EP0316234A1 - Verfahren und Einrichtung für die hydrierende Pyrolyse von schweren Kohlenwasserstoffen durch einen Plasmastrahl, insbesondere ein H2/CH4-Plasma - Google Patents

Verfahren und Einrichtung für die hydrierende Pyrolyse von schweren Kohlenwasserstoffen durch einen Plasmastrahl, insbesondere ein H2/CH4-Plasma Download PDF

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Publication number
EP0316234A1
EP0316234A1 EP88402817A EP88402817A EP0316234A1 EP 0316234 A1 EP0316234 A1 EP 0316234A1 EP 88402817 A EP88402817 A EP 88402817A EP 88402817 A EP88402817 A EP 88402817A EP 0316234 A1 EP0316234 A1 EP 0316234A1
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EP
European Patent Office
Prior art keywords
plasma
hydrocarbons
gas
injection
free radicals
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Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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EP88402817A
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English (en)
French (fr)
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EP0316234B1 (de
Inventor
Jean-Marie Baronnet
Christian Daumas
Renée Derai
François Pingaud
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
AGENCE FRANCAISE POUR LA MAITRISE DE L'ENERGIE
Electricite de France SA
Universite de Limoges
Original Assignee
AGENCE FRANCAISE POUR LA MAITRISE DE L'ENERGIE
Electricite de France SA
Universite de Limoges
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G15/00—Cracking of hydrocarbon oils by electric means, electromagnetic or mechanical vibrations, by particle radiation or with gases superheated in electric arcs
    • C10G15/12—Cracking of hydrocarbon oils by electric means, electromagnetic or mechanical vibrations, by particle radiation or with gases superheated in electric arcs with gases superheated in an electric arc, e.g. plasma

Definitions

  • the present invention relates to a process and an installation for hydropyrolysis of heavy hydrocarbons.
  • hydropyrolysis of hydrocarbons which mainly applies to the cracking of liquid hydrocarbons with a high number of carbons and / or comprising a large proportion of aromatic constituents, consists in carrying out thermal cracking in the presence of hydrogen by diluting the hydrocarbons in a phase hydrogenated gas at moderate pressure (a few bars to a few tens of bars).
  • the hydrogen present in excess during this reaction exerts a blocking effect on undesirable polymerization, condensation and aromatization reactions between two molecules of unsaturated hydrocarbons.
  • the reactions involve essentially play free radicals (mainly H., But also CH., CH2., CH3.), A phenomenon characteristic of the hydropyrolysis relative to thermal cracking without hydrogen, the presence and the kinetics of recombination of these radicals free being essential parameters determining the efficiency and the yield of the hydropyrolysis reaction envisaged.
  • Hydropyrolysis cracking applies particularly well to the transformation of heavy residues comprising a high proportion of non-volatile aromatic components as well as a high proportion of residual materials (Ni, V, S) which make direct hydrogenation by catalysis difficult and expensive, in particular due to the rapid degradation of the catalyst due to the residual materials.
  • cracking by hydropyrolysis provides an almost complete conversion of these heavy residues with a high number of carbons into liquid and gaseous products.
  • FR-A-2 542 004 describes in particular a process and a device, assisted by electricity, for cracking by hydropyrolysis, in which an electric arc is produced between an anode and a distant cathode placed opposite, the hydrocarbons being injected in the form of a vortex flow around the arc column.
  • the aforementioned document proposes to produce a vortex flow of the hydrocarbons injected around the electric arc, in the vicinity of the anode (that is to say in the region of the electric arc richest in free radicals).
  • the injection of hydrocarbons is preferably done there tangentially or obliquely against the flow of the arc jet, or by vortex sheathing the arc and striking the foot of the anode.
  • This flow mode intended to improve the mixing of free radicals with the products to be converted, however limits the exchange zone to the region where the arc plasma is confined by the hydrocarbons injected around the arc column.
  • One of the aims of the present invention is to overcome these difficulties, by proposing a method and an installation providing a large exchange surface between the hydrocarbons and the free radicals, which allows: - ensuring rapid and intimate mixing of the two reactive phases, with the consequence of a very short reaction time, and - to keep a high proportion of free radicals throughout the duration of the cracking reaction and hydrogenation.
  • the process of the present invention proposes carrying out the hydropyrolysis of hydrocarbons by the following steps: - production and ejection of a pressurized jet of plasma generated from a plasma gas, free radical generator H. , - injection, into the plasma jet thus produced, of a gas generating free radicals, in particular H radicals . , CH . , CH2 . and CH3 . , - injection into the resulting gas stream of hydrocarbons to be hydropyrolyzed to react with the gas generating free radicals, - recovery of the hydropyrolysis products thus obtained.
  • the gas generating free radicals is injected radially into the plasma jet.
  • the gas stream is non-vortex at the point of injection of the hydrocarbons, and it is accelerated prior to the injection of the hydrocarbons.
  • the radial injection of the gas generating free radicals does not create any vortex and allows a very fine spraying of the charge ensuring a very superior plasma / hydrocarbon mixture.
  • the invention also relates to a hydropyrolysis installation, comprising: - a plasma torch, to produce and eject a jet of plasma under pressure produced from a plasma gas, - an intermediate stage comprising means for inject a gas generating free radicals, in particular H radicals, into this plasma jet . , CH . , CH2 . and CH3 . , means for injecting, into the resulting downstream gas stream, the hydrocarbons to be hydropyrolyzed, - means for collecting, downstream, the hydropyrolysis products.
  • a convergent-divergent oriented in the axis of the plasma jet, the injection of hydrocarbons being carried out at this convergent-divergent.
  • This convergent-divergent allows to obtain all the advantages mentioned above, ensuring an excellent mixture of the two reactive phases and a cooling of the flow which causes a slowdown of the recombination reactions of free radicals.
  • FIG 1 there is shown schematically a conversion unit implementing the installation of the present invention.
  • This conversion unit includes a plasma torch 100, which is of a conventional type of plasma projection torch. As can be seen in detail in FIG. 2 which shows the lower part of this torch, this comprises a cathode 101 of the hot cathode type in thoriated tungsten, placed in the axis of a nozzle-anode 102 comprising a channel axial 103 at the outlet of which the plasma jet will be projected, at a temperature between 2000 and 3500 K, for example of the order of 3250 K.
  • a cooling jacket 104 makes it possible to limit the temperature of the anode so as to allow the latter to be kept at its optimum operating temperature.
  • This torch 100 is supplied with plasma gas (FIG. 1) by a pipe 110 connected to reserves 120 of hydrogen and argon by means of a series of valves V and sensors of flow rate D, pressure P and temperature T.
  • the plasma torch operates continuously, both with an argon-hydrogen mixture (for example, at around 10% argon) as with pure hydrogen.
  • a direct current generator 130 makes it possible to supply the torch 100 with the desired voltages and intensities, for example in a range going from 300 V / 400 A to 1200 V / 100 A, the output voltage being regulated, for example by semiconductors controlled in phase.
  • the installation then comprises an intermediate stage 200 for injecting the gas generating free radicals.
  • This stage 200 which will be described in more detail below with reference to FIGS. 2 to 5, makes it possible to inject at the outlet of the anode a gas which may be either hydrogen or natural gas (essentially methane ), to enrich by free radicals such as H. or CH . (and possibly CH2 . or CH3 . ) the plasma projected by the torch into this intermediate stage.
  • Hydrogen and methane are brought to the intermediate stage 200 by a line 210 connected to reserves 220 by means of valves V and means for measuring the flow rate D, the pressure P and the temperature T of the gases. injected.
  • stage 300 Downstream of this intermediate stage, there is provided a stage 300 for injecting the charge to be cracked, this injection being carried out at the level of the throttle of a convergent-divergent, also described below with reference to FIGS. 2 to 5, which has the function of accelerating the flow and avoiding making it swirling at the injection point.
  • the charge to be hydropyrolyzed is brought to this stage 300 by a pipe 310 connected to the reservoir 320 containing this charge, in liquid form; the tank 320 is possibly preheated to a temperature slightly lower than the boiling or decomposition temperature of the charge, by a heating tape 321 so that all the constituents of the charge are in liquid form (even those which could solidify at a temperature close to room temperature) and have a viscosity sufficiently reduced to allow their nebulization at the time of injection.
  • the reservoir 320 is pressurized, for example by a gas 322, such as natural gas or methane, to allow the charge to be injected under pressure into the stage 300.
  • a gas 322 such as natural gas or methane
  • the injection of the charge at the location of the throttle of the convergent-divergent creates a suction of liquid allowing a very effective injection, due to the vacuum produced at this location by plasma flow.
  • stage 300 Downstream of stage 300, the mixed constituents react at the outlet of the convergent-divergent in a stage 400 forming an actual reactor, the gaseous and liquid reaction products being collected, separated and analyzed by circuits 500 of conventional type which do not will not be described in detail.
  • a probe 410 also makes it possible to take a sample and measure its temperature at the very heart of the reactor 400.
  • the game of plasma is projected into a mixing chamber 230 supplied in addition with gas generating free radicals by a series of orifices 240, preferably radial, connected to the gas supply line 210 (usually hydrogen, or a mixture of hydrogen and methane).
  • gas supply line 210 usually hydrogen, or a mixture of hydrogen and methane.
  • the injection of cold gas (at a temperature close to room temperature) has the effect of lowering the temperature of the plasma set at the anode outlet (where the temperature of the argon / hydrogen mixture or of pure hydrogen is between 2000 and 3500 K, for example of the order of approximately 3250 K as indicated above) at a temperature remaining below approximately 2800 K in the lower part of the chamber 230.
  • the cylinder 250 constituting the wall of the mixing chamber can be formed from an external piece 251 of copper provided with a sleeve 252 formed of a material limiting the transfer of heat to the room. made of copper, for example a 5 mm thick boron nitride sleeve.
  • the stage 300 for injecting the liquid charge essentially comprises a convergent-divergent 310,320 forming a throttle 330 at the level of which the liquid charge is injected.
  • the charge is preferably injected through a plurality of orifices 340 (for example three in number, arranged radially at 120 °), with a radial orientation and perpendicular to the axis nozzle.
  • the homogeneity of the injection of the charge through these orifices is obtained by a distributor interposed between the orifices injection line and supply line for the liquid charge.
  • the holes have for example a diameter of 1.5 mm for a nozzle diameter at the location of the neck of 3 mm and an angle at the top of the diverging point of 16 °.
  • the piece constituting the convergent-divergent can be made of copper, or else of stainless steel to have a higher wall temperature.
  • a bore 350 makes it possible to introduce a thermocouple making it possible to measure approximately the temperature in the vicinity of the wall at the level of the constriction.
  • the depression produced at the constriction of the convergent-divergent and the suction of the resulting charge make it possible to divide and nebulize very finely the injected charge (which correlatively increases the exchange surface), the shape of the convergent- divergent favoring an intimate mixture of hydrocarbons within the plasma rich in free radicals.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Physics & Mathematics (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Mechanical Engineering (AREA)
  • Electromagnetism (AREA)
  • General Chemical & Material Sciences (AREA)
  • Plasma & Fusion (AREA)
  • Organic Chemistry (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Plasma Technology (AREA)
EP19880402817 1987-11-10 1988-11-09 Verfahren und Einrichtung für die hydrierende Pyrolyse von schweren Kohlenwasserstoffen durch einen Plasmastrahl, insbesondere ein H2/CH4-Plasma Expired - Lifetime EP0316234B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR8715546 1987-11-10
FR8715546A FR2622894B1 (fr) 1987-11-10 1987-11-10 Procede et installation d'hydropyrolyse d'hydrocarbures lourds par jet de plasma,notamment de plasma d'h2/ch4

Publications (2)

Publication Number Publication Date
EP0316234A1 true EP0316234A1 (de) 1989-05-17
EP0316234B1 EP0316234B1 (de) 1992-06-03

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EP19880402817 Expired - Lifetime EP0316234B1 (de) 1987-11-10 1988-11-09 Verfahren und Einrichtung für die hydrierende Pyrolyse von schweren Kohlenwasserstoffen durch einen Plasmastrahl, insbesondere ein H2/CH4-Plasma

Country Status (3)

Country Link
EP (1) EP0316234B1 (de)
DE (1) DE3871723T2 (de)
FR (1) FR2622894B1 (de)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2639354A1 (fr) * 1988-11-24 1990-05-25 Gaz De France Procede de craquage d'une charge d'hydrocarbures lourds en hydrocarbures plus legers et dispositif pour la mise en oeuvre de ce procede
NL1010288C2 (nl) * 1998-10-12 2000-04-13 Stichting Energie Werkwijze voor de conversie van waterstof in substituut aardgas.
US6800336B1 (en) * 1999-10-30 2004-10-05 Foernsel Peter Method and device for plasma coating surfaces
CN113247881A (zh) * 2021-05-17 2021-08-13 常州大学 一种甲烷等离子体裂解制备纳米碳的装置及方法

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2304243A1 (fr) * 1975-03-14 1976-10-08 Inst Teplo I Massoobmena Akade Procede de chauffage de gaz et reacteur plasmochimique a arc electrique pour sa mise en oeuvre
FR2320977A1 (fr) * 1975-08-11 1977-03-11 Westinghouse Electric Corp Procede pour transformer les hydrocarbures naturels en produit gazeux au moyen d'un appareil de chauffage a arc
US4144444A (en) * 1975-03-20 1979-03-13 Dementiev Valentin V Method of heating gas and electric arc plasmochemical reactor realizing same
FR2542004A1 (fr) * 1983-03-02 1984-09-07 British Petroleum Co Procede de conversion assistee a l'electricite de produits carbones lourds

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2304243A1 (fr) * 1975-03-14 1976-10-08 Inst Teplo I Massoobmena Akade Procede de chauffage de gaz et reacteur plasmochimique a arc electrique pour sa mise en oeuvre
US4144444A (en) * 1975-03-20 1979-03-13 Dementiev Valentin V Method of heating gas and electric arc plasmochemical reactor realizing same
FR2320977A1 (fr) * 1975-08-11 1977-03-11 Westinghouse Electric Corp Procede pour transformer les hydrocarbures naturels en produit gazeux au moyen d'un appareil de chauffage a arc
FR2542004A1 (fr) * 1983-03-02 1984-09-07 British Petroleum Co Procede de conversion assistee a l'electricite de produits carbones lourds
EP0120625A1 (de) * 1983-03-02 1984-10-03 The British Petroleum Company p.l.c. Verfahren zur Umwandlung mit elektrischem Bogen und Apparat

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2639354A1 (fr) * 1988-11-24 1990-05-25 Gaz De France Procede de craquage d'une charge d'hydrocarbures lourds en hydrocarbures plus legers et dispositif pour la mise en oeuvre de ce procede
EP0370910A1 (de) * 1988-11-24 1990-05-30 Gaz De France Krackverfahren von schweren Kohlenwasserstoff-Einsätzen und Vorrichtung zur Ausführung des Verfahrens
US5026949A (en) * 1988-11-24 1991-06-25 Gaz De France Method of cracking a batch of heavy hydrocarbons into lighter hydrocarbons
NL1010288C2 (nl) * 1998-10-12 2000-04-13 Stichting Energie Werkwijze voor de conversie van waterstof in substituut aardgas.
WO2000021911A1 (en) * 1998-10-12 2000-04-20 Stichting Energieonderzoek Centrum Nederland Process for converting hydrogen into substitute natural gas
US6800336B1 (en) * 1999-10-30 2004-10-05 Foernsel Peter Method and device for plasma coating surfaces
CN113247881A (zh) * 2021-05-17 2021-08-13 常州大学 一种甲烷等离子体裂解制备纳米碳的装置及方法

Also Published As

Publication number Publication date
FR2622894A1 (fr) 1989-05-12
DE3871723D1 (de) 1992-07-09
DE3871723T2 (de) 1992-12-24
EP0316234B1 (de) 1992-06-03
FR2622894B1 (fr) 1990-03-23

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