US3868331A - Process for the partial combustion of hydrocarbonaceous fuels to produce substantially soot-free gases - Google Patents

Process for the partial combustion of hydrocarbonaceous fuels to produce substantially soot-free gases Download PDF

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US3868331A
US3868331A US370996A US37099673A US3868331A US 3868331 A US3868331 A US 3868331A US 370996 A US370996 A US 370996A US 37099673 A US37099673 A US 37099673A US 3868331 A US3868331 A US 3868331A
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soot
gases
particles
partial combustion
gas mixture
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Expired - Lifetime
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US370996A
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English (en)
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Lookeren Campagne Nicolaas Van
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Shell USA Inc
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Shell Oil Co
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/36—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using oxygen or mixtures containing oxygen as gasifying agents
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency
    • Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines

Definitions

  • ABSTRACT The soot content of a hydrogen and carbon monoxidecontaining gas mixture obtained by the partial combustion of a hydrocarbonaceous fuel is substantially reduced by passing the partially-combusted gases through a soot-conversion zone maintained at an elevated temperature and pressure, and retarding the passage of soot particles through the zone for a sufficient period of time that the soot is substantially converted to carbon monoxide.
  • An apparatus suitable for effecting soot-conversion is also disclosed.
  • the present invention relates to a process and an apparatus for the partial combustion of hydrocarbonaceous fuels to produce gases having a substantially reduced soot content.
  • the gases produced by processes for the partial combustion of hydrocarbonaceous fuels invariably contain a substantial amount of free carbon (i.e., soot) which is undesirable for the subsequent utilization or processing of the gases and which should therefore be removed.
  • soot free carbon
  • the removal of the soot is normally achieved by scrubbing the gases with water.
  • the resulting dispersion of soot particles in water is then processed in order to recover substantially soot-free water and soot.
  • the soot removal facilities are expensive and the recovered soot generally has a low value. It is therefore an object of the present invention to provide a process for the combustion of hydrocarbonaceous fuels to produce gases having a substantially reduced soot content and thus eliminate the need for expensive soot-removal facilities. It is also an object of the invention to increase the efficiency of the partial combustion process by ensuring that substantially all the carbon content of the hydrocarbonaceous fuels combusted is converted into more valuable carbon monoxide.
  • soot particles are retained in the soot-conversion zone for this length of time, they are substantially converted into carbon monoxide by reaction with steam and/or carbon dioxide which is also present in the crude gas mixture.
  • This substantial reduction in in soot concentration correspondingly reduces or eliminates the need for downstream soot removal facilities and permits the use of conventional straight tube heat exchangers to abstract heat from the hot crude gas mixture, instead of more expensive helical coil heat exchangers which are commonly employed in this service.
  • the conversion of the carbon to carbon monoxide in the soot conversion zone increases the calorific value of the gases produced.
  • the relative proportions of steam and carbon dioxide present in the partially combusted gases is not critical. It is only required that the combined steam and carbon dioxide concentrations be stoichiometrically sufficient to effect conversion of the free carbon to carbon monoxide in accordance with the above equations.
  • the operation of the soot-conversion zone can therefore be seen to comprise firstly retarding the passage of soot particles and secondly to allow sufficient time for conversion of the particles so retarded into carbon monoxide.
  • the advantage of this operation is two-fold. Firstly it enables the production of substantially sootreduced gases, and secondly it allows substantial conversion of the carbon content of the hydrocarbonaceous fuel into carbon monoxide, thus increasing the calorific value of the gases produced as previously mentioned.
  • the retardation and conversion of the soot particles in the soot-conversion zone is such that the percentage by weight of soot particles present in the gases leaving said zone is reduced to less than 1 percent. Preferably, however, the percentage by weight of soot particles present in the gases leaving said zone is reduced to less than 0.3 percent.
  • soot particles are sufficiently retarded in the soot-conversion zone that their residence time therein allows substantial conversion to carbon monoxide to take place. Accordingly, the soot particles suitably remain in the soot-conversion zone for at least 5 seconds. It is, however, preferred that the time that the soot particles remain in the soot-conversion zone is between 15 and 50 seconds.
  • Retardation of the soot particles is suitably effected by a soot-conversion zone consisting of at least one bed of ceramic material or any equivalent material which is resistant to high temperatures.
  • a soot-conversion zone consisting of at least one bed of ceramic material or any equivalent material which is resistant to high temperatures.
  • any ceramic material capable of resisting the high temperatures present in the soot-conversion zone e.g., l,O-l,600C or higher, can be employed. Ceramic materials having the requisite refractory properties are known to those skilled in this art and are described, for example, in Encyclopedia of Chemical Technology by Kirk and Othmer, Second Edition, 1968, Vol. 4, pages 762775.
  • Suitable ceramic materials include various carbides, e.g., the carbides of silicon, boron, zirconium, hafnium, tantalum, vanadium, molybdenum, tungsten and niobium; various aluminum silicates, particularly sillimanite and Korund (a special alumina refractory material containing at least 95 percent alumina); various borides, nitrides and sulfides of high melting point metals, and various oxides such asmullite, zircon and the like.
  • the soot particles adhere to the surface of the ceramic material under the influence of Van der Waals-type forces.
  • the bed of ceramic material advantageously consists of packed perforated bricks.
  • the bricks are preferably packed on top of one another in layers such that the perforations of the bricks in a lower layer interconnect with the perforations of the bricks in an upper layer.
  • the interconnecting perforations form elongated tubes in the direction of gas flow within the sootconversion zone.
  • the gases pass through the elongated tubes but the soot particles adhere to the walls thereof and are therefore retarded.
  • the perforated bricks are preferably made from Korund, carbides or sillimanite, although they may be made from any other suitable ceramic material which can resist high gas temperatures.
  • the diameter of the elongated tubes may vary over a wide range.
  • the diameter preferably is between 0.5 cm and 2.5 cm.
  • the surface area of the elongated tubes for gas contact may also vary considerably. Preferably the surface area is between 30 square mete rs and 200 square meters per cubic meter of perforated bricks.
  • the average gas velocity through the elongated tubes is not critical, but in general lies between 1 meter per second and meters per second.
  • the ash particles in the hot gases are temporarily retarded in the sootconversion zone.
  • the soot particles do not react further with the hot gases but pass through the said zone unchanged.
  • a very small proportion of the ash particles however is retained within the soot-conversion zone and thus a gradual build-up of ash particles therein occurs. This build-up is accelerated if the ash content of the hydrocarbonaceous fuel is high. This eventually leads to plugging of the perforations of the bricks and inefficient soot conversion. Accordingly, after a shorter or longer period of operation it is necessary to remove the old bricks from the soot-conversion zone and install new ones.
  • intervals between successive brick renewal periods depend to a large extent on the ash content of the hydrocarbonaceous fuel combusted, but in general are between 1 month and 12 months.
  • a swing reactor system is suitably utilized, whereby while a bed of bricks in one reactor is being replaced, another bed of bricks in another reactor is in operation.
  • the bed of ceramic material suitably consists of at least one fluid bed of ceramic particles.
  • the particles are made from any suitable ceramic material and in particular from Korund, carbides or sillimanite.
  • the diameter of the particles may vary over a wide range, but as in the case of perforated bricks, consideration of gas flow rate through the bed and surface area for gas contact requires the diameter to be in general between 10 and 1,000 microns.
  • the superficial velocity of the gases passing through the fluid bed preferably lies between 0.1 and 1 meter per second, although operation above and below these figures is quite possible.
  • the temperature and pressure at which soot conversion in the soot-conversion zone takes place are substantially the same as the temperature and pressure at which partial combustion occurs.
  • the pressure in the partial combustion zone can be from 1 to 300 atmospheres, but'preferably is between 10 and 150 atmospheres.
  • the temperature within the partial combustion zone is, in general, from about 1,000C to about 1,600C, but preferably from 1,300C to 1,500C. These same ranges of pressure and temperature apply to the soot conversion zone.
  • a considerable advantage of the present invention lies in the fact that the production of substantially sootreduced gases greatly simplifies and facilitates the subsequent heat recovery operation therefrom.
  • the soot content of the gases is negligible, it is possible to recover heat from the gases in a conventional straight tube type heat exchanger since soot deposition on the inside walls of the tubes no longer occurs.
  • the more expensive helical tube heat exchangers are no longer necessary and also heat recovery at higher steam pressures becomes possible, since conventional straight-tube exchangers can operate at higher pressures than helical tube exchangers.
  • Any suitable hydrocarbonaceous or carbonaceous fuel may be partially combusted according to the present invention including natural gas, heavy oils, coal, coke and shale oil, tar sands oil, etc.
  • the fuel will be a liquid hydrocarbon fuel. If a solid fuel is employed, it may be combusted in either a dry pulverized form or in a slurry with liquid.
  • the invention also relates to an apparatus suitable for carrying out the process described hereinbefore.
  • This apparatus comprises:
  • soot-conversion vessel connected to the partial combustion reactor containing a bed of ceramic material of sufficient thickness and porosity to retard passage of the soot particles through said soot conversion vessel for at least 5 seconds whereby the soot particles are substantially converted to carbon monoxide, said soot-conversion vessel having an inlet for the partially combusted, sootcontaining gases from the partial combustion reactor, and an outlet through which the soot-reduced gases are discharged from the soot-conversion vessel.
  • the outlet of the sootconversion vessel is connected to a waste heat boiler.
  • the waste heat boiler is suitably of the conventional straight tube type if the gases leaving the sootconversion vessel contain negligible amounts of soot. If small amounts of soot are still present in the gases then a helical tube type heat exchanger may be employed.
  • the number of beds of ceramic material contained within the soot-conversion vessel is not of critical importance. Accordingly any number of separate beds, within reason, may be contained within the sootconversion vessel although one single bed is preferred.
  • the bed(s) of ceramic material must be of sufficient porosity to permit the passage of the gases therethrough while retaining the soot particles for the prescribed length of time to effect their conversion to carbon monoxide, i.e., at least 5 seconds.
  • the soot-conversion vessel contains a bed of packed perforated bricks.
  • the perforated bricks are packed on top of one another in layers such that the perforations in the bricks in a lower layer interconnect with the perforations of the bricks in an upper layer.
  • the interconnecting perforations form elongated tubes in the direction of gas flow within the soot-conversion vessel.
  • the total length of the elongated tubes formed by the packed perforated bricks varies according to, inter alia, the surface area required for soot retardation, the diameter of the perforations and the soot content of the combustion gases entering the sootconversion zone, but in general is between 0.5 and 5 meters.
  • the surface area of the elongated tubes suitably lies between square meters and 200 square meters per cubic meter of the packed perforated bricks.
  • the number of layers of perforated bricks within the soot-conversion zone depends on the length of elongated tubes required and the size of the individual bricks but advantageously lies between 2 and 100.
  • the number of perforations per brick suitably lies between 5 and 750, and the diameter of the perforations between 0.5 cm and 2.5 cm.
  • the soot conversion vessel contains at least one bed of fluidizable particles.
  • the size of the particles is not critical but advantageously the average diameter thereof is between 10 and 1000 microns.
  • FIG. 1 is a diagrammatic representation of an apparatus for the partial combustion of hydrocarbonaceous fuels to produce substantially soot-reduced gases.
  • FIG. 2 is a partially cutaway, perspective view of a perforated ceramic brick suitable for use in the sootconversion vessel.
  • hydrocarbonaceous fuel is introduced via line 1 and oxygen is introduced via line 2 into burner part 3 of partial combustion reactor 4. Steam if required may be introduced via both lines 1 and 2.
  • the hot combustion gases pass through a con necting piece 5 which connects the reactor to sootconversion vessel 6.
  • the bed of ceramic material can suitably comprise ceramic bricks as shown in FIG. 2, consisting of ceramic material 13 and having perforations 14 through which the soot-containing combustion gases flow, the soot particles adhering to the inside surfaces of the perforations thus retarding their passage and permitting their conversion to carbon monoxide.
  • the gases leaving the top of the soot-conversion vessel enter heat exchanger 8 via line 9 and leave the heat exchanger via line 10. Water enters the heat exchanger via line 11 and steam leaves via line 12.
  • a liquid hydrocarbon fuel may be combusted in the presence of oxygen and steam in a reactor and the combustion gases passed at a temperature of I,400C and a pressure of 60 atmospheres from the reactor to a sootconversion vessel containing a bed of packed perforated ceramic bricks.
  • the combustion gases entering the soot-conversion vessel contain 3 percent by weight of soot particles.
  • the bed is packed with perforated bricks having dimensions of 36 centimeters long, 12 centimeters wide and 10 centimeters deep and the height and diameter of the packed bed are 2 meters and 1.4 meters, respectively.
  • Each brick contains 50 perforations of 1.5 centimeters diameter and the surface area of the tubes formed by the interconnecting perforations is square meters per cubic 'meter of packed bricks.
  • the volume flow rate of the combustion gases flowing through the soot-conversion vessel is 1.45 cubic meters per second and the average gas flow through the tubes is 4.5 meters per second
  • the average soot retardation time is 20 seconds and the average thickness of the soot layer formed on the surface of the perforations of the packed bricks is 0.8 millimeters.
  • the gases passing out of the soot conversion vessel contain 0.03 percent by weight of soot particles. Hence a 99 percent conversion of the soot particles present in the gases entering the soot-conversion vessel is achieved.
  • a liquid hydrocarbon fuel may be combusted in the presence of oxygen and steam in a reactor and the combustion gases passed at a temperature of 1,400C and a pressure of 60 atmospheres from the reactor to a soot-conversion vessel containing a fluidized bed of ceramic particles.
  • the combustion gases entering the soot-conversion vessel contain 3 percent by weight of soot particles and 300 ppm of ash particles.
  • the bed consists of 9.2 cubic meters or 12 tons of Korund particles having an average diameter of 50 to 200 microns.
  • the height and diameter of the fluidized bed are 2 meters and 2.4 meters respectively.
  • the soot retardation time is greater than seconds and the gases passing out of the sootconversion vessel contain 0.03 percent by weight of soot particles. Hence a 99 percent conversion of the soot particles present in the gases entering the soot conversion is achieved.
  • Operation of the process at this soot conversion level may be continued for 3 months until the amount of ash which builds up within the fluidized bed is 6.5 tons. At this point replacement of the bed with fresh particles is considered desirable since the bed contains about 30 percent by weight of ash particles.
  • the bed of ceramic material through which the crude gas mixture is flowed comprises layers of perforated bricks, the perforations of the bricks in each lower layer interconnecting with the perforations of adjoining upper layers to form elongated tubes in the direction of gas flow.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Health & Medical Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Industrial Gases (AREA)
  • Catalysts (AREA)
  • Fluidized-Bed Combustion And Resonant Combustion (AREA)
  • Filtering Of Dispersed Particles In Gases (AREA)
US370996A 1972-06-26 1973-06-18 Process for the partial combustion of hydrocarbonaceous fuels to produce substantially soot-free gases Expired - Lifetime US3868331A (en)

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GB2976872A GB1437090A (en) 1972-06-26 1972-06-26 Process and apparatus for the partial combustion of carbona ceous fuels to produce substantially soot-free gases

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US (1) US3868331A (fr)
JP (1) JPS5710156B2 (fr)
BE (1) BE800947A (fr)
CA (1) CA1004465A (fr)
DE (1) DE2332172A1 (fr)
FR (1) FR2190905B1 (fr)
GB (1) GB1437090A (fr)
IT (1) IT989352B (fr)
NL (1) NL7308788A (fr)
ZA (1) ZA734280B (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3964882A (en) * 1973-10-19 1976-06-22 Shell Oil Company Partial combustion process
US6213033B1 (en) * 1996-09-02 2001-04-10 Fioter Oy Method for treating waste material containing hydrocarbons
WO2009065792A1 (fr) * 2007-11-19 2009-05-28 Shell Internationale Research Maatschappij B.V. Procédé de préparation d'un mélange d'hydrogène et de monoxyde de carbone

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2804933A1 (de) * 1978-02-06 1979-08-09 Ght Hochtemperaturreak Tech Produktion von synthesegas aus kohle
JPS61211396A (ja) * 1985-03-16 1986-09-19 Tsumoru Tajima 燃料・水燃焼法及びその装置
JPH0726107B2 (ja) * 1986-06-16 1995-03-22 積 田島 燃料・水燃焼法
US5266346A (en) * 1989-02-16 1993-11-30 Nabisco, Inc. Extended ester derivatives as low calorie fat mimetics

Citations (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US408674A (en) * 1889-08-06 Apparatus for the manufacture of gas
US2605178A (en) * 1946-09-27 1952-07-29 Standard Oil Dev Co Preparation of gaseous fuel
US2709646A (en) * 1951-03-29 1955-05-31 United Eng & Constructors Inc Method for producing oil gas
US2779667A (en) * 1952-08-05 1957-01-29 Percival C Keith Gas generation
US2844452A (en) * 1950-04-05 1958-07-22 Rudolph L Hasche Self-sustaining regenerative process
US3042507A (en) * 1959-03-28 1962-07-03 Hilgers Giovanni Method for cracking and subsequent gasifying of hydrocarbons
US3048481A (en) * 1958-06-18 1962-08-07 Texaco Inc Method of forming gas tight seal between vessel wall and refractory lining of a synthesis gas generator
US3536455A (en) * 1959-02-24 1970-10-27 Huettenwerk Oberhausen Ag Plant for the production of metallurgical reducing gas
US3607154A (en) * 1969-11-06 1971-09-21 Washington Gas Light Co Refractory bed for gas machine and process for producing oil gas
US3682605A (en) * 1969-07-15 1972-08-08 Tokyo Heat Treating Co Method and apparatus for soot controlling in a thermal decomposition of a hydrocarbon gas
US3715301A (en) * 1971-06-30 1973-02-06 Texaco Inc Multi-hydrotorting of coal

Patent Citations (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US408674A (en) * 1889-08-06 Apparatus for the manufacture of gas
US2605178A (en) * 1946-09-27 1952-07-29 Standard Oil Dev Co Preparation of gaseous fuel
US2844452A (en) * 1950-04-05 1958-07-22 Rudolph L Hasche Self-sustaining regenerative process
US2709646A (en) * 1951-03-29 1955-05-31 United Eng & Constructors Inc Method for producing oil gas
US2779667A (en) * 1952-08-05 1957-01-29 Percival C Keith Gas generation
US3048481A (en) * 1958-06-18 1962-08-07 Texaco Inc Method of forming gas tight seal between vessel wall and refractory lining of a synthesis gas generator
US3536455A (en) * 1959-02-24 1970-10-27 Huettenwerk Oberhausen Ag Plant for the production of metallurgical reducing gas
US3042507A (en) * 1959-03-28 1962-07-03 Hilgers Giovanni Method for cracking and subsequent gasifying of hydrocarbons
US3682605A (en) * 1969-07-15 1972-08-08 Tokyo Heat Treating Co Method and apparatus for soot controlling in a thermal decomposition of a hydrocarbon gas
US3607154A (en) * 1969-11-06 1971-09-21 Washington Gas Light Co Refractory bed for gas machine and process for producing oil gas
US3715301A (en) * 1971-06-30 1973-02-06 Texaco Inc Multi-hydrotorting of coal

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3964882A (en) * 1973-10-19 1976-06-22 Shell Oil Company Partial combustion process
US6213033B1 (en) * 1996-09-02 2001-04-10 Fioter Oy Method for treating waste material containing hydrocarbons
WO2009065792A1 (fr) * 2007-11-19 2009-05-28 Shell Internationale Research Maatschappij B.V. Procédé de préparation d'un mélange d'hydrogène et de monoxyde de carbone
US20090224209A1 (en) * 2007-11-19 2009-09-10 Jacobus Eilers Process to prepare a mixture of hydrogen and carbon monoxide

Also Published As

Publication number Publication date
JPS4958101A (fr) 1974-06-05
GB1437090A (en) 1976-05-26
JPS5710156B2 (fr) 1982-02-25
IT989352B (it) 1975-05-20
CA1004465A (en) 1977-02-01
NL7308788A (fr) 1973-12-28
FR2190905B1 (fr) 1978-09-29
FR2190905A1 (fr) 1974-02-01
BE800947A (nl) 1973-12-17
ZA734280B (en) 1974-05-29
DE2332172A1 (de) 1974-01-24

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