EP1031623A2 - 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
EP1031623A2
EP1031623A2 EP00101992A EP00101992A EP1031623A2 EP 1031623 A2 EP1031623 A2 EP 1031623A2 EP 00101992 A EP00101992 A EP 00101992A EP 00101992 A EP00101992 A EP 00101992A EP 1031623 A2 EP1031623 A2 EP 1031623A2
Authority
EP
European Patent Office
Prior art keywords
fluidized bed
raw gas
particles forming
particles
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.)
Granted
Application number
EP00101992A
Other languages
German (de)
English (en)
Other versions
EP1031623A3 (fr
EP1031623B1 (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
Original Assignee
Metallgesellschaft AG
MG Technologies 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 Metallgesellschaft AG, MG Technologies AG filed Critical Metallgesellschaft AG
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
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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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 splitting of in the gasification of carbon-containing masses, in particular biomass and sewage sludge, in a fluidized bed at temperatures from 700 to 1200 ° C, preferably 850 to 950 ° C, and a stoichiometric air factor ⁇ , based on the C. - and H content of the carbon-containing masses, from 0.28 to 0.60 volatile higher, preferably aromatic hydrocarbons of the C 6 to C 22 binding systems contained in the raw gas.
  • the raw gas produced during the gasification of carbonaceous masses such as bio-waste, waste, sewage sludge, coal and the like, in a fluidized bed under lack of oxygen at temperatures from 700 to 1200 ° C. contains up to 20 g / Nm 3 higher, preferably aromatic hydrocarbons of the C 6 -bis C 22 binding systems.
  • the raw gas usually has to be before gasification downstream recycling, for example in Rotary kilns, boiler systems for power generation, Current machines, piston machines or the like Be subjected to gas cleaning. Often condensing higher aromatic Hydrocarbons significantly hamper gas cleaning.
  • the tar content of the raw gas is usually reduced by washing.
  • the formation of aerosols that occurs makes it difficult to remove tar.
  • This disadvantage tries to remedy by means of a method known from EP-B 0 310 584 for the purification of raw gas produced from a carbon-containing material by gasification.
  • the raw gas generated in a first stage is subjected to a catalytic treatment in a second stage formed from a circulating fluidized bed in the presence of magnesium-calcium carbonate-containing material.
  • the tar content in the raw gas is reduced to less than 500 mm / Nm 3 .
  • Such a low tar content generally allows the raw gas to be cleaned by means of bag filters, since the low tar contents are absorbed by the carbon-rich dust particles still present, so that the particles remain free-flowing and the bag filters do not stick together.
  • the particles forming the fluidized bed consist of at least one of the substances selected from oxides, hydroxides and carbonates of calcium, aluminum, silicon, nickel, magnesium, titanium, iron, cobalt and molybdenum, and related on the content of hydrocarbons in the raw gas, are used in stoichiometric excess.
  • This measure considerably reduces the content of higher aromatic carbons, in particular the C 6 to C 22 binding systems, to contents of ⁇ 500 mg / Nm 3 .
  • an "in-situ" cleavage ie a cleavage of the higher aromatic hydrocarbons, is achieved during the gasification of the carbon-containing masses.
  • a special training of the invention The process can be seen in the fact that this is the fluidized bed leaving raw gas after pre-dedusting, d. H. to the separation of those from the fluidized bed Dust particles, a catalytic aftertreatment is subjected to, in which the residual contents at higher Hydrocarbons are almost completely split.
  • the fluid bed is expediently left and dedusted raw gas over honeycomb catalysts or Bulk catalysts directed. They are still existing higher hydrocarbons at those there prevailing gasification temperatures catalytically in at Ambient temperatures of non-condensable gas components split. However, such catalysts can to be waived if up to 15% of the fluidized bed forming particles from a common cobalt / molybdenum and / or nickel catalyst exist.
  • the Raw gas at the entrance to the catalyst is so high Airborne dust concentration, that a cleaning effect entry.
  • the invention is based on one in the Drawing (Fig. 1) and a flow chart Embodiment explained in more detail.
  • 2 is the Influence of different substances on the fluidized bed forming particles on the tar reduction in the raw gas as Column chart reproduced.
  • the raw gas formed by the gasification and emerging from 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 .
  • the naphthalene is predominantly present in the volatile higher aromatic hydrocarbons and can be regarded as a key parameter for the splitting of the hydrocarbons, ie if the naphthalene content can be reduced to ⁇ 50 mg / Nm 3 , it can be assumed that The hydrocarbon content is so pure that it is suitable for further use in boiler systems, gas turbines, gas engines or the like without any problems.
  • the raw gas is directly dedusted from the particles forming the fluidized bed in the recycle cyclone (2) downstream of the fluidized bed reactor (1) and the separated particles are fed back to the fluidized bed reactor (1) via line (11).
  • the raw gas is passed over a honeycomb catalyst (10) arranged in the dip tube (9) of the recycle cyclone (2).
  • the raw gas leaving the honeycomb catalyst (10) via line (8) is almost ⁇ 0.05 g / Nm 3 free of higher aromatic hydrocarbons and can thus be fed to further gas cleaning without the use of special separator stages.
  • the dedusted raw gas is fed to a boiler system (12) with a heat exchanger and leaves it via line (16).
  • the raw gas is cleaned in a downstream bag filter (13) and then fed to a thermal utilization via line (15).
  • the fly ash and abrasion particles of the particles forming the fluidized bed still contained therein are removed from the raw gas leaving the return cyclone (2), discharged via line (17), agglomerated and returned to the fluidized bed reactor.
  • the bar diagram shown in FIG. 2 shows the effect of different substances forming the fluidized bed 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 hydrocarbon content 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)
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 true EP1031623A2 (fr) 2000-08-30
EP1031623A3 EP1031623A3 (fr) 2002-12-18
EP1031623B1 EP1031623B1 (fr) 2007-06-13

Family

ID=7898658

Family Applications (1)

Application Number Title Priority Date Filing Date
EP00101992A Expired - Lifetime EP1031623B1 (fr) 1999-02-24 2000-02-02 Procédé de craquage catalytique d'hydrocarbures volatils lourds

Country Status (3)

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

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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
WO2010019319A2 (fr) 2008-08-15 2010-02-18 Conocophillips Company Système et processus de gazéification par entraînement à deux étages
EP2316280A1 (fr) 2004-01-13 2011-05-04 DSM IP Assets B.V. Blanchiment enzymatique dans les lessives de foyer et blanchiment a la pierre
CN102827641A (zh) * 2012-09-10 2012-12-19 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

Families Citing this family (2)

* 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
DE102007025420B4 (de) * 2007-05-31 2011-12-08 Karlsruher Institut für Technologie Verfahren zur Entfernung von Teersubstanzen aus Rohsynthesegasen mittels Katalysator

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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
EP2316280A1 (fr) 2004-01-13 2011-05-04 DSM IP Assets B.V. Blanchiment enzymatique dans les lessives de foyer et blanchiment a la pierre
WO2010019319A2 (fr) 2008-08-15 2010-02-18 Conocophillips Company Système et processus de gazéification par entraînement à deux étages
WO2010019319A3 (fr) * 2008-08-15 2010-06-24 Conocophillips Company Système et processus de gazéification par entraînement à deux étages
US8460410B2 (en) 2008-08-15 2013-06-11 Phillips 66 Company Two stage entrained gasification system and process
US8888876B2 (en) 2008-08-15 2014-11-18 Lummus Technology Inc. Two stage entrained gasification system and process
AU2009282334B2 (en) * 2008-08-15 2015-11-12 Lummus Technology Llc Two stage entrained gasification system and process
CN102827641A (zh) * 2012-09-10 2012-12-19 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

Also Published As

Publication number Publication date
DE19907901C2 (de) 2001-11-29
ATE364672T1 (de) 2007-07-15
DE50014394D1 (de) 2007-07-26
EP1031623A3 (fr) 2002-12-18
EP1031623B1 (fr) 2007-06-13
DE19907901A1 (de) 2000-09-07

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