EP1031623B1 - Procédé de craquage catalytique d'hydrocarbures volatils lourds - Google Patents

Procédé de craquage catalytique d'hydrocarbures volatils lourds Download PDF

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Publication number
EP1031623B1
EP1031623B1 EP00101992A EP00101992A EP1031623B1 EP 1031623 B1 EP1031623 B1 EP 1031623B1 EP 00101992 A EP00101992 A EP 00101992A EP 00101992 A EP00101992 A EP 00101992A EP 1031623 B1 EP1031623 B1 EP 1031623B1
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EP
European Patent Office
Prior art keywords
fluidised bed
particles
raw gas
gas
catalyst
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.)
Expired - Lifetime
Application number
EP00101992A
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German (de)
English (en)
Other versions
EP1031623A2 (fr
EP1031623A3 (fr
Inventor
Johannes Dr. Albrecht
Claus Gretl
Ernst Bareuther
Peter Sturm
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.)
Envirotherm GmbH
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Envirotherm GmbH
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Filing date
Publication date
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Publication of EP1031623A2 publication Critical patent/EP1031623A2/fr
Publication of EP1031623A3 publication Critical patent/EP1031623A3/fr
Application granted granted Critical
Publication of EP1031623B1 publication Critical patent/EP1031623B1/fr
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Classifications

    • 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
    • C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
    • C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/48—Apparatus; Plants
    • C10J3/482—Gasifiers with stationary fluidised bed
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/54—Gasification of granular or pulverulent fuels by the Winkler technique, i.e. by fluidisation
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/02—Dust removal
    • C10K1/024—Dust removal by filtration
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/02—Dust removal
    • C10K1/026—Dust removal by centrifugal forces
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
    • C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
    • C10K3/023—Reducing the tar content
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0916—Biomass
    • C10J2300/092—Wood, cellulose
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0983—Additives
    • C10J2300/0996—Calcium-containing inorganic materials, e.g. lime
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
    • C10J2300/1807—Recycle loops, e.g. gas, solids, heating medium, water
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
    • C10J2300/1861—Heat exchange between at least two process streams
    • C10J2300/1884—Heat exchange between at least two process streams with one stream being synthesis gas

Definitions

  • the invention relates to a process for the catalytic cleavage of in the gasification of carbonaceous masses, in particular biomass and sewage sludge, in a fluidized bed at temperatures of 700 to 1200 ° C, preferably 850 to 950 ° C, and a stoichiometric air factor ⁇ , based on the C. - and H content of the carbonaceous masses, from 0.28 to 0.60 incurred, contained in the crude gas volatile higher, preferably aromatic hydrocarbons of C 6 - to C 22 binding systems.
  • the raw gas must be subjected to gas purification prior to gasification downstream reuse, for example in rotary kilns, boiler plants for energy production, electricity machines, piston engines or the like.
  • gas purification prior to gasification downstream reuse, for example in rotary kilns, boiler plants for energy production, electricity machines, piston engines or the like.
  • the frequently condensing out higher aromatic hydrocarbons hinder gas purification considerably.
  • the D1 refers instead to a process for the production of synthesis gas.
  • the CO and hydrogen synthesis gas is recovered in a gasification process of solid fuels at a pressure of about 5 bar to 150 bar by treatment with oxygen and water vapor at 350 ° C to 700 ° C.
  • the crude gas thus obtained is post-treated in a subsequent reactor at a temperature between 800 ° C and 1400 ° C with the addition of a dust fuel or liquid hydrocarbons and oxygen in the presence of catalysts in a fluidized bed to remove higher hydrocarbons.
  • nickel, cobalt or chromium oxides and / or sulfides are disclosed.
  • the fluidized bed also contains oxides, spinels or silicates of aluminum and / or magnesium.
  • the particles forming the fluidized bed consist of at least one of oxides, hydroxides and carbonates of calcium, aluminum, silicon, nickel, magnesium, titanium, iron, cobalt and molybdenum and are based on the content of hydrocarbons in the raw gas, in stoichiometric Excess used.
  • a considerable reduction in the content of higher aromatic carbons, in particular the C 6 - to C 22 binding systems to contents ⁇ 500 mg / Nm 3 is achieved.
  • an "in-situ" cleavage ie a splitting of the higher aromatic hydrocarbons, is already achieved during the gasification of the carbonaceous masses by the substances forming the fluidized bed.
  • a particular embodiment of the method according to the invention is to be seen in that the fluidized bed leaving raw gas after a dedusting, ie after the deposition of the resulting from the fluidized bed dust particles, is subjected to a catalytic aftertreatment, in which the residual contents of higher hydrocarbons are almost completely split.
  • the fluidized bed leaving and dedusted raw gas is passed through honeycomb catalysts or bulk catalysts.
  • the still existing higher hydrocarbons are split catalytically at the gasification temperatures prevailing there in gas components which are not condensable at ambient temperatures.
  • catalysts can be dispensed with if up to 15% of the particles forming the fluidized bed consist of a conventional cobalt / molybdenum and / or nickel catalyst.
  • the raw gas at the inlet into the catalyst has such a high concentration of flue dust that this results in a cleaning effect.
  • FIG. 1 a flow chart shown in the drawing (FIG. 1) and an exemplary embodiment.
  • FIG. 2 the influence of different substances of the fluidized bed forming particles on the tar reduction in the raw gas is shown as a bar chart.
  • the crude gas formed by the gasification and leaving the reactor in an amount of 800 m 3 / hour still contains 0.329 g / Nm 3 of hydrocarbons which consist of 0.012 g / Nm 3 of naphthalene and 0.285 g / Nm 3 of BTX aromatics ,
  • naphthalene is dominantly present in the volatile higher aromatic hydrocarbons and can be considered as a guide for the cleavage of hydrocarbons, ie, if it is possible to reduce the naphthalene content to ⁇ 50 mg / Nm 3 , it can be assumed that the raw gas in terms of Content of hydrocarbons is so pure that it is easily suitable for further use in boiler systems, gas turbines, gas engines or the like.
  • the Rchgas is directly in the downstream of the fluidized bed reactor (1) recirculation cyclone (2) pre-dedusted from the particles forming the fluidized bed and fed the deposited particles to the fluidized bed reactor (1) via line (11) again.
  • the raw gas is passed through a in the dip tube (9) of the recycle cyclone (2) arranged honeycomb catalyst (10).
  • the honeycomb catalyst (10) via line (8) leaving raw gas is almost ⁇ 0.05 g / Nm 3 free of higher aromatic hydrocarbons and thus can be supplied to the further gas cleaning without the use of special separator stages.
  • the dedusted raw gas is fed to a boiler plant (12) with a heat exchanger and leaves it via line (16).
  • the crude gas is purified in a downstream bag filter (13) and then fed via line (15) for thermal utilization.
  • the fly ash and debris particles of the particles forming the fluidized bed are removed, discharged via line (17), agglomerated and returned to the fluidized-bed reactor.
  • the column diagram shown in Fig. 2 shows the effect of different fluidizing bed forming materials with a grain size of 0.03 to 3 mm on higher hydrocarbons contained in the raw gas.
  • the value of 100% corresponds to a content of hydrocarbons of 3 to 20 g / Nm 3 .

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Catalysts (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Treating Waste Gases (AREA)
  • Treatment Of Sludge (AREA)

Claims (10)

  1. Procédé de craquage catalytique d'hydrocarbures lourds volatils, de préférence aromatiques, des systèmes de liaisons C6 à C22 contenus dans le gaz brut résultant de la gazéification de masses carbonées, en particulier de biomasses et de boues résiduaires, dans un lit fluidisé à des températures allant de 700 à 1200°C, de préférence de 850 à 950°C, et à un coefficient d'air stoechiométrique À de 0,28 à 0,60, ramené à la teneur en C et H des masses carbonées, caractérisé en ce que le craquage catalytique a lieu dès la gazéification et en ce que les particules qui forment le lit fluidisé se composent d'au moins une substance qui est choisie parmi des oxydes, des hydroxydes et des carbonates de calcium, aluminium, silicium, nickel, magnésium, titane, fer, cobalt et molybdène et qui est utilisée en excès stoechiométrique, ramené à la teneur en hydrocarbures du gaz brut, les particules qui forment le lit fluidisé étant constituées jusqu'à concurrence de 15% d'un catalyseur au cobalt/molybdène classique et/ou d'un catalyseur au nickel dont la granulométrie moyenne d50 se situe dans la plage de 0,5 à 3,0 mm.
  2. Procédé selon la revendication 1, caractérisé en ce que les particules qui forment le lit fluidisé sont constituées d'au moins une substance choisie parmi le sable, la dolomite, la zéolithe, l'argile, la latérite et des matériaux contenant du nickel.
  3. Procédé selon l'une des revendications 1 et 2, caractérisé en ce que la granulométrie moyenne d50 des particules qui forment le lit fluidisé se situe dans la plage de 0,03 à 3,0 mm.
  4. Procédé selon l'une des revendications 1 à 3, caractérisé en ce que la vitesse du gaz se situe dans la plage de 1,0 à 7,0 m/s.
  5. Procédé selon l'une des revendications 1 à 4, caractérisé en ce que le temps de séjour du gaz se situe dans la plage de 2,0 à 15,0 secondes.
  6. Procédé selon l'une des revendications 1 à 5, caractérisé en ce que le gaz brut est soumis à un dépoussiérage préalable dans un cyclone de recyclage disposé en amont du réacteur à lit fluidisé, les cendres volantes et les particules d'abrasion qu'il contient étant séparées des particules qui forment le lit fluidisé et renvoyées dans le lit fluidisé.
  7. Procédé selon la revendication 6, caractérisé en ce que les cendres volantes et les particules d'abrasion sont agglomérées après la séparation.
  8. Procédé selon l'une des revendications 1 à 5, caractérisé en ce que le gaz brut préalablement dépoussiéré qui sort ensuite du lit fluidisé est soumis à un retraitement catalytique.
  9. Procédé selon la revendication 8, caractérisé en ce que le gaz brut s'écoule dans un catalyseur en nid d'abeilles.
  10. Procédé selon la revendication 8, caractérisé en ce que le gaz brut s'écoule dans un catalyseur en vrac.
EP00101992A 1999-02-24 2000-02-02 Procédé de craquage catalytique d'hydrocarbures volatils lourds Expired - Lifetime EP1031623B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19907901 1999-02-24
DE19907901A DE19907901C2 (de) 1999-02-24 1999-02-24 Verfahren zur katalytischen Spaltung von flüchtigen höheren Kohlenwasserstoffen

Publications (3)

Publication Number Publication Date
EP1031623A2 EP1031623A2 (fr) 2000-08-30
EP1031623A3 EP1031623A3 (fr) 2002-12-18
EP1031623B1 true EP1031623B1 (fr) 2007-06-13

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EP00101992A Expired - Lifetime EP1031623B1 (fr) 1999-02-24 2000-02-02 Procédé de craquage catalytique d'hydrocarbures volatils lourds

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EP (1) EP1031623B1 (fr)
AT (1) ATE364672T1 (fr)
DE (2) DE19907901C2 (fr)

Families Citing this family (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10037762B4 (de) * 2000-03-23 2010-01-28 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Vorrichtung zur Stromerzeugung aus Biomasse durch Vergasung mit anschließender katalytischer Beseitigung von Teerverbindungen aus dem Brenngas
EP1142981A3 (fr) * 2000-03-23 2003-04-02 Fraunhofer-Gesellschaft Zur Förderung Der Angewandten Forschung E.V. Appareillage de génération d'électricité par gazéification de biomasse suivi par l'élimination catalytique des composés du goudron
AR047413A1 (es) 2004-01-13 2006-01-18 Dsm Ip Assets Bv Proceso para el blanqueado enzimatico de productos alimenticios
DE102007025420B4 (de) * 2007-05-31 2011-12-08 Karlsruher Institut für Technologie Verfahren zur Entfernung von Teersubstanzen aus Rohsynthesegasen mittels Katalysator
US8460410B2 (en) 2008-08-15 2013-06-11 Phillips 66 Company Two stage entrained gasification system and process
CN102827641B (zh) * 2012-09-10 2014-07-23 庆华集团新疆和丰能源化工有限公司 一种煤气化热解炉
CN114836225A (zh) * 2022-04-29 2022-08-02 浙江科技学院 一种酸性生物炭的制备方法

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DE2532197C3 (de) * 1975-07-18 1980-05-22 Metallgesellschaft Ag, 6000 Frankfurt Verfahren zur Erzeugung von Synthesegasen
GB1558996A (en) * 1976-07-27 1980-01-09 Gulf Oil Corp Fliud bed gasifier
US4828581A (en) * 1985-09-20 1989-05-09 Battelle Development Corporation Low inlet gas velocity high throughput biomass gasifier
SE8605211L (sv) * 1986-12-04 1988-06-05 Skf Steel Eng Ab Sett att framstella en gas lempad for energiproduktion
SE459584B (sv) * 1987-10-02 1989-07-17 Studsvik Ab Foerfarande foer foeraedling av raagas framstaelld ur ett kolhaltigt material
AT392079B (de) * 1988-03-11 1991-01-25 Voest Alpine Ind Anlagen Verfahren zum druckvergasen von kohle fuer den betrieb eines kraftwerkes
CA2127394A1 (fr) * 1993-07-12 1995-01-13 William Martin Campbell Reacteur de gazeification

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Title
"Biomass Gasification and Pyrolysis", August 1997, M. KALTSCHMITT & A.V. BRIDGEWATER, EUROPEAN COMMISION *
"Catalytic hot gas cleaning of gasification gas", VALTION TEKNILLINEN TUTKIMUSKESKUS (VTT), 1997, VTT Publication 330 *
IND. ENG. RES., vol. 36, 1997, pages 3800 - 3808 *
IND. ENG. RES., vol. 36, 1997, pages 5220 - 5226 *
IND. ENG. RES., vol. 36, 1997, pages 5227 - 5239 *
POWDER TECHNOLOGY, vol. 93, 1997, pages 93 - 100 *

Also Published As

Publication number Publication date
DE19907901C2 (de) 2001-11-29
ATE364672T1 (de) 2007-07-15
EP1031623A2 (fr) 2000-08-30
DE50014394D1 (de) 2007-07-26
EP1031623A3 (fr) 2002-12-18
DE19907901A1 (de) 2000-09-07

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