EP3455162A1 - Procédé pour former un gaz de synthèse - Google Patents

Procédé pour former un gaz de synthèse

Info

Publication number
EP3455162A1
EP3455162A1 EP17723320.2A EP17723320A EP3455162A1 EP 3455162 A1 EP3455162 A1 EP 3455162A1 EP 17723320 A EP17723320 A EP 17723320A EP 3455162 A1 EP3455162 A1 EP 3455162A1
Authority
EP
European Patent Office
Prior art keywords
range
parameters
hydrocarbon
vapor mixture
pressure vessel
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.)
Pending
Application number
EP17723320.2A
Other languages
German (de)
English (en)
Inventor
Evgeni Dr. Gorval
Joachim Dr. Johanning
Bernd Dr. KEIL
Katja Dr. POSCHLAD
Christiane Potthoff
Dennis Dr. REBIEN
Josef Kurt
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.)
GORVAL, EVGENI
Original Assignee
ThyssenKrupp AG
ThyssenKrupp Industrial Solutions AG
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by ThyssenKrupp AG, ThyssenKrupp Industrial Solutions AG filed Critical ThyssenKrupp AG
Publication of EP3455162A1 publication Critical patent/EP3455162A1/fr
Pending legal-status Critical Current

Links

Classifications

    • 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
    • C01B3/38—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 catalysts
    • C01B3/382—Multi-step processes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0244—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being an autothermal reforming step, e.g. secondary reforming processes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1276—Mixing of different feed components

Definitions

  • the present invention relates to a process for the formation of a synthesis gas by autothermal reforming.
  • synthesis gas is an important step in the production of a variety of substances such as ammonia, methanol and synthetic fuels from carbonaceous feedstocks.
  • the reforming of hydrocarbonaceous feedstocks, especially natural gas, with steam is today the predominant process for the production of synthesis gas.
  • synthesis gases gas mixtures with the main components H 2 and CO are referred to, depending on the technology and application they may contain other components such as, for example, proportions of H 2 0, C0 2 , N 2 , CH 4 and argon.
  • Synthesis gases are the basis for the large-scale production of ammonia, pure hydrogen, methanol and synthetic fuels.
  • hydrocarbonaceous feedstocks can usually be carried out either in a cracking furnace with external heating (steam reformer) or in an autothermal reformer (ATR) with an internal heating.
  • steam reformer steam reformer
  • ATR autothermal reformer
  • Hydrocarbon-containing feedstocks include natural gas, liquefied petroleum gas and biogas , Butane, gasoline or another type of hydrocarbon.
  • the autothermal reforming is a combination of partial oxidation of the feed gas with an oxygen-containing oxidant and steam reforming of hydrocarbon-containing feedstocks, wherein both the partial oxidation and the steam reforming take place within a reactor.
  • the advantage of autothermal reforming is the elimination of the external heat source.
  • the exothermic partial oxidation reaction (1) and the exothermic water gas shift reaction (3) partially cover the energy requirements for the endothermic steam reforming reaction (2).
  • the additional energy requirement is at least partially covered by the combustion reactions (4) and (5).
  • These reactions are exemplary for the reforming of methane formulated: CH 4 + 1/2 0 2 ⁇ CO (1)
  • the reactions usually run at operating temperatures of 500-1250 ° C and pressures up to 70 bar abs.
  • the combustion of the hydrocarbon-containing feedstocks takes place with a substoichiometric amount of oxygen with the aid of a flame reaction in the combustion zone of a reactor.
  • the steam reforming reaction begins in the combustion zone, but occurs predominantly in the same reactor in the fixed bed of a steam reforming catalyst.
  • autothermal reforming has many advantages compared to steam reforming with only external heating. It is characterized by a compact design of the reformer, by significantly lower construction costs and better controllability compared to steam reforming, is mechanically relatively easy to carry out and allows a quick startup and shutdown of the reformer.
  • the combustion of hydrocarbon-containing feedstocks with substoichiometric amounts of oxygen takes place essentially in the region of the partial oxidation above the catalyst (POX zone).
  • POX zone the region of the partial oxidation above the catalyst
  • the geometry of the POX zone should be designed so that extremely hot zones keep a certain distance from the walls of the pressure vessel and the surface of the packed bed, so that a local overheating of areas of the refractory lining of the pressure vessel, the catalyst or of Nozzle for feeding the oxygen-containing oxidant can be avoided.
  • the object of the invention is to increase the service life of a reactor for autothermal reforming.
  • This object is achieved by a process for the formation of a synthesis gas by autothermal reforming, wherein a hydrocarbons and water vapor-containing hydrocarbon vapor mixture and an oxygen-containing gas are introduced into a pressure vessel, the hydrocarbons are partially oxidized in a reaction zone of the pressure vessel and a Catalyst bed of the pressure vessel to be supplied, wherein the reaction zone of the pressure vessel has a conical portion and a cylindrical portion with a cylinder height, wherein the pressure vessel, a hydrocarbon vapor mixture volume flow V in the range of 37,000 / P m 3 / h to 1 .000,000 / P m 3 / h is supplied and from the pressure vessel, a synthesis gas flow N in the range of 1090 kmol / h to 40,000 kmol / h with a molecular density A in the range of P
  • the gas pressure P [bar abs] at the outlet of the pressure vessel is in the range from 10 bar abs to 73.5 bar abs, preferably in the range from 10 bar abs to 71.7 bar abs, in the range from 10 bar abs to 70 bar abs, in the range of 10 bar abs to 60 bar abs, in the range of 10 bar abs to 50 bar abs, in the range of 10 bar abs to 40 bar abs, in the range of 10 bar abs to 30 bar abs or in the range of 10 bar abs up to 28.5 bar abs.
  • the gas pressure at the outlet of the pressure vessel can be 42 bar abs.
  • the vapor / carbon ratio (S / C) of the hydrocarbon vapor mixture is the molar ratio of water vapor molecules to carbon atoms in the gas mixture, but only those carbon atoms of compounds which are pure hydrocarbons, ie free from oxygen, are included; Carbon atoms of alcohols, aldehydes, etc. are not included accordingly.
  • the steam / carbon ratio (S / C) has the unit [mol / mol] and is accordingly dimensionless.
  • the S / C ratio at the inlet of the autothermal reformer is preferably in the range of 0.1 to 3.0, more preferably in the range of 0.5 to 2.7, more preferably in the range of 1.0 to 2.5, more preferably in the range of 1.5 to 2.4, more preferably in the range of 0.3 to 1.0, or in the range of 2.2 to 3.0.
  • a preferred embodiment provides that the cylinder height hi as a function of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ] in the range of
  • cylinder height hi as a function of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ]) in the range from
  • cylinder height h- ⁇ as a function of speed of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ] In the range of N 3
  • cylinder height h- ⁇ as a function of speed of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ] In the range of N 3
  • An alternative, preferred embodiment provides that the cylinder height hi as a function of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ] in the range of
  • cylinder height h- ⁇ as a function of speed of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ] In the range of N 3
  • cylinder height h- ⁇ as a function of speed of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ] In the range of N 3
  • An alternative, preferred embodiment provides that the cylinder height hi as a function of the hydrocarbon-vapor mixture volume flow V [m 3 / h], the synthesis gas flow N [kmol / h] and the molar density A [mol / m 3 ] in the range of
  • the hydrocarbon-vapor mixture is twisted around a longitudinal axis of the pressure vessel and the oxygen-containing gas is twisted around the longitudinal axis of the pressure vessel.
  • the temperature distribution in the reaction zone can be further improved.
  • the hydrocarbon-vapor mixture is produced by mixing hydrocarbons with steam and then the hydrocarbon-vapor mixture is twisted in a subsequent process step.
  • the twisting of the Hydrocarbon vapor mixture can be carried out, for example, by a swirl generator, in particular a swirl generator with wing-like guide plates for a tangential supply to the reactor, in which the untwisted hydrocarbon vapor mixture is introduced and flows as a twisted hydrocarbon vapor mixture into the reactor.
  • the oxygen-containing gas can be vaporized by means of an inflow device which has nozzles which each extend along a nozzle longitudinal axis and wherein the nozzle longitudinal axes have no point of intersection with the longitudinal axis of the pressure container.
  • the hydrocarbon-vapor mixture and the oxygen-containing gas are counter-twisted.
  • the ratio of the amount of an angular momentum of the hydrocarbon vapor mixture to the amount of an angular momentum of the oxygen-containing gas is in the range from 1 to 8, preferably in the range from 3 to 6, particularly preferably 4.
  • An advantageous embodiment of the method provides that the oxygen-containing gas is introduced via nozzles into the pressure vessel, wherein the nozzles are arranged on a conical inner wall of the pressure vessel.
  • a lower overall height of the pressure vessel can be made possible.
  • a more uniform flow of the catalyst bed can be made possible, whereby the thermal load of the bed is reduced.
  • the oxygen-containing gas can be introduced into the pressure vessel, in particular into the POX zone of the pressure vessel, in such a way that it has an angular momentum, i. that it is twisted.
  • the oxygen-containing gas is supplied via the nozzles in a direction having an inclination angle with respect to a radial plane extending through the longitudinal axis of the pressure vessel and the point of the nozzle entrance into the pressure vessel greater than 0 ° is in the range of 7 ° to 89 °, more preferably in the range of 10 ° to 45 °.
  • FIG. 1 shows an autothermal reformer for carrying out the method according to the invention in a schematic sectional view.
  • FIG. 2 shows a schematic sectional view through the autothermal reformer of Figure 1 along a sectional plane in the region of the nozzle.
  • Figures 3 to 23 show various embodiments of an autothermal reformer for carrying out the method according to the invention in schematic sectional views.
  • FIG. 1 shows an apparatus designed as an autothermal reformer for carrying out the method according to the invention for forming a synthesis gas.
  • the apparatus comprises a pressure vessel 10 having an inlet 14, via which a hydrocarbon-vapor mixture containing hydrocarbons and water vapor is introduced into the pressure vessel 10.
  • a swirl generator 17 is arranged, via which the hydrocarbon-vapor mixture is twisted.
  • a reaction zone 11 is formed, in which the introduced hydrocarbons are partially oxidized.
  • an oxygen-containing gas is introduced via several nozzles 13 in the reaction zone 1 1, in which the partial oxidation takes place with flame formation.
  • the reaction zone 1 1 has a the inlet 14 facing conical region 1 1.1. Further, the reaction zone 1 1 comprises a cylindrical portion 1 1 .2, which immediately adjacent to the conical portion 1 1 .1 and is arranged on a side 14 opposite the inlet of the conical region 1 1.1. On the conical region 1 1 .1 opposite side of the cylindrical portion 1 1 .2 of the reaction zone 1 1, a catalyst bed 12 adjacent to the reaction zone 1 1 at.
  • the pressure vessel 10 further comprises an outlet 15, which is arranged on one of the reaction zone 1 1 opposite side of the catalyst bed 12.
  • a refractory lining is arranged both in the reaction zone 1 1 and in the region of the catalyst bed 12.
  • the pressure vessel 10 has a manhole 16, which is provided in the cylindrical region 11.2 of the reaction zone 11.
  • the pressure vessel 10 is supplied with a hydrocarbon-vapor mixture volume flow V in the range from 37,000 / P m 3 / h to 1,000,000 / P m 3 / h.
  • the hydrocarbon-vapor mixture is partially oxidized in the reaction zone 1 1 with the addition of an oxygen-containing gas and then fed to the catalyst bed 12.
  • a synthesis gas stream N in the range of 1090 kmol / h to 40,000 kmol / h with a density A in the range from P-6.9 mol / m 3 to P-9.5 mol / subtracted 3 m.
  • P denotes the dimensionless numerical value of the gas pressure [bar abs] at the outlet 15 of the pressure vessel 10.
  • the height of the catalyst bed 12 is designated by the reference numeral H, the cylinder height of the cylindrical portion 1 1.2 of the reaction zone with h- ⁇ .
  • the nozzles 13 for introducing the oxygen-containing gas are arranged in the conical region 1.1 of the reaction zone 11.
  • the height of the conical region 1 1 .1 of the reaction zone is h 2 + h 3 , where h 2 is the distance of the nozzles 13 from the cylindrical portion 1 1.2 and h 3 the distance of the nozzles 13 from the inlet 14 in the direction of a longitudinal axis L of Pressure vessel 10 denotes.
  • FIG. 2 shows a sectional view along the section line II-II 'shown in FIG.
  • the illustration shows a radial plane R which encloses the longitudinal axis L and corresponds to the plane of the sheet of FIG.
  • the nozzles 13 are arranged in the conical region 1.1 in such a way that the nozzles 13 enclose an angle of inclination ⁇ with the radial plane R.
  • the oxygen-containing gas is supplied via the nozzles 13 in a direction which has an inclination angle ⁇ with respect to the plane passing through the longitudinal axis L of the pressure vessel 10 radial plane R.
  • the inclination angle ⁇ is greater than 0 °; it is preferably in the range of 7 ° to 89 °, more preferably in the range of 10 ° to 45 °.
  • a total of five nozzles 13 are provided in the pressure vessel 10.
  • the nozzles 13 each have an identical distance from each other.
  • a different number of nozzles 13 may be provided, for example, three, four, six, seven, eight, nine, ten or more nozzles 13.
  • the hydrocarbon vapor mixture and the oxygen-containing gas are counter-twisted, wherein the ratio of the amount of Angular momentum of the hydrocarbon substance vapor mixture to the amount of an angular momentum of the oxygen-containing gas in the range of 1 to 8, preferably in the range of 3 to 6, particularly preferably 4.
  • exemplary embodiments of geometries of the pressure vessel 10 are shown, which are suitable for carrying out the method according to the invention. All embodiments are based on the following common operating conditions:
  • the ratio of the volume flow in Nm 3 / h to DIN 1343 at the outlet 15 to the volume of the catalyst bed in m 3 is in the range of 5,000 (Nm 3 / h) / (m 3 ) to 55,000 (Nm 3 / h) / (m 3 ).
  • the residence time 3600 s V PO x [m 3 ] / V OUT [m 3 / h] is in the range of 0.5 s to 6 s.
  • the ratio of the height H of the catalyst bed 12 to the diameter D of the catalyst bed is in the range of 0.5 to 4.
  • the inlet velocity of the carbon-steam mixture is in the range of 1 m / s to 40 m / s.
  • the walls of the conical region include a cone angle of 2a.
  • the halved cone angle ⁇ is in the range of 10 ° to 60 °.
  • the distance h 3 is in the range of 0.25 m to 3 m.
  • the dimensionless numerical value P of the gas pressure [bar abs] at the outlet 15 of the pressure vessel 10 is in the range of 10 to 73.5.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

La présente invention concerne un procédé pour former un gaz de synthèse par reformage autotherme. Un mélange de vapeurs d'hydrocarbures contenant des hydrocarbures et de la vapeur d'eau et un gaz contenant de l'oxygène sont introduits dans un réservoir sous pression, les hydrocarbures étant partiellement oxydés dans une zone de réaction du réservoir sous pression et amenés à un lit catalytique du réservoir sous pression. La zone de réaction du réservoir sous pression comprend une zone conique et une zone cylindrique ayant une hauteur de cylindre, le mélange de vapeurs d'hydrocarbures étant amené dans le réservoir sous pression à un débit V situé dans une plage de 37 000/P m3/h à 1 000 000/P m3/h et un courant de gaz de synthèse N étant extrait du réservoir sous pression à un débit situé dans une plage de 1 090 kmol/h à 40 000 kmol/h avec une densité molaire A située dans une plage de P.6,9 mol/m3 à P.9,5 mol/m3, P étant la valeur numérique sans dimensions de la pression gazeuse [bar abs], au niveau d'une évacuation du réservoir sous pression, ladite valeur se situant dans une plage de 10 à 73,5.
EP17723320.2A 2016-05-12 2017-05-05 Procédé pour former un gaz de synthèse Pending EP3455162A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102016108792.0A DE102016108792A1 (de) 2016-05-12 2016-05-12 Verfahren zur Bildung eines Synthesegases
PCT/EP2017/060830 WO2017194427A1 (fr) 2016-05-12 2017-05-05 Procédé pour former un gaz de synthèse

Publications (1)

Publication Number Publication Date
EP3455162A1 true EP3455162A1 (fr) 2019-03-20

Family

ID=58707513

Family Applications (1)

Application Number Title Priority Date Filing Date
EP17723320.2A Pending EP3455162A1 (fr) 2016-05-12 2017-05-05 Procédé pour former un gaz de synthèse

Country Status (3)

Country Link
EP (1) EP3455162A1 (fr)
DE (1) DE102016108792A1 (fr)
WO (1) WO2017194427A1 (fr)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114505014B (zh) * 2022-04-19 2022-06-28 北京中科富海低温科技有限公司 一种压力容器

Family Cites Families (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2943062A (en) * 1956-01-19 1960-06-28 Kellogg M W Co Conversion of hydrocarbons to a hydrogen-rich gas
GB0120071D0 (en) * 2001-08-17 2001-10-10 Ici Plc Steam reforming
US7261749B2 (en) * 2002-09-05 2007-08-28 General Motors Corporation Multi-port autothermal reformer
US6818198B2 (en) * 2002-09-23 2004-11-16 Kellogg Brown & Root, Inc. Hydrogen enrichment scheme for autothermal reforming
EP1728761A1 (fr) * 2005-06-02 2006-12-06 Casale Chemicals S.A. Procédé pour la production de gaz de synthèse et appareil correspondant
DE102008039014A1 (de) * 2008-08-21 2010-02-25 Uhde Gmbh Mehrstufige Reaktorkaskade zur rußfreien Herstellung von Systhesegas
EP2676924A1 (fr) * 2012-06-21 2013-12-25 Haldor Topsoe A/S Procédé de reformage d'hydrocarbures
WO2015128456A1 (fr) * 2014-02-28 2015-09-03 Haldor Topsøe A/S Procédé de production de gaz de synthèse
EP2915780A1 (fr) * 2014-03-05 2015-09-09 Air Products And Chemicals, Inc. Systèmes et procédés basés sur un réacteur à membrane de transport d'ions pour la production de gaz de synthèse

Also Published As

Publication number Publication date
DE102016108792A1 (de) 2017-11-16
WO2017194427A1 (fr) 2017-11-16

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