EP2169035B1 - Procédé de réglage de la valeur de combustion dans des gaz de combustion contenant du méthane - Google Patents

Procédé de réglage de la valeur de combustion dans des gaz de combustion contenant du méthane Download PDF

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Publication number
EP2169035B1
EP2169035B1 EP20090171002 EP09171002A EP2169035B1 EP 2169035 B1 EP2169035 B1 EP 2169035B1 EP 20090171002 EP20090171002 EP 20090171002 EP 09171002 A EP09171002 A EP 09171002A EP 2169035 B1 EP2169035 B1 EP 2169035B1
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EP
European Patent Office
Prior art keywords
calorific value
fuel gas
gas
methane
plasma
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.)
Not-in-force
Application number
EP20090171002
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German (de)
English (en)
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EP2169035A1 (fr
Inventor
Michael Goschin
Thomas Ryll
Klaus Rademann
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.)
Begatec GmbH
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Begatec GmbH
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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
    • 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

Definitions

  • the invention relates to a method for adjusting the calorific value in methane-containing fuel gases.
  • Methane-containing fuel gases such as biogas, digester gases, mine gases, thermally produced fuel gases and combustion gases produced by degassing can often be fed into the public gas network only by suitable measures.
  • the reason for the limitation of the feed into the public gas network is justified by the German calibration law, since this allows only a deviation of 2% of the average settlement value within a billing period with supply of gas from different sources or directions. In Germany are z.Zt. two fundamentally different natural gases distributed in public gas networks. First, the natural gas H with a calorific value between 9.5 - 13.1 kWh / m 3 and secondly, the natural gas L with a calorific value between 8.4 - 9.5 kWh / m 3 .
  • biogas After processing the raw biogas, biogas has a calorific value of 10.4 - 10.8 kWh / m 3 . Usually this means that the limit of 2% compared to the billing period is exceeded with a standard combustion value of 11.1-11.5 kWh / m 3 .
  • LPG Liquefied petroleum gas
  • propane / butane mixture is now used to increase the calorific value.
  • This mixture comes from fossil sources and is as finite as natural gas and subject to variable market prices.
  • gas biogas or natural gas H
  • air is mixed with air via elaborate filtering and drying systems.
  • the fuel gas is excited by energy input to form a plasma, whereby the fuel gas or product gas then has a modified calorific value.
  • the plasma is preferably generated in a reactor, through which the fuel gas is passed continuously.
  • the energy input is preferably discontinuous, so that short-term plasmas are generated in the reactor.
  • the plasmas are generated by electric sparks, electric arcs, lasers, microwaves or the like.
  • the electrodes used in this case are preferably made of metal or carbon, with platinum or stainless steel being preferred. Platinum is the most preferred.
  • the calorific value of the fuel gas is changed, wherein the formation can be controlled so that a predetermined calorific value can be achieved, which can be set by a suitable means, which will be described below, to a defined value.
  • the basic organic component methane acetylene / ethyne is formed as the main product.
  • Other products include ethene, ethane, propene, propane, various hydrocarbons with a four carbon carbon skeleton, and hydrogen. There will also be connections with up to six Carbon atoms in the product gas obtained. In addition, carbon black or coal is obtained in good yields.
  • the unsaturated compounds are catalytically hydrogenated and the remaining portion of hydrogen can be separated.
  • the hydrogenation catalyst known catalysts such as metal asbestos, metals and metal oxides are used. Further suitable catalysts are known to the person skilled in the art.
  • the calorific value of the fuel gas is of course also influenced.
  • the separation is carried out by known methods. These are, for example, the diffusion through clay or ceramic components or hydrogen-permeable membranes of palladium alloys. Further suitable methods are known to the person skilled in the art.
  • the entire process can advantageously be carried out continuously in all steps.
  • An apparatus for carrying out the method essentially comprises a reactor, preferably a tubular reactor for the continuous passage of the methane-containing fuel gas.
  • the tubular reactor is provided with means for introducing energy into the fuel gas to form a plasma.
  • This device preferably generates pulsed short-time plasmas.
  • this has after the reactor to a device for the separation of the hydrogen, as described above in the method.
  • this has between the reactor and the means for separating the hydrogen, a means for the catalytic hydrogenation of the unsaturated compounds in the fuel gas, which flows out of the reactor after the plasma treatment.
  • a means for the catalytic hydrogenation of the unsaturated compounds in the fuel gas which flows out of the reactor after the plasma treatment.
  • the yield of the various products depends on the electrical power, the electrode geometry of the energy input device, its polarity, the flow rate of the fuel gas in the reactor, the gas pressure and the electrode material.
  • the selectivity is controlled according to the invention by varying these parameters, so that an increase in the calorific value of a methane-containing fuel gas by formation of higher-energy hydrocarbons or a reduction of the calorific value by formation of soot, which is removed from the gas stream occurs. Also by means of hydrogenation and / or separation of the hydrogen, the calorific value is influenced.
  • the most important and most easily varied parameters in the control of the process are the power of the plasma and the flow rate of the methane-containing fuel gas.
  • the main products can be classified according to the number of carbon atoms.
  • the C2 group two C atoms
  • the C3 group three C atoms
  • the C4 group four C atoms
  • Fig. 1 and Fig. 2 compare each of the products obtained in the different plasma performances. Shown are the C2 in Fig. 1 and C3-in Fig. 2 ,
  • Table 1 represents the percent yields of the carbon compounds and the calorific value produced as a function of the voltage and current of the reactor. Tab.1 Dependence of the reaction products on the reaction voltage Flow (l / h) 30 Sample 1 Sample 2 Sample 3 Sample 4 Sample 5 unit tension kV 4.7 6.0 9.0 12.0 15.0 electricity mA 2.4 4.1 7.4 10.6 14.0 hydrogen % 1.51 2.60 3.81 5.10 4.77 methane % 96.81 94.51 90.90 82.52 77,70 Ethan % 0.55 0.48 0.97 1.57 1.39 ethene % 0.17 0.37 0.66 1.57 1.90 acetylene % 0.85 1.73 3.24 7.43 11.34 propane % 0.00 0.00 0.00 0.05 0.04 propene % 0.00 0.00 0.04 0.11 0.14 1,2- % 0.00 0.04 0.05 0.17 0.26 propyne % 0.04 0.10 0.14 0.47 0.77 1,3-butadiene % 0.00 0.00 0.00 0.07 0.
  • Fig. 1 shows superimposed chromatograms and represents the increase in peak height (area) for ethane, ethene, and acetylene.
  • concentration can be found in Table 1.
  • Sample 1 corresponds to the lowest plasma power (4.7 kV) and Sample 5 to the highest plasma power (15 kV).
  • Particularly noteworthy here is the enormous increase in acetylene. With a voltage of approx. 15 kV, acetylene reaches a peak area of more than ten percent, making it the main product.
  • the sum of the C2 connections is about 15 kV voltage with over 15 percent higher than all other connections.
  • Fig. 2 shows propene and propadiene as a function of increasing plasma power. There is also a significant increase in peak height with increasing voltage.
  • the proportional peak area of propene and propadiene is about ten times smaller than the sum of the peak areas of the C2 group at about 15 kV. Propane is detectable only at voltages above 9 kV.
  • Table 2 shows that higher concentrations of higher hydrocarbons are obtained at 60 l / h than at 30 l / h.
  • the concentration of hydrogen in the product gas mixture correlates with low gas flows and high voltages. At low gas flows carbon is formed, which is recognizable as carbon fouling. The hydrogen yield then increases, the concentration of higher hydrocarbons decreases as carbon is formed.
  • Table 2 Dependence of the concentration as a function of the flow rate Flow (l / h) 60 30 unit tension kV 9.1 9.0 electricity mA 7.2 7.4 hydrogen 3,542 2.43 3.81 methane % 11,064 89.56 90.90 Ethan % 19.537 1.11 0.97 ethene % 19.537 0.96 0.66 acetylene % 19.537 5.04 3.24 propane % 25 0.00 0.00 propene % 25 0.07 0.04 1,2-propadiene % 25 0.10 0.05 propyne % 25 0.00 0.14 1,3-butadiene % 35 0.26 0.00 1.3 Butadiyne % 35 0.03 0.13 1-butyn % 35 0.33 0.00 n-pentane %
  • Fig. 5 shows that acetylene concentrations of over one percent at 30 l / h and about 15 kV are obtained.
  • the concentration of hydrogen in the product gas mixture correlates with low gas flows and high voltages.
  • Fig. 6 shows that more than 5% by volume hydrogen was measurable at reaction conditions of 30 l / h and 15 kV in the product gas.
  • Table 3 shows the results of methane conversion at 60 l / h with a platinum and a stainless steel electrode
  • Fig. 7 shows a schematic structure of a device.
  • This device 10 has a fuel gas source 11 with a discharge valve 12, from which the fuel gas is passed via a gas line to the flow reactor 13, in which a device for energy input 14 is arranged. Subsequently, the fuel gas / product gas changed in the calorific value is first conducted to a device for hydrogenation 15 and then to a device for the separation of hydrogen 16. In addition, the last device provided is a gas chromatograph 17 with which the composition of the product gas can be analyzed.
  • the gas analysis after carrying out the process with the device prototype described below shows, in addition to the main component methane, exclusively saturated higher hydrocarbons and no hydrogen.
  • the partial conversion of methane into higher hydrocarbons and the complete hydrogenation of unsaturated hydrocarbons such as acetylene and the complete separation of hydrogen has succeeded.
  • the increase in calorific value was over 11%.
  • the control of the ignition energy of the plasma allows adjustment of the calorific value. This means that almost every calorific value that is greater than 11.064 kWh / m3 can be set by varying the process parameters.
  • the methane reactor consists of a square tube (edge length 10 cm) in which at a distance of 5 cm twelve spark plugs are screwed.
  • the electrical mains voltage 230V, 50Hz
  • the required high voltage is achieved by a relay circuit with a very high clock frequency.
  • semiconductor relays are controlled by means of high-frequency pulsed DC voltage and thus clock the supply voltage of the coils.
  • the control of the ignition energy via a frequency controller and the amount of supply voltage for the coils.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Claims (4)

  1. Procédé de réglage du pouvoir calorifique dans des gaz combustibles contenant du méthane, caractérisé en ce que le gaz combustible est conduit en continu à travers un réacteur, ce gaz étant excité par une fourniture d'énergie pour la formation d'un plasma de telle sorte que, à partir du méthane, il est formé de l'acétylène en tant que produit principal, et qu'un gaz combustible d'un pouvoir calorifique accru, indiqué en kWh/m3, sort du réacteur, le plasma étant produit par des étincelles électriques, des arcs électriques, un laser, des microondes, et le gaz dont le pouvoir calorifique a été modifié étant hydrogéné.
  2. Procédé selon la revendication 1, caractérisé en ce que l'hydrogénation s'effectue par voie catalytique.
  3. Procédé selon la revendication 1 ou 2, caractérisé en ce que l'hydrogène encore présent dans le gaz combustible du fait de la modification du pouvoir calorifique et après l'hydrogénation est séparé du gaz combustible.
  4. Procédé selon une des revendications 1 à 3, caractérisé en ce que le réglage du pouvoir calorifique s'effectue par la variation d'au moins un des paramètres suivants :
    puissance électrique du plasma,
    vitesse d'écoulement du gaz combustible,
    géométrie des électrodes,
    polarité des électrodes,
    pression du gaz combustible et
    matériau des électrodes.
EP20090171002 2008-09-22 2009-09-22 Procédé de réglage de la valeur de combustion dans des gaz de combustion contenant du méthane Not-in-force EP2169035B1 (fr)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE102008048819 2008-09-22

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EP2169035A1 EP2169035A1 (fr) 2010-03-31
EP2169035B1 true EP2169035B1 (fr) 2013-07-24

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Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102010010896B4 (de) * 2010-03-03 2014-12-04 Scharr Tec Gmbh & Co. Kg Verfahren und Vorrichtung zur Konditionierung von biomethanhaltigem Gas
DE102011077788A1 (de) 2011-06-20 2012-12-20 Evonik Degussa Gmbh Verfahren zur Modifizierung eines methanhaltigen Gasvolumenstroms
PL227975B1 (pl) * 2012-07-31 2018-02-28 Inst Tele I Radiotech Sposób i urzadzenie do zwiekszania wartosci opałowej biogazu

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* Cited by examiner, † Cited by third party
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NO175984C (no) * 1991-12-12 1995-01-18 Kvaerner Eng Fremgangsmåte for å redusere karboninnholdet i en innmatingsström av naturgass eller andre hydrokarbongasser og anvendelse derav
NL1010288C2 (nl) * 1998-10-12 2000-04-13 Stichting Energie Werkwijze voor de conversie van waterstof in substituut aardgas.
DE10163475C1 (de) * 2001-12-21 2003-09-25 Siemens Ag Verfahren und Vorrichtung zur Behandlung oder Umwandlung von gasförmigen Brennstoffen
AP2008004698A0 (en) * 2006-06-05 2008-12-31 Plascoenergy Ip Holdings S L A gasifier comprising vertically successive processing regions
US8075869B2 (en) * 2007-01-24 2011-12-13 Eden Energy Ltd. Method and system for producing a hydrogen enriched fuel using microwave assisted methane decomposition on catalyst

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EP2169035A1 (fr) 2010-03-31

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