WO2017064059A1 - Dispositif et procédé de production de gaz de synthèse - Google Patents

Dispositif et procédé de production de gaz de synthèse Download PDF

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Publication number
WO2017064059A1
WO2017064059A1 PCT/EP2016/074339 EP2016074339W WO2017064059A1 WO 2017064059 A1 WO2017064059 A1 WO 2017064059A1 EP 2016074339 W EP2016074339 W EP 2016074339W WO 2017064059 A1 WO2017064059 A1 WO 2017064059A1
Authority
WO
WIPO (PCT)
Prior art keywords
gas
reaction zone
synthesis gas
synthesis
plasma
Prior art date
Application number
PCT/EP2016/074339
Other languages
German (de)
English (en)
Inventor
Stephan Fabig
Original Assignee
Deutsche Lufthansa Ag
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Deutsche Lufthansa Ag filed Critical Deutsche Lufthansa Ag
Publication of WO2017064059A1 publication Critical patent/WO2017064059A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J19/087—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J19/088—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/342—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents with the aid of electrical means, electromagnetic or mechanical vibrations, or particle radiations
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0869—Feeding or evacuating the reactor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0873—Materials to be treated
    • B01J2219/0881—Two or more materials
    • B01J2219/0883—Gas-gas
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0894—Processes carried out in the presence of a plasma
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
    • C01B2203/0272—Processes for making hydrogen or synthesis gas containing a decomposition step containing a non-catalytic decomposition step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0861—Methods of heating the process for making hydrogen or synthesis gas by plasma
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1241—Natural gas or methane

Definitions

  • the invention relates to an apparatus and a method for the production of synthesis gas.
  • a thermal decomposition of Kohlenwas ⁇ hydrobromofluorocarbons wherein a hydrogen-containing carrier gas (synthesis gas) a signal generated by a plasma torch plasma flows and the hydrocarbons by the thermal energy of the plasma (and of the arc) may be cleaved in a ers ⁇ th reaction zone takes place.
  • synthesis gas is generated using the cleavage products of the first reaction zone, thereby typically ⁇ additionally C02 and / or H20 is supplied.
  • Plasma done This is especially advantageous if Excess electrical energy is available for example from rege ⁇ nerative sources, which can be implemented in this way advantageous in ultimately bound in a fuel ⁇ fuel chemical energy.
  • This synthesis gas is allowed to react for example by the above ge ⁇ called Fischer-Tropsch process to produce liquid fuel.
  • the invention has for its object to provide a device and a method of the type mentioned, or allow efficient operation. Furthermore, there should be a possibility in the use of regeneratively generated electrical energy to take into account the fluctuations of energy sources such as, for example, wind power or solar power.
  • a device according to the invention for the production of synthesis gas which comprises: a. a first reaction zone (1) for thermal Spal ⁇ processing of hydrocarbons in a plasma, b. a second reaction zone (2) for generating
  • Synthesis gas using the fission products of the first reaction zone a first gas inlet (3) upstream of the first action zone (1), d. a second gas inlet (8) in the region of the first reaction zone, e. a third gas inlet (9) in the region of the second reaction zone, characterized in that it further comprises: f. a device for setting an operating state in which all gas inlets (7, 8, 9) are fed exclusively with synthesis gas.
  • a first reaction zone is designed for thermal cracking of hydrocarbons in a plasma. Plas A ⁇ mafackel generated from constituents of the carrier gas (Synthe ⁇ segas) by an electrical discharge between two Electrodes a high-temperature plasma. Such a Plasmafa ⁇ ckel is the skilled worker in general and needs no further explanation. The thermal energy of the plasma serves to cleave the hydrocarbons (usually methane) preferably in elemental hydrogen and carbon.
  • a first reaction zone may be designed, for example, as a Kvaerner reactor.
  • a second reaction zone serves to generate synthesis gas using the cleavage products of the first reaction zone.
  • synthesis gas Gasmi designates a ⁇ research, whose main constituents are hydrogen and Kohlenmono- hydroxide (optionally in different mixing behaves ⁇ nits).
  • "Using the cleavage products” means that additional reactants can be used in the second reaction zone, typically CO 2 and / or water
  • One embodiment of such a second reaction zone is the CO 2 converter or Boudouard reactor as described above.
  • Boudouard reactor means in this context always that there in addition to a Boudouard reaction (in the case of the supply of C02) even when supplying water, a - known to the expert -.
  • the first gas inlet upstream of the the first reaction zone serves in normal operation of the device the supply of carrier gas for the plasma, typically syngas.
  • Optional can ⁇ additionally in normal operation by this first gas inlet for cleaving hydrocarbons in certain micro research are introduced with the carrier gas.
  • the optional second gas inlet in the region of the first reaction zone is used in normal operation of the supply of for cleavage of certain hydrocarbons.
  • This second gas inlet can be designed, for example, as a central feed lance, which is guided through a plasma flare designed as a tubular hollow body.
  • the second gas inlet can be arranged somewhat downstream of the plasma electrodes, in order to avoid or reduce direct contact of the hydrocarbons with the electrodes and an electrode filling caused thereby by deposition of elemental carbon.
  • the third gas inlet in the region of the second reaction zone is used in normal operation of the supply of carbon dioxide and / or water to the Boudouard reactor or water gas conversion reactor.
  • Synthesis gas are fed, an operation of Vorrich ⁇ tion can be done in a state in which in particular in the first reaction zone at least no appreciable amounts regardsifies ⁇ thermally cleavable hydrocarbons are not or present.
  • the invention has recognized that, in particular when starting or stopping a device according to the invention unfavorable operating conditions can occur. When starting and stopping the operation, a slow heating or cooling of the device is required to avoid temperature-induced stress and damage. The device runs through temperatures or states in which a normal operation is no longer possible because, for example, the temperature threshold from which a splitting of the hydrocarbons takes place, is not or no longer reached.
  • the core of the invention is such load change states as start-up or shut-down or even idling operation (operation in a basically suitable for normal operation operating point, but without a splitting of
  • Hydrocarbons or generation of synthesis gas takes place without it can lead to undesirable side reactions and thus, for example, associated impurities of the device.
  • a slow start of the retraction o- or a setting of the desired operating point can be carried out without causing tr foundedungen to any affected.
  • the carrier gas for the plasma also referred to as plasma gas
  • ⁇ finished syngas under all operating conditions (including starting up or shutting and normal operation) in the behaves inertly first reaction zone and the second reaction zone in ⁇ We sentlichen and there are no adverse reactions or side reactions.
  • Essentially means inertness that the synthesis gas while the plasma magas enables the plasma formation and to the extent, of course, responds that it does not come to chemical Reginareaktio ⁇ nen that significantly change the chemical composition of the Plasmaga ⁇ ses. Only after reaching a desired and defined operating point of the normal operation is absorbed by feeding the intended for normal operation gases in the gas inlets.
  • the invention is of particular advantage in particular when a device according to the invention is fed with regeneratively generated electrical energy which is subject to fluctuations.
  • the then regularly required change of operating conditions can be carried out according to the invention, without causing undesirable high signs of wear or frequent operating conditions with non-optimal implementation of the starting materials used.
  • means are provided for recirculating gas from the outlet of the second reaction zone to the gas inlets.
  • a means for recirculating gas from the exit of the second reaction zone to the gas inlets means that synthesis gas can be recirculated and recycled to some or all of the existing gas inlets.
  • the device according to the invention may additionally have a reservoir for synthesis gas.
  • a reservoir for synthesis gas.
  • the reservoir may be provided for temporarily stored synthesis gas from the previous operation han ⁇ punching, alternatively or additionally, the synthesis gas from an external source, for example by mixing externally provided carbon monoxide and hydrogen.
  • the plasma introduces an energy input into the device, which is not used for chemical reactions (splitting up of the hydrocarbons). Since this energy input ⁇ possible greater than the desired energy input for heating the device when starting, advantageously, a means for cooling at least a partial flow of the recirculated synthesis gas can be provided. It may be that cooler, which is usually provided anyway for cooling the synthesis gas before Wei ⁇ tergabe to the Fischer-Tropsch reactor. Cooling at least a part-stream allows to adjust by mixing of cooled and uncooled parts of the synthesis gas a ge ⁇ desired energy input or a desired temperature profile.
  • At least one mixing device is provided for mixing an uncooled recirculated partial flow of the gas recirculated from the outlet of the second reaction zone to the gas inlets with a cooled partial stream of this gas and / or a partial stream taken from the synthesis gas reservoir.
  • a separate mixing device may preferably be provided for each gas inlet, so that the introduction temperature at each gas inlet set different and thus the total setting ⁇ ment a desired temperature profile is facilitated in the device.
  • Another object of the invention is a method for operating a device for generating synthesis gas during a load change state and / or in an idle ⁇ running state. This device has a first reaction zone for the thermal cleavage of hydrocarbons in a plasma and a second reaction zone for the production of synthesis gas using the cleavage products of the first reaction zone.
  • Idle operation essentially without chemical reactions, side reactions or other unwanted accompanying circumstances.
  • the method according to the invention can be carried out particularly advantageously with a device according to the invention described above.
  • An operation exclusively with synthesis gas over at least one subsection includes that, for example, a further subsection of a load change can already take place with supply of reactive gas components such as, for example, hydrocarbons. If, for example, in the first reaction zone, a cleavage of the hydrocarbons in a certain temperature window and / or
  • Pressure window can be done, can be started with the introduction of hydrocarbons as soon as the lower limit of this temperature window is reached when starting. It can then ⁇ follow with already hydrocarbon feeds another load change through, for example, in the middle of this temperature window and / or pressure window.
  • an operation according to the invention can exclu ⁇ Lich with synthesis gas to the slow cooling of the apparatus take place.
  • the operation can eventually be made from ⁇ with synthesis gas to maintain a desired temperature and / or pressure levels.
  • a short-term idle state can be useful, for example, in the operation of the plasma with regeneratively generated electrical energy to provide short-term control energy for the operation of an electrical grid.
  • This device according to the invention will initially be described in its normal operation.
  • the device according to the invention has a first reaction zone 1 (designed as a Kvaerner reactor) and a second reaction zone 2 (designed as a Boudouard reactor and / or a water gas conversion reactor).
  • Synthesis gas is introduced as plasma gas into the first reaction zone through a first gas inlet 7 arranged upstream of the electrodes 3. Between the electrodes 3, a plasma is ignited.
  • Hydrocarbons are introduced through the second gas inlet 8, which are thermally partly directly in the plasma, partly split in the hot zone of the plasma slightly downstream on ⁇ into hydrogen and elemental carbon.
  • the gas / solid mixture thus produced enters the second reaction zone 2.
  • Through the third gas inlet 9 C02 and / or water is supplied. Elemental carbon can be converted into carbon monoxide with carbon dioxide in a Boudouard reaction. Alternatively or additionally, a water gas conversion reaction can be carried out with water introduced.
  • the ⁇ segas is removed. In normal operation, this is cooled in a kuh ⁇ ler 4 to a desired temperature level and supplied for example to a subsequent reactor for the production of liquid hydrocarbons at 15, in ⁇ game as a Fischer-Tropsch reactor.
  • synthesis gas (uncooled or cooled) can be recycled before the cooler 4 at 16 and after the cooler at 17 and pumped by means of pumps 18, 19 in the direction of the gas inlets 7, 8, 9.
  • Mixer 10, 11, 12 allow to set for each of the gas inlets to flow a desired mixing ratio of refrigerated and unrefrigerated part ⁇ and thus to control the inlet temperature at each of the gas inlets individually.
  • a reservoir 5 is additionally provided. It can be a tank that is fed with syngas in normal operation and keeps it in stock for the next start-up.
  • 13 may be used hydrogen or carbon monoxide from supply containers ⁇ 6, if necessary.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Inorganic Chemistry (AREA)
  • Combustion & Propulsion (AREA)
  • Toxicology (AREA)
  • Physics & Mathematics (AREA)
  • Electromagnetism (AREA)
  • Mechanical Engineering (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)

Abstract

L'invention a pour objet un dispositif de production de gaz de synthèse, comprenant une première zone réactionnelle (1) pour le craquage thermique d'hydrocarbures dans un plasma, une deuxième zone réactionnelle (2) pour la production de gaz de synthèse à partir des produits de craquage de la première zone réactionnelle, une première entrée de gaz (7) en amont de la première zone réactionnelle (1), éventuellement une deuxième entrée de gaz (8) dans la région de la première zone réactionnelle (1), ainsi qu'une troisième entrée de gaz (9) dans la région de la deuxième zone réactionnelle (2). Selon l'invention le dispositif comprend un système pour recirculer le gaz de la sortie de la seconde zone réactionnelle (2) vers les entrées de gaz (7, 8, 9), ainsi qu'un système de mise en oeuvre d'un mode de fonctionnement dans lequel toutes les entrées de gaz (7, 8, 9) sont alimentées uniquement avec du gaz de synthèse. L'invention concerne en outre un procédé pour faire fonctionner un tel réacteur à des régimes de changement charge, ainsi qu'à vide. Un fonctionnement uniquement au gaz de synthèse à ces régimes permet d'obtenir un démarrage et un arrêt contrôlés sans réactions secondaires indésirables.
PCT/EP2016/074339 2015-10-13 2016-10-11 Dispositif et procédé de production de gaz de synthèse WO2017064059A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102015219862.6 2015-10-13
DE102015219862.6A DE102015219862A1 (de) 2015-10-13 2015-10-13 Vorrichtung und Verfahren zur Erzeugung von Synthesegas

Publications (1)

Publication Number Publication Date
WO2017064059A1 true WO2017064059A1 (fr) 2017-04-20

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PCT/EP2016/074339 WO2017064059A1 (fr) 2015-10-13 2016-10-11 Dispositif et procédé de production de gaz de synthèse

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WO (1) WO2017064059A1 (fr)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR3112767B1 (fr) * 2020-07-27 2023-05-12 Plenesys Production optimisée d’hydrogène à partir d’un hydrocarbure.

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2013091879A1 (fr) 2011-12-20 2013-06-27 CCP Technology GmbH Procédé et installation de production de gaz de synthèse
DE102013020375A1 (de) * 2013-12-06 2015-06-11 CCP Technology GmbH Plasma-reaktor zum aufspalten eines kohlenwasserstoff-fluids
WO2015128673A2 (fr) * 2014-02-27 2015-09-03 C-Tech Innovation Limited Procédé et appareil de conversion catalytique assistée par plasma

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7407634B2 (en) * 2003-04-11 2008-08-05 Massachusetts Institute Of Technology Plasmatron fuel converter having decoupled air flow control
US20140239232A1 (en) * 2011-06-21 2014-08-28 Vernon Eric Staton Apparatus and method for hydrocarbon pyrolysis
US9574770B2 (en) * 2012-04-17 2017-02-21 Alter Nrg Corp. Start-up torch
WO2015105607A1 (fr) * 2014-01-08 2015-07-16 Drexel University Nettoyage au plasma non thermique de gaz de synthèse sale

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2013091879A1 (fr) 2011-12-20 2013-06-27 CCP Technology GmbH Procédé et installation de production de gaz de synthèse
DE102013020375A1 (de) * 2013-12-06 2015-06-11 CCP Technology GmbH Plasma-reaktor zum aufspalten eines kohlenwasserstoff-fluids
WO2015128673A2 (fr) * 2014-02-27 2015-09-03 C-Tech Innovation Limited Procédé et appareil de conversion catalytique assistée par plasma

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