EP0806467A1 - Verfahren und Einrichtung zur thermischen Umsetzung von Kohlenwasserstoffen zu ungesättigten aliphatischen Kohlenwasserstoffen durch Kombination einer Dampfkrackung und einer Pyrolysestufe - Google Patents

Verfahren und Einrichtung zur thermischen Umsetzung von Kohlenwasserstoffen zu ungesättigten aliphatischen Kohlenwasserstoffen durch Kombination einer Dampfkrackung und einer Pyrolysestufe Download PDF

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Publication number
EP0806467A1
EP0806467A1 EP97400998A EP97400998A EP0806467A1 EP 0806467 A1 EP0806467 A1 EP 0806467A1 EP 97400998 A EP97400998 A EP 97400998A EP 97400998 A EP97400998 A EP 97400998A EP 0806467 A1 EP0806467 A1 EP 0806467A1
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EP
European Patent Office
Prior art keywords
zone
pyrolysis
steam cracking
water vapor
rows
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
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EP97400998A
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English (en)
French (fr)
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EP0806467B1 (de
Inventor
Christian Busson
Pierre Marache
Jean-Pierre Burzynski
Christian Dubois
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
IFP Energies Nouvelles IFPEN
Engie SA
Original Assignee
IFP Energies Nouvelles IFPEN
Gaz de France SA
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G51/00—Treatment of hydrocarbon oils, in the absence of hydrogen, by two or more cracking processes only
    • C10G51/02—Treatment of hydrocarbon oils, in the absence of hydrogen, by two or more cracking processes only plural serial stages only
    • C10G51/023—Treatment of hydrocarbon oils, in the absence of hydrogen, by two or more cracking processes only plural serial stages only only thermal cracking steps
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G9/00—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G9/14—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils in pipes or coils with or without auxiliary means, e.g. digesters, soaking drums, expansion means
    • C10G9/16—Preventing or removing incrustation
    • 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
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S585/00—Chemistry of hydrocarbon compounds
    • Y10S585/949—Miscellaneous considerations
    • Y10S585/95—Prevention or removal of corrosion or solid deposits

Definitions

  • the invention relates to a process for the pyrolysis of a hydrocarbon feedstock with at least two carbon atoms and simultaneously a process for decoking the coke deposited on the walls of the reactor.
  • pyrolysis reactors made of ceramic material have been used in which non-watertight partitions advantageously made of ceramic material determine the channels in which the charge and the reaction effluents circulate.
  • These partitions advantageously have a shape adapted to create turbulence and comprise for example cells or cavities at the level of the heating means. These are generally ducts containing an electric heater or a gas burner.
  • a pyrolysis oven operating at a higher temperature should be decoked more often, every four to five days for example. During the decoking stage, this oven must be isolated. Unfortunately, there are no sealing valves operating between 800 and 900 ° C.
  • a variant then consists in sending the effluent from the steam cracker, cooled after passing through a quench exchanger, into the pyrolysis oven, but the benefit of using hot gas is lost and the gain then becomes small. Furthermore, the dead volume of the quench exchanger promotes side reactions to the detriment of the ethylene yield.
  • Another drawback is related to the frequency of decoking of the tubes, every two or three months. Indeed, at the end of the cycle, the interior of the tubes is covered with a thick layer of coke. Coke is liable to detach at times and is entrained by the gas flow at speeds of the order of 200 m / s, risking damage to the ceramic sheaths of the pyrolysis oven downstream from the steam cracking oven.
  • An object of the invention is to provide a method for pyrolyzing a hydrocarbon feedstock without stopping the unit while allowing decoking of this unit.
  • Another object is to reduce the investment and operating costs of the unit.
  • Another object of the invention is to keep the temperature of the installation substantially constant during its operation, to avoid the thermal stresses which would not fail to occur, in particular when using a gas containing oxygen. for the decoking step which implements an exothermic reaction while the pyrolysis step implements an endothermic reaction.
  • the invention relates to a continuous pyrolysis and decoking process in a reaction zone comprising a pyrolysis zone (40) made of refractory material, of elongated shape in a direction (an axis) comprising a heating zone and a cooling zone following the heating zone, the heating zone comprising at least two rows (1, 2) substantially parallel to the axis, separated by a partition (70), advantageously not leaktight, made of refractory material between two successive rows, at least one of said rows (1) receiving hydrocarbons and water vapor, at least one other (2) of said rows receiving essentially water vapor, said rows comprising heating means (8) surrounded by sheaths (7) substantially parallel to each other and substantially perpendicular to the axis of the reactor, coke depositing in the reaction zone, the process being characterized in that circulates a hydrocarbon charge containing at least one hydrocarbon containing at least two carbon atoms at an adequate steam cracking temperature in a steam cracking zone containing at least two steam cracking tubes,
  • the decoking current is circulated in at least the other row of the heating zone so as to at least partially decoker said row and to have an outlet temperature of said zone heating at least 850 ° C and collecting hydrocarbons comprising at least one acetylene compound for example acetylene and a decoking effluent.
  • the exit temperature from the steam cracking zone is generally lower than the exit temperature from the heating zone from the pyrolysis zone.
  • the temperature in the steam cracking tube or tubes where the steam cracking takes place is advantageously maintained substantially equal to the temperature in the tube or tubes where the decoking takes place.
  • the temperature in the row or rows where the pyrolysis of the gas stream leaving the steam cracking zone is carried out is advantageously maintained substantially equal to the temperature in the row or rows where the decoking takes place.
  • the exit temperature from the heating zone relative to the hydrocarbons and the exit temperature from the heating zone relative to the decoking effluent are approximately 1000 to 1400 ° C.
  • the quantity of water vapor introduced into the steam cracking zone, relative to that of the charge, in other words the weight ratio of water vapor to charge, for a determined charge is greater than that corresponding to conventional steam cracking of the same charge.
  • the one which is most suitable for the pyrolysis reaction following the steam cracking reaction is generally adopted.
  • this ratio is greater than 0.5 whereas it is usually around 0.2.
  • the ratio is greater than 0.7 while it is usually about 0.5.
  • the ratio is greater than 1, for example equal to 2 while it is usually close to 1.
  • the choice of a high water vapor to charge ratio has the advantage of reducing the deposition of coke. This will not be able to grow significantly since it is planned to decoker every four or five days for example, that is to say at a frequency corresponding to that of decoking the pyrolysis reactor, at instead of decoking every two to three months in the case of industrial steam crackers.
  • the hydrocarbon supply is cut off in the tube intended to be decoked and the water flow introduced is substantially increased so as not to cause excessive thermal disturbance in the gas preheating furnace. upstream of the steam cracking zone.
  • the steam cracking furnace is usually heated by conventional gas burners, of the radiant burner type.
  • the load is generally preheated between 300 and 400 ° C.
  • the temperature of the steam cracking zone is usually at most equal to 900 ° C.
  • the means for heating the pyrolysis reactor may be electrical resistances contained in sheaths as described in the above patents or they may consist of sheaths containing a gas burner as described in the applicant's patent application ( FR 2715583).
  • Each row may comprise at least one layer of heating means surrounded by sheaths, substantially parallel to the axis of the reaction zone, these sheaths being substantially perpendicular to said axis.
  • heating elements either electric or comprising gas burners, their number, the distance between them and their configuration are described in the patents cited above.
  • a sheath gas containing hydrogen and / or water vapor and / or carbon monoxide and / or an inert gas could be used and moreover could diffuse from the inside towards the outside of the sheaths without disturbing the pyrolysis reaction and without disturbing the reaction of decoking.
  • the collected hydrocarbons and the decoking effluent can be mixed before being introduced into the cooling zone.
  • the collected hydrocarbons and the decoking effluent are cooled separately in their respective rows, located at the level of the cooling zone, then optionally mixed.
  • the cooling zone is usually a zone of direct quenching by a cooling fluid, known to those skilled in the art, advantageously followed by an indirect contact exchanger generating steam (TLE: transfer line exchanger).
  • TLE transfer line exchanger
  • the installation has the advantage of being safe, reliable and easy to implement. It uses in the pyrolysis zone, refractory materials and more particularly ceramic materials known to those skilled in the art such as cordierite, mullite, silicon nitride or silicon carbide.
  • the invention also relates to a continuous pyrolysis and decoking unit for the implementation in particular of the method according to the invention, comprising a pyrolysis reactor (40) of elongated shape in a direction (an axis) comprising at least two rows (1, 2) substantially parallel to the axis separated by a partition, (70) advantageously not leaktight, of refractory material between two successive rows, each row comprising a plurality of heating means (8) arranged in at least one layer of heating elements surrounded by sheaths (7) made of ceramic material substantially parallel to each other and substantially perpendicular to the axis of the reactor, at least one of the rows (1) being adapted to receive hydrocarbons and steam, at least one other ( 2) said rows being adapted to receive water vapor, said pyrolysis reactor comprising means for controlling and modulating heating connected to the heating means, the pyrolysis reactor further comprising cooling means (47) effluents produced in each row, said unit being characterized in that it comprises a steam cracking reactor (30)
  • Hydrocarbon supply lines 11, 12, 13, 14, 15, 16 controlled respectively by valves V1, V2, V3, V4, V5 and V6 introduce into a steam cracker 30 then into a reactor 40 for pyrolysis and decoking of the hydrocarbons, ethane for example, coming from a line 10 in mixture with water generally in vapor form brought by a line 60.
  • This line distributes it in lines 17, 18, 19, 20, 21 and 22 controlled respectively by valves V7, V8, V9, V10, V11 and V12.
  • valves V1 to V12 are adapted to allow the circulation of a mixture of hydrocarbons and steam in a certain number of tubes of the steam cracker 30 and of adjacent rows of the so-called pyrolysis reactor 40 and only water vapor in other tubes of the steam cracker 30 and other adjacent rows of the so-called decoking reactor 40 to remove the coke which has deposited during the reaction respectively steam cracking and pyrolysis.
  • Steam cracker tubes 31, 32, 33, 34, 35, 36 transporting the mixture of hydrocarbons and water or transporting water alone, connected respectively to lines 11 and 22, 12 and 21, 13 and 20, 14 and 19, 15 and 18 and finally, 16 and 17, are heated in the steam cracker 30 to a temperature of 850 to 900 ° C so as to crack part of the hydrocarbon charge and are connected respectively to rows 1, 2, 3, 4 , 5 and 6 of the pyrolysis reactor 40.
  • valve V1 closing the line 11
  • the tube 31 receives only water vapor supplied by the line 22 controlled by the valve V12.
  • the tubes 32, 33, 34, 35 and 36 receive the mixture of hydrocarbons and water, all the other valves mentioned being open.
  • the set of tubes is preheated to about 400 ° C, essentially by convective heating in the first part of the heating furnace, then to about 900 ° C in the second part of the furnace, essentially by radiative heating, by means of a plurality burners.
  • the steam cracking effluent is introduced into the pyrolysis reactor 40 by very short junction lines, not performing the function of quenching.
  • the pyrolysis reactor 40 adjacent to the steam cracking reactor 30 is divided into longitudinal rows (1, 2, 3, 4, 5 and 6) substantially parallel to its axis. These rows are separated from each other by partitions, 70, not leaktight in ceramic material, of shape comprising cells adapted to promote turbulence inside the row and therefore to promote the reaction. These rows contain sheaths of ceramic material 7 forming a sheet substantially parallel to the axis of the reactor. These sheaths are substantially parallel to each other and substantially perpendicular to the axis of the reactor. They contain, for example, a plurality of electrical resistances 8 immersed in a sheath gas, chosen from the group formed by water vapor, hydrogen, carbon monoxide, an inert gas and a mixture of two or more of these gases.
  • the tube 31 containing water vapor is connected by a shortest possible heated line with row 1 of the reactor 40.
  • the flow rate of water vapor introduced into the tube and in the row where s' is increased decokings for example 2 to 3 times that used in the other tubes 32, 33, 34, 35 and the other rows 2, 3, 4, 5 and 6 where the pyrolysis takes place.
  • the outlet temperature of the pyrolysis reactor 40 is heated to around 1200 ° C.
  • the terminal part of the various rows of the reactor 40 intended for pyrolysis or decoking, receives the effluents from pyrolysis or decoking and each row is connected to a line 47 for direct quenching, comprising an injector with controlled flow rate, for example of ethane if the charge is ethane, which allows these effluents to be cooled.
  • a line 47 for direct quenching comprising an injector with controlled flow rate, for example of ethane if the charge is ethane, which allows these effluents to be cooled.
  • lines 41, 42, 43, 44, 45 and 46 connected respectively to rows 1, 2, 3, 4, 5 and 6 mix the various effluents which are discharged through a line 50.
  • the effluents can be cooled by circulating through sealed conduits arranged in the terminal part of the rows by indirect quenching, then mixed as described above.
  • the pyrolysis and decoking effluents from rows 1, 2, 3, 4, 5 and 6 are collected by lines 41, 42, 43, 44, 45 and 46, then mixed and sent to a direct or indirect quenching zone and once cooled discharged via line 50.
  • the heating elements 8 of the pyrolysis reactor are supplied with electrical energy independently by means of a pair of electrodes not shown in the figure, pyrometric thermocouple probes not shown are housed in the spaces where the charge circulates and make it possible to regulate automatically the temperature of each heating section, by a conventional regulation and modulation device not shown in the figure, as a function of the temperature profile chosen which applies to both the pyrolysis reaction and that of decoking the walls sheaths.
  • a temperature regulation device which may be the same, moreover makes it possible to control the temperature of the burners of the steam cracking reactor so that this temperature is lower than the outlet temperature of the hydrocarbons collected and of the final effluent from decoking of the pyrolysis reactor.
  • a steam cracker-pyrolysis reactor assembly described according to FIG. 1 is used to crack a mixture of ethane and steam in order to produce a mixture of ethylene and acetylene.
  • the weight ratio of water vapor to ethane is 1.8.
  • the mixture (ethane-water) and the decoking vapor are brought to 900 ° C in the steam cracking reactor 30 and heated in a substantially linear manner to 1200 ° C in the pyrolysis reactor under an absolute pressure of 1.3 bar.
  • the steam cracker has six heating tubes.
  • the pyrolysis reactor has six heating rows substantially parallel to its axis and separated by partitions in the form of cells and made of ceramic material such as silicon carbide for example. Each row includes a sheet parallel to the axis of electric heating elements.
  • the sheaths perpendicular to the axis of the reactor, surrounding the electrical resistances are made of silicon carbide and contain a sheath gas which is nitrogen.
  • each steam cracking tube 258 kg / h of ethane and 464 kg / h of water vapor are introduced, while in the tube operating in decoking, 979 kg / h of water vapor is introduced via the valve V11 , the hydrocarbon valve V2 being closed.
  • the steam cracking effluent containing hydrocarbons, hydrogen and water vapor is introduced directly into the appropriate rows of the pyrolysis reactor.
  • the tube decoking effluent is introduced directly into the row of the pyrolysis reactor subjected to decoking.
  • the pyrolysis effluent is cooled to 800 ° C by direct contact with 91 kg / h of ethane at 16 ° C while the decoking effluent is cooled to 800 ° C by direct contact with 85 kg / h of ethane at 16 ° C.
  • the ethane flow is cut by the valve V1 and to avoid a disturbance of the thermal regime of the steam cracker and the pyrolysis oven, the water vapor flow rate is increased (valve V12) until 979 kg / h.
  • the tube 32 and the row No. 2 are again supplied with 258 kg / h of ethane and 464 kg / h of steam, by opening the valve V2 and the valve V11.
  • decoking is checked by disappearance of carbon monoxide, which is analyzed online by infrared, for example at the outlet of the pyrolysis oven. It is found that decoking is almost complete after 14 hours in each tube and row where it is carried out and we immediately go back into a steam cracking reaction situation for the tube which has been decoked and pyrolysis for the row which has been decoked.
  • An industrial ethane steam cracker effluent having operated at a temperature of 900 ° C. is used as the pyrolysis hydrocarbon charge, this effluent being cooled by indirect quenching to 450 ° C.
  • This charge, introduced by line 10, is distributed between five lines (n ° 11, 13, 14, 15 and 16) corresponding as for the example above to the five rows working in pyrolysis (n ° 1, 3, 4 , 5 and 6).
  • each row of the pyrolysis zone 258 kg / h of hydrocarbons and hydrogen and 86 kg / h of water from the conventional steam cracker are introduced and each line 17, 18, 19, 20 or 22, 378 kg / h of water.
  • valve V2 of hydrocarbons being closed, 979 kg / h of water vapor are sent via the valve V11 and the line 21.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Feeding, Discharge, Calcimining, Fusing, And Gas-Generation Devices (AREA)
EP97400998A 1996-05-06 1997-05-02 Verfahren und Einrichtung zur thermischen Umsetzung von Kohlenwasserstoffen zu ungesättigten aliphatischen Kohlenwasserstoffen durch Kombination einer Dampfkrackung und einer Pyrolysestufe Expired - Lifetime EP0806467B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR9605760A FR2748273B1 (fr) 1996-05-06 1996-05-06 Procede et dispositif de conversion thermique d'hydrocarbures en hydrocarbures aliphatiques plus insatures que les produits de depart, combinant une etape de vapocraquage et une etape de pyrolyse
FR9605760 1996-05-06

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EP0806467A1 true EP0806467A1 (de) 1997-11-12
EP0806467B1 EP0806467B1 (de) 2000-12-27

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EP97400998A Expired - Lifetime EP0806467B1 (de) 1996-05-06 1997-05-02 Verfahren und Einrichtung zur thermischen Umsetzung von Kohlenwasserstoffen zu ungesättigten aliphatischen Kohlenwasserstoffen durch Kombination einer Dampfkrackung und einer Pyrolysestufe

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US (2) US5976352A (de)
EP (1) EP0806467B1 (de)
JP (1) JP4251303B2 (de)
AU (1) AU726569B2 (de)
CA (1) CA2204541C (de)
DE (1) DE69703763T2 (de)
ES (1) ES2154448T3 (de)
FR (1) FR2748273B1 (de)
ID (1) ID17841A (de)
MY (1) MY113653A (de)
NO (1) NO314507B1 (de)

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US8450552B2 (en) 2009-05-18 2013-05-28 Exxonmobil Chemical Patents Inc. Pyrolysis reactor materials and methods
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FR1501836A (fr) * 1966-04-29 1967-11-18 Exxon Research Engineering Co Procédé de craquage thermique avec décokage des tubes de fours de craquage
EP0542597A1 (de) * 1991-11-08 1993-05-19 Institut Francais Du Petrole Verfahren zur thermischen Pyrolyse von Kohlenwasserstoffen mit Elektroofen
EP0666104A1 (de) * 1994-02-02 1995-08-09 Institut Français du Pétrole Vorrichtung zur Durchführung von chemischen Reaktionen welche, mindestens während des Startens, eine Zuführ von Kalorien nötig haben
EP0733609A1 (de) * 1995-03-23 1996-09-25 Institut Francais Du Petrole Verfahren zur thermischen Umsetzung von aliphatischen gesättigten oder ungesättigten Kohlenwasserstoffen in acetylenischen Kohlenwasserstoffen

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2796078A1 (fr) * 1999-07-07 2001-01-12 Bp Chemicals Snc Procede et dispositif de vapocraquage d'hydrocarbures
WO2001004236A1 (fr) * 1999-07-07 2001-01-18 Naphtachimie Sa Procede et dispositif de vapocraquage d'hydrocarbures
US7288690B2 (en) 1999-07-07 2007-10-30 Bp Chemicals Limited Method and apparatus for steam cracking hydrocarbons

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NO314507B1 (no) 2003-03-31
US5976352A (en) 1999-11-02
NO972070L (no) 1997-11-07
DE69703763T2 (de) 2001-04-19
NO972070D0 (no) 1997-05-05
AU2002997A (en) 1997-11-13
CA2204541C (fr) 2008-07-15
ID17841A (id) 1998-01-29
FR2748273A1 (fr) 1997-11-07
DE69703763D1 (de) 2001-02-01
EP0806467B1 (de) 2000-12-27
CA2204541A1 (fr) 1997-11-06
ES2154448T3 (es) 2001-04-01
JPH10279507A (ja) 1998-10-20
US6322760B1 (en) 2001-11-27
JP4251303B2 (ja) 2009-04-08
AU726569B2 (en) 2000-11-09
MY113653A (en) 2002-04-30
FR2748273B1 (fr) 1998-06-26

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