Source: HANDBOOK OF PETROLEUM REFINING PROCESSES

CHAPTER 15.2

THE SYNTROLEUM PROCESS OF CONVERTING NATURAL GAS INTO ULTRACLEAN HYDROCARBONS

Larry Weick and Matthew Nimmo
Syntroleum Corporation Tulsa, Oklahoma

INTRODUCTION
As used in this chapter, the term gas-to-liquids (or GTL) refers to a process that converts natural gas into synthetic, ultraclean liquid fuels that contain no sulfur, aromatics, or heavy metals. GTL technology is increasingly being considered as a tool for monetizing stranded gas reserves and for mitigating some of the environmentally driven challenges that are currently confronting the petroleum industry. From the perspective of energy supply, there are increasing pressures to monetize ever-growing reserves of natural gas. Currently, proven world reserves of natural gas are estimated to be in excess of 5200 Tft3.1 More than one-half of these resources are considered strandeduneconomic to transport due to the proximity of potential markets and/or the size of gas deposits, or subquality because of contamination by nitrogen, carbon dioxide, hydrogen sulfide, aromatics, etc.2 These stranded reserves represent potentially large additions to oil company balance sheets if they can be monetized. From the perspective of energy demand, the petroleum industry faces a number of challenges with fuels derived from conventional crude oilenvironmental mandates for cleaner fuels, raw materials getting heavier and dirtier, process upgrading investments becoming more difficult to justify, and tightening supplies of middle distillates and naphtha. Coupled with improved economics, the possibility of meeting these challenges with GTL technology is spurring increased interest in its commercialization. This chapter summarizes Fischer-Tropsch (FT) chemistry and provides an overview of Syntroleums GTL technology, including descriptions for each major section of the process. Quality of fuels produced from a GTL plant is also discussed, including descriptions of emissions, fuel properties, and applications. The report concludes with discussion on the advantages and economics of the Syntroleum Process.

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GAS-TO-LIQUIDS TECHNOLOGIES

HISTORY OF FISCHER-TROPSCH REACTION

In 1923, Franz Fischer and Hans Tropsch of Germany observed that alkalized iron turnings in an atmosphere of carbon monoxide and hydrogen at elevated temperatures and pressures catalyzed the production of oxygenated compounds and hydrocarbons.3 After 2 years of experimentation, the first Fischer-Tropsch catalyst was reported and consisted of an ironzinc preparation. After the pioneering work of Fischer and Tropsch in the 1920s, it was several years before Fischer and Kuster first published a report of liquid (slurry) phase carbon monoxide hydrogenation.4 The earliest known liquid-phase FT patent, awarded to Dr. Mathias Pier of I. G. Farbenindustrie in 1936,5 was applied for in late 1928, predating Fischers publications by about 3 years. Subsequent patents issued in the United States and a number of European countries in the late 1930s through the early 1950s624 indicate a fairly high degree of R&D was occurring immediately before and during World War II. The major players were I. G. Farbenindustrie and Ruhrchemie in Germany, while liquid-phase/slurry FT patents were also issued to a number of U.S. companies (M. W. Kellogg Company, Celanese Corporation, The Texas Company, and Standard Oil Development Company). Today, the leading GTL technology holders are Syntroleum, Sasol, Shell, BP Amoco, and ExxonMobil.

HISTORY OF THE SYNTROLEUM PROCESS

Syntroleums history began in 1984 when the founder, Ken Agee, began experimenting with the use of air as a source of oxygen for the GTL process. After several years of experimenting, the first series of patents were filed in 1988 that were later issued in 1989. In 1990, Syntroleum began the operation of its first pilot plant, which still operates today. The pilot plant has a production rate of 2 barrels per day (BPD) and is used to test a variety of operating conditions for various catalysts. In 1998, Syntroleums research and development facilities quadrupled with the purchase of a new building and the surrounding 100 acres. During the following year, Syntroleum, along with Arco (now BP), began the operation of a 70-BPD facility using slurry reactor designs. After approximately one year of operation, the demonstration plant was relocated to Tulsa. The demonstration plant will begin operation in 2003 as part of the U.S. Department of Energys ultraclean fuels program. Fuel demonstrations are planned in the bus fleets of Washington, D.C., Metropolitan Area Transit Authority and Denali National Park. As of 2001, Syntroleum had licensed its technology to several companies, including Texaco, Marathon, Arco, YPF, Enron, Kerr McGee, Ivanhoe, and the Commonwealth of Australia. Syntroleum has also formed many alliances related to fuel production, testing, and certification; catalyst testing and production; and the design of both onshore and floating GTL plants.

PROCESS DESCRIPTION
The Syntroleum Process consists of the following steps for converting natural gas to finished fuel products: (1) gas pretreating, (2) air compression, (3) synthesis gas generation, (4) Fischer-Tropsch synthesis, and (5) product upgrading. The process converts approximately 10,000 standard cubic feet (SCE) of gas into 1 barrel (bbl) of synthetic hydrocarbons. The maximum capacity of each GTL train is about 11,500 BPD. The process produces several by-products, tailgas, water, and heat, which can be used to generate other products from the plant, such as exportable electricity and steam for desalination. The Syntroleum Process can be adapted for either offshore or onshore applications and can be designed for small gas fields. Figure 15.2.1 is a process flow diagram of the inside-battery-limits (ISBL) portion of the Syntroleum Process.
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Tailgas Natural Gas Gas Treating Fischer Tropsch Products Ultraclean Liquid Fuels

Air

Gas/Steam Turbine-Driven Air Compression

Syngas Production (ATR)

Fischer Tropsch Reactors

Product Upgrading

Steam

FIGURE 15.2.1 Process flow diagram of Syntroleum Process.

TABLE 15.2.1 Components

Syntroleum Gas Feed Specifications Limit Less than 5 mol % Less than 20 mol % Less than 25 mol % Less than 10 ppm

Ethane and heavier CO2 N2 Sulfur compounds

Feed Gas Pretreating The feed gas pretreating section is determined by the gas composition and Syntroleums feed gas specifications, which are based upon those components that are detrimental to the catalytic reactor systems. The gas feed specifications are summarized in Table 15.2.1. For example, for a gas composition that does not exceed the limitations in Table 15.2.1, minimal gas pretreating is required. In this case, sulfur removal is the only gas treatment needed. Cobalt/molybdenum (Co/Mo) and zinc oxide (ZnO) guard beds are used to reduce the sulfur concentration to 100 ppb for the catalytic processes. When the limitations of CO2 and/or sulfur are exceeded, the cost of treatment determines whether the gas is feasible for use. Finally, gas that exceeds the specification for ethane and heavier molecules either can be processed to recover and sell natural gas liquids (NGLs) for additional revenue or can be processed to reform the C2 components into methane for use as feedstock. The choice will depend on the amount of recoverable NGLs and market conditions. Overall, the robust gas specifications of the Syntroleum Process enable many gas fields that are considered marginal to be monetized.

Air Compression Unique to the Syntroleum Process is its use of air as an oxygen source. A process air compressor driven by a steam or gas turbine supplies the synthesis gas generation section with the stochiometric amount of oxygen (as contained in air) required to generate a synthesis gas ratio of approximately 2 : 1 (H2:CO). The inlet air is filtered to avoid corrosion and erosion of the rotating components and deactivation of the downstream catalyst. Gas turbines are commercially available that will burn low-Btu tailgas, a by-product generated from the FT reactors. In addition to providing fuel value, this tailgas stream represents a large mass flow of high-pressure gas that aids in the generation of shaft power from the expander end of the gas turbine. For a steam turbine, the tailgas is utilized for the production of steam.

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GAS-TO-LIQUIDS TECHNOLOGIES

Synthesis Gas Production The Syntroleum Process produces a nitrogen-diluted stream of synthesis gas, a mixture of carbon monoxide and hydrogen, using Syntroleums proprietary autothermal reactor (ATR). Pretreated natural gas, steam, and air are thoroughly mixed before entering the bed in the ATR. The reaction proceeds over a commercially available catalyst and yields syngas having a H2:CO ratio of approximately 2 : 1. The reactions that take place in the ATR are shown in Fig. 15.2.2. The net thermal result of all three reactions is a surplus of heat, which is used to raise high-pressure steam. Water coproduced within the syngas is recovered, treated, and used as makeup water. The catalyst can be regenerated periodically, if required, with air and hydrogen to remove any coke formation and has an expected minimal life of 4 years. After exiting the vessel, the synthesis gas is cooled and compressed prior to entering the FischerTropsch reactors.

Fischer-Tropsch Synthesis Nitrogen-diluted synthesis gas from the ATR is compressed and enters the Fischer-Tropsch reactors to predominantly produce paraffinic, synthetic hydrocarbons. The compressed synthesis gas flows into the bottom of the FT reactor and is bubbled through a slurry of Fischer-Tropsch liquid and suspended solid particles of a proprietary and commercially available cobalt catalyst. On the active surface of the catalyst, carbon monoxide is hydrogenated into paraffinic hydrocarbons of various molecular weights. The balanced reaction is shown in Fig. 15.2.3. Excess heat produced from the Fischer-Tropsch reactions is removed by raising low-pressure steam. Syntroleum catalysts yield a Shultz-FluoryAnderson distribution corresponding to an alpha ranging from 0.88 to 0.94, depending on the formulation. Unreacted synthesis gas exits the top of the reactor and may become the feedstream for the subsequent stage or a fuel for the gas turbine. The cobalt catalyst has an expected minimal life of 4 years and is continuously regenerated to sustain high levels of activity. Each reactor produces two streams of hydrocarbonslight Fischer-Tropsch liquid (LFTL) and heavy Fischer-Tropsch liquid (HFTL); and three by-productswater, tailgas, and heat. The unrefined heavy and light Fischer-Tropsch streams are sent to the product upgrading section for processing into fuels. Syntroleum has also developed and licenses the Fischer-Tropsch reaction of a fixed bed design.

Reaction 1: CH4 Reaction 2: CH4 Reaction 3: CO

Catalyst 1.5O2 H2O H2O

CO 2H2O 3H2 CO H2 CO2

FIGURE 15.2.2 Synthesis gas generation.

Synthesis gas (diluted with nitrogen) n(2H2 CO) N2

Catalyst

Hydrocarbons (CH2 )n

Water nH2O

Nitrogen N2

FIGURE 15.2.3 Fisher-Tropsch reaction.

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Product Upgrading The final step in a Syntroleum GTL fuels plant is product upgrading (upgrader), which converts the waxy effluent from the FT reactions into useful fuels. The upgrader consists of distillation and hydroprocessing units that are of similar configurations found in conventional petroleum-based refineries. As in petroleum-based refineries, the upgraders exact configuration and processing scheme will depend upon the facilitys particular product slate and associated specifications. Although the processing schemes may be varied, several general processing requirements are needed and can be broken down into the following major areas: 1. Distillation of the FT effluent into two or more fractions 2. Hydroprocessing of one or more of the fractions to improve low-temperature properties 3. Distillation of the hydroprocessed effluent streams into finished products Due to the high purity and low variability of the FT stream, the Syntroleum upgrader will have a lower capital and operating cost than that of an equivalent petroleum-based system. Specific areas of cost savings include these:

Since there is no sulfur in the feed, the metallurgical requirements of the hydroprocessing unit are reduced, resulting in a lower cost (e.g., no stainless overlay is required for the reactor). Also, sulfur recovery requirements are completely eliminated. Hydrogen consumption is lower ( 50 percent of a typical sour feedstock), which reduces not only the operating costs associated with producing hydrogen, but also compression requirements on both the makeup and reactor recycle gas loop. Hydroprocessing conditions are milder (i.e., lower pressures and temperatures) and bear more resemblance to a fuels hydrotreating unit than to a fuels hydrocracker. The need for an independent residual cracker or coking unit is eliminated due to the ability of high-molecular-weight normal paraffins to crack into lower-molecular-weight paraffins in the fuels hydroprocessing unit itself. Contaminants, such as polynuclear aromatics and heavy metals (e.g., nickel and vanadium), are not present in the feed, and therefore the unconverted bottoms can be recycled to extinction.

Syntroleum uses commercially available hydroprocessing catalysts in its licensed hydrocracker and hydrotreating units. Overall, these attributes reduce the complexity and cost of producing ultraclean fuels compared to a conventional crude oil refinery.

ADVANTAGES OF THE SYNTROLEUM PROCESS

The Syntroleum Process has several advantages over competing processes. The process utilizes air instead of pure oxygen to generate FT liquids. This reduces the cost of the plant and increases the safety of plant personnel. Additionally, the process produces several recoverable by-productstailgas, heat, and water. These by-products are used to reduce the operating costs of the plant and to provide additional revenue. The process has the advantage of being flexible in terms of operating configuration and feedstock quality, allowing the process to be adapted to a range of environments. Finally, as detailed earlier, the lack of contaminants, sulfur, aromatics, and heavy metals simplifies the refining section of the plant.

Oxygen versus Air The use of ambient air as the source of oxygen in the ATR is a unique characteristic of the Syntroleum Process that has several advantages over competing processes, which utilize
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air separation units to obtain a pure stream of oxygen. First, ambient air utilization has significantly lower capital and operating costs, because no refrigeration, which requires costly metallurgy and a considerable amount of electricity (often not included in efficiency calculations), is avoided. The Syntroleum Process uses off-the-shelf turbines and compressors to supply air to the reactors. These turbines and compressors are commonly used in power plant projects and oil and gas operations. Second, liquid oxygen is extremely explosive and requires highly trained and experienced personnel and a rigorous maintenance schedule to reduce the risk of accidents. To the contrary, the use of air reduces increases safety of the plant, because the presence of inert nitrogen in the Syntroleum Process provides additional thermal control of the energy released from the ATR and FTR reactions. The resulting thermal control benefits of nitrogen from the use of air are (1) a fairly uniform temperature profile, (2) moderation of the temperature rise in the ATR, (3) more efficient heat removal in the FT reactor, and (4) minimal coke formation. Even though the Syntroleum Process uses air instead of pure oxygen, the Syntroleum FT reactors are not twice as big and therefore not more expensive than oxygen-blown FT reactors. The Syntroleum Process operates on a single-pass basis; the oxygen-blown processes operate with a recycle loop. Due to recycle, inerts (CO2, C1, C2, etc.) accumulate, dilute the synthesis gas, and act in much the same manner as nitrogen in the Syntroleum Process. The net effect is that the combined air feed system and the FT reactor system of the Syntroleum Process will in most cases cost less than the air separation unit and FT reactor system of an oxygen-blown system.

By-products All three by-productswater, tailgas, and heatare recovered and utilized in the process for makeup water, plant fuel, steam generation, and/or producing additional exportable products to nearby markets. Approximately 1.1 bbl of water is produced for every barrel of unrefined hydrocarbon. The water contains contaminants including suspended paraffins and small amounts of dissolved oxygenates, such as alcohols, and inorganic ions, such as ammonia. The water is fed to a wastewater stripper, where volatiles are removed and sent to a pre-reformer for recovery of hydrocarbon value. The stripped water is routed to the wastewater treatment plant for conditioning as makeup water for cooling towers and process boilers. The second by-product, tailgas, is a clean-burning and abundant source of energy that fuels low-Btu heaters, gas turbines, and any additional power generation. The tailgas displaces the use of natural gas and therefore reduces operating costs and increases plant efficiency. The tailgas can also be sold to nearby refineries for steam or power generation. The final by-product is high-pressure and medium-pressure steam, raised from the ATR and FT reactor, respectively. The steam is used in a variety of applications, ranging from steam turbine operations for power generation and/or compression to water reclamation, such as water stripping and desalination.

Process Flexibility and Simplicity The Syntroleum Process has a tremendous amount of flexibility. Under appropriate conditions, the process can be economically designed to produce as little as 6000 BPD of synthetic fuels. Reserves of less than 500 BCF recoverable gas would be required to produce 6000 BPD of synthetic fuels for 20 years. The process can also be configured to produce surplus electricity for sale. For example, the tailgas and steam can be used as fuel for power generation in gas turbine(s), and flue gas from the gas turbines can be routed to heat recovery steam generators (HRSGs) to raise additional steam for additional power. Also, the process can be designed for marine applications with the use of floating production, storage, and

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off-loading systems (FPSOs) and barges. Offshore infrastructure for processing and transporting gas to markets is typically designed around a collection of gas and oil discoveries. In many cases, the cost of transporting the gas onshore is prohibitive, and therefore the gas is reinjected, flared, and/or vented after condensate and/or LPG has been removed. Floating plants of the Syntroleum Process would enable gas in such isolated fields to be produced and converted to higher-valued products. Finally, perhaps someday, surplus steam and tailgas generated from the process will be used to produce gas from the largest known source of natural gasmethane hydrates. Conceptually, the tailgas and steam from the plant would be used to heat seawater to produce a heated brine solution, which would be used to melt the hydrates and free the gas for conversion into synthetic hydrocarbons.

QUALITY OF FUELS PRODUCED FROM SYNTROLEUM PROCESS

The attributes of the synthetic fuels are discussed in the following sections. The synthetic fuel data reflect a 2001 analysis conducted by Syntroleum at its laboratories, national laboratories, including Southwest Research Institute, and car manufacturers, including Volkswagen and Daimler Chrysler.

Synthetic Diesel (S-2) Synthetic diesel produced from the Syntroleum Process, also known as S-2, is a highly paraffinic, high-cetane distillate product suitable for conventional and advanced compression ignition diesel engines and fuel cells. S-2 is physically similar to petroleum-based diesel fuels, but with superior combustion emission characteristics. At ambient temperature and pressure, S-2 is a colorless, stable, environmentally safe liquid that can be shipped, stored, and dispensed using the same fuel distribution and handling procedures as petroleum diesel. A comparison of the S-2 to other conventional diesel fuels is shown in Table 15.2.2. Due to its attributes, S-2 outperforms diesel fuel produced from crude oil. First, due to its high paraffin content (99 percent) and absence of aromatics, S-2 has a cetane number of 74. As a comparison, the minimum cetane number in the United States is 40 and in Europe is 50. With its inherent high cetane number, S-2 will reduce the ignition delay periods, especially for cold starts, and increase power and performance without the need of cetane additive. Also S-2 contains no detectable amounts of sulfur, aromatics, or heavy metals. Because of this attribute, tests by Southwest Research Institute have confirmed that S-2 has reduced emissions in every category of criteria pollutant compared to EPA no. 2 diesel, CARB diesel, and Swedish City diesel. The results of these tests are summarized in Table 15.2.3. Furthermore, since S-2 contains no measurable olefins or aromatics, the fuel does not exhibit stability problems, such as gum formation and insoluble organics associated with conventional diesel fuels. Another advantage due to the absence of contaminants is S-2s compatibility with emission after-treatment devices and fuel cells, which are sensitive to
TABLE 15.2.2 Specifications Specific gravity Sulfur, ppm Aromatics, vol % Cetane number Specifications of Diesel Fuels Tested by SWRI S-2 0.77 0 0 74 EPA no. 2 0.85 350 31 47 CARB 0.83 155 8 51 Swedish 0.82 10 4 52

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TABLE 15.2.3

Criteria Pollutant Emissions from S-2 Measured emission, g (bhp h)r

Fuel tested EPA no. 2 diesel CARB diesel Swedish City diesel S-2

HC 0.12 0.09 0.09 0.07

CO 1.2 1.1 1.2 0.8

NOx 4.0 3.7 3.6 3.2

PM 0.10 0.08 0.08 0.06

the sulfur levels in diesel fuel. Since S-2 contains no sulfur or heavy metals, these catalytic after-treatment devices are not susceptible to deactivation caused by contaminants normally found in conventional fuels. Finally, S-2 has excellent low-temperature properties due to a high percentage of isoparaffins. Testing has demonstrated that the cloud point and the cold filter plugging can be as low as 30 and 34C, respectively. This implies that S-2 will not require additives to improve the low-temperature properties and that engines using S-2 in cold environments will not be as susceptible to clogged fuel lines and filters as engines using conventional diesel.

Synthetic Naphtha (FC-2) FC-2 is an ultraclean, synthetic naphtha that is saturated with hydrogen and has many applications in the petrochemical and fuels industry. FC-2 is free of aromatics, metals, and sulfur and is composed of 99.99 percent naphtha. With these qualities, FC-2 can be utilized for feedstocks in ethylene crackers, fuel cells, and low-compression engines (4 : 1 or less) or undergo further processing into upgraded products, such as high-octane gasoline and liquefied petroleum gas. Ethylene Feedstock Applications. FC-2 is an excellent ethylene cracker feedstock. Naphtha feedstocks with a high paraffin content are preferred, because they produce much higher yields of light olefins. As stated earlier, FC-2 has a paraffin content of 99.99 percent, a content higher than that of any naphtha isolated from a conventional crude oil, such as Saudi Arabias A-180 natural gasoline, which has a paraffin content in the range of 90 to 95 percent. Combustion Engine/Heating Applications. Due to its high paraffin content, FC-2 has a low octane rating of approximately 30, making it an ideal straight-run fuel for lowcompression (4:1) engines. However, the octane level of FC-2 can be upgraded for vehicular use with the addition of an akylation unit. Alternatively, FC-2 can be cracked into liquefied petroleum gas (LPG). This would provide a sulfur-free fuel for residential and commercial heating needs. Finally, FC-2 is an excellent fuel substitute that is currently being used in industrial turbines. A significant reduction of emissions would result, eliminating the need for expensive scrubbing of the exhaust. Fuel Cell Applications. As a fuel-cell fuel, FC-2 is a very attractive fuel for generating hydrogen. The paraffinic nature of FC-2, more specifically the lack of unsaturated and aromatic hydrocarbons, favors minimal coking in the reforming step of the fuel cell. Additionally, the lack of sulfur and heavy metals in FC-2 prevents the need for sulfur removal beds or guard beds to protect the reforming catalyst. In comparison to other fuels, tests conducted by IdaTech showed that the hydrogen yield
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per unit volume is nearly double that of CNG or methanol. These attributes are expected to contribute significantly toward minimal operating costs and favorable overall economics of a FC-2 fuel cell.

Synthetic LPG Synthetic LPG is used for domestic heating, cooking, and transportation and has outstanding qualities when compared to conventional LPG. Synthetic LPG contains no contaminants such as hydrogen sulfide, carbon dioxide, oxygen compounds, and moisture that are commonly found in conventional LPG. Because of these attributes, synthetic LPG does not require any gas conditioning, such as dehydration or amine processing. The lack of contaminants also implies that synthetic LPG can be handled more safely and will have a higher performance for end-use markets, especially in terms of emissions.

CAPITAL INVESTMENT REQUIREMENTS

Several key variables affect the profitability of a GTL plant; these variables include the capacity of the plant, capital cost of the plant (Table 15.2.4), gas price, operating and maintenance costs, and transportation costs. Only a detailed front-end engineering design for a site-specific project can provide a definitive cost estimate. The cost information provided here is based on generic studies, which typically have an accuracy of 30 percent. The cost estimate is based upon the following:

Capital cost estimate is based on U.S. Gulf Coast pricing in 2001 U.S. dollars. Capital cost estimate includes home office/EPC costs of 15 percent. Capital cost estimate has an accuracy of 30 percent. Operating cost estimate excludes cost of natural gas. The following exclusions apply: gas pipeline and other gas transportation costs outside plant fence, cost of recovering NGLs from feed gas, unusual water acquisition costs, cost of land, taxes, licenses, permits, duties, start-up costs, insurance, and cost of frontend engineering design.

REFERENCES
1. Energy Information Administration Web site: www.eia.doe.gov. 2. B. Eisenberg et al., Advanced Gas Conversion Technology for Remote Natural Gas Utilization, GPA Convention Paper, March 1994, p. 1. 3. Henry H. Storch, The Fischer-Tropsch and Related Synthesis, Wiley, New York, 1951, p. 1.

TABLE 15.2.4 GTL Plant

Generic Economics of Syntroleum Capital cost estimate

Capital cost of plant Operating cost

$25,000/bbl of daily capacity $5.00/bbl

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4. F. Fischer and K. Peters, Catalytic Gas Reactions in Liquid Medium, Brennstoff-Chem., 12: 286293, 1931. 5. M. Pier, (I. G. Farbenindustrie), Verfahren zur katalytischen Reduktion der Oxyde des Kohlenstoffs, German Patent 630,824, May 14, 1936. 6. I. G. Farbenindustrie, Improvements in the Manufacture and Production of Hydrocarbons of High Boiling Point, British Patent 449,274, June 24, 1936. 7. I. G. Farbenindustrie, Improvements in and Apparatus for the Conversion of Oxides of Carbon and Hydrogen, British Patent 468,434, June 29, 1937. 8. Standard Oil Development Company, An Improved Method of Controlling Exothermic Catalytic Reactions, British Patent 496,159, Nov. 25, 1938. 9. H. Dreyfus, Improvements in or Relating to the Manufacture of Hydrocarbons and Other Products from Carbon Monoxide and Hydrogen, British Patent 505,121, May 5, 1939. 10. F. Duftschmid, E. Linckh, and F. Winkler, (I. G. Farbenindustrie), Production of Valuable Hydrocarbons and Their Derivatives Containing Oxygen, U.S. Patent 2,159,077, May 23, 1939. 11. International Hydrocarbon Synthesis Company, Procd de synthse catalytique en gnral et plus particulirement applicable la production synthtique dhydrocarbures liquides partir de mlanges gazeux synthse comprenant du monoxyde de carbone et de lhydrogne, French Patent 855,378, Feb. 12, 1940. 12. H. Tramm (Internal Hydrocarbon Synthesis Company), Forfaringssatt vid syntetisk framstalling av kolvaten ur koloxid och vate samt pa sa satt framstalla produkter, Swedish Patent 104,113, June 18, 1941. 13. E. W. Riblett, (M. W. Kellogg Company), Method of Catalytic Synthesis, U.S. Patent 2,250,421, July 22, 1941. 14. International Hydrocarbon Synthesis Company, Procedimento per aumentare la resa in indrocarburi che bollono nel campo di ebollizione di olio per diesel, nella sintesi da monoossido di carbonio e idrogeno, Italian Patent 389,201, Oct. 29, 1941. 15. International Hydrocarbon Synthesis Company, Procedimento per la produzione di olio da gas nellidrogenazione catalitica di ossidi di carbonio, Italian Patent 390,152, Nov. 27, 1941. 16. International Hydrocarbon Synthesis Company (H. Tramm), Forfaringssatt vid syntetisk framstalling av kolvaten ur koloxid och vate samt pa sa satt framstalla produkter 482kb, Swedish Patent 104,113, Mar. 31, 1942. 17. H. Tramm and W. Wischermann, (Ruhrchemie), Verfahren zur Durchfhrung der Kohlenoxydhydrierung ber in flssigem Medium aufgeschlmmten Kontakten, German Patent 744,185, Nov. 18, 1943. 18. H. Dreyfus, Improvements Relating to the Production of Hydrocarbons, British Patent 564,730, Oct. 11, 1944. 19. H. Dreyfus (Celanese Corporation), Production of Organic Compounds, U.S. Patent 2,361,997, Nov. 7, 1944. 20. H. Kolbel and P. Ackermann, (Steinkohlenbergwerk Rhienpreussen), Verfahren zur Durchfhrung der Kohlenoxydhydrierung, German Patent 766,025, Feb. 8, 1945. 21. M. M. Stewart, R. C. Garrett, and E. E. Sensel, (The Texas Company), Method of Effecting Catalytic Reaction between Carbon Monoxide and Hydrogen, U.S. Patent 2,433,072, Dec. 23, 1947. 22. F. J. Moore (The Texas Company), Method of Effecting Catalytic Reactions, U.S. Patent 2,440,109, Apr. 20, 1948. 23. F. Schnur (Ruhrchemie), Verfahren zur katalytischen Kohlenoxydhydrierung in flussiger Phase, German Patent 817,596, Aug. 30, 1951. 24. H. Kolbel and P. Ackermann, (Steinkohlenbergwerk Rhienpreussen), Verfahren zur Durchfhrung der Kohlenoxydhydrierung in einem flssigen Medium, German Patent 764,166, Dec. 4, 1952.

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