EP0349090B1 - Méthode pour altérer les contaminants dans un flux de gaz de synthèse brut à haute température et à haute pression - Google Patents

Méthode pour altérer les contaminants dans un flux de gaz de synthèse brut à haute température et à haute pression Download PDF

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Publication number
EP0349090B1
EP0349090B1 EP19890201730 EP89201730A EP0349090B1 EP 0349090 B1 EP0349090 B1 EP 0349090B1 EP 19890201730 EP19890201730 EP 19890201730 EP 89201730 A EP89201730 A EP 89201730A EP 0349090 B1 EP0349090 B1 EP 0349090B1
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EP
European Patent Office
Prior art keywords
gas
synthesis gas
quench
coal
particles
Prior art date
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Expired - Lifetime
Application number
EP19890201730
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German (de)
English (en)
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EP0349090A1 (fr
Inventor
Charles Victor Sternling
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Shell Internationale Research Maatschappij BV
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Shell Internationale Research Maatschappij BV
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Classifications

    • 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
    • C10J3/72—Other features
    • C10J3/82—Gas withdrawal means
    • C10J3/84—Gas withdrawal means with means for removing dust or tar from the gas
    • 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
    • C10J3/466—Entrained flow processes
    • 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
    • C10K1/04—Purifying combustible gases containing carbon monoxide by cooling to condense non-gaseous materials
    • 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
    • C10J2300/093—Coal
    • 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
    • C10J2300/0953—Gasifying agents
    • C10J2300/0959—Oxygen
    • 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
    • C10J2300/12—Heating the gasifier
    • C10J2300/1223—Heating the gasifier by burners
    • 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 partial combustion of finely-divided solid fuel, such as pulverized coal, in which the latter is introduced together with oxygen-containing gas via a burner into a reactor or gasifier from which a stream of high-temperature raw synthesis gas is discharged together with a minor amount of contaminating material, some of which may be in the form of particles having a sticky outer surface, that tend to adhere to equipment located downstream of the reactor.
  • finely-divided solid fuel such as pulverized coal
  • Partial combustion is the reaction of all of the fuel particles with a substoichiometrical amount of oxygen, either introduced in pure form or admixed with other gases, such as a transport stream of nitrogen, whereby the fuel is partially oxidized to hydrogen and carbon monoxide. This partial combustion differs from complete combustion wherein the fuel would be completely oxidized to carbon dioxide and water.
  • the present invention is directed to a process for the partial combustion of finely divided carbonaceous fuel containing at least 1% by weight ash in a reactor or gasifier to produce a product gas (mainly carbon monoxide and hydrogen) which carries along with it, as it leaves the reactor, sticky particles of fly ash or fly slag, or ash-forming constituents which may consist of alkali metal chlorides, silicon and/or aluminium oxides or other mineral species.
  • a product gas mainly carbon monoxide and hydrogen
  • the ash is usually sticky.
  • the residence time in the gasifier or reactor is very short compared with gasification in a fluidized or moving bed process, and the temperature is very high.
  • the ash that is formed during the present gasification process is at least partly in liquid form at the conditions that prevail in the reactor, usually temperatures from 1050 to 2200 °C. If the ash particles are not fully in liquid form, they will generally consist at least partly of a molten slag or be a combustion product or residue having a partly molten consistency.
  • the high temperature of a reactor is sufficient to vaporize certain other by-products which may assume a sticky form when cooled in the process equipment.
  • the invention therefore provides a process for the production of synthesis gas comprising the steps of
  • GB-A-2,053,262 discloses a process for production of synthesis gas from coal involving injection to the synthesis gas of a lower temperature quench gas and mixing of the combined gases under turbulant flow in order to reduce the sticky characteristic of sticky particles.
  • the temperature of the product gas at this point may be, say 1400 °C for example.
  • a stream of product gas, which has been cooled several hundred degrees, is recycled from a selected point in the process and injected as a quench gas into the upstream end of the quench section of the reactor discharge duct.
  • the hot synthesis product gas and the sticky particles carried thereby are thoroughly mixed with the cooler quench gas thereby allowing the molten or sticky particles to "freeze” or at least cause the outer surfaces of the particles to become non-sticky to the extent that they do not stick to the walls of any downstream equipment or piping.
  • the raw synthesis gas also contains minor amounts of vaporized mineral matter and said reducing step includes condensing the vaporized mineral matter by the injection of a volume of quench gas at a lower temperature than the synthesis gas stream into which it is injected.
  • the quench gas stream is injected into the raw synthesis gas stream at a plurality of points around the periphery thereof so as to form at said gas injection area a sheath of cooler quench gas around the hot stream of synthesis gas and the sticky particles carried thereby.
  • the quench gas is synthesis gas taken from a point downstream which contains a minor amount of lower temperature solid particles of the contaminating impurity, said particles being of the same composition as at least one of the impurities in the effluent raw synthesis gas stream leaving the reactor.
  • the steam generated in the gasifier shell may be passed to a heat exchange zone where it may be superheated and then sent for utilization.
  • the gasification may be carried out utilizing techniques suitable for producing a synthesis gas having a gasifier outlet temperature of from about 1050 °C to about 1650 °C.
  • the process is advantageously carried out with a gasifier comprising at least one burner.
  • a gasifier comprising at least one burner.
  • Such a process will advantageously include combustion, with oxygen, of dry particulate coal, i.e., coal having less than about 10 per cent water content. Steam may be added in some instances to assist in the combustion.
  • the type of coal utilized is not critical, but it is an advantage of the invention that lower grade coals, such as lignite or brown coal, may be used. If the water content of the coal is too high to meet the requirements mentioned, supra, the coal should be dried before use.
  • the atmosphere will be maintained reducing by the regulation of the weight ratio of the oxygen to moisture and ash free coal in the range of about 0.6 to 1.2, in particular 0.9 to 1.0.
  • the specific details of the equipment and procedures employed form no part of the invention, but those described in U.S. patent specification No. 4,350,103, and U.S. patent specification No. 4,458,607, may be employed.
  • suitable structural materials such as the Inconels and Incoloy 800, i.e., high chrome-molybdenum steels, should be employed for superheating duty for long exchanger life. It is an advantage of the invention that, by carrying out the advantageous procedure described herein, or utilizing the advantageous structural aspects mentioned, as described, a synthesis gas stream is produced free of particles of sticky material that might adhere to and/or clog flow lines or equipment.
  • the drawing is a schematic representation of the process flow type, and illustrates the efficient integration of the specialized gasifier with equipment for substantially eliminating the particles of sticky material that are produced in a gasifier. All values specified in the description relating thereto hereinafter are calculated, or merely illustrative.
  • dry particulate coal (average particle size about 30 to 50 microns and moisture content of less than about 10 per cent by weight) is fed via a line (1) to burners (2) of a gasifier (3).
  • the gasifier (3) may be a vertical oblong vessel, for example cylindrical in the burner area, with substantially conical or convex upper and lower ends, and is defined by a surrounding membrane wall structure (4) for circulation of cooling fluid.
  • the generally cylindrical reactor wall will comprise a plurality of heat exchange tubes, spaced apart from each other by "membranes" or curved plates, the tubes being connected at their extremities for continuous flow of a heat exchange fluid, such as water, and also having multiple inlets/outlets for the fluid, in a manner well known to the art.
  • a heat exchange fluid such as water
  • oxygen is introduced to the burners (2) via a line (5), the weight ratio of oxygen to moisture and ash free coal being about 0.9, for example.
  • the combustion produces a flame temperature of about 2200 °C, with a gas temperature at the outlet of the gasifier being about 1250 °C to about 1450 °C. Regulation of gasifier and outlet temperature is assisted by coolant in the membrane wall structure (4). Slag is discharged at the outlet (1a).
  • Hot raw synthesis gas with impurities leaves the gasifier (3) through a straight elongated quench line (8) of selected length the interior of which forms a quench chamber in which the raw synthesis gas and the impurities carried thereby are quenched by cooler synthesis gas through line (6) from any suitable point in the process.
  • the quench gas may be from 140 °C to about 540 °C.
  • the quench line (8) may also be jacketed for heat recovery, although this is not illustrated.
  • the quenched gas then passes to a cooler or heat exchanger (7).
  • the heat exchanger (7) is advantageously a multiple section exchanger, the quenched synthesis gas being cooled by fluid in the tubes.
  • the raw synthesis gas now cooled in the low temperature section of the heat exchanger (7) to a temperature of about 315 °C to 140 °C, passes via a line (14) to a cleanup section (15) or solids separator where particulates and various impurity gases, such as H2S, may be removed.
  • the details of the gas cleanup form no part of the invention. Steam requirements for cleanup activities may be supplied from that generated by the overall process.
  • the purified synthesis gas passes from the section (15) in the line (17), and is ready for use. Dry solids impurities are discharged at the outlet (17a).
  • the quench line (8) of Fig. 1 running horizontally from the gasifier (3)
  • the quench line (8) from the gasifier (3) in Fig. 2 is illustrated as extending vertically from the top of the gasifier for a calculated distance.
  • the length of the quench line (8) depends on many factors such as flow rates or volumes in the quench lines and the recycled quench gas supply lines, the temperatures of the raw synthesis gas from the gasifier and that of the quench gas, the nature of the vaporized impurities in the raw synthesis gas to be condensed, the nature of the sticky ash particles in the synthesis gas to be rendered non-sticky, etc.
  • Tests were conducted in a pilot operation in which 200 tons per day of finely-divided coal were burned with an equal weight of oxygen.
  • the gasifier in one test was operated at about 25 bar (10 to 100 bar range) with the product gas being discharged from the gasifier with contaminants at about 1450 °C. After being cleaned and cooled, a portion of the product gas flow stream at about 315 °C was recycled and injected as a quench gas into the upstream end of the quench section which forms substantially the first section of gas discharge line from the gasifier.
  • Equal masses of product gas and quench gas may be used although this ratio may be varied with from 0.5 to 4.0 mass of quench gas being used for each mass of product gas depending on operating conditions.
  • the length of the quench line it is necessary for the length of the quench line to be between 5 and 20 times the inner diameter of the line. It is advantageous that this minimum length of quench line have no bends in it until the particles have passed a point in the line where they are no longer sticky.
  • certain impurities such as the lower oxides of silica and many of the alkali metals are vaporized. The materials are then condensed and cooled in the quench section of the process equipment.
  • a quench section having a straight run of 14 times the section diameter handled a 9 metres per sec flow of hot synthesis gas in a system burning 200 tons of coal per day.
  • Fig. 2 The remaining equipment shown in Fig. 2 are similar to the components of Fig. 1. Fig. 2 is included to show that the quench line (8) may leave the gasifier in a vertical direction and enter the heat exchanger (7) from the top, if desired.

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  • 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)
  • Industrial Gases (AREA)

Claims (3)

  1. Un procédé pour la fabrication d'un gaz de synthèse, comportant les étapes consistant
    a) à oxyder partiellement du charbon à une température élevée en introduisant dans une zone de gazéification du charbon particulaire sec et de l'oxygène, la zone de gazéification comportant au moins un brûleur pour oxyder le charbon, le rapport du charbon a l'oxygène étant déterminé de façon à maintenir une atmosphère réductrice, et à produire un gaz de synthèse brut présentant une température d'environ 1050°C à environ 2200°C, et à éliminer la chaleur dudit gaz de synthèse dans ladite zone de gazéification par échange thermique indirect avec de la vapeur et de l'eau à une température d'environ 100°C à environ 350°C;
    b) à faire passer le gaz de synthèse et les particules collantes qu'il transporte à travers une zone de trempe.
    c) à injecter un gaz de refroidissement pour trempe dans ladite zone de trempe et à mélanger le gaz de refroidissement pour trempe avec le gaz de synthèse chaud sous des conditions d'écoulement turbulent afin de modifier au moins les surfaces externes des particules collantes en un état non-collant.
    d) à transférer le gaz de synthèse brut provenant de l'étape c) dans une zone d'échange thermique et a éliminer la chaleur dudit gaz de synthèse et du matériau particulaire qu'il transporte; et
    e) à éliminer les particules dudit gaz de synthèse brut pour obtenir un gaz de synthèse pratiquement exempt de particules, une partie du gaz étant susceptible d'être recyclée vers et d'être injectée dans la zone de trempe;
    caractérisé en ce que le gaz de synthèse brut quittant la zone de gazéification renferme de faibles quantités de matière minérale vaporisée et dans lequel ladite matière minérale vaporisée est condensée par l'injection d'un gaz de trempe dans la zone d'extrémité amont de ladite zone de trempe, la zone de trempe étant constituée d'un conduit de trempe allongé et rectiligne, montée au niveau de la zone d'extrémité amont du conduit d'évacuation des gaz à partir de ladite zone de gazéification et en communication d'écoulement avec celle-ci, dans lequel la longueur de la section droite du conduit en aval du point d'injection du gaz de trempe est de 5 à 20 fois le diamètre du conduit, et dans lequel la masse du gaz de trempe injecté dans le courant de gaz de synthèse brut est de 0,5 à 4 fois la masse du gaz de synthèse;
    et dans lequel les particules non-collantes conjointement avec la matière minérale vaporisée et condensée, passent avec le gaz de synthèse à travers la zone d'échange thermique en aval de l'étape d).
  2. Le procédé tel que revendiqué dans la revendication 1, caractérisé en ce que le gaz de trempe est un produit gazeux à basse température, exempt d'eau et de particules, qui est fabriqué par le présent procédé.
  3. Le procédé tel que revendiqué dans les revendications 1 ou 2, caractérisé en ce que le courant de gaz de trempe est injecté dans le courant de gaz de synthèse brut en une pluralité d'endroits autour de sa périphérie de façon à former, au niveau de cette zone d'injection de gaz, une gaine de gaz de trempe très froid autour du courant chaud de gaz de synthèse et des particules collantes transportées par celui-ci.
EP19890201730 1988-06-30 1989-06-28 Méthode pour altérer les contaminants dans un flux de gaz de synthèse brut à haute température et à haute pression Expired - Lifetime EP0349090B1 (fr)

Applications Claiming Priority (2)

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US21341888A 1988-06-30 1988-06-30
US213418 1988-06-30

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EP0349090A1 EP0349090A1 (fr) 1990-01-03
EP0349090B1 true EP0349090B1 (fr) 1993-03-31

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EP (1) EP0349090B1 (fr)
JP (1) JP2668266B2 (fr)
DE (1) DE68905681T2 (fr)
DK (1) DK315289A (fr)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE4310447A1 (de) * 1993-03-31 1994-10-06 Krupp Koppers Gmbh Verfahren zur Kühlung von durch Vergasung gewonnenem Rohgas
DE102007046260A1 (de) 2007-09-26 2009-04-09 Uhde Gmbh Verfahren zur Reinigung des Rohgases aus einer Feststoffvergasung
US20120255301A1 (en) * 2011-04-06 2012-10-11 Bell Peter S System for generating power from a syngas fermentation process
CN103666580B (zh) * 2013-11-29 2015-07-22 武汉凯迪工程技术研究总院有限公司 一种耦合式生物质加压热解工艺及系统

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* Cited by examiner, † Cited by third party
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GB2053262B (en) * 1979-07-13 1983-08-24 Texaco Development Corp Process and apparatus for producing gaseous mixtures including h2 and co
DE2942804A1 (de) * 1979-10-23 1981-05-07 Janich, geb.Fischer, Elsbeth, 4720 Beckum Vorrichtung und verfahren zur gaserzeugung
DE3808729A1 (de) * 1988-03-16 1989-10-05 Krupp Koppers Gmbh Verfahren und vorrichtung zur abkuehlung des aus einem vergasungsreaktor austretenden heissen produktgases
DE3809313A1 (de) * 1988-03-19 1989-10-05 Krupp Koppers Gmbh Verfahren und vorrichtung zum kuehlen von partialoxidationsgas

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Publication number Publication date
JP2668266B2 (ja) 1997-10-27
DE68905681D1 (de) 1993-05-06
DE68905681T2 (de) 1993-07-08
DK315289D0 (da) 1989-06-26
JPH0247193A (ja) 1990-02-16
EP0349090A1 (fr) 1990-01-03
DK315289A (da) 1989-12-31

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