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SCALE-UP OF MICROCHANNEL REACTORS FOR FISCHER-TROPSCH
SYNTHESIS
Anna Lee Tonkovich*, Soumitra Deshmukh, Kai Jarosch, Luke Schrader, Sean
Fitzgerald, Dave Kilanowski, Jan Lerou, and Terry Mazanec
Velocys, Inc.
Summary
The scale-up of a microchannel reactor for Fischer-Tropsch (FT) synthesis has progressed through
multiple scales. Equivalent process performance was demonstrated across each scale. Small single
channel test reactors (~4 cm in length) have demonstrated excellent performance of an FT catalyst
provided by Oxford Catalysts, Ltd. Catalyst from the same batch was tested in two long microchannel
reactors (~62 cm in length), with equal performance at a GHSV of 12,400 hr-1
. Further the same
catalyst replicated the performance from both short and long single channel reactors in a pilot reactor
with 276 parallel process channels (~ 16 cm in length). The elusive premise of numbering up
microchannel has been demonstrated, enabling the scale-up of reactor capacity.
Keywords
Scale-up, multichannel, Fischer-Tropsch synthesis, Numbering-up
* To whom all correspondence should be addressed
Introduction
The early development of the FT process was
undertaken by Franz Fischer and Hanz Tropsch in
Germany in the 1920s and 1930s (1). The chemistry
discovered by Fischer and Tropsch is based on creating
long chain paraffinic hydrocarbons by polymerizing a
mixture of carbon monoxide (CO) and hydrogen (H2),
referred to as “synthesis gas”, at an elevated pressure and
temperature and in the presence of a cobalt catalyst. The
reaction is highly exothermic and selectivity to the
primary by-product, methane, is temperature sensitive
thus control of catalyst bed temperature is important for
high yield operation.
Over cobalt catalysts the primary products of FT
synthesis are paraffins with a carbon number distribution,
usually following the Anderson-Schulz-Flory distribution
with the exception of carbon numbers less than C4. The
reaction can be represented by the following chemical
equation:
nCO + (2n+1)H2 CnH2n+2 + H2O
Typical byproducts are liquefied petroleum gas (LPG)
and naphtha. After the FT process, heavier hydrocarbons
can be hydrocracked to produce distillate products,
notably diesel and jet fuels (2). FT derived transportation
fuels are typically referred to as synthetic fuels. Recently,
there has been interest in synthetic fuels for four reasons:
increasing world demand for fuels, the clean burning
nature of synthetic fuels due to the absence of impurities
(2), the increased desire to monetize stranded gas as
energy prices rise, and the growing interest in producing
renewable, environmentally-sustainable fuel from the
gasification of non-edible biomass.
The demonstration of nearly isothermal performance of
FT in a single microchannel has been described early in
the literature by Wang and co-workers (2). A
multichannel FT reactor was described by Jarosch and
co-workers (3) and the performance was compared to
predicted performance. This report compares the
performance of multiple microchannel reactors evaluated
with the identical F-T catalyst to clearly show how to
scale-up the microchannel reactors. Neither channel
length nor number of channels substantially changes the
catalyst performance, when it is operated in a nearly
isothermal microchannel reactor.
Experimental and Results
The scalability of microchannel reactors was
demonstrated by testing four reactors using an identical
catalyst (each reactor operated with fresh catalyst from the
same batch). This study also addresses the effect of
increasing channel length to increase productivity.
The first microchannel reactor (Short) had a characteristic
dimension (gap) of 1 mm, a width of 0.76 cm width and a
catalyst bed length of 3.8 cm length. The second reactor
(Long-A) contained one process microchannel with a
dual gap of 1 mm for two-thirds of the channel width and
0.5 mm for one-third of the channel width. The channel
width was 0.6 cm and the catalyst bed length was 61.6
cm. The third reactor (Long B) had a catalyst bed length
of 61.6 cm, a width of 0.6 cm and a uniform gap of 1 mm.
The final reactor, (Pilot), had 276 process channels where
each process channel had a dimension of 0.3 cm width, 1
mm gap, and 16.5 cm length. For the first three single
channel reactors, heat was removed using hot oil flowing
co-currently in microchannels flanking the process
channel. The cooling medium employed in the pilot
reactor was water maintained under partial boiling
conditions. In the pilot reactor layers with catalyst
containing process microchannels were flanked on either
side by layers containing coolant microchannels. Process
and coolant microchannels were oriented at with their
major axes orthogonal to produce a cross-flow
architecture.
Each reactor was loaded with a catalyst obtained from
Oxford Catalysts, Ltd (OCL). The Co-based catalyst is
based on the OCL patented OMX method for producing
highly active and selective FT catalysts (5).
Figure 1. Pilot-scale FT Microchannel reactor with 276
parallel process channels and 132 coolant channels. The
reactor is shown as it is installed in a pressure
containment shell.
The operating conditions were varied for each reactor, but
similar conditions were also tested across each reactor to
validate scale-up in both length and number of channels.
The FT feed was held constant with a 2:1 ratio of
hydrogen to carbon monoxide and 16% diluent of
nitrogen. The feed pressure inlet was held constant at 350
psig and the average reaction temperature was maintained
at about 210 C. The feed gas flowrate was set to achieve a
GHSV of 12,400 hr-1
for each of the four reactors. The
results are shown in Figure 2.
For all four reactors the selectivity to methane averaged
between 8% and 9% while the CO conversion ranged
from 70% to 75% over the range of time-on-stream. The
performance as a function of time-on-stream was similar
across the four reactors and shows the natural deactivation
of the FT process that is expected with the build up of
waxes. Each reactor was regenerated and the
performance was brought back to near initial levels.
0.0%
10.0%
20.0%
30.0%
40.0%
50.0%
60.0%
70.0%
80.0%
90.0%
100.0%
0.0 50.0 100.0 150.0 200.0 250.0 300.0 350.0
Time on stream [hrs]
COConversion,CH4Selectivity[%]
Single Channel (Long-A) - CO Conv
Single Channel (Short) - CO Conv
Single Channel (Long-A) - CH4 Sel
Single Channel (Short) - CH4 Sel
Single Channel (Long-B) - CO Conv
Single Channel (Long-B) - CH4 Sel
Pilot - CO Conv
Pilot - CH4 Sel
Figure 3. Performance comparison is shown for four
microchannel reactors under equal reaction conditions.
Conclusions
The scalability of microchannel reactors was
demonstrated experimentally using four reactors,
demonstrating an increase in microchannel length and
number of channels with equivalent performance.
References
(1) Strange, A. M.; AIChE 2003 Spring National Meeting,
New Orleans, LA, 2003.
(2) Dry, M.E., High quality diesel via the Fischer-Tropsch
process – a review, J Chem Technol Biotechnol, v77, pp43-
50, 2001
(3) Wang, Y, Vanderwiel, D., Tonkovich, A., Gao, Y., Baker,
E., US 6,451,864, issued 2002
(4) Jarosch, K., Yang, B., Fitzgerald, S., Taha, R., Mazanec,
T., Tonkovich, A., Reduced Complexity in the
Representation of Fischer Tropsch Chemistry, Prepr. Pap.-
Am. Chem. Soc., Div. Fuel Chem, 2008, 53 (1), 1-2.
(5) Green, M., Xiao, T., US 2005 0250863 A1

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SCALE-UP OF MICROCHANNEL REACTORS FOR FISCHER-TROPSCH

  • 1. SCALE-UP OF MICROCHANNEL REACTORS FOR FISCHER-TROPSCH SYNTHESIS Anna Lee Tonkovich*, Soumitra Deshmukh, Kai Jarosch, Luke Schrader, Sean Fitzgerald, Dave Kilanowski, Jan Lerou, and Terry Mazanec Velocys, Inc. Summary The scale-up of a microchannel reactor for Fischer-Tropsch (FT) synthesis has progressed through multiple scales. Equivalent process performance was demonstrated across each scale. Small single channel test reactors (~4 cm in length) have demonstrated excellent performance of an FT catalyst provided by Oxford Catalysts, Ltd. Catalyst from the same batch was tested in two long microchannel reactors (~62 cm in length), with equal performance at a GHSV of 12,400 hr-1 . Further the same catalyst replicated the performance from both short and long single channel reactors in a pilot reactor with 276 parallel process channels (~ 16 cm in length). The elusive premise of numbering up microchannel has been demonstrated, enabling the scale-up of reactor capacity. Keywords Scale-up, multichannel, Fischer-Tropsch synthesis, Numbering-up * To whom all correspondence should be addressed Introduction The early development of the FT process was undertaken by Franz Fischer and Hanz Tropsch in Germany in the 1920s and 1930s (1). The chemistry discovered by Fischer and Tropsch is based on creating long chain paraffinic hydrocarbons by polymerizing a mixture of carbon monoxide (CO) and hydrogen (H2), referred to as “synthesis gas”, at an elevated pressure and temperature and in the presence of a cobalt catalyst. The reaction is highly exothermic and selectivity to the primary by-product, methane, is temperature sensitive thus control of catalyst bed temperature is important for high yield operation. Over cobalt catalysts the primary products of FT synthesis are paraffins with a carbon number distribution, usually following the Anderson-Schulz-Flory distribution with the exception of carbon numbers less than C4. The reaction can be represented by the following chemical equation: nCO + (2n+1)H2 CnH2n+2 + H2O Typical byproducts are liquefied petroleum gas (LPG) and naphtha. After the FT process, heavier hydrocarbons can be hydrocracked to produce distillate products, notably diesel and jet fuels (2). FT derived transportation fuels are typically referred to as synthetic fuels. Recently, there has been interest in synthetic fuels for four reasons: increasing world demand for fuels, the clean burning nature of synthetic fuels due to the absence of impurities (2), the increased desire to monetize stranded gas as energy prices rise, and the growing interest in producing renewable, environmentally-sustainable fuel from the gasification of non-edible biomass. The demonstration of nearly isothermal performance of FT in a single microchannel has been described early in the literature by Wang and co-workers (2). A multichannel FT reactor was described by Jarosch and co-workers (3) and the performance was compared to predicted performance. This report compares the performance of multiple microchannel reactors evaluated with the identical F-T catalyst to clearly show how to scale-up the microchannel reactors. Neither channel length nor number of channels substantially changes the catalyst performance, when it is operated in a nearly isothermal microchannel reactor.
  • 2. Experimental and Results The scalability of microchannel reactors was demonstrated by testing four reactors using an identical catalyst (each reactor operated with fresh catalyst from the same batch). This study also addresses the effect of increasing channel length to increase productivity. The first microchannel reactor (Short) had a characteristic dimension (gap) of 1 mm, a width of 0.76 cm width and a catalyst bed length of 3.8 cm length. The second reactor (Long-A) contained one process microchannel with a dual gap of 1 mm for two-thirds of the channel width and 0.5 mm for one-third of the channel width. The channel width was 0.6 cm and the catalyst bed length was 61.6 cm. The third reactor (Long B) had a catalyst bed length of 61.6 cm, a width of 0.6 cm and a uniform gap of 1 mm. The final reactor, (Pilot), had 276 process channels where each process channel had a dimension of 0.3 cm width, 1 mm gap, and 16.5 cm length. For the first three single channel reactors, heat was removed using hot oil flowing co-currently in microchannels flanking the process channel. The cooling medium employed in the pilot reactor was water maintained under partial boiling conditions. In the pilot reactor layers with catalyst containing process microchannels were flanked on either side by layers containing coolant microchannels. Process and coolant microchannels were oriented at with their major axes orthogonal to produce a cross-flow architecture. Each reactor was loaded with a catalyst obtained from Oxford Catalysts, Ltd (OCL). The Co-based catalyst is based on the OCL patented OMX method for producing highly active and selective FT catalysts (5). Figure 1. Pilot-scale FT Microchannel reactor with 276 parallel process channels and 132 coolant channels. The reactor is shown as it is installed in a pressure containment shell. The operating conditions were varied for each reactor, but similar conditions were also tested across each reactor to validate scale-up in both length and number of channels. The FT feed was held constant with a 2:1 ratio of hydrogen to carbon monoxide and 16% diluent of nitrogen. The feed pressure inlet was held constant at 350 psig and the average reaction temperature was maintained at about 210 C. The feed gas flowrate was set to achieve a GHSV of 12,400 hr-1 for each of the four reactors. The results are shown in Figure 2. For all four reactors the selectivity to methane averaged between 8% and 9% while the CO conversion ranged from 70% to 75% over the range of time-on-stream. The performance as a function of time-on-stream was similar across the four reactors and shows the natural deactivation of the FT process that is expected with the build up of waxes. Each reactor was regenerated and the performance was brought back to near initial levels. 0.0% 10.0% 20.0% 30.0% 40.0% 50.0% 60.0% 70.0% 80.0% 90.0% 100.0% 0.0 50.0 100.0 150.0 200.0 250.0 300.0 350.0 Time on stream [hrs] COConversion,CH4Selectivity[%] Single Channel (Long-A) - CO Conv Single Channel (Short) - CO Conv Single Channel (Long-A) - CH4 Sel Single Channel (Short) - CH4 Sel Single Channel (Long-B) - CO Conv Single Channel (Long-B) - CH4 Sel Pilot - CO Conv Pilot - CH4 Sel Figure 3. Performance comparison is shown for four microchannel reactors under equal reaction conditions. Conclusions The scalability of microchannel reactors was demonstrated experimentally using four reactors, demonstrating an increase in microchannel length and number of channels with equivalent performance. References (1) Strange, A. M.; AIChE 2003 Spring National Meeting, New Orleans, LA, 2003. (2) Dry, M.E., High quality diesel via the Fischer-Tropsch process – a review, J Chem Technol Biotechnol, v77, pp43- 50, 2001 (3) Wang, Y, Vanderwiel, D., Tonkovich, A., Gao, Y., Baker, E., US 6,451,864, issued 2002 (4) Jarosch, K., Yang, B., Fitzgerald, S., Taha, R., Mazanec, T., Tonkovich, A., Reduced Complexity in the Representation of Fischer Tropsch Chemistry, Prepr. Pap.- Am. Chem. Soc., Div. Fuel Chem, 2008, 53 (1), 1-2. (5) Green, M., Xiao, T., US 2005 0250863 A1