressure.
The C9+ lump consists of alkylated benzenes, and the
strong pressure dependency as with ethylbenzene is
probably a result of higher dealkylation tendency for
larger alkyl groups on benzene. For C9+ aromatics, this
results in a net loss to lighter aromatics such as benzene
and toluene with increasing severity. As RON is closely
linked to the total concentration of aromatics in the
reformate (Figure 2), changing the operating variables
will only affect the distribution between the different
aromatic components, while the total content of aromat-
ics in the reformate is defined by the RON value.
The content of benzene in the reformate is shown as
function of RON for different pressures in Figure 6. It
is clearly seen that at high severity the benzene content
depends on the reaction pressure. At severities above
ca. 99 RON the content of benzene increased with
increasing pressure as a result of increased benzene
(and toluene) formation from heavier aromatics. At 102
RON the content of benzene in the reformate differed
by 1.0 wt % (10%) when comparing the results at 12
and 25 bar pressure. At high severity the benzene
content of the reformate will therefore be significantly
reduced when reformer pressure is lowered. However,
at severities below 99 RON the opposite effect was
observed.
i-Paraffins. Isomerizations of n-paraffins to i-paraf-
fins, and particularly multibranched i-paraffins, are
 Ind. Eng. Chem. Res., Vol. 35, No. 1, 1996 103

Figure 5. Yield of different aromatics as a function of reaction temperature at different reaction pressures: (a) benzene, (b) toluene, (c)
ethylbenzene, (d) p-xylene, (e) m-xylene, (f) o-xylene, and (g) C9+ aromatics.

desired reactions that contribute to the increase in
octane numbers during naphtha reforming. It is com-
mon to assume that the isomerization reactions are
rapid enough to closely approach thermodynamic equi-
librium at normal reforming conditions (Gates et al.,
1979). However, the reactivity of the paraffins de-
creases as their carbon number decreases (Van Trim-
pont et al., 1988). Furthermore, multibranched isomers
are secondary products formed via single-branched
isomers (Van Trimpont et al., 1988), and equilibrium
is largely attained between normal paraffins and their
single-branched isomers (Kmak and Stuckey, 1973).
Since the i-paraffins crack much easier than the corre-
sponding n-paraffins, it is not obvious that the i- to
n-ratios for all paraffins are defined by their thermo-
dynamic equilibrium at high-severity reforming. As the
paraffin isomerization reactions are slightly exothermic,
the equilibrium ratio between i- and n-paraffins dimin-
ishes slightly with increasing reaction temperature.
Furthermore, the isomerization equilibrium is indepen-
dent of the reaction pressure.
Figure 7 shows the experimental i/n-ratios for C4, C5,
C6, and C7 paraffins at different pressures and temper-
atures. The i/n-ratios for C6 and C7 increase from 480
to 495 °C, signifying that chemical equilibrium is not
attained between i- and n-paraffins for hexanes and
104 Ind. Eng. Chem. Res., Vol. 35, No. 1, 1996

Figure 6. Concentration of benzene in the reformate as a function

of RON at different reaction pressures.

heptanes at these severities. At higher temperatures

(510 °C) the i/n-ratios for C6 and C7 paraffins approach
thermodynamic values only at the lowest pressures, 12
and 16 bar. At higher pressures an increase in the
temperature above 495 °C results in a net consumption
of i-heptanes, exceeding the consumption of n-heptane
due to hydrocracking. The same was observed for the
hexanes as well, although to a lesser extent. For C6 and
C7 paraffins the i/n-ratios at high severity seem to be
governed by the consumption of i- and n-paraffins by
hydrocracking. The isomerization reactions are obvi-
ously not fast enough at those reaction conditions to
compete with the hydrocracking reactions, in particular
at high pressures.
On the contrary, the i/n-ratios of the pentanes dimin-
ish with increasing temperature independent of the
pressure, as is expected for the isomerization reaction
at thermodynamic equilibrium. The measured value at
480 °C (Kexp ) 1.8) corresponds very well with the
calculated equilibrium constant (Kth ) 1.89, with data
from Stull et al., 1969) but falls more rapidly with
increasing temperature than expected. This could be
caused by either extensive cracking of i-pentane or
formation of n-pentane from cracking. As can be seen
from Figure 2, the variations in the degree of paraffin
isomerization with the operating conditions did not
influence RON significantly.
Hydrogen. For a given feedstock the yield of hydro-
gen is determined by the balance between hydrogen-
producing and hydrogen-consuming reactions. Dehy-
drogenation and dehydrocyclization are the most im-
portant hydrogen-producing reactions, while hydro-
cracking and hydrogenolysis, both undesired reactions
which lower the reformate yield, are hydrogen consum-
ing.
Figure 8 shows the yield of hydrogen as a function of
RON at different pressures. Hydrogen production is
Figure 7. i/n-ratios for different paraffins as a function of reaction
favored by low pressures, and more so the higher the temperature at different reaction pressures: (a) butanes, (b)
severity. At 102 RON, the yield of hydrogen increased pentanes, (c) hexanes, and (d) heptanes.
by 0.35 wt % (16%) when the pressure was lowered from
16 to 12 bar and by 0.60 wt % (50%) when the pressure effect of severity on hydrogen yields therefore depends
was lowered from 25 to 20 bar. The same pressure on the operating conditions: At reformer pressures
reductions at 99 RON gave lower hydrogen yield ben- below 16 bar the hydrogen yields decrease when the
efits, 0.25 and 0.52 wt %, respectively. severity is reduced, while at higher pressures the
At 12 and 16 bar the hydrogen yield increases with hydrogen yields may even increase when lowering the
increasing severity. At higher pressures the hydrogen- severity.
consuming reactions are favored and the hydrogen
yields diminish with increasing severity. The severity Conclusions
at which the hydrogen-consuming reactions balance the
hydrogen-producing reactions decreases with increasing The study shows that a reduction of the reaction
pressure. At 25 bar the maximum hydrogen yield was pressure results in higher reformate and hydrogen
attained at a severity below 98 RON, while at 12 bar yields. This effect is more pronounced at high-severity
the maximum hydrogen yield was above 104 RON. The operation and in the high-pressure range. Maximum

Figure 8. Yield of hydrogen as a function of RON at different
reaction pressures.
hydrogen yields were observed at lower severity the
higher the pressure.
A linear correlation between RON and the content of
aromatics in the reformate was found: Independent of
the reaction conditions, a given concentration of aro-
matics in the reformate is needed to achieve a certain
RON value. However, the relative amount of the
different aromatic components depends on the operating
conditions. Less hydrodealkylation to benzene and
toluene results in a shift toward xylenes and heavier
aromatics at lower reaction pressure. Therefore, the
benzene content of the reformate decreases when the
pressure is lowered at high-severity operation.
Variations in the degree of paraffin isomerization as
a result of changing reaction conditions did not influence
RON significantly at those severities. The i/n-ratios of
C6 and C7 paraffins approach chemical equilibrium
values only at low reaction pressures and high severity.
At low severity chemical equilibrium apparently was not
reached for those isomerization reactions, while at high
pressure and high severity the branched isomers were
hydrocracked to give lower than equilibrium i- to
n-ratios.
Acknowledgment
The authors are grateful to Statoil for supporting this
work and for the permission to publish the results.
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Received for review October 6, 1994
Revised manuscript received May 19, 1995
Accepted September 12, 1995X
IE940582R
X
Abstract published in Advance ACS Abstracts, November
15, 1995.