EP0061339B1 - Composition combustible et méthode de sa préparation - Google Patents

Composition combustible et méthode de sa préparation Download PDF

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Publication number
EP0061339B1
EP0061339B1 EP82301473A EP82301473A EP0061339B1 EP 0061339 B1 EP0061339 B1 EP 0061339B1 EP 82301473 A EP82301473 A EP 82301473A EP 82301473 A EP82301473 A EP 82301473A EP 0061339 B1 EP0061339 B1 EP 0061339B1
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EP
European Patent Office
Prior art keywords
coal
char
liquid
particulate
fuel composition
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Expired
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EP82301473A
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German (de)
English (en)
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EP0061339A3 (en
EP0061339A2 (fr
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Edmond Gerald Meyer
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Individual
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Priority to AT82301473T priority Critical patent/ATE20905T1/de
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Publication of EP0061339A3 publication Critical patent/EP0061339A3/en
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
    • C10L1/322—Coal-oil suspensions

Definitions

  • This invention relates to a fuel composition and to a method of manufacturing a fuel composition.
  • the invention may have specific application in making carbonaceous fuel supplies, such as coal, which are located in remote areas available to populous areas. More particularly, this invention relates to transportable fuel compositions, and to methods of making such compositions.
  • coal from whatever source contain various pollutants which heretofore have been difficult or impossible to remove. The nature and amount of these depends upon the geographical area from which the coal is mined. Ash, sulfur, and nitrogen comprise the most objectionable of these pollutants.
  • hydrocarbon containing fuels including synfuels
  • hydrocarbon containing fuels are likewise valuable as feedstock for the manufacture of chemical synthetics including all types of plastics, elastomers, resins, polymers and the like. It would therefore appear advantageous to utilize coal for stationary energy needs while utilizing the liquid crude supply and synfuels for transportation as well as feed-stock purposes.
  • coal slurries which comprise a pulverized, comminuted or ground coal admixed with water, and which may contain various additives to, for example, increase the wetability of the coal.
  • This slurry while capable of being transmitted by pipeline, requires special pipelines and pumping equipment.
  • Aqueous coal slurries have additional drawbacks. First the water which is necessary to slurry the coal is in short supply at the geographic region of the western U.S. coal reserve. Second, water must be removed from the slurry prior to introduction of the fuel into a furnace or boiler.
  • Non-aqueous or hydrocarbon containing liquid can also be used as the transmission medium to form a slurry of pulverized coal. These slurries still have attendant problems. Non-aqueous coal slurries also require special pipelines and pumping equipment. Since coal is still the main fuel constituent in such slurries, furnace and stack modifications are still required to burn coals from different regions. Non-aqueous fractions, unlike aqueous solutions, tend to solubilize constituents as well as impurities in the coal. This renders the slurrying liquid substantially unusable as a feed- stock for many chemical syntheses. Additionally, burning of the slurry mixture results in emission of the pollutants present in the coal.
  • Coke is an expensive product which is produced from metallurgical coal. Methods have been proposed for producing coke slurry by adding coke which has been formed by conventional specialized coke production techniques, to certain hydrocarbon materials. Coke is an agglomerated material which has poor fluidity. It does, therefore, not form a readily transportable slurry which can be effectively conveyed in conventional pipeline systems. Coke, being an agglomerated product, tends to settle out. Coke particles, because of their surface and geometric characteristics, and because of their agglomerated structure, do not roll over each other and do not pack effectively.
  • a fuel composition comprising a liquid-solid admixture characterized in that it includes a portion of a particulate coal char material, derived from coal, dispersed in an amount of a liquid organic material effective to produce a fluidic, combustible, transportable composition, wherein said liquid, organic fraction is at least partially derived from the pyrolytic destructive distillation of coal, or is a lower chain alcohol of from 1 to 4 carbon atoms or a mixture thereof.
  • the invention further extends to a method of producing a fuel composition, which comprises admixing a coal char with an amount of a liquid organic material effective to produce a fluidic transportable, combustible composition.
  • the coal char may be produced by the pyrolytic destructive distillation of a carbonaceous material in the absence of oxygen, and the liquid organic material may be derived entirely or at least partially from the pyrolytic destructive distillation.
  • composition of this invention is formed to create a composition which has fluidic characteristics such that it can be transported by certain existing pipeline facilities.
  • the liquid organic fraction which acts as a continuous phase in the admixture does not contain the impurities of the prior art slurries and thus is capable of being separated from the liquid-solid mixture prior to the ignition of the char.
  • the separated liquid is then available for use as a feedstock for synthesis of chemical compounds.
  • the liquid organic fraction is derived during the pyrolysis of the coal.
  • both the char and the liquid organic fraction are beneficiated.
  • the fuel composition of the instant invention can be produced by subjecting coal to pyrolytic destructive distillation in the absence of oxygen to produce a particulate char which is admixed in suitable proportions with a liquid organic fraction to produce a liquid/ solid fluidic mixture.
  • the combustible liquid-solid mixture is produced by first subjecting coal to pyrolytic destructive thermal distillation in the absence of oxygen to produce a coal char.
  • the char is then pulverized or otherwise ground to produce a particulate matter.
  • the particulate matter is then beneficiated to produce a substantially pollutant-free char material.
  • the lower boiling organic fraction obtained from the pyrolysis of coal is admixed with the particulate beneficiated char in proportions so as to form the fluidic, solid-liquid, combustible fuel mixture.
  • the lower boiling organic fraction used does not contain sulfur or nitrogen pollutants.
  • the beneficiated particulate char is admixed with a lower chain alcohol which is produced by well known synthetic methods utilizing coal and water or natural gas.
  • the ground, beneficiated char is sized to yield a particulate distribution which is bi-modal or tri- modal.
  • a particulate distribution which is bi-modal or tri- modal.
  • the drawing shows a schematic of process steps for producing a coal derived fuel composition of the instant invention wherein raw coal 12 from a coal mine 10 is conveyed continuously to a crusher means 14. Within crusher means 14 the raw coal 12 is fragmented to particles in the range of 1/2" to 1/4" (12 to 6 mm) in diameter to produce a crushed coal product 16.
  • the crushed coal 16 is conveyed continuously to a pyrolytic destructive distillation means 18 which preferably contains a preheating chamber to remove moisture and entrained gases.
  • the pyrolytic destructive distillation means 18 provides for thermal destructive distillation of the coal in the absence of oxygen to produce a char portion 20 and a liquid organic fraction 34.
  • the char portion 20 is continuously conveyed to a grinding means 22.
  • the char is pulverized or otherwise comminuted to produce a ground char product 24 which is inherently spherical in shape.
  • the ground char 24 is conveyed to a beneficiation means 26.
  • the ground char 24 is beneficiated by removal of undesirable constituents and pollutants such as sulfur and ash.
  • the open pore structure of the char facilitates this process.
  • the beneficiaated char 28 is conveyed to a particulate sizing means 30.
  • the particulate is mechanically separated by particle size to produce a sized distribution of particulate char.
  • the sized char mixture 32 is continuously conveyed to a mixing means 42.
  • the liquid organic fraction 34 is conveyed from the pyrolytic destructive distillation means 18 to a separation means 36 where the higher boiling fraction 38 containing the bulk of the nitrogen is separated for example by distillation from the remainder and conveyed to storage for use directly as a chemical reagent and feedstock.
  • the separation means 36 the lower boiling fraction 40 is rendered substantially free of combined and entrained materials which on combustion would produce sulfur oxides, nitrogen oxides, and like pollutants.
  • the lower boiling pollutant free fraction 40 is continuously conveyed to the mixing means 42.
  • the char mixture 32 and the liquid lower boiling fraction 40 are combined in appropriate proportions to produce the easily transportable char containing fuel composition 44 of the instant invention which is passed to storage 46 for distribution by pipeline or tanker vehicle in a manner similar to crude oil.
  • the coal that can be employed in accordance with the instant invention can be generally termed "combustible carbonaceous material". It is any of the combustible, carbon containing materials that will undergo pyrolytic destructive distillation to form char. Such materials comprise carbon containing shales, anthracite coal, bituminous coal, and all of the soft coals, lignites, and the like.
  • coal is mined from a coal mine by either strip or underground methods as appropriate and well known in the art.
  • the raw coal material 12 is preferably subjected to preliminary crushing to reduce the particle size. Particle sizes of from 1/2" (12 mm) to about 1/4" (6 mm) in lateral dimension (diameter) are found useful, with particles of about 3/8" (9 mm) being preferred.
  • the need for size reduction and the size of the reduced material will depend upon the pyrolytic conditions utilized as well as the composition of the coal material.
  • the crushing and/or grinding is preferably accomplished with impact mills such as counterrotating cage mills, hammer mills of the like. This is done to impart an impact type shock to the coal to separate material along natural planes, faulted surfaces, solution channels and the like.
  • the coal is sized by, for example, rough screening and gangue material is removed to assure a more uniform product for pyrolysis.
  • carbonaceous fines and the like are readily utilized and can be separated from the macro coal particles and conveyed directly to the pyrolytic destructive distillation means 18.
  • the macro coal particles are passed continuously through a preheater within pyrolytic destructive distillation means 18 which is operated at 150° to 220°F (65° to 104°C) in order to remove gases and moisture. This is a well known process and is of value in that the BTU content of the resultant coal per unit weight is increased. This preheating also removes certain entrained gases which may have further value as fuel for the pyrolysis step.
  • the pyrolytic destructive distillation means 18 can be any pyrolysis apparatus which is well known in the art. Preferably, the pyrolysis is performed in a continuous process. As the crushed coal 16 is heated in the absence of oxygen, the entrained materials are vaporized and collected. Lower boiling organic fractions including hydrocarbons, cyclics, and aromatics as well as higher boiling organic fractions are emitted from the coal leaving a char material of essentially carbon which is of a porous structure and substantially spherical in shape. Included in the emitted constituents are the nitrogen containing polluting compounds such as pyridine, piperazine and the like.
  • the char 20 is continually conveyed to the grinding means 22.
  • the grinding means 22 reduces the char to a suitable fineness to facilitate beneficiation and subsequent sizing for use in the fuel admixture. Any conventional crushing and grinding means, wet or dry, may be employed. This would include ball grinders, roll grinders, rod mills, pebble mills and the like.
  • the particles are sized within the grinding means 22 and recycled to produce a uniform distribution of particles.
  • the char particles are of sufficient fineness to pass a 10 mesh screen and the majority of the particles are in the 100 to 200 mesh size. The mesh sizes refer to the Tyler Standard Screens.
  • the char 24 is continuously conveyed to the beneficiation means 26.
  • the beneficiation means 26 can be any device known in the art utilized to extract pollutants and other undesirable inorganics such as sulfur and ash from a particulate char material. This can be done for example, by washing, jigging, extraction, flotation, chemical reaction, and/or electro: beam techniques. The exact method employed will depend largely on the coal constituent utilized in forming the char, the sizes of the char particles and the conditions of pyrolysis.
  • the beneficiated char 28 is sized in particulate sizing means 30 which can be any apparatus known in the art for separating particles of a size in the order of 100 micro-metres. Economically, screens or sieves are utilized, however cyclone separators or the like can also be employed. In sizing selections made so as to assure combustion, a second and/or third particle size is chosen to effect so-called "modal" packing.
  • the spheriod shape of the primary particle provides spacing or voids between adjacent particles which can be filled by a distribution of second or third finer particle sizes to provide bi-modal or tri-modal packing. This packing concept allows the compaction of substantially more fuel in a given volume of fuel mixture while still retaining good fluidity.
  • the resultant char mix 32 is conveyed by means of for example an air conduit to the mixing means 42 where it is combined in appropriate proportion with the lower boiling organic fraction 40.
  • the organic fraction 34 entering the separation means 36 is continuously fractionally distilled or otherwise separated to provide the lower boiling pollutant free organic fraction 40.
  • the exact amount of this fraction utilized will depend upon the properties of the combustible char containing admixture which are desired. Normally, fractions having boiling points up to about 200°F (94°C) have been found useful in carrying out the instant invention. Any remaining pollutant fraction could be separated by other means as, for example, steam stripping.
  • the higher boiling fractions 38 of the liquid organic fraction 34 advantageously contain certain sulfur and nitrogen compounds. This fraction is removed and can be based directly as a feedstock for chemical synthesis.
  • the particulate char and the lower boiling pollutant-free organic fraction 40 are admixed in the desired proportions and sent to storage 46.
  • an admixture is formed of char and the liquid constituent.
  • the ratio of char to liquid that can be utilized will depend upon the properties of the fuel desired.
  • the char constituent should comprise not less than about 45% by weight of the composition and preferably from about 45% to about 75% by weight.
  • the mixing means 42 can be any well known mixing apparatus in which an organic constituent and a coal char can be mixed together in specific proportions and pumped continuously to a storage tank such as 46.
  • Certain well known surfactant stabilizers may be added depending on the viscosity and non- settling characteristics desired.
  • Within the storage tank 46 it is generally not required to agitate the fuel admixture of the instant invention unless such storage is to be for an extended period.
  • From the storage tank the fuel of the.- instant invention is preferably continuously conveyed by means of pipelines well known in the art to distant fixed source heat and electric generators.
  • liquid organic fraction 34 derived from the pyrolytic destructive distillation of coal can be utilized directly as a feedstock for chemical synthesis, transportation fuels or the like rather than as the liquid phase of the instant fuel admixture.
  • coal and water are utilized to produce first CO and H 2 and then methanol and other lower alcohols which are utilized as the liquid phase for the combustible fuel admixture of the instant invention.
  • Water released from the coal during preheating can be used as part of the water required in the synthesis, thus further preserving precious resources.
  • alcohol is employed to mean alcohols which contain from 1 to 4 carbon atoms. These include for example, methanol, ethanol, propanol, butanol and the like.
  • the alcohol may range from substantially pure methanol to various mixtures of alcohols as are produced by the catalyzed reaction of synthesis gas or natural gas.
  • the alcohol constituent can be produced on site at the mine in conjunction with the pyrolytic destructive distillation. The process can be fired by coal, thereby negating the necessity to transport fuels long distances.
  • carbon monoxide and hydrogen are initially formed in accordance with equation I: A portion of the gas is subjected to the shift reaction with steam to produce hydrogen for hydrogen enrichment in accordance with equation II: The C0 2 is scrubbed from the gaseous product leaving only hydrogen. The hydrogen is admixed with gaseous products of equation I to produce a "syn gas" having desired ratio of hydrogen to carbon monoxide from which methanol and similar products are synthesized catalytically.
  • the respective constituents such as carbon monoxide and hydrogen are combined to produce methanol.
  • the synthesis of methanol is described in page 370-398 of vol. 13 of the above referenced Kirk-Othmer Encyclopedia.
  • the carbon monoxide and hydrogen are controlled in a ratio and temperature pressure combination to obtain maximum yields of the methanol fuel product.
  • Other methods for methanol synthesis at lower temperatures and pressures are also known, as for example, the ICI low pressure process as described in "Here's how ICI Synthesizes Methanol at Low Pressure" Oil and Gas Journal, vol. 66, pp. 106-9, February 12, 1968.
  • the methanol is used as the liquid phase to slurry the char 32 in mixing means 42.
  • the lower boiling organic fraction and/or the synthesized methanol will not dissolve or otherwise solubilize impurities since the coal has been charred and the char has been beneficiated.
  • the liquid phase of the composition can be readily extracted at the fuel mixture destination for use as a chemical synthesis feedstock.
  • the fuel composition of the instant invention can be mobilized or transported by all conventional means used for crude oil transportation, permitting the efficacious foreign export of coal derived fuels which has not heretofore been readily and easily accomplished.
  • the existing pipelines to docks and tanking facilities can readily be utilized. Oil tankers can empty their crude oil load in this country, and be refilled with the char containing composition of the instant invention which can be exported to other countries, thus improving the balance of payments of this country.
  • the liquid solid admixture upon reaching its ultimate destination, may be employed directly as a fuel for heating; for utilities such as power plants; or for process converters such as in the preparation of synthetic materials. On the other hand it may be separated into its constituents, char and the lower boiling organic fractions and/or methanol.
  • the char portion is employed as fuel, while the organic fraction and/or methanol can be employed as a feedstock or as a transportation fuel such as a gasoline additive or as an extender.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Solid Fuels And Fuel-Associated Substances (AREA)
  • Liquid Carbonaceous Fuels (AREA)

Claims (9)

1. Une composition combustible comprenant un mélange ajouté liquide-solide, caractérisé en ce qu'il inclut une portion de matière particulaire de noir de carbone (char), provenant du charbon, dispersé dans une quantité de matière organique liquide susceptible de produire une composition fluidique, combustible, transportable, et dans laquelle ladite fraction organique liquide est au moins en partie obtenue à partir de la cuisson pyrolytique du charbon, ou est un alcool à chaîne courte de 1 à 4 atomes de carbone, ou un mélange de tout cela.
2. Une composition combustible d'après la demande 1, caractérisée en ce que le noir de carbone est produit par la cuisson pyrolytique du charbon en l'absence d'oxygène.
3. Une composition combustible d'après la demande 2, caractérisée en ce que ladite fraction organique liquide provient au moins en partie de la cuisson pyrolytique dudit charbon.
4. Une composition combustible d'après les demandes 1, 2, 3, caractérisée en ce que la proportion de matière particulaire, par rapport au liquide, n'est pas inférieure à 45% en poids.
5. Une composition combustible d'après n'importe laquelle des demandes 1 à 4, caractérisée en ce que le noir de carbone est enrichi, et en ce que la fraction organique liquide est essentiellement dépourvue de polluants sulfureux et azotés.
6: Une composition combustibles d'après n'importe laquelle des demandes 1 à 5, caractérisée en ce que l'alcool de chaîne courte est un alcool produit par la réaction catalytique de gaz de synthèse ou de gaz naturel.
7. Une composition combustible d'après n'importe laquelle des demandes 1 à 6, caractérisée en ce que la dimension des particules de ladite matière particulaire est de l'ordre de 100 micromètres, et en ce que de telles particules sont essentiellement de forme sphérique.
8. Une méthode de production d'une composition combustible caractérisée en ce qu'elle comprend les étapes de l'adjonction d'un noir de carbone (char) à une quantité de matière organique liquide susceptible de produire une composition fluidique, transportable et combustible, dans laquelle ledit noir de carbone (char) est obtenu par cuisson pyrolytique du charbon, et ladite matière organique liquide provient en grande partie de la cuisson pyrolytique du charbon, ou bien est un alcool à chaîne courte ayant de 1 à 4 atomes de carbone, ou un mélange de tout cela.
9. Une méthode d'après la demande 8, caractérisée en ce qu'elle comprend les étapes qui consistent 1) à soumettre le charbon à la cuisson pyrolytique thermique en l'absence d'oxygène pour produire un noir de carbone (char) particulaire et une fraction organique liquide; 2) à réduire le noir de carbone (char) en une matière particulaire calibrée afin de créer un compactage bimodal ou trimodal; 3) à enrichir la matière particulaire pour produire un noir de carbone (char) particulaire enrichi essentiellement dépourvu de polluant; 4) à séparer la fraction organique liquide et à la transformer en une fraction pyrolytique à point d'ébullition plus élevé contenant des composés sulfureux et azotés, ainsi qu'en une fraction pyrolytique à point d'ébullition moins élevé qui est essentiellement dépourvue de composés sulfureux ou azotés; 5) et à mélanger le noir de carbone (char) particulaire enrichi, ainsi qu'un liquide organique choisi dans le groupe comprenant la fraction pyrolytique à point d'ébullition moins élevé, les alcools à courte chaîne ayant de 1 à 4 atomes de carbone, et les mélanges ayant des proportions telles que le noir de carbone (char) particulaire ne représente pas moins de 45% du poids.
EP82301473A 1981-03-24 1982-03-22 Composition combustible et méthode de sa préparation Expired EP0061339B1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AT82301473T ATE20905T1 (de) 1981-03-24 1982-03-22 Brennstoffzusammensetzung und methode zur herstellung.

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US24738281A 1981-03-24 1981-03-24
US247382 1981-03-24

Publications (3)

Publication Number Publication Date
EP0061339A2 EP0061339A2 (fr) 1982-09-29
EP0061339A3 EP0061339A3 (en) 1983-09-21
EP0061339B1 true EP0061339B1 (fr) 1986-07-23

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EP82301473A Expired EP0061339B1 (fr) 1981-03-24 1982-03-22 Composition combustible et méthode de sa préparation

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EP (1) EP0061339B1 (fr)
AT (1) ATE20905T1 (fr)
AU (1) AU549579B2 (fr)
CA (1) CA1172851A (fr)
DE (1) DE3272077D1 (fr)
WO (1) WO1982003405A1 (fr)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3340971A1 (de) * 1983-11-11 1985-05-23 Johannes Dipl.-Ing. 6200 Wiesbaden Linneborn Verfahren zur herstellung von aus mindestens zwei komponenten bestehenden fluessigen brennbaren medien

Family Cites Families (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB292217A (en) * 1927-03-11 1928-06-11 James Yate Johnson Improvements in the production of stable suspensions or pastes of coal
US4014661A (en) * 1975-03-17 1977-03-29 Texaco Inc. Fuel making process
US4030893A (en) * 1976-05-20 1977-06-21 The Keller Corporation Method of preparing low-sulfur, low-ash fuel
US4192651A (en) * 1977-11-21 1980-03-11 The Keller Corporation Method of producing pulverulent carbonaceous fuel
US4208251A (en) * 1978-06-19 1980-06-17 Rasmussen Ross H Process and apparatus for producing nonaqueous coke slurry and pipeline transport thereof
US4249911A (en) * 1979-02-15 1981-02-10 Hydrocarbon Research, Inc. Combustible fuel composition

Also Published As

Publication number Publication date
DE3272077D1 (en) 1986-08-28
AU549579B2 (en) 1986-01-30
AU8392182A (en) 1982-10-19
EP0061339A3 (en) 1983-09-21
CA1172851A (fr) 1984-08-21
WO1982003405A1 (fr) 1982-10-14
EP0061339A2 (fr) 1982-09-29
ATE20905T1 (de) 1986-08-15

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