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Oxidative Dehydrogenation of Propane To Propylene With Carbon Dioxide
Oxidative Dehydrogenation of Propane To Propylene With Carbon Dioxide
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اﻟﺨـﻼﺻــﺔ :
ﺗﺘﻨﺎول هﺬﻩ اﻟﻮرﻗﺔ ﻣﻮﺿﻮع ﺗﻄﻮﻳﺮ ﻋﻤﻠﻴﺔ ﺟﺪﻳﺪة ﻟﻠﺘﻜﺴﻴﺮ اﻟﺤﻔﺰي اﻟﻤﻤﻴﻊ ) (HS-FCCﻋﻨﺪ ﻋﻮاﻣﻞ ﺗ ﺸﻐﻴﻞ ﻣﺮﺗﻔﻌ ﺔ ﺑﻬ ﺪف زﻳ ﺎدة إﻧﺘﺎﺟﻴ ﺔ
اﻟﺒﺮوﺑﻴﻠﻴﻦ ﺑﻮﺳﺎﻃﺔ ﻓﺮﻳﻘﻲ ﺑﺤﺚ ﻣﻦ اﻟﻤﻤﻠﻜﺔ اﻟﻌﺮﺑﻴﺔ اﻟﺴﻌﻮدﻳﺔ واﻟﻴﺎﺑﺎن .وﻟﻘﺪ ﺗﻢ ﺗﺸﻐﻴﻞ اﻟﻌﻤﻠﻴﺔ ﻓ ﻲ ﻣ ﺼﻨﻊ ﺗﺠﺮﻳﺒ ﻲ ﺷ ﺒﻪ ﺻ ﻨﺎﻋﻲ ﺑﻄﺎﻗ ﺔ )(30
ﻼ ﺑﺎﻟﻴﻮم ﺑﺎﻟﻘﺮب ﻣﻦ ﻣﺼﻔﺎة أراﻣﻜﻮ اﻟﺴﻌﻮدﻳﺔ ،إﺿﺎﻓﺔ إﻟﻰ وﺣﺪة دﻓﻘﻴﺔ ﺑ ﺎردة )ﺑ ﺪون ﻟﻘ ﻴﻢ( ﺑﻄﺎﻗ ﺔ ) (500ﺑﺮﻣﻴ ﻞ ﺑ ﺎﻟﻴﻮم ﻓ ﻲ ﺷ ﺮآﺔ ﻧﻴﺒ ﻮن ﺑﺮﻣﻴ ً
ﻟﻠﺒﺘﺮول ﻓﻲ اﻟﻴﺎﺑ ﺎن .وﻣ ﻦ ﻣﻼﻣ ﺢ اﻟﻌﻤﻠﻴ ﺔ اﻟﺠﺪﻳ ﺪة إﺿ ﺎﻓﺔ ﺗﻌ ﺪﻳﻼت ﻣﻴﻜﺎﻧﻴﻜﻴ ﺔ إﻟ ﻰ ﻋﻤﻠﻴ ﺔ اﻟﺘﻜ ﺴﻴﺮ اﻟﺘﻘﻠﻴﺪﻳ ﺔ ) (FCCﻣ ﻊ ﺗﻐﻴ ﺮات ﻓ ﻲ ﻇ ﺮوف
اﻟﺘﺸﻐﻴﻞ وﺗﺮآﻴﺒﺎت اﻟﺤﻔ ﺎز .وﺗﺘﻤﺜ ﻞ ﻣﻼﻣ ﺢ اﻟﺘ ﺸﻐﻴﻞ اﻟﺮﺋﻴ ﺴﻴﺔ ﻟﻠﻌﻤﻠﻴ ﺔ ﺑﻨﻈ ﺎم ﺗﻔ ﺎﻋﻠﻲ ذات دﻓ ﻖ ﻣ ﻦ أﻋﻠ ﻰ إﻟ ﻰ أﺳ ﻔﻞ ،وإرﺗﻔ ﺎع درﺟ ﺔ ﺣ ﺮارة
اﻟﺘﻔﺎﻋﻞ وﻗﺼﺮ زﻣﻦ ﺗﻼﻣﺲ اﻟﻠﻘﻴﻢ ﻣﻊ اﻟﺤﻔﺎز ،إﺿﺎﻓﺔ إﻟﻰ ارﺗﻔﺎع ﻣﻌﺪل اﻟﺤﻔﺎز ﺑﺎﻟﻨﺴﺒﺔ ﻟﻠﺰﻳﺖ .وﺗﻢ إﺟﺮاء اﻟﺘﺠ ﺎرب اﻟﻤﻌﻤﻠﻴ ﺔ ﻓ ﻲ وﺣ ﺪﺗﻴﻦ ذات
دﻓﻖ ﻣﺨﺘﻠﻒ ،إﺿﺎﻓﺔ إﻟﻰ ﻣﺼﻨﻊ ﺗﺠﺮﻳﺒ ـﻲ ﺷ ﺒﻪ ﺻ ﻨﺎﻋﻲ ﺑﺎﺳ ﺘﺨﺪام ﺣﻔ ﺎزات ،وإﺿ ﺎﻓﺎت وﻟﻘ ﺎﺋﻢ زﻳ ﻮت ﻣﺨﺘﻠﻔ ﺔ .وأﻇﻬ ﺮت ﻧﺘ ﺎﺋﺞ اﻟﻔﺤ ﺺ ﺗﻔﻮﻗ ًﺎ
ﻷداء اﻟﻤﻔﺎﻋﻞ ذات اﻟﺪﻓﻖ ﻣﻦ أﻋﻠﻰ إﻟﻰ أﺳﻔﻞ وذﻟﻚ ﻟﻤﻨﻌﻪ اﻟﺨﻠﻂ اﻟﻌﻜﺴﻲ ﻣﻤﺎ أدى إﻟﻰ زﻳﺎدة إﻧﺘﺎﺟﻴﺔ اﻷﻟﻴﻔﻴﻨﺎت اﻟﺨﻔﻴﻔ ﺔ ) اﻹﻳﺜﻴﻠ ﻴﻦ واﻟﺒ ﺮوﺑﻴﻠﻴﻦ
واﻟﺒﻴﻮﺗﻴﻠﻴﻦ ( وﺗﻘﻠﻴﻞ إﻧﺘﺎج اﻟﻐﺎز اﻟﺨﻔﻴﻒ .وﺑﺎﺳﺘﺨﺪام زﻳﺖ اﻟﻐﺎز اﻟﻔﺮاﻏ ﻲ اﻟﻤ ﺸﺘﻖ ﻣ ﻦ ﺑﺘ ﺮول ﺧ ﺎم ﺑﺮاﻓﻴﻨ ﻲ وﺣﻔ ﺎز ﺧ ﺎص ﻧ ﻮع ) (USYذات
ﺛﺒﺎت ﻋﺎل وﺻﻠﺖ إﻧﺘﺎﺟﻴﺔ اﻟﺒﺮوﺑﻴﻠﻴﻦ إﻟﻰ ) (%25وزن ،وإﻧﺘﺎﺟﻴﺔ اﻟﺠﺎزوﻟﻴﻦ إﻟﻰ ) (%30وزن ﻋﻨﺪ ﻇﺮوف ﺗﺸﻐﻴﻞ اﻟﻌﻤﻠﻴﺔ .
Paper Received 9 May 2006; Revised 11 December 2006; Accepted 20 December 2006
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
ABSTRACT
A novel high-severity FCC process that maximizes propylene production is under
development by research teams in Saudi Arabia and Japan. The process has been
proven in a 30-BPD demonstration plant at Saudi Aramco’s refinery, Saudi Arabia,
and at a 500-BPD cold flow model at Nippon Oil Corporation, Japan. The HS–FCC
process combines mechanical modifications to conventional FCC with changes in
process variables and catalyst formulations. The process main operating features are
a down-flow reactor system, high reaction temperature, short contact time, and high
catalyst to oil ratio. Experimental runs were conducted in a downer- and riser-type
pilot plants and a demonstration plant using various catalysts, additives and feed oils.
The experimental results demonstrated the advantage of downer in suppressing back-
mixing, thus increasing the yield of light olefins (ethylene, propylene, and butylenes)
and reducing dry gas. Using paraffinic crude base VGO feed and proprietary USY
FCC catalyst, propylene yield of 25 wt% (feed basis) and gasoline yield of 30 wt%
were obtained under HS-FCC reaction conditions.
Key words: aromatics, cracking, downer, FCC catalysts, gasoline, octane, olefins,
propylene, riser.
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
1. INTRODUCTION
Increasing the yield of the valuable light olefins, especially propylene and butylenes, remains a major challenge for
many integrated refineries. As global petrochemical demand for propylene continues to grow, opportunities for
improved production routes will emerge. Propylene is used as a feedstock for a wide range of polymers, product
intermediates, and chemicals. Major propylene derivatives include polypropylene, acrylonitrile, propylene oxide, oxo-
alcohols, and cumene. These derivatives account for almost 90% of global propylene demand. In 2005, global demand
for propylene reached about 67 million tons and its annual demand is expected to increase by 4.8% during 2005–2010
[1,2]. The processing of propylene to polypropylene improves refinery margins and increases revenues because of the
high value of polypropylene.
Propylene has been considered a by-product of ethylene production via steam cracking of naphtha or other
feedstocks. However, this route has not been able to keep up with propylene demand. To make up this shortfall,
refineries capture propylene from fluid catalytic cracking (FCC) units and purify it to either chemical grade or polymer
grade propylene. Currently, FCC supplies 30 wt% of the world’s propylene and the remainder is co-produced from
steam cracking.
FCC continues to be the dominant conversion process for gasoline and light olefins production with a global capacity
of 14.2 million BPD. While refiners are under pressure to process heavier crudes, the FCC product slate is increasingly
shifting towards light olefins production (mainly propylene). More stringent specifications for gasoline are needed in the
future, for which the current FCC product slate is not optimal, because of high aromatics and olefins content.
2. FCC OPTIONS TO MAXIMIZE REFINERY PROPYLENE
The conventional FCC unit is typically operated at low to moderate severity with flexibility to swing between
maximum distillate and maximum gasoline mode [2,3]. This unit yields 3–4 wt% propylene. Improvements in FCC
catalysts, process design, hardware, and operation severity can boost propylene yield up to 25 wt% or higher. In FCC
practice, there are several options to increase the selectivity to light olefins [2]. The major options are as follows:
• Dedicated FCC catalysts
• ZSM-5 additives
• Higher severity operation (higher cracking temperature)
• Naphtha recycle and
• Dedicated new petrochemical FCC processes
Conventional FCC catalyst compositions contain a catalytic cracking component and amorphous alumina which is
necessary to provide the bottoms conversion. Catalytic cracking components are crystalline compounds such as
faujasite-type Y zeolite. Amorphous alumina may also be used as a binder to provide a matrix with enough binding
function to properly bind the crystalline cracking component when present. ZSM-5 based additive containing a small
pore zeolite (5.5 to 7.5 Å) is commonly added to the cracking catalyst in FCC to enhance gasoline octane and LPG
olefins production, especially propylene.
One cost effective way to increase the propylene yield from the FCC unit is the use of specialized catalysts that
contain ZSM-5 zeolite. An increasing number of refiners use as much as 10 wt% of ZSM-5 additives to obtain more than
9 wt% propylene. Because of its unique pore structure, ZSM-5 limits access to only linear or slightly branched
hydrocarbon molecules within the gasoline boiling point range. ZSM-5 based additive acts mainly by cracking C6+
gasoline olefins to smaller olefins such as propylene and butylenes [4]. These catalysts and additives increase the yield
of propylene and other light olefins at the expense of gasoline and distillate products.
The cracking of light hydrocarbons is another excellent option for an FCC-based refiner to produce and recover
propylene. Naphtha is the most common feedstock used in FCC cracking units for the incremental production of
propylene. Various process schemes for naphtha cracking in the FCC unit have been suggested and the simplest option
consists of feeding and cracking naphtha together with gas oil feed. Naphtha may also be injected at the bottom of the
fluidized riser reactor, before regenerated catalyst contacts gas oil feed, where it may be cracked at higher temperature
and catalyst/oil (C/O) ratio [5].
April 2008 The Arabian Journal for Science and Engineering, Volume 33, Number 1B
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
The need for a higher cracking temperature, a shorter contact time, and a higher C/O ratio lead to the conclusion that
the mechanical restrictions of existing FCC units prevent the optimization of the conventional process for maximum
olefin production [6]. Despite the various FCC technologies available to increase propylene yield, intense research
activity in this field is still being conducted. Table 1 presents a summary of emerging FCC processes for enhancing
refinery propylene [2].
3. FEATURES OF HS–FCC
The main objective of the high-severity FCC process is to produce significantly more propylene and high octane
number gasoline. The conceptual process and preliminary feasibility study of the HS–FCC process started in the mid
1990s [7]. For a 36 000 BPD conceptual unit and depending on the operating mode (gasoline mode operates at 550 ºC),
the HS–FCC doubles the amount of light olefins. At high-olefins mode (600 ºC), the unit provides three times more light
olefins accompanied with a minimum loss in gasoline as shown in Figure 1. The production of propylene is 2 to 4 times
higher than in the conventional FCC process. The study showed the high feasibility of HS–FCC even though the olefin
yield was not so high during the forepart of the development.
The special features of this new process (Table 2) include rapid feed vaporization, down-flow reactor, high severity,
short contact time, and high C/O ratio. Since the FCC process involves successive reactions, the desired products such as
olefins and gasoline are considered intermediate products. A suppression of back-mixing by using the downer reactor is
the key to achieving maximum yield of these intermediates. Compared to conventional FCC processes, the HS–FCC has
modifications in the reactor/regenerator and stripper sections [8–12]. An efficient product separator suppresses side
reactions (oligomerization and hydrogenation of light olefins) and coke formation accelerated by condensation.
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
100 Ethylene
Propylene
80
Product yields, (wt%)
Butylenes
60
Gasoline
40
20 Others
LCO+HCO
0
Conventional HSFCC Gasoline HSFCC Light
FCC Mode Olefin Mode
Figure 1. Comparison of typical product yields of conventional and HS–FCC processes
April 2008 The Arabian Journal for Science and Engineering, Volume 33, Number 1B
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
Flue Gas
Hopper
Stripper
Steam
Regenerator
Air
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
9 75
Light Olefins+Gasoline, (wt%)
Riser Downer
Dry Gas, (wt%)
7 70
Downer Riser
5 65
3
60
70 75 80 85 90
70 75 80 85 90
Conversion
Conversion (wt%)
Figure 3. Comparison of product yields from riser and downer pilot plants
The advantage of downer operation over riser is clearly shown in Figure 4. The downer, operated at HS–FCC
conditions, offers more gasoline at the same yield of light olefins compared to the riser. At the same gasoline yield, the
downer offers higher light olefins yield. Several studies were conducted with different feed oils, catalysts, and olefin
boosting additive combinations.
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
60
More gasoline at Downer
50 same light olefins
Gasoline (wt%)
40
Riser
30
20
More light olefins at
10 same gasoline
0
0 10 20 30 40
Light Olefins (wt%)
The quality of feed also has an impact on the cracking activity and yield structure. Aromatic base feeds are difficult
to crack and produce more coke, whereas paraffinic base feeds are easily cracked and can produce more light olefins. A
set of experiments were conducted using different feed oils of various origins. VGO and AR obtained from paraffinic
low-sulfur crude of East Asia showed high reactivity. The results are presented in Table 6 [14].
Table 6. Effect of Feed Oil Type on Product Yields
Low Sulfur Crude East
Arabian Light Crude
Yields Asia
VGO AR VGO AR
C2 4.3 3.8 5.4 5.1
Light olefins C3 20.7 19.2 25.0 23.8
(wt% feed basis) C4 17.4 16.6 19.5 18.5
Total 42.4 39.5 49.9 47.4
Dry gas 6.5 6.2 7.8 7.9
LPG 42.4 39.7 49.8 46.7
Others
Gasoline 33.6 35.1 29.0 29.2
(wt% feed basis)
LCO+ 14.5 14.6 11.0 11.9
Coke 2.9 4.5 2.3 4.3
Hydrotreated feed oils gave high propylene and gasoline yield even when hydrotreated AR was used. At low C/O
ratios, the performance of Arabian Light VGO was better, whereas at higher C/O ratios, the conversion of paraffinic
VGO was higher. In terms of light olefins yield, paraffinic VGO gave the best performance. At a C/O ratio of 40,
paraffinic VGO yielded 50 wt% light olefins (25 wt% propylene). The gasoline yield was found higher for hydrotreated
VGO compared to paraffinic VGO. A similar trend was also observed for the two atmospheric residue feed oils.
Figure 5 shows the features of the developed proprietary catalyst for HS–FCC. The proprietary catalyst with an
additive gave higher propylene yield compared to a conventional catalyst mixed with 10% of the same additive. Table 7
compares the yields of light olefins, LPG, gasoline, LCO, HCO, and coke make for a base catalyst and with and without
10 wt% ZSM-5 additive. The base catalyst yielded about 29 wt% olefins and 45 wt% gasoline compared to 39 wt% light
olefins and 34 wt% gasoline in catalyst blended with additive.
April 2008 The Arabian Journal for Science and Engineering, Volume 33, Number 1B
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
25
15
Additive C onventional
10 10% C atalyst
P roprietary
5 C atalyst
0
75 80 85 90
C onversion (221℃), m ass%
Figure 5. Advantage of proprietary catalyst
The rise in propylene was accompanied with a drop in gasoline yield since the additive is effective in catalytic
systems where the catalyst have low-hydrogen transfer activity. While fresh ZSM-5 is sufficiently active to crack
gasoline paraffins, ZSM-5 in the FCC, which has been subjected to severe hydrothermal conditions, is not active enough
to crack gasoline paraffins [13, 15,16].
5.2. Demonstration Plant versus Pilot Plant
The operation of the demonstration plant was very successful and the obtained results were very close to those of the
0.1 BPD pilot plant. The two plants were operated using conventional FCC catalyst and untreated VGO to compare the
difference of the scale. The yields of light olefins, gasoline, LCO, HCO, and coke in the pilot and demonstration plants
are compared in Table 8. At a C/O ratio of 30, the conversion in both plants was high about 80 wt %. Gasoline yields
were similar in both plants; and a small decrease in the yield of light olefins occurred in the demonstration plant. Coke
make was also higher in the demonstration plant. The results in Table 8 confirm that the pilot plant and demonstration
plant performed similarly. It also confirmed that scaling up the process was successful.
The experimental results of demo plant operation using a catalyst (a blend of conventional catalyst, developed
proprietary catalyst and ZSM-5 based additive) and feed oil (obtained from the bottom of the first stage of hydrocracker)
are shown in Table 9. The propylene yield was 20 wt% accompanied with a drop in gasoline yield. This drop was likely
due to ZSM-5 accelerating the catalytic cracking of the gasoline lighter components to produce low molecular weight
olefins.
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
Table 8. Effect of ZSM-5 Addition on HS–FCC Product Yields at 600°C Using Untreated VGO
Conventional FCC HS–FCC Pilot Plant HS–FCC Demo Plant
Product
Base Base Base +
Base Base Base
Yields wt% +10wt% +10wt% 8wt% ZSM-
Catalyst Catalyst Catalyst
ZSM-5 ZSM-5t 5*
Dry Gas 5.3 5.8 4.6 5.5 5.4 10.4
Propylene 7.5 13.0 10.7 18.4 10.6 20.4
Butylenes 8.8 13.6 16.1 17.8 13.4 19.0
Total C3-C4
16.3 26.6 28.7 39.3 25.7 43.9
Olefins
Gasoline 43.4 34.1 45.4 34.0 36.0 35.7
Light Cycle
15.0 15.4 9.4 9.3 10.5 1.1
Oil
Heavy Cycle
14.3 13.4 6.6 7.1 7.7 4.4
Oil
Coke 2.3 2.1 3.1 3.5 9.1 2.3
April 2008 The Arabian Journal for Science and Engineering, Volume 33, Number 1B
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A. Maadhah, Y. Fujiyama, H. Redhwi, M. Abul-Hamayel, A. Aitani, M. Saeed, and C. Dean
6. CONCLUDING REMARKS
Stand-alone fuel refinery is not any more profitable and FCC is no more a fuel producer only. With proper design
and operation, the HS–FCC process is in best position to produce light olefins for petrochemicals usage along with fuel
products. Catalytic cracking under high severity in a downer-type reactor boosts overall conversion and enhances the
production of gasoline and light olefins. Based on the intrinsic features of HS–FCC, maximum propylene yield and
aromatics can be obtained by the combination of an optimized catalyst system and operating conditions. The recovery of
propylene and paraxylene enhances the economics of an upgraded refinery with HS–FCC option.
ACKNOWLEDGMENTS
The authors acknowledge the support of NOC, Saudi Aramco, KFUPM, and Japan Cooperation Center, Petroleum
(JCCP) in publishing this paper.
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