EP1652906A1 - Procédé de production de clathrates de gaz - Google Patents

Procédé de production de clathrates de gaz Download PDF

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Publication number
EP1652906A1
EP1652906A1 EP05023230A EP05023230A EP1652906A1 EP 1652906 A1 EP1652906 A1 EP 1652906A1 EP 05023230 A EP05023230 A EP 05023230A EP 05023230 A EP05023230 A EP 05023230A EP 1652906 A1 EP1652906 A1 EP 1652906A1
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EP
European Patent Office
Prior art keywords
transport
reaction
liquid
ice
gas
Prior art date
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.)
Granted
Application number
EP05023230A
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German (de)
English (en)
Other versions
EP1652906B1 (fr
Inventor
Bernd Bonso
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.)
Mebes Reto
Original Assignee
Bernd Bonso
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Filing date
Publication date
Application filed by Bernd Bonso filed Critical Bernd Bonso
Publication of EP1652906A1 publication Critical patent/EP1652906A1/fr
Application granted granted Critical
Publication of EP1652906B1 publication Critical patent/EP1652906B1/fr
Not-in-force legal-status Critical Current
Anticipated expiration legal-status Critical

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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10—Working-up natural gas or synthetic natural gas
    • C10L3/108—Production of gas hydrates
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C11/00—Use of gas-solvents or gas-sorbents in vessels
    • F17C11/007—Use of gas-solvents or gas-sorbents in vessels for hydrocarbon gases, such as methane or natural gas, propane, butane or mixtures thereof [LPG]
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25C—PRODUCING, WORKING OR HANDLING ICE
    • F25C1/00—Producing ice
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25C—PRODUCING, WORKING OR HANDLING ICE
    • F25C5/00—Working or handling ice
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25B—REFRIGERATION MACHINES, PLANTS OR SYSTEMS; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS
    • F25B2315/00—Sorption refrigeration cycles or details thereof
    • F25B2315/003—Hydrates for sorption cycles

Definitions

  • the invention relates to a method for producing gas clathrates, wherein at least one required for the clathrate reaction gas and at least one required for the clathrate reaction liquid are introduced into a reaction vessel and wherein in the reaction vessel, the conditions are set with the proviso that a clathrate formation from the reaction gas and from the reaction liquid.
  • gas clathrates or gas hydrates are known in principle.
  • hydrocarbon-containing gases for example methane or else hydrogen are bound in the form of clathrates or hydrates.
  • the gases can be stored in a less voluminous and relatively easy to handle manner.
  • the gases for example natural gas, can thus be stored primarily as energy sources and can be transported simply and easily compared to the free gaseous state.
  • the invention is based on the technical problem to provide a method of the type mentioned, with the less expensive and effective way Clathrates with high yield and high Production speed can be generated. Above all, the invention is also based on the technical problem of specifying a method which can be carried out continuously.
  • the invention teaches a process for the production of gas clathrates, wherein at least one reaction gas required for clathrate formation and at least one reaction liquid required for the formation of clathrates are introduced into a reaction vessel, wherein the conditions in the reaction vessel are set with the proviso that a clathrate formation takes place from the reaction gas and from the reaction liquid, further wherein the conditions in the reaction vessel are adjusted with the proviso that in an outlet region of the reaction vessel clathrat inconveniences ice is formed, which closes the outlet region reaction chamber side, wherein the clathrat hair ice is crushed with at least one crushing device into pieces of ice and wherein the clathrat ambiencen pieces of ice are transported away via a connected to the outlet region transport line.
  • gas clathrates of hydrocarbon-containing gases for example methane
  • gas hydrates for the production of which water is used as the reaction liquid. It is above all also within the scope of the invention that gas clathrates or gas hydrates are formed by natural gases or by natural gas.
  • the process according to the invention is carried out continuously, that is to say that reaction gas and / or reaction liquid are fed continuously to the reaction vessel, and that ice pieces containing clathrate are continuously produced and removed.
  • the method can also be carried out with a periodic supply of reaction gas and / or reaction liquid and / or with a periodic removal of clathrat restroomn pieces of ice.
  • Clathrate-containing pieces of ice means in the context of the invention in particular pieces of ice which consist entirely of the gas clathrate or at least consist essentially of the gas clathrate.
  • a particularly preferred embodiment of the method according to the invention is characterized in that the reaction gas used for the clathrate formation is purified and compressed prior to its introduction into the reaction vessel. This procedure has proved particularly suitable for continuous clathrate production.
  • Such a simultaneous cleaning and compression of a reaction gas is disclosed in EP 1 329 253 A1. Thereafter, work is preferably carried out within the scope of the invention.
  • the cleaning and compression (compression) of the reaction gas is advantageously carried out in at least one cleaning / compression tank by a cleaning liquid is introduced into the cleaning / filling container filled with the reaction gas, so that the reaction gas is purified on the one hand and on the other hand Filling the cleaning / compression tank is compressed.
  • reaction gas is first expediently introduced into the cleaning nerdichtungs matterer filled with the cleaning liquid from below.
  • the reaction gas has as small a bubble size as possible when it is introduced into the cleaning fluid, so that a large contact surface is provided.
  • the reaction gas is purified by means of the cleaning liquid.
  • cleaning liquid is displaced from the cleaning Nerdichtungs concerneder and transferred, for example, in a reservoir.
  • the cleaning liquid is then introduced into the cleaning Nerdichtungs actually filled with the reaction gas and preferably injected or sprayed, for which purpose a corresponding spray head or a corresponding spray nozzle is provided in the upper region of the cleaning Nerdichtungs matterers. This then results in an effective final cleaning of the reaction gas and at the same time the cleaning Nerdichtungs actuallyer is filled with the cleaning liquid, so that the reaction gas is compressed.
  • a cleaning liquid is used in the above-described cleaning, which absorbs only small amounts of the reaction gas to be purified under the conditions in the cleaning Nerdichtungstic matterer.
  • the cleaning liquid may be, for example, a glycol, which in particular absorbs only small amounts of methane under the conditions mentioned.
  • the cleaning liquid is selected with the proviso that it easily absorbs other impurities in the reaction gas, for example, carbon dioxide or water.
  • the reaction gas which is preferably purified and compressed in the manner described above, is then pressurized at least partially initiated with the reaction liquid filled reaction vessel.
  • the introduction is expediently carried out via a corresponding valve. It is within the scope of the invention that the reaction gas is introduced into the reaction vessel under the pre-pressure set in the cleaning / compression tank. During the introduction into the reaction vessel, care is also taken to ensure that the reaction gas enters the reaction liquid with the smallest possible bubble size, so that the largest possible contact surface is provided.
  • at least one mixing device for effective mixing of reaction liquid and reaction gas is located in the reaction vessel.
  • the conditions in the reaction vessel are adjusted so that a Clathrat Struktur takes place. Setting the conditions means in particular adjustment of the pressure and / or the temperature and / or the concentrations of the reactants.
  • reaction liquid for adjusting the conditions in the reaction vessel is introduced continuously or periodically into the reaction vessel and / or withdrawn continuously or periodically from the reaction vessel. With the help of the reaction liquid in particular the required pressure setting for clathrate formation takes place.
  • the reaction liquid in the case of the production of gas hydrates is water.
  • water is used to produce methane hydrate as the reaction liquid.
  • the density and / or the adsorption capacity and / or the absorption capacity of the reaction liquid is influenced or controlled by the addition of salts for effective clathrate formation.
  • the formation of the clathrat inconveniencen ice induced by adjusting the conditions in particular by adjusting the pressure and / or the temperature in the reaction vessel or is encouraged.
  • the clathrate can then collect due to its density in the outlet area in the form of ice.
  • the clathrat inconveniencen ice is formed with at least one arranged in the outlet region cooling device or the formation of the clathrat inconveniencen ice is promoted in the outlet region with this at least one cooling device.
  • both measures that is, cooling device and setting the conditions.
  • the clathrate-containing ice preferably consists entirely or essentially of the gas clathrate. It is also within the scope of the invention that the clathrat inconvenience ice is pressed in the form of an ice plug in the outlet region under the pressure prevailing in the reaction vessel. This formation of the ice plug contributes particularly effectively to the solution of the problem according to the invention.
  • the conditions required for clathrate formation in the reaction vessel that is to say in particular pressure and / or temperature, can be maintained in a simple and effective manner.
  • the outlet region is expediently formed by at least one outlet connection piece connected to the reaction container. It is within the scope of the invention that the outlet region or the outlet nozzle is arranged in the upper part or at the top of the reaction container.
  • the comminuting device can be an active comminuting device, that is to say a comminution device driven by a motor or the like.
  • the comminution device can also be a passive, that is to say non-driven, comminuting device, for example comprising cutting devices consists. Active and passive crushers can also be combined.
  • this transport liquid is supplied in the reaction vessel facing away or transport line side region of the outlet region and / or at the beginning of the transport line.
  • the transport liquid may at least partially consist of the reaction liquid.
  • the transport liquid can also consist at least partially or completely of water.
  • at least part of the transport liquid consists of a liquid for generating energy, in particular of a liquid fuel, for example of gasoline. Then both the gas stored in the clathrates and the transport liquid can be used to generate energy.
  • Methanclathrat can be treated with gasoline as a transport liquid and both the methane stored in the clathrate and the gasoline can be used to generate energy and, for example, be supplied to a corresponding engine.
  • a special transport liquid so the simultaneous storage of the gas in the clathrate and a fuel liquid, for example for vehicle engines is possible.
  • the transport line has at least one pump for conveying the pieces of ice or the transport liquid.
  • the transport liquid is introduced with the entrained ice pieces in a transport and / or storage container and that at least part of the transport liquid is withdrawn from this transport and / or storage container.
  • transport liquid is introduced with ice pieces in the container and at the same time excess transport liquid is withdrawn from the transport and / or storage container.
  • at least a portion of the withdrawn from the transport and / or storage container transport liquid is returned to the transport of the ice pieces through the transport line. In that regard, therefore, a corresponding cycle of the transport liquid is realized.
  • the transport liquid withdrawn from the transport and / or storage container is expediently filtered clathrate-free.
  • the invention is based on the finding that with the aid of the method according to the invention a very effective and at the same time inexpensive preparation of gas clathrates or gas hydrates is possible. It should be emphasized in particular that the process according to the invention permits an advantageously high clathrate yield and is distinguished in particular by a high production rate for gas clathrates. It should also be emphasized that the process according to the invention can be carried out continuously in an advantageous manner and that a very high production rate with high clathrate yield is possible, especially in a continuous process. It should also be pointed out that the method according to the invention or a device for the method according to the invention operates very reliably and without interference. Such a device can also be realized in a relatively simple, inexpensive and cost-effective manner.
  • FIGURE shows a device according to the invention for carrying out the method according to the invention in a schematic representation.
  • the figure first shows a cleaning Nerdichtungs concerneder 1 for the simultaneous cleaning and compression of a reaction gas.
  • the reaction gas may be a hydrocarbon-containing gas, for example methane.
  • the cleaning / compression tank is initially filled with a cleaning liquid, for example with a glycol.
  • the reaction gas is then introduced via the supply line 2 from below into the cleaning Nerdichtungsiter 1. It is expediently ensured that the reaction gas is passed through the cleaning liquid with the smallest possible bubble size, so that the largest possible contact surface results. In this way, the reaction gas is purified by means of the cleaning liquid.
  • the cleaning liquid is displaced in a manner not shown from the cleaning / compression tank. Subsequently, the cleaning / compression tank 1 is filled with the reaction gas.
  • cleaning liquid is introduced via the supply line 3 again in the cleaning / compression tank 1 and expediently injected from above.
  • the reaction gas is further purified with the cleaning liquid.
  • the reaction gas is compressed.
  • reaction gas is fed from the cleaning / compression vessel 1 via the feed line 4 under the admission pressure into the reaction vessel 5 filled with reaction liquid.
  • the reaction gas is introduced from below through the reaction liquid. Appropriately, care is also taken here that the injected reaction gas enters the reaction liquid with a small bubble size in order to ensure the largest possible contact surface.
  • the conditions, that is, in particular, the pressure and the temperature are adjusted so that a gas clathrate forms from the reaction gas and the reaction liquid.
  • About the Eiri Operations convinced 6 more reaction liquid is introduced into the reaction vessel 5.
  • excess reaction liquid can be removed from the reaction vessel 5 via the discharge line 7. Excess reaction gas can be withdrawn as needed via the discharge line 8 from the reaction vessel 5.
  • reaction gas is fed through the feed line 4 and reaction liquid is continuously supplied through the introduction line 6 and expediently, the gas clathrate formed is continuously removed from the reaction vessel 5.
  • an outlet nozzle 9 is provided in the upper region of the reaction vessel 5.
  • a cooling device 10 is connected in the embodiment of the figure, with the clathrat inconveniences ice in the outlet nozzle 9 is generated.
  • This clathrate-containing ice preferably closes off as an ice plug the outlet nozzle 9 during the formation of the clathrate in the reaction vessel 5.
  • the ice plug is as it were pressed in under pressure in the reaction vessel 5 in the outlet nozzle 9.
  • comminution device 11 In the outlet direction behind the cooling device 10 of the outlet nozzle 9 a not shown in the figure comminution device 11 is arranged, with the clathrat inconvenience ice behind the cooling device 10 and before a transport line 12 and / or in the front region of the transport line 12 is crushed into transportable pieces of ice , The transportable pieces of ice are then removed via the transport line 12.
  • a transport liquid is supplied via a supply line 13.
  • the transport liquid is expediently supplied in the transport-line-side region of the outlet nozzle 9 and / or in the initial region of the transport line 12.
  • the transport liquid in the transport line side region of the outlet nozzle 9 is supplied.
  • the pieces of ice can then be easily removed with the transport liquid through the transport line 12. It is within the scope of the invention that here takes place a continuous removal of ice pieces with the transport liquid.
  • the pieces of ice are then fed by means of the transport liquid via the transport line 12 to a transport and / or storage container 14.
  • the transport liquid present in the transport and / or storage container 14 can be removed simultaneously via the discharge line 15 and preferably completely fed back to the supply line 13.
  • By discharging the transport liquid from the transport and / or storage container 14 results in a very volume-saving storage of Gasclathrates in the transport and / or storage container 14. If, for example, methane hydrate is prepared in the process of the invention and water is used as a transport liquid can the methane hydrate in the transport and / or storage container to float in the water and the water can be removed as a transport liquid in a simple manner via the discharge line 15.
  • the transport of a gas clathrate produced according to the invention with the aid of the transport liquid is much safer than the transport of the respective gas under pressure in conventional lines.
  • the gas stored in the form of the gas clathrate can be passed in a substantially larger amount in the same time unit through the same pipeline.
  • the gas clathrate accommodated in the transport and / or storage container 14 can in particular be converted back into the respective gas by heating and this gas can then be withdrawn via the withdrawal line 16 from the transport and / or storage container and fed to its intended use.
  • transport liquid can be introduced into the transport and / or storage container 14 via the feed line 17, in order in particular to set the discharge pressure of the resulting gas.
  • penetration of undesired gases into the transport and / or storage container 14 can be prevented.
  • the gas clathrate is transported with a fuel liquid as transport liquid or introduced into the transport and / or storage container 14.
  • Methanclathrat can be transported with gasoline as transport liquid.
  • the methane can then first be developed, for example by heating, and used or consumed in particular in an engine.
  • the transport liquid gasoline from the transport and / or storage container 14 can then be supplied to the engine for use or for consumption.
  • the stored gas from the gas clathrate is expediently released by heating the gas clathrate or the gas clathrate / transport liquid mixture.
  • the heating is preferably carried out via the transport liquid, wherein a corresponding heat source in the transport liquid and / or outside of the wall of the transport and / or storage container 14 may be provided.
EP05023230A 2004-11-01 2005-10-25 Procédé de production de clathrates de gaz Not-in-force EP1652906B1 (fr)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE102004053627A DE102004053627A1 (de) 2004-11-01 2004-11-01 Verfahren zur Herstellung, Transport und Lagerung von Gashydraten (Gasclathrat)

Publications (2)

Publication Number Publication Date
EP1652906A1 true EP1652906A1 (fr) 2006-05-03
EP1652906B1 EP1652906B1 (fr) 2008-12-31

Family

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Family Applications (1)

Application Number Title Priority Date Filing Date
EP05023230A Not-in-force EP1652906B1 (fr) 2004-11-01 2005-10-25 Procédé de production de clathrates de gaz

Country Status (7)

Country Link
US (1) US7863491B1 (fr)
EP (1) EP1652906B1 (fr)
AT (1) ATE419321T1 (fr)
DE (2) DE102004053627A1 (fr)
DK (1) DK1652906T3 (fr)
ES (1) ES2320237T3 (fr)
WO (1) WO2006048197A2 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2434002A1 (fr) * 2010-09-28 2012-03-28 Mebes, Reto Dispositif de fabrication de clathrate de gaz

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Publication number Priority date Publication date Assignee Title
US9149782B2 (en) * 2010-01-25 2015-10-06 Stx Offshore & Shipbuilding Co., Ltd. Method for the fast formation of a gas hydrate
US8354565B1 (en) * 2010-06-14 2013-01-15 U.S. Department Of Energy Rapid gas hydrate formation process
DE102011108065A1 (de) * 2011-07-21 2013-01-24 Rwe Ag Verfahren zur energetischen Nutzung von Brenngasen

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CH677618A5 (fr) * 1988-01-14 1991-06-14 Sulzer Ag
CH679222A5 (en) * 1988-10-04 1992-01-15 Sulzer Ag Hydrate prodn. from hydrocarbon gas esp. natural gas - by contacting gas bubbles with ice crystal suspension in pressure vessel to form solid methane hydrate
US5473904A (en) * 1993-11-12 1995-12-12 New Mexico Tech Research Foundation Method and apparatus for generating, transporting and dissociating gas hydrates
US5536893A (en) * 1994-01-07 1996-07-16 Gudmundsson; Jon S. Method for production of gas hydrates for transportation and storage
US6028234A (en) * 1996-12-17 2000-02-22 Mobil Oil Corporation Process for making gas hydrates
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CA2300521C (fr) * 1999-03-15 2004-11-30 Takahiro Kimura Methode et dispositif de production d'hydrates
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EP2434002A1 (fr) * 2010-09-28 2012-03-28 Mebes, Reto Dispositif de fabrication de clathrate de gaz

Also Published As

Publication number Publication date
ATE419321T1 (de) 2009-01-15
US7863491B1 (en) 2011-01-04
ES2320237T3 (es) 2009-05-20
WO2006048197A2 (fr) 2006-05-11
DE102004053627A1 (de) 2006-05-04
DK1652906T3 (da) 2009-04-14
DE502005006365D1 (de) 2009-02-12
EP1652906B1 (fr) 2008-12-31

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