DE2853011A1 - PRODUCTION OF HYDROGEN CARBONS - Google Patents

Description

OCCIDEMTM. PETROLEUM CORPORATION, 10889 Wilshire Boulevard,

Los Angeles, California 9-24, U.S.A.

Production of hydrogenated hydrocarbons

The invention relates to a - method for continuous Production of hydrogenated hydrocarbons from a carbonaceous feedstock by pyrolysis of the carbonaceous feedstock Materials.

In the pyrolysis of solid, carbonaceous substances, such as Coal or oil shale, mostly hydrocarbons are formed of little economic value due to their high carbon: hydrogen ratio. They tend because of the high Content of unsaturated alkenes and alkynes for self-polymerization. Consequently, attempts are made to improve the economic viability of such pyrolysis processes by the inferior hydrocarbons in a hydrogenation reactor

Buaaoni / Biemen Office:
Posuadi / RO. Box 10 7127

Feldstafe 24 "D-28ÖB Bremen 1
• Telephone: Ρ421 | “7 4044

Telegr. / Cafetes: diagram Bremen
Tl 244 "S ³ SS btd

098 2 4/0831

Accounts Bremen: Bremer Bank, Bremen (BLZ 290 80010) 100 1449 Deutsche Bank. Bremen (BLZ 290 700 50) 1112002 l'SchA Hamburg (BLZ 20010020) 1260 83-202

Office! Munich / Munich Office:

P.O. Box / R O. Box 14 01 08

SchtoiÜaaucisJiaße 3

D ^ OOO Munich 5

Telephone: (089) 6523 21

Telegr. / Cables: Telepalent Munich

Telex: 523937 jus d (code: forbo)

BDEHMEKE & BQEKMSRT

hydrogenated with hydrogen after leaving the product stream the pyrolysis reaction zone. If catalytic When hydrogenation is used, pesticides such as the carbonaceous remains of pyrolysis and any ash contaminants become of very small grain size generally from the liquid ones Products separated in a solids separation step.

From US-PS 38 55 O7o a hydropyroLysis process is known, in which highly heated coal and hydrogen in a liquid reactor in which the coal is pyrolyzed to coke and hydrocarbons, while the hydrocarbons are hydrogenated at the same time. The temperature of the liquid bed is practically by circulating small Solid particles, e.g., coke, between an area above the liquid bed and a device for heating or cooling the fine particles, kept constant, depending on whether the hydropyrolysis reaction is exothermic or endothermic. The hydrogen required for the process can come from the gaseous products of hydropyrolysis or by gasifying coke produced by hydrolysis with a gasifying agent including oxygen will.

The production of the necessary hydrogen gas by a Hydrogen generator is expensive and the investment and operating costs for another hydrogenation reactor are very high. Furthermore, in this case, the inferior hydrocarbons sometimes not hydrogenated before being cooled down and condensed by a product collection process are, then these hydrocarbons must be in a very expensive and heat-wasting reheating step be heated again. Such a hydrogenation is thermally inefficient. The economy of a process continues to depend on solids separation steps, the very depend on the "quality" of the fluids; the separation

909824/0 8

BOEHMERT & BOEHM2RT

becomes lighter and the economy improves as the "quality" of the liquids increases.

The object of the invention is thus to create a process for the hydropyrolysis of solid, carbonaceous substances for the production of hydrogenated hydrocarbons, especially those of the valuable "middle fraction", whereby the use of an external hydrogen source should be avoided in order to avoid unnecessary separation steps, especially liquid / fixed ₇ to bypass.

According to the invention, this object is achieved by providing a method such that there is oxidation in the presence of an oxygen source for the production of hot, carbonaceous residual material and a combustion gas, wherein at least a portion of the particulate, carbonaceous residue originates from the pyrolysis of the carbonaceous feed material; Reacting at least a portion of the particulate carbonaceous residue with water vapor in the practical absence of unpyrolysed carbonaceous material to form hydrogen; simultaneous pyrolysis and hydrogenation of the pyrolysis products of the carbonaceous material by bringing together gaseous hydrogen, formed from the particulate carbonaceous residue, the carbonaceous feed material and a particulate heat source containing at least a portion of the hot, carbonaceous residue, in a flash pyrolysis Reaction zone with temperatures between 315 to 395 ° C (600 to 2000 ° F), a pressure of up to about 6.89 χ 10 ⁷ N / m ² (10,000 psig) and a solids residence time less than 5 seconds to produce a pyrolysis product stream which particulate, carbonaceous pyrolysis residues, the particulate heat source and a gas mixture consisting of volatilized hydrocarbons, including the middle fraction and unused hydrogen gas, * condensable hydrocarbons, which contains the middle fraction of the

909824/0 831

BOEHMERT & BOEHMERT

Contain gas mixture, has.

The oxidation and the generation of hydrogen gas from the carbonaceous residue can take place in separate oxidation and conversion zones be performed. In this case, at least a portion of the particulate carbonaceous residue undergoes pyrolysis introduced into an oxidation zone to produce hot, particulate, To bring forth carbonaceous residues and a combustion gas, these products are passed through a separation zone in which the hot, particulate, carbonaceous residue is separated from the combustion gas, sent at least part of the separated hot, particulate carbonaceous residue is passed on to a conversion zone, in which it is used Formation of hydrogen gas is used.

Alternatively, these reactions can be carried out simultaneously in a combined oxidation-conversion zone Be: In this case, at least a portion of the particulate, carbonaceous residue is pyrolysed with an oxygen source and water vapor in an oxidation conversion zone in the absence of non-pyrolyzed carbonaceous material brought together to hot, particulate, carbonaceous residue and combustion gas through at least partially Oxidation of the carbon in the carbonaceous residue and simultaneous production of hydrogen gas by reaction of Allow water vapor with carbon in the carbonaceous residue. This arrangement is preferably practically purer Oxygen used in the oxidation conversion zone.

Steam and / or carbon dioxide can enter the pyrolysis reaction zone be introduced in order to with the hot, particulate, carbonaceous residual material that is located therein, to react to provide additional hydrogen gas for the hydrogenation of the volatilized hydrocarbons that are involved the pyrolysis of the carbonaceous material arise.

909824/08 3 1

i BOEHMER ¹ F & BQEHMERT

-228590H

The & id is barren pyrolysis! Resulting GasmischTingcikannl iiit ferine

ürl Gas.e,: -: die: - _: ^^ ieiTteri
v: w erden. ' Ini-der '^ ^; Hy-drierzane
: flüchitigteri; hydrocarbons · further: duarchö dsas'cWassers ± IAF f- -Tgas: in: '= Gaismischun, g _r <IThe from the EYJ £ oiys-e - iReaktieais: Koene. ; ab zo gBn, jwir _ä d, i hydr.t.

~ L ^The: Eyrolyse-Reaktxonszone works ^b: egg; pure ü emperatur?

: -between; 3:15 > to tQ55 ^O C '(600 - 2000 ° F), .-. Ieiiiem: Dnick 3fon- we-

7 2

liiiger as: χ 6 + 89 10'N / m ( "10,000 psi ^) -n residence time of less than 5 Sekunden.i'iDie '. under Fabrics: ±> ^e: fihden widget accordingly all the while; deüi hydrogenation in the Gas phase. " It is particularly preferred; ; eiii ^r between 315 and 76O ^O C (600 ⁰ F to 14O0 ° F) :. oide.r, - even better, between 480 and 76O ° C (900 to T.4D0 ° F),; a: pressure of about 3, VxIO ⁶ N / m ² to 2.41 χ 10 ⁷ H / m ² Γ45Ο: to: 3500-psig) and a vacation time between 0.5 to about 3 seconds to achieve a maximum To achieve yield of liquid hydrocarbons in the process according to the invention.

The method according to the invention shows "many advantages compared to known of this type. As hydrogen for the: hydrogenation steps is obtained directly from "the circulated particulate, carbonaceous residue, one needs no separate hydrogen source. In addition, none fall Investment and operating costs with separate pyrolysis "and Hydrogenation reactors are connected to. Due to the immediate hydrogenation of the carbonaceous during the pyrolysis The hydrocarbons produced by the material run cheap Kinetics. Fundamentally new and inventive is the use of the same solid residue from pyrolysis for Production of hydrogen as well as a partial heat source in the pyrolysis reaction zone.

The inventive method can be used for the recovery of Hydrocarbons from a variety of carbonaceous

909824/0831

BOEHMERT & BOEHMERT

Materials ,, ζ-B- Gllsonlt, tar sand / oil shale ,, the organic Share of iron solid MSH, coal, etc. and also from mixtures from the same, can be applied. All different Types of coal and coal-like materials, such as Luster charcoal, Bituminous coal, sub-bituminous coal, lignite and peat can be used in the process of the invention.

Further features and advantages of the invention emerge from the claims and from the following description, In which the exemplary embodiments are explained in detail with reference to the drawing. It shows:

Fig. 1 shows the schematic representation of an inventive Procedure;

Fig. ' 2 shows the schematic representation of a further according to the invention Procedure;

Fig. 3

up to 6 views, partially longitudinal sections of pyrolysis reactors for use in the invention proper procedures; and

7 is a flow diagram of a laboratory-scale arrangement; to clarify details of the method according to the invention.

Fig. 1 shows a preferred embodiment of the method according to the invention, in which a stream 10, the artificial coal from the pyrolysis of a solid carbonaceous material, such as coal, with a source of oxygen, such as air, in an oxidation zone 12 to produce hot char and combustion gases. The combustion gases contain oxidation products of coal such as carbon monoxide, carbon dioxide and sulfur dioxide and can also be inert Contain components of the oxygen source, e.g. nitrogen if air is used as the oxygen supplier. In the oxidation zone at least part of the charcoal is oxidized. Oxidation of the particulate char is one exothermic reaction and provides at least partially the for

- 6 909824/0831

BOEHMERT & BOEHMSRT

required pyrolysis of the carbonaceous material, e.g. coal Warmth.

The hot, crushed char in the oxidation zone 12 is separated from the combustion gases by a separation stage 13, e.g. one or more cyclones connected in series. In a preferred embodiment, an oxidation-separation cyclone is used as the oxidation zone, see above that the charcoal is both heated and separated from the gaseous products of combustion in a single device can be, with substantial savings in capital and operating costs.

The separated, heated charcoal particles 32 flow in a conversion zone 14, in which it is used with water vapor Reaction are brought about, according to the following reaction steps:

C + H 0 } CO + H. (1)

CO + H 0 '■ > CO + H (2)

The extent of coal gasification to hydrogen and carbon monoxide is determined by the amount of water vapor added in the conversion zone, also by the temperature there and pressure. If more water vapor is added, more hydrogen is formed.

The charcoal is preferably gasified in zone 14 to produce hydrogen and carbon monoxide in a virtually complete absence from unpyrolysed carbonaceous material. If there is a significant amount of unpyrolysed carbonaceous Material would be present, the amount of liquid hydrocarbons would be reduced: hydrogen would by reaction of the Vapor with volatile components of the carbonaceous material used, condensable, volatile carbon

- 7 -

909824/083

BOEHMERT & BOEHMERT

Hydrogen, which is normally produced by pyrolysis of the carbonaceous material used, would be released by the Reaction with steam consumed even before the feed reaches the pyrolysis reactor. That way you can there will be a significant decrease in the yield of liquid hydrocarbons.

The gas produced in the conversion zone 14 contains hydrogen, Carbon monoxide, water vapor and some carbon dioxide. This synthetic gas mixture is known under the common name "Syngas" known.

The temperature of the stream 5, which consists of the synthetic gas and hot, crushed charcoal exiting the conversion zone 14, is determined by changing process parameters such as the temperature of the crushed coal from the oxidation zone 12 and the temperature of the water vapor, that is let into the charcoal turnover zone. The temperature of the emerging from the char converter current 15 is controlled to obtain the desired for the pyrolysis of the coal temperature: It is common for a Auslaßtemperatür 55-278 ° C (100 ⁰ F to 500 ⁰ F) higher than the pyrolysis temperature to use.

A carbonaceous material, in this case coal, the inflow 16, syngas from the conversion zone 14 and a heat source are brought together in a coal pyrolysis reaction zone 18. At least some of the heat is obtained by the particulate charcoal from the conversion zone. Before the char reaches the pyrolysis reaction zone 18, can they are used for charging the pyrolysis reaction chamber by methods such as grinding to the surface-to-volume ratio to increase effective pyrolysis, by separating magnetic particles, by at least partial pre-drying the coal to reduce the heat absorption in the pyrolysis reactor to evaporate the water from this coal

- 8 909824/0831

BOEHMERT & BOEHMSRT

to be ridden.

Carrier gas, which can only lead to "harmless" reactions with respect to the pyrolysis products, can preferably be used to transfer the coal into the pyrolysis reaction zone. A gas flow that is in principle free of oxygen is referred to as "unsehädlicli — reactive" transport gas. ■ Gases such as nitrogen or water vapor, preferably «gases that arise during the pyrolysis of coal, can be used as carrier gases. Another preferred form of the process uses a hydrogen-enriched transport gas in which the hydrogen is preferably part of the hydrogen produced in the charcoal converter.

© as transport gas can be used for both coal and synthetic coal be the gas resulting from the pyrolysis of coal, either before or after condensable hydrocarbons removed and "compounds such as hydrogen sulfide from the Have been gas scrubbed. To a maximum degree of utilization To achieve the heat source, the transport gas should be used Heat source have a temperature approximately equal to that of the heat source. ·

A high solids content in the pyrolysis feed stream becomes a problem desirable in order to reduce the size and cost of the inventive To keep the device as small as possible. A preferred embodiment of such a pyrolysis reaction zone is described in US Pat. No. 3,736,233. There contains the pyrolysis feed stream enough transport gas so that the Besclhickungs stream has a low solids content between 0.1 to 10% by volume, calculated for the total volume of the stream, has to create turbulence for rapid heating of the coal and cause the carbon particles to dilute and prevent them from agglomeration, particularly when Coals with agglomeration tendencies are implemented.

24/0831

BOEHMERT & BOEHMERT

In the pyrolysis reaction zone 18, the coal is pyrolyzed to give "char" and "volatile hydrocarbons". The "artificial charcoal" is a combustible charcoal residual mass, which after the evaporation of volatile constituents from Coal is created. The "volatilized hydrocarbons" are the hydrocarbon-containing gases that are released during pyrolysis can be obtained from coal. Generally, these gases consist of condensable hydrocarbons that are produced by conventional Recycled condensation processes and non-condensable gases such as methane and other hydrocarbons gases that cannot be recovered by ordinary condensation devices. A high proportion of these Volatilized hydrocarbons consist of heavy, highly viscous tars with a high carbon-to-hydrogen ratio. In addition, these volatilized hydrocarbons can be contaminated with organic sulfur compounds be. Om increase the value of volatilized hydrocarbons and organic sulfur compounds, too To convert hydrogen sulfide, which is easily separated from the hydrocarbons can be removed by washing, the volatilized hydrocarbons in the pyrolysis react. tion zone 18 with the hydrogen gas in the conversion zone the char was produced, hydrogenated, hydrogenation in the gas phase in the pyrolysis reaction zone 18 also serves to reduce the viscosity and lower the average boiling point of the volatilized hydrocarbons, also a more successful separation of the solid impurities from the condensable volatilized Hydrocarbons is possible.

The process according to the invention can be carried out with any coal pyrolysis reactor, such as fluidized bed reactors, as described in the publication "Multi-Stage Fluidized-Bed Pyrolysis of Coal at the Project COED Pilot Plant "by Scott et al, American Institute of Chemical Engineers at Pittsburg, Pa., June 1974, or by fast fluidized bed reactors, as in US-PS 38 55 O7O loading

- 10 -

909824/0831

BOEHMERT & BOEHM £ RT

written, be applied. To maximize the yield However, a particularly preferred process medium for liquids is a flash pyrolysis reactor, as described in US Pat. No. 3,736,233.

The solids residence time in the pyrolysis reaction zone varies from 0.01 to 3600 seconds, depending on the reactor type is used. For a high yield of condensable volatilized hydrocarbons, use a flash pyrolysis reactor particularly favorable. The solids residence time in a flash pyrolysis reactor is advantageous less than 5 seconds, better between 0.1 to 3 seconds.

As used herein, the term "solids residence time" relates refer to the mean residence time of the carbonaceous Material stream, the heat source and the solid products of the Pyrolysis of the carbonaceous material in a reactor.

A favorable charcoal-to-charcoal weight ratio moves between 2: 1 to about 20: 1. This high ratio from charcoal to charcoal helps keep the agglomeration-prone charcoal particles from sticking together, if an agglomerable coal or other agglomeration-prone material is used as the carbon-containing substance will. The charcoal temperature corresponds to the requirements of the pyrolysis zone, those of the coal and carrier gas temperature and also of the weight ratios of coal and synthetic charcoal and carrier gas depends. For the charcoal: charcoal ratios given above, the temperature of the charcoal is between 55 to 278 higher than that of the pyrolysis zone.

The temperature of the pyrolysis reaction zone 18 depends on such Process parameters such as temperature of the carrier gas, temperature of the syngas, temperature of the hot, crushed charcoal and the weight ratio of coal, carrier gas and synthetic

909 824/0831

BOEHMERT & BOEHMiPT

coal from; the temperature in the reaction zone is preferably between 315 and 1095 ° C (600 ° F to 2000 ° F). It has been found that the product composition and the overall yield of product are highly dependent on temperature depend in the reaction zone and the solids residence time. With a higher temperature in the reaction zone 18 and longer Solid residence time, the volatilized hydrocarbons contain increasing amounts of non-condensable hydrocarbons.

It is advisable to control the solids residence time in the pyrolysis reactor and the temperature of the coal in the pyrolysis reactor so that the yield of liquid hydrocarbons from the pyrolysis reactor is at least 60%, determined according to Fischer. A maximum pyrolysis zone temperature of approximately 650 ° C (1200 ° F) is required for a dwell time of 5 seconds. In solid-residence times of 4, 3, 2 and 0.3 seconds arise as a maximum allowable temperature in the pyrolysis reactor about 76o ° C (1400 ° F), 815 ° C (1500 ⁰ F), about 900 ° C (about 1600 ° F), about 95O ° C (1700 ° F) and about 1000 ° C (about 1800 ⁰ F). As the solids residence time in the pyrolysis reaction zone 18 decreases, the minimum temperature for degassing the carbonaceous feed material increases to a Fischer yield of 60%. The minimum temperatures of the Pyrolysereaktionszone are about for solids residence times of 5, 4, 3, 2, 1 and 0.3 seconds 300 ⁰ C (600 ° F), about 37o ° C (about 700 ° F), about 400 ° C (about 750 ⁰ F), about 500 ° C (about 900 ⁰ F), about 54O ° C (about 1000 ⁰ F) and about 600 ° C (about 1100 ⁰ F) to a yield of at least 60% by Fischer obtain.

The crushed coal is (F ⁰ 900) heated to a temperature of about 48O ° C to about 76o ° C (1400 ° F), wherein the optimum temperature at about 58o ° C (1O75 ° F)

- 12 -

909824/0631

BOEHMERT & BOEHMEFT

is, iamhohe yields of volatilized hydrocarbons with a high percentage of valuable medium "fractions to obtain if a flash pyrolysis reactor is wetted, the wom a solids residence time is less than 5 seconds. midfractions are hydrocarbons having average boiling points, ie the highest Boiling point is around 520 ° C (95O ° F).

Those hydrocarbons "are used for the production of gasoline, Diesel oil, heating oil and the like are required.

The maximum temperature of the pyrolysis reaction zone 18 is limited by the temperature at which the inorganic part the heat source or the coal due to mold processes or slagging begins to soften. Since the heat source existing on the particle is in front of the entry rank in the pyrolysis reaction zone 18 usually at a higher temperature when the pyrolysis reactor is located, the limiting factor is usually its softening temperature, it is found that a pyrolysis temperature of about 1095 ° C

O- "

((2OO0 Fl about the maximum, is that without slag formation can be reached. ". .-"

The pyrolysis reaction zone 18 is under Überdoack to -zn

~ 1 2

6, S9 χ IO Newton ^ per m (1O 000 psig) "driven" ¹ . An addition

of the pressure increases the hydrogen partial pressure in the Pyrolysis reaction zone and thus the degree of hydrogenation, as well as the investment and operating costs of the process. A usual pressure range for the pyrolysis reaction zone 18 in the economic range of the process is between

6 2 7

3 χ 10 Mewtons per m (450 psig) to about 2.41 x IO

2
Mewtons per m (35OO psig).

Beworzaagterweise the conversion zone 14 is at least operated at the same high pressure as the coal pyrolysis zone 1® » so that no high capacity compressors zjib transfer

- 13 -

90 98 2 4/0831

BOEHMERT & BOEHiV-ERT

of the stream 15 from the coal converter to the pyrolysis reaction zone are required.

Be preferably between O _r O1248 to 2.5 m (O, 1 to 20 standard cubic feet per pound) brought carbon dioxide in the Pyro-Iysereaktionszone 18 per kilogram of charcoal. It has been found that

the presence of the carbon dioxide in the pyrolysis reaction zone increases the yield of condensable hydrocarbons. This ratio of carbon dioxide to charcoal is obtained when the transport gas is introduced into the pyrolysis reaction zone is, contains between 10 to 90 vol .-% carbon dioxide, the charcoal to coal weight ratios between 2: 1 to 20: 1 and the feed stream has a solids content of 0.1 to 10% by volume, based on the total volume of the feed stream. Particularly preferred the remainder of the feed stream is liquid or evaporated water, i.e. the transport gas contains between 10 to about 90% by volume of carbon dioxide and between 90 to 10% by volume of water vapor.

Four examples of pyrolysis reactors which are suitable for contact between hot, crushed charcoal and coal in the invention Process suitable are shown in Figs. The illustrated reactors are detailed in the U.S. Patent 15 04 409.

In such reactors, the char and coal flows and the hydrogen gas under turbulent flow to the better heat transfer from the hot, crushed charcoal particles to the coal stream and more efficient pyrolysis and hydrogenation reaction mixed. These devices are particularly useful for coals with agglomeration properties, since turbulent flow leads to rapid heating of the coal and rapid passage through the "sticky" phases leads to the build-up of carbon particles on the reactor walls

- 14 -

909824/0831

BOEHMERT & BOEHMERT

to prevent.

In Fig. 3 is a device with generally perpendicular Inlet 1311 shown terminating in an end piece 1324 which partially in an annular liquefaction chamber 1308 is narrowed to form a nozzle 1313 which is along the axis of the vertically oriented, descending pyrolysis flow reactor 1380 is directed.

In operation of this device there is a stream of coal feed given through inlet 1311 in a carrier gas and emerges from the nozzle 1313 as a liquid jet which enters the vertically directed mixing part 1312 of the reactor 1380 entry. The upper end 1314 of the reactor 1380 is larger in diameter than the nozzle 1313 and extends into the annular liquefaction chamber 1308, wherein a annular opening 1316 between nozzle 1313 and the wall of the reactor end 1314 is formed.

The reactor 1380 has an elbow 1317 in the middle that rests on a bracket 1318 and its low End 1319 in a reactor product stream cyclone 1321 for separation the gaseous pyrolysis products from the solid pyrolysis products ends.

An annular member 1312 with inwardly extending flanges 1365 is attached to the first inlet 1311 and to the reactor 1380, with the end piece 1324 of the inlet 1311 directly above the constriction which the nozzle 1313 forms and with the upper end 1314 of the reactor 1380, is connected, the part 1323 thus forms the annular liquefaction chamber 1308 with the nozzle 1313 and part of the upper end 1314 of the reactor.

A second annular inlet 1326 is connected generally horizontally to the annular liquefaction chamber 1308 to

- 15 -

824/0831

BOEHMERT & BOEHMEFT

to deliver a liquefied charcoal stream into the chamber. The second inlet 1326 is preferably positioned tangentially with respect to the annular chamber wall, around the incoming Imposing electricity vortices. Artificial charcoal is preferably fed into the liquefaction chamber via the second annular inlet 1308 below the uppermost end 1340 of the reactor chamber 1380 introduced so that the incoming charcoal in the liquefaction chamber 1308 and retained by the weir formed by the upper end 1314 of the reactor and forms a solid barrier. The char is kept in a liquefied state in the chamber 1308 by a liquefying or aerating gas is supplied through inlet 1326 which is "harmless" reactive in terms of Must be on the pyrolysis products. The charcoal from chamber 1308 reaches the upper end of the overflow weir that comes from the top end 1314 is formed by the opening 1316 between weir and nozzle in the mixing chamber 1312 of the reactor. The success of this defense-like arrangement is that a steady flow of liquefied charcoal enters the mixing chamber 1312 enforced; the one behind the top 1314 of the reactor stored mass of charcoal acts as a damping for minor fluctuations in charcoal flow.

The syngas can be introduced into the reactor with the charcoal. Alternatively, it can be separated in a separation zone, like a separating cyclone, from which the charcoal is separated after the conversion zone and as a separate stream be introduced into the pyrolysis reactor or as at least a portion of the stream of carrier gas for the coal.

A preferred embodiment of the invention provides that the syngas by direct injection of the water vapor into the annular Chamber 1308 is formed. In the chamber 1308, water vapor reacts accordingly with the synthetic charcoal present reactions 1 and 2, the ring-shaped chamber acts as a conversion zone. The advantages of this version of the process

909824/083 1

BOEHMERT & BOEHMEFT

rens are that investment and operating costs, which are derive from a separate charcoal converter, do not appear. Direct injection of water vapor into the ring-shaped Chamber 13OS for using the annular chamber as a Charcoal conversion chamber can also be used in the reactor variants 4 and 5 described below, but not with that described in FIG. 6, in the coal introduced instead of charcoal in the annular chamber 1308 will be used. .

In the mixing chamber 1312 of the pyrolysis reactor of FIG. 3 occurs the carbonaceous material contained in the carrier gas from the nozzle 1313 as a liquid jet 1394, which is in the direction on the reactor wämde by about 20 or less, as shown by the broken lines 1395 indicating the periphery of the liquid jet. As soon the "particulate heat source" has arrived in the mixing chamber is, it follows the path of the liquid jet 1394 and is carried away by it, a turbulent one follows Mixing the particulate heat source, the coal feed, and the carrier gas. The beam has a free core 1396, as indicated by the V-shaped dotted line 1397 in FIG which extends significantly into the reactor. In area 1308, between the reactor walls and the liquid jet 1394, there is un-entrained particulate heat source material. The particulate heat source along the periphery 1395 of the liquid jet preferably heats the carbonaceous material if coal is also used Agglomeration properties are used because of the "agglomerate" state before the coal touches the reactor walls. This mixing of the particulate heat source with the solid carbonaceous material in the mixing zone 1312 causes heat transfer from the particulate solid heat source to the coal, which is pyrolysis in the mainly vertically oriented Pyrol ^ sezone 13O7 of the pyrolysis reactor for Consequence.

- 17 -

9824/0831

BOEHMERT & ΒΟΕΗΜΕΚΓ

FIG. 4 shows a reactor similar to FIG. 3, which however has a different second inlet. Here is an inlet 1328 with a horizontal part 1329 with. equipped with a riveting device 1331, which is approved by the approved Transport gas stream 13Q9, which is preferred to the pyrolysis should come from coal, to the inlet 1329 as liquefied— ble gas flow allows. The inlet 132S for the charcoal also has a vertical part 1332, through the charcoal is fed to the edge of the horizontal part 1329 connected is. In this arrangement, charcoal is placed vertically has been introduced through the part 1332, liquefied by the transport gas stream 13-9 before it enters the liquefaction chamber H 3OS enters.

In Fig. 5, a similar to Fig. 3-type device is described, which is through a second inlet 1333 for vertical charging with Kumstkohle, instead of horizontal, in the ¥ eriquidumgskameer 13OS ramd a porous bed or plate 1334 at the bottom of the chamber 13Ο8 above a Feed line from "" Recycling ¹ "or transport gas 13Ο9, which enters through the plate 1334 to the ¥ erlussigumg of the coal through the inlet 1333, differs. The reactor shown in FIG. 6 is similar to that of FIG. 5, except that the coal flow through the first inlet 1336 and the coal flow is generally introduced vertically into the condensing canals via an upright second inlet 1337. This arrangement is only suitable for non-agglomerative coal burners.

The charcoal stream in Fig. 6 is then introduced accordingly, to form a jet that acts on the stream of coal, like represented by the umterbrochemeia lines 1339 in FIG will. The artificial coal can also be added to the first inlet be enteredin, and non-agglomerative charcoal comb through enter the second inlet of Figs.

909824/0831

BOEHMERT & BOEHIV'EFT

An advantage of the arrangements in Figs. 4 to 6 is that that the charcoal is heated very quickly, so that in the case of agglomeration-friendly coals the sticky or The adhesive phase is passed through quickly enough for the To prevent char particles from sticking to the reactor walls and clogging of the reactor.

In the arrangements shown in FIGS. 3 to 6, the speed of the streams of particles, either coal or charcoal, entering through the second inlet below incoming turbulence selected, the particle flow entering through the first inlet is kept in turbulent flow, the speed should be high enough that the resulting mixed flow from the contact of the Both of the supplied streams are in a turbulent flow, resulting in a very good contact between the charcoal and the charcoal particles are created and so the charcoal is heated very quickly by the charcoal particles to increase the yield can be achieved. In the case of agglomeration-friendly coal, the build-up of "sticky" Coal particles on the reactor walls, as discussed above, by rapidly heating the coal in turbulent flow is prevented. Here, turbulent refers to a current that is greater than a Reynolds number 2000 has. The Reynolds number is related to the carrier gas under the process conditions. Laminar flow in the The pyrolysis reactor limits the speed of heat transfer in the pyrolysis zone. Further variable process parameters are e.g. the diameter of the nozzle and the mass flow rate of particulate material and its carrier gas. They are changed until the flow velocity of the particle stream that passes through the first Inlet enters, gets into the area of turbulent mixing.

It is advisable to remove the nozzle 1313 from wear and tear by heat-repellent Lining, e.g. stress-free stainless steel

'83 1

BOEHMERT & BOEHMERT

2853G11

Inconel (trademark) cast steels or others made of wear-resistant Protect material.

The end of the coal flow inlet is advantageously cooled, e.g. with water, especially if the one prone to agglomeration Coals are pyrolyzed because otherwise this inlet can be heated to above the temperature at which such Coals become sticky due to a heat transfer from the particulate heat source at the end of the solids stream inlet.

Although the devices of Figures 3 to 6 show the solids stream inlet terminating in a nozzle 1313, for high inlet velocities To reach the mixing zone, it is not absolutely necessary to have a nozzle at the end of the inlet to be provided. Alternatively, the carbonaceous material and its carrier gas may enter the inlet at such a rate be supplied so that the resulting mixture gets into turbulent flows without the use of a nozzle.

Referring again to Figure 1, the pyrolysis product stream contains 20 exiting the pyrolysis reaction zone 18, char and a mixture of gases consisting of volatilized hydrocarbons and the unreacted components of the syngas consists. The char is separated from the gaseous mixture in a solid / gas separator 22, e.g. highly efficient cyclones, connected in series, separated. At least part of the separated charcoal is recovered introduced into the oxidation zone 12 as charcoal stream 10. The rest of the charcoal corresponds to the pure solid product, that is contained in the pyrolysis of coal and is withdrawn as a charcoal product.

The device according to the invention is started up by the oxidation zone 12 with a supply of charcoal

- 20 -

9098 2A / 0831

BOEHMERT & BOEHMEET

is loaded. after this! the process has started The carbon particles formed can be useful in the process as new, "© nelle the coal part required in the process be used Bmd are komsegiaemterwelse, as described above, reinstated. Kianstkohle is in such a Surplus produced that at least part of the art- coal is available for further processes or uses stands, e.g. as fuel in a «power plant or as raw material for the chemical industry; this improves the economic viability of the process.

The gases 24 sms de «solid / gas separator 22 include volatile hydrocarbons, mn ^ erbramchtem hydrogen and gaseous products ,, as Kohlenraönoxid, carbon dioxide, hydrogen sulfide IMD water, the germs Kohlemwasserstoffe.sind. The more condensed volatilized hydrocarbons can be separated and recovered similarly by conventional methods such as venturi-hunters, indirect heat ataestatijischer, washing mod. , mnkondensierbarein Kohleiuwasserstoffe can be sold as Prodiuik-tgass'troüii: are or as a carrier gas ¹ ZVM moving the coal Zior K'oiilepyrolYsereaktionszone mutzt be sawn. They can also be used as tramsport gas. ¹ ZViX. Movement of the KTmmsfSsshleteilchen in the oxidation zone

As shown in Fig- 1, the ans der Fest / (Gasseparatiomszoae: 22 MeraTHSsferimiiiBiiide gas preferably in a hydrogenation zone 2tS fair gases escort-fe ^ in the volatilized hydrocarbons in the. can be further hydrogenated in the presence of a catalyst the value of the volatile hydrocarbons further increases -

- 21 -

24/0831

BOEHMERT & BOEHMERT

The hydrogenation zone for gas 26 is preferably operated at high temperatures under a high partial pressure of hydrogen, since the degree of hydrogenation of the volatile hydrocarbons increases with the magnitude of these hydrogenation conditions. In order to avoid the need and expense of a high temperature compressor for the transfer of the gas from the solids / gas separation 22 to the gas hydrogenator 26, the pressure in the second hydrogenation zone for gases is preferably kept no greater than that in the coal pyrolysis reaction zone 18, ie , up to about 6.89 10 N / m (10,000 psig), and most commonly between 3.1 10 ⁶ to 2.41 χ 10 ⁷ N / m ² (450 to 3500 psig).

The gas stream 28, which also contains hydrogen, can be passed into the hydrogenation zone for gases in order to increase the concentration and so the partial pressure of the hydrogen in the hydrogenation zone for gases to increase. This improves the degree of hydrogenation of the volatile hydrocarbons. Hydrogen that from the conversion zone for charcoal 14 or a combined one Oxidation conversion zone is related, can also can be conveniently used for this purpose.

A variety of catalysts can be used to facilitate the hydrogenation reaction. Among these are hydro cracking and hydrogenation catalysts such as cobalt, molybdenum, nickel and tungsten containing compositions, the are applied to silica-aluminum or aluminum substrates.

In the pyrolysis reaction zone 18 and in the hydrogenation zone for vapors 26 there is partial thermal cracking of the higher molecular weight components of the coal. This process is desirable because it increases the overall yield of volatile hydrocarbons. At temperatures above 76O ° C (1400 ⁰ F) the cracking process becomes rampant, so that the yield of the valuable middle fraction distillates decreases. The pyrolysis reaction zone 18 and the hydrogenation zone 26 for vapors

- 22 -

909824/083 1

BOEHMERT & BOEHMERT

are therefore favorably operated at temperatures below 760 C (1400 ⁰ F).

Fig. 2 shows a further inventive method that is similar to that of Fig. 1, but differs in two respects:

1. The oxidation and conversion zones are in a single one Level combined and

2. Is hydrogen sulfide in the gas flowing out of the hydrogenation zone 26 by scrubbing, preferably after the gas flow was cooled, removed.

Either or both of these variations can also be used in the method of FIG. 1.

In Fig. 2, the char stream 10 resulting from the pyrolysis of the supplied coal in the coal pyrolysis reaction zone 18, with preferably pure oxygen and steam in the complete absence of non-pyrolysed coal in a single oxidation conversion zone 13 'mixed to to produce hot, particulate charcoal and hydrogen. Economically, this version is particularly advantageous, since hot particulate char and syngas are made in a single step, and so is a reaction vessel and the associated feed and discharge lines can be saved.

In the preferred process shown in Fig. 2, in which practically pure oxygen is used to oxidize the charcoal no diluents that are present in the commonly used oxygen sources, such as e.g. Nitrogen present in the air in the pyrolysis reaction zone 18 and the char converter in any significant quantities supplied. Therefore, with the same

9 0 982-Ιί g8 3 1

BOEHMERT & BOEHlViERT

Total pressure, the partial pressures of the reacting gases in these areas are higher.

As shown in FIG. 2, hydrogen for the hydrogenation zone 26 from the syngas stream 30 coming from the oxidation conversion zone 13 ¹ is fed into a solid / gas separator, such as the cyclone 32 ', which is used to separate any entrained char particles of the gas in stream 30 and recirculation of this to the oxidation conversion zone 13 '. The syngas is then passed through the agitation line 28 into the hydrogenation zone for gases 26 for conversion to increase the yield of hydrogenated volatile hydrocarbons.

If the coal used contains sulfur, at least some of the sulfur is hydrogenated to form hydrogen sulfide in the pyrolysis reaction zone and the hydrogenation zone for gases. This side reaction is desirable because it removes the char and the hydrocarbon products of pyrolysis by reduction the sulfur content, which thereby gain in value as non-polluting super fuels.

As shown in FIG. 2, hydrogen sulfide can be volatilized from the Hydrocarbons by contact with the absorption solution stream 36, in which hydrogen sulfide is soluble, can be freed in a washing stage 38. The absorption solution 36, which is capable of absorbing hydrogen sulfide, typically contains compounds such as amines. A stream 40 of loaded absorbent solution can be degassed to recover the hydrogen sulfide, which then can be transferred to a Claus unit to recover the sulfur.

Example 1 to 8

Tests were carried out with the system shown in FIG

- 24 -

909824/08

BOEHMEET & BOEHMERT

<carried out, ran to demonstrate ^ that the encore of steam and / or carbon dioxide in a flash pyrolysis reaction zone -the yield of iron liquid products is increased »

The plant in Iiabormaßstab contains a Knnst & öhlebesch.ikäkun <gsvorxic: n-tung 104 ,, by the charcoal through a Zufühirung; sleitung 1 04 with the aid of a transport gas, it preferably sticiksifcoff- or carbon dioxide-containing, is conveyed to a preheater 106th Helium is fed to the feed line 104 from a tank 18, as measured by the Roots flow meter 110. Further includes the facility devices for producing and introducing you steam into the preheater "1iQ6, these devices _r containing a water tank 112, from CDEM water to the electric power generator is fed to 116, ·, which previously passes through the IRooter flow meter 116 in order to thy water stream to monitor, 'the steam generated in the generator 116 is fed to the upper end of the preheater 106. The contaminants fed into the preheater 106 are transported by the transport gas from this into a pyrolysis reactor 118, into which coal is fed by a coal loading device 120. Solids and gases from the pyrolysis reactor 118 are passed through the first cyclone 120 and the second cyclone 122 connected in series with the second cyclone 122, and the pesticides separated from both are collected in the respective first and second carbon sumps 124 and 126. The The gases leaving the second cyclone 122 are switched by several gases in series The cooled gases then pass through an electrostatic precipitator (not shown), an activated carbon column 132 and a Drierite drying column 134. The purified and dried gases are then measured by a Rockwell dry gas flow meter 136 and divided into samples .

- 25 -

909824/0831

BOEHMERT & BOEHMERT

Eight test runs were carried out with the arrangement according to the invention, in which heating was carried out in different ways became. In example 1 electric heating was used, example 2 worked with highly heated aluminum a solids ratio of aluminum particles to coal feed of 5: 1. In Examples 3 to 8, heated charcoal was used as a heat source at different solids ratios, as indicated in Table 1 was used. The preheater 106 was at a temperature of 665 - 28 ° C (1225 - 25 F), the feed rate of the pyrolysis reactor 118 was approximately 0.0624 m per kg of carrier gas (1 pound per SCF) in each test run - The type of heating, the solids ratio and the transport gas composition and the liquid yield can be found in Table 1 for each example.

Table 1

Tar yield from flash pyrolysis of subbituminous coal / carrier gas

B3i-
played ¹ Type of heating Solid
relationship Transport
(Vol-%)
N ₂ + He CO - tgas
2 ^H 2 ° Fluid outlet
loot (% according to Fi
shear) 1 electric 0 100 - - 154 2 aluminum 5 100 - - 155 3 Kunstkchle 3.3 100 0 106 4th Kunstkchle 3.3 90 0 10 140 C.
~> Kunstkchle 6.7 78 58 22nd 158 6th Kunstkchle 3.3 0 98 42 151 7th Kunstkchle 3.3 2 88 0 145 8th Kunstkchle 18th 2 10 172

The comparison of the results of Example 3 with those of Experiments 1 and 2 shows _/ that the use of charcoal increases the liquid yield, which in the pyrolysis of subbitu-

BOEHMERT & BOEHMERT

coal is obtained as compared with that of electric Heating or aluminum particles caused heat transfer can be reduced. It is believed that this belittling the yield is achieved through catalysis of the cracking of the volatilized hydrocarbons by the artificial charcoal. By comparing experiments 3, 4 and 5 it can be shown that the addition of increased amounts of water vapor in the Reactor increase the liquid yield to the same extent as obtained in the absence of char can. Furthermore, as shown in Example 7, the yield of liquids compared to that by using inert Transport gas achievable increases when carbon dioxide is used as part of the transport gas in the pyrolysis reactor.

From the results of the experiments described here and other experiments, it could be concluded that when using hot artificial coal as a heat source for coal pyrolysis is the best transport gas to maximize the liquid yield Water vapor alone is second, water vapor and carbon dioxide mixed comes second, followed by carbon dioxide alone; an inert transport gas leads to the lowest liquid yield. The method according to the invention has compared to previously known for the pyrolysis of carbonaceous material such as coal and hydrogenation of the hydrocarbon products the carbonaceous material has many advantages. E.g. direct hydrogenation in the gas phase demonstrates higher Reactivity and higher selectivity, resulting in better hydrogenation and therefore better utilization of the hydrogen possible than when hydrogenation of the collected liquid hydrocarbons is carried out.

Compared to processes in which the volatilized hydrocarbons condensed, collected, reheated and then hydrogenated, there are fewer investments and costs Operating costs as the stages for condensation, collecting

- 27 -

90 98 2 4/083 1

BOEHMERT & BOEHMERT

and reheating have been eliminated. Another advantage of the method according to the invention is that if the volatilized hydrocarbons have been condensed, they are a relative due to the hydrogenation that has taken place have low viscosity and are therefore easy to collect and transport. By using the same particulate Heat source in the pyrolysis reaction zone and the syngas source is, since only one charcoal cycle process is required is also achieved a lower use of investment capital and lower operating costs.

Although this method is described on the basis of preferred embodiments has been, there are also other embodiments possible. These include, for example, the use of a single cyclone reactor for the pyrolysis reaction zone and the solids / gas separation zone a, whereby the costs for a separate cyclone for the solid / gas separation are omitted. Alternatively for this purpose, part of the hot particulate charcoal which is obtained in the oxidation zone can be fed directly into the pyrolysis reaction zone are recycled, the coal conversion zone is bypassed and thus not all, but enough hot, particulate charcoal in the charcoal conversion ions ζ one is directed to the production of the required amount of syngas.

- 28 -

909824/08 31

Claims (23)

BOEHMERT & BOEHMERT O 189 Expectations 1 '. A process for the continuous production of hydrogenated hydrocarbons from a carbonaceous feedstock characterized in that it comprises oxidation in the presence of an oxygen source to produce hot carbonaceous residue and a combustion gas, at least a portion of the particulate carbonaceous residue originating from pyrolysis of the carbonaceous batch; Reacting at least a portion of the particulate carbonaceous residue with water vapor in the practical absence of non-pyrolyzed carbonaceous material to form hydrogen; simultaneous pyrolysis and hydrolysis of the pyrolysis products of the carbonaceous material by bringing together gaseous hydrogen - formed from the particulate carbonaceous residue, the carbonaceous charge material and a particulate heat source containing at least a portion of the hot, carbonaceous residue, in a flash pyrolysis reaction zone with temperatures between 315 to 1095 ° C (600 to 2000 ⁰ F), a pressure up to about 6.89 c 10 N / m ² (TO 000 psig) and a solids residence time less than 5 seconds, for the production of a pyrolysis product stream, the particulate carbonaceous pyrolysis residues containing particulate heat source and a gas mixture consisting of volatilized hydrocarbons including the middle fraction and unused hydrogen gas; having condensable hydrocarbons, which contain the middle fraction of the gas mixture. 2. The method according to claim 1, characterized in that the ORIGINAL INSPECTED - 29 - 909824/0831 BOEHMERT & BOEHMERT particulate, carbonaceous residue in an oxidation zone is oxidized, the resulting hot, particulate carbonaceous residue and the combustion gas by a Separation zone are passed in which the hot, particulate, carbonaceous residue is separated from the combustion gas is, wherein at least a portion of the separated hot, particulate, carbonaceous residue is passed to a conversion zone in which it is used for hydrogen gas production is used. 3. The method according to claim 1, characterized in that for the production of hot, particulate, carbonaceous Residual and combustion gases of the particulate, carbonaceous Rest with a source of oxygen and steam in one Oxidation conversion zone in the practical absence of unpyrolysed carbonaceous material is implemented, with at least partial oxidation of the carbon in the carbonaceous The rest with simultaneous production of hydrogen gas through reaction of the water vapor with carbon in the carbonaceous Rest is done. 4. The method of claim 3, wherein the oxygen source should be pure oxygen. 5. The method according to any one of claims 1 to 4, characterized in that that there is a separation of the gas mixture from the carbonaceous remainder of the pyrolysis and hydrogenation of at least a part of the volatilized hydrocarbons of the separated gas mixture in the presence of a catalyst in a Has gas hydrogenation zone. 6. The method of claim 5, wherein the volatilized hydrocarbons at least partially hydrogenated by unreacted hydrogen contained in the gas mixture will. - 30 - 909824/0831 - - - BOEHMEKT & BOEHMERT " 7. Procedure. according to .tospriich 5 or 6, characterized by the fact that a hydrogen pool is introduced into the hydrogenation zone for gases . - - 8. Method - according to iitaspriich 7, characterized * that the Hydrogen gas, the .ans the particulate, carbonaceous Rest formed. wiiirie, introduced into the hydrogenation zone for gases 9- Process according to buckets of claims 5 to 8, characterized in that the carbonaceous feed material contains sulfur, which reacts with hydrogen gas in the pyrolysis reaction zone and forms hydrogen sulfide gas, since hydrogen sulfide gas is the volatilized hydrocarbons that are present in the hydrogenation zone for gases have been hydrogenated, "äknurch 2bsammmenbringen of the hydrocarbons -verflüchtigten end the current hydrogen sulfide contained tionslösnng with a Äbsorp- ^1, is soluble in the hydrogen sulfide removed 1O. Is introduced Method according to one of the preceding claims, characterized .gekennzeichnet _ff that water vapor for reaction with carbonaceous residue for the production of hydrogen gas in AEIE Fyrolysereaktionszone, wa. further fflyttojernamg of the volatile hydrocarbons which were formed from the pyrolysis of the carbonaceous Besdhickiiingsüiaterlals # dnarchznfuhren, ■ ■ Π. Method according to one of the preceding claims, characterized marked »that carbon dioxide in the Pycolysere— Action zone is introduced. 12. Method according to Samspruich 11, thereby. marked that Carbon dioxide in sufficient quantity to react with the carbonaceous Best rand the carbon-containing residues of the! Pyrolysis in the EYrolysereaktiomszone is introduced to the cracking - 31 - 90SS24 / 0831 BOEHMERT & BOETO-IERT to prevent the hydrocarbons. 13. The method according to claim 11 or 12, characterized in that that the carbon dioxide in amounts between 0.0624 to 3
about 1.25 m per kg of coal is (0.1 to 20 SCF per pound). 3
mixed in approximately 1.25 m per kg of the coal-containing residue 14. The method according to any one of claims 11, 12 or 13, characterized characterized in that the pyrolysis zone fed carbon dioxide between 10 to 90 vol .-% of the total in the Is pyrolysis reaction zone introduced gas. 15. The method according to any one of claims 10 to 14, wherein practically only water vapor and carbon dioxide are introduced into the pyrolysis reaction zone as gases. 16. The method according to any one of the preceding claims, characterized in that the pyrolysis reaction zone a Temperature between about 315 ° C to 76O ° C {600 ° F to 1400 ° F). 17. The method according to claim 16, characterized in that the Pyrolysereaktionszone is at a temperature above about 48O ° C (900 ⁰ F). 18. The method according to any one of the preceding claims, characterized characterized in that the solids residence time in the pyrolysis reaction zone is between 0.5 to about 3 seconds amounts to. 19. The method according to any one of the preceding claims, characterized in that the pyrolysis reaction zone has a pressure between approximately 3.1 χ 10 Ν / πΤ to 2.41 χ 10 N / m (450 to 3500 psig). - 32 - 909824/0831 BOEHMERT & BOEHMERT 20. The method according to any one of the preceding claims, characterized in that the charcoal feed material Coal and the carbonaceous remainder has artificial charcoal. 21. The method according to claim 20, characterized in that the charcoal feed comprises a particulate agglomerable char. 22. The method according to any one of the preceding claims, characterized in that a particulate, solid, carbonaceous feed material is subjected to flash pyrolysis by a continuous transport of a carbonaceous feed material in a carrier gas that is practically "harmless" reactive for the pyrolysis products of the solid, carbonaceous feedstock is arranged a vertically to the inlet, descending flow Blitzpyrolysereaktors with a vertically arranged pyrolysis, which (to 2000 ⁰ F 600) and a pressure between 3.1 χ between 315 ° C and 1O95 ° C 10 ⁶ to 2.41 χ 10 ⁷ N / m ² (450 to 3500 psig) operating and having a solids residence time of less than 5 seconds is being transported; feeding the particulate heat source into a vertically arranged, annular chamber surrounding the upper wall of the pyrolysis reactor, the inner, peripheral wall of the chamber forming an overflow weir for a vertically arranged mixing zone of the vertical, descending flow-through flash pyrolysis reactor, the particulate heat source takes place in this chamber in the flow of an aerating gas which is kept practically "harmless" reactive to the pyrolysis products of the particulate, carbonaceous feed material; introducing the particulate, carbonaceous feed material and the carrier gas through the solids inlet into the mixing chamber to achieve turbulent mixing of the particulate heat source and the particulate, carbonaceous feed material and the carrier gas - 33 - 90982A / 08 31 BOEHMERT & BOEHMERT follows; the flow rate of the turbulent mixture from the mixing area down to the pyrolysis zone for pyrolysis of the particulate carbonaceous feed material in the presence of gaseous hydrogen, which is formed from the particulate carbonaceous residue, at the same time the pyrolysis products of the particulate charcoal feed material are hydrogenated to form a pyrolysis product stream the solids, including the particulate heat source and a carbonaceous solid residue pyrolysis of the particulate, carbonaceous feed material and a gas mixture of carrier gas and pyrolysis gases, the unreacted hydrogen and hydrogenated, volatilized hydrocarbons, including the middle fraction, contains, takes place. 23. The method according to claim 22, characterized in that additionally water vapor in the vertical annular chamber is introduced to react with at least a portion of the carbonaceous residue to form hydrogen gas. - 34 - 909824/0