Methods for the Biomethanation of H2 and CO2

Abstract

The invention relates to means and methods for the biomethanation of H.sub.2 and CO.sub.2. In particular, the invention relates to devices for producing methane by means of methanogenic microorganisms by converting H.sub.2 and CO.sub.2, wherein the devices comprise at least one reactor, an aqueous medium, which is provided in the at least one reactor, wherein the methanogenic microorganisms are contained in the aqueous medium, a feeding apparatus, which is designed to introduce H.sub.2 and CO.sub.2 into the at least one reactor, wherein H.sub.2 and CO.sub.2 form a gaseous mixture therein, and a reaction-increasing device, which is designed to enlarge the contact surface between the aqueous medium having the methanogenic microorganisms and the gaseous mixture. The invention further relates to methods for producing methane in a reactor device by means of methanogenic microorganisms.

Claims

1-29. (canceled)

20. Method for production of methane in a reactor device by means of methanogenic microorganisms, which are located in the reactor device in an aqueous medium, by conversion of H.sub.2 and CO.sub.2 as the reaction gas mixture, characterized in that the contact surface between the aqueous medium with the methanogenic microorganisms and the gaseous mixture is increased by means of a reaction boosting device during the conversion and further characterized in that by means of a return mechanism at least a portion of the gas, which accumulates in the reactor, is returned in the reactor device, wherein a return rate of the gas accumulating in the reactor is greater than a feed rate of the reaction mixture in the reactor.

21. Method according to claim 20, characterized in that the methanogenic microorganisms are a mixture of different microorganisms of the phylum Euryarchaeota.

22. Method according to claim 20, characterized in that the methanogenic microorganisms are supplied in the form of macroscopic colonies (pellets) to the aqueous medium.

23-25. (canceled)

26. Method according to claim 20, characterized in that the reactor device has: at least one reactor; an aqueous medium, which is prepared in the at least one reactor, the methanogenic microorganisms being located in the aqueous medium; a feed mechanism, which is designed to channel H.sub.2 and CO.sub.2 into the at least one reactor, wherein the H.sub.2 and CO.sub.2 form a gaseous mixture inside it; a reaction boosting device, which is designed to increase the contact surface between the aqueous medium with the methanogenic microorganisms and the gaseous mixture; a return mechanism, which is designed to return at least a portion of the gas, which accumulates in the reactor, wherein the return rate of the gas accumulating in the reactor is greater than the feed rate of the substrate gas in the reactor.

27. Method according to claim 26, characterized in that the reactor device further has a drainage mechanism, which is designed to drain a gas from the at least one reactor.

28. Method according to claim 27, characterized in that the gas has methane.

29. Method according to claim 28, characterized in that the quantitative fraction of methane in the gas is at least 50%.

30. Method according to claim 20, characterized in that the return rate of the gas accumulating in the reactor exceeds the feed rate of the substrate gas in the reactor by at least a factor of 100.

31. Method according to claim 20, characterized in that the return mechanism has a pump or a compressor.

32. Method according to claim 20, characterized in that the device further has a circulation mechanism, which is designed to circulate the aqueous medium through the at least one reactor.

33. Method according to claim 32, characterized in that the circulation mechanism has at least one pump.

34. Method according to claim 33, characterized in the pump is a driving jet pump.

35. Method according to claim 20, characterized in that the device is set up as stationary or nonstationary reactor.

36. Method according to claim 35, characterized in that the device is a solid state reactor or a submerse reactor.

37. Method according to claim 20, characterized in that the device is set up as continuous ideal stirred tank (CSTR), discontinuous ideal stirred tank (STR), tube reactor, loop reactor, reactors switched in series, or as cascade of reactors.

38. Method according to claim 20, characterized in that the reaction boosting device has at least one trickling bed, one spray tower, one in-line mixer or one pump.

39. Method according to claim 38, characterized in that the pump is a driving jet pump.

40. Method according to claim 26, characterized in that the feed mechanism further has: a device for enrichment of carbon dioxide from a gas mixture; and optionally a mechanism for electrolytic splitting of water; wherein the feed mechanism preferably is designed so that when the H.sub.2 and CO.sub.2 are channeled into the at least one reactor, the gaseous mixture forms a turbulent flow.

41. Method according to claim 26, characterized in that the feed mechanism is further designed so that, in operation, the volume of introduced H.sub.2 and CO.sub.2 per hour exceeds the volume capacity of the at least one reactor by at least the factor of 2, wherein the pressure in the reactor is optionally greater than or equal to 0.1 bar.

42. Method according to claim 20, characterized in that the methanogenic microorganisms are not immobilized in the aqueous medium.

Description

BRIEF DESCRIPTION OF THE FIGURES

Nonlimiting Examples and Figures

[0083] With the aid of the enclosed representations (figures) and sample embodiments, the invention shall be explained more closely.

[0084] FIG. 1: Flow chart of a sample device for production of methane by means of methanogenic microorganisms making use of a tube reactor

[0085] FIG. 2: Flow chart of a sample device for production of methane by means of methanogenic microorganisms making use of a stirred tank

[0086] FIG. 3: Flow chart of a sample device for production of methane by means of methanogenic microorganisms making use of a submerse reactor

[0087] FIG. 4: Flow chart of a sample device for production of methane by means of methanogenic microorganisms making use of a spray tower

[0088] FIG. 5: Flow chart of a sample device for production of methane by means of methanogenic microorganisms making use of a trickle-bed reactor

[0089] FIG. 6: Flow chart of a sample device for production of methane by means of methanogenic microorganisms making use of a jet reactor

[0090] FIG. 7: Flow chart of a submerse reactor for conversion of gaseous substrates. For example, methane bacteria are introduced as compact pellet in a submerse bioreactor and gasified with H.sub.2 and CO.sub.2 at pressure under physiological conditions. An effective phase transition of the gaseous substrate is achieved by an internal recirculation (4) of gases from the reactor gas space (2) into the liquid phase (1). Several reactors (Rn) or reactor parts with different conditions are operated as a cascade in series. Advantages of the method: low temperatures, high organism density, short startup times, flexible operation, simple controls.

[0091] FIG. 8: Flow chart of a cascade of reactors R.sub.1 to R.sub.n with common gas recirculation

[0092] FIG. 9: Flow chart of a cascade of reactors R.sub.1 to R.sub.n with separate gas recirculation

[0093] FIG. 10: Arrangement of several reactors (R.sub.1 to R.sub.n) in a common water body (C), cross section

LIST OF REFERENCES FOR FIGS. 1 TO 6

[0094] 100 Device for production of methane with a tube reactor [0095] 102 Inlet line [0096] 104 First valve [0097] 106 Nozzle [0098] 108 Reactor (designed as a tube reactor) [0099] 110 Gas separation device [0100] 112 Second valve [0101] 114 First outlet [0102] 116 Aqueous medium [0103] 118 First return branch [0104] 120 Pump [0105] 122 Second return branch [0106] 124 Mixing element [0107] 126 Feed mechanism [0108] 128 Liquid surface [0109] 200 Device for production of methane with a stirred tank [0110] 202 Reactor (designed as a stirred tank) [0111] 204 Stirrer [0112] 300 Device for production of methane with a submerse reactor [0113] 302 Reactor (designed as a submerse reactor) [0114] 400 Device for production of methane with a spray tower [0115] 402 Reactor (designed as a spray tower) [0116] 404 Dispersion device [0117] 500 Device for production of methane with a trickle-bed reactor [0118] 502 Reactor (designed as a trickle-bed reactor) [0119] 504 Matrix [0120] 600 Device for production of methane with a trickle-bed reactor [0121] 602 Reactor (designed as a driving jet reactor)

LIST OF REFERENCES FOR FIG. 7 TO 10

[0122] (A) Gasified reactor part with up flow [0123] (B) Nongasified reactor part with down flow [0124] (C) Water body by which several reactors can be tempered [0125] (1) Primarily water filled volume fraction of the reactor [0126] (2) Primarily gas filled volume fraction of the reactor [0127] (3) Gas supply [0128] (4) Gas recirculation [0129] (5) Inlet for nutrient and bacteria supply, pH adjustment, taking samples, etc. [0130] (6) Defoamer dosage [0131] (7) Defoaming device, foam trap [0132] (8) Drainage of solid, liquid and dissolved products from (1) [0133] (9) Drainage of gaseous products from (2) [0134] (10) Gas recirculation pump [0135] (11) Shutoff element [0136] (12) Pressure sustaining valve

DETAILED DESCRIPTION OF SPECIFIC SAMPLE EMBODIMENTS OF THE INVENTION

[0137] FIG. 1 shows a sample embodiment of a device 100 for production of methane by means of methanogenic microorganisms by conversion of hydrogen and carbon dioxide. The sample device 100 has a reactor 108. An inlet line 102 is connected across a first valve 104, such as a first pressure sustaining valve 104, to a first inlet of a nozzle 106, for example, a driving jet nozzle. The nozzle 106 is connected across a corresponding line to the reactor 108. The reactor 108 is connected at its end by means of a line to an inlet of a gas separation device 110. The gas separation device 110 can be filled with a liquid, such as water, and it has three outlets. At a first outlet 114, a gaseous phase can be taken away across a second valve 112, such as a second pressure sustaining valve, containing at least the end product of the microbial conversion, the methane gas, or consisting essentially of this. By a second outlet, optionally a portion of the same gaseous phase can be drained from the gas separation device and supplied via a first return branch 118 to the nozzle 106. The gaseous phase can be fed by means of a separate line to the nozzle 106 or it can be fed into the line by means of which the first valve 104 is connected to the nozzle 106. The first return branch 118 is an optional device, especially in the case of sufficiently long tube reactors, which is not essential to the function of the invention presented here, but which can be entirely suitable for the optimization of its operation. At a third outlet of the gas separation device 110 a liquid phase can be drained away and supplied by means of a second return branch 122, in which a pump 120 is provided, to the nozzle 106.

[0138] In the sample embodiment represented in FIG. 1, the reactor 108 is a tube reactor. By a tube reactor is meant here a tubular container in which the methanogenic microorganisms are contained, and in which a microbial conversion reaction takes place, during which methane is made from H.sub.2 and CO.sub.2. The H.sub.2 and CO.sub.2 together form the substrate gasthe starting product of the microbial conversion reaction. These two gases can be supplied separated from each other by means of separate lines or already as a gas mixture by means of one line to the nozzle 106. The latter case is implemented in the embodiment shown in FIG. 1. The reactor 108 can be designed so that its interior can be maintained at a particular temperature which ensures an optimal course of the reaction. In the present case of production of methane by means of methanogenic microorganisms, the temperature can be for example in a range of around 30 C. to around 80 C., for example in a range of around 40 C. to around 70 C., for example at around 40 to around 50 C. In the reactor 108 there is present an aqueous medium 116, and the methanogenic microorganisms are present in the aqueous medium 116. The aqueous medium 116 can be a gas/liquid mixture, for example a foamy gas/water mixture. The substrate gas, which contains H.sub.2 and CO.sub.2, is fed by means of the nozzle 106 via a feed mechanism 126 to the reactor 108. The feed mechanism 126 can be a correspondingly designed pipe system, which is arranged to introduce a fluid into the reactor 108. In the context of this description, a fluid can mean a gas, a liquid, or a mixture thereof, such as a finely atomized liquid, which is furthermore mixed with a gas. Of course, other substances such as additives encouraging the microbial conversion reaction, such as heavy metals in small amounts which are partly required by methanogenic microorganisms, can also be conveyed into the reactor 108.

[0139] By means of the first return branch 118 the gaseous phase from the gas separation device 110 can be fed to the nozzle 106 and thus recycled. The gaseous phase taken away by means of the first return branch 118 can involve predominantly components of the substrate gas which have not been converted to methane in the reactor 108. These unreacted residues can be so to speak recycled in this way and are again available to the microbial reaction. The first return branch 118 can be omitted in very long tube reactors 108, since the substrate gas introduced at the inlet of such a tube reactor 108 is converted with high probability by the end of the reactor 108. In other words, it can be assumed that with increasing length of the tube reactor 108 the portion of the unreacted substrate gas at the end of such a reactor becomes increasingly smaller.

[0140] The nozzle 106 arranged between the first valve 104 and the reactor 108 serves to introduce at least the substrate gas into the reactor 108 such that at the same time a recirculation or throughput of the liquid medium 116 with the substrate gas so introduced takes place. By means of the nozzle 106 the kinetic energy of the substrate gas can be increased before it is introduced into the reactor 108. In this way, the substrate gas introduced can be as it were blown into the aqueous medium containing the methanogenic microorganisms, producing a strong recirculation of the aqueous medium 116. In other words, by introducing the substrate gas into the reactor 108 by means of the nozzle 106 one can produce numerous gas bubbles which push the aqueous phase 116 through (hereinafter called the dynamic case). In this way, the reaction surface between the substrate gas and the aqueous medium 116 is drastically increased as compared to the case (hereinafter called the static case) when the substrate gas is introduced into a tube reactor 108 without the above-described recirculation of the aqueous phase 116.

[0141] The driving jet can be formed by the nozzle 106 with the help of the liquid phase which is drained off from the gas separation device 110. The nozzle 106 can be, for example, a jet pump in which, depending on the design of the device, the gaseous medium or the liquid phase drained away from the gas separation device 110 can be used. The liquid phase drained away through the second return branch 122 is the aqueous medium 116 from the reactor 108. The gas separation device 110 can be seen functionally as a settling or separation device. In the reactor 108, due to the turbulent mixing processes, the aqueous medium 116 can be present as a foamy gas/water mixture. In other words, the liquid containing the methanogenic microorganisms is heavily enriched with the gaseous phasemethane and residues of the substrate gas. In this state, the aqueous medium 116 is transferred to the gas separation device 110 and a separation of the gaseous phase from the liquid phase occurs there, while the aqueous medium 116 can still be foamy. This gas separation process can naturally occur by uplifting of the gaseous phase (unreacted residues of the substrate gas and methane) from the mixture 116 of liquid and gas. The liquid essentially cleansed of the gaseous phase together with the methanogenic microorganisms can then, as shown in FIG. 1, be removed at the third outlet of the gas separation device 110 and be fed by means of the pump 120 across the second return branch 122 to the nozzle 106 and used to form the driving jet entering the reactor 108. In this way, a closed circulation of the aqueous medium 116 can be achieved.

[0142] The gas which can be drained away at the second outlet of the gas separation device 110 and which can be fed to the nozzle 106 by means of the optional first return branch 118 contains essentially only methane in the optimal case, and possibly slight residues of the unreacted substrate gas. The recirculation rate of the gaseous phase from the gas separation device 110 can be adapted to the length of the reactor 108 and, as already mentioned, will tend toward zero in sufficiently long reactors 108, in which the recirculated gaseous phase from the gas separation device 110 consists essentially of methane. Since the production method presented here is very efficient, i.e., thanks to the strong mixing of the aqueous medium 116 in the reactor 108 with the substrate gas, conversion rates of more than 90% for example, more than 95% for example, practically 100% for example can be achieved. When the first recirculation branch 118 is present, the recirculation rate of the gaseous phase from the gas separation device 110 can always be larger than the feed rate of the substrate gas into the reactor 108 by means of the inlet line 102, for example by factors on the order of 1 to 100, for example, to 200 for example, to 500 for example, to 1000 or more, for example. With very long tube reactors 108, as mentioned above, almost the entire substrate gas is converted to methane. An appropriately designed return branch 118 can also be provided in this case, despite a vanishingly small fraction of the substrate gas residue in the recirculated gas. Regardless of the conversion rate inside the reactor 108, with the help of a high gas recirculation rate by means of the first return branch 118, which thus corresponds functionally to a recirculation branch, the gas fraction in the gas/water mixture inside the reactor 108 and thus the degree of turbulence can be increased. By means of the gas recirculation, the mixing of the gas/water mixture inside the reactor 108, i.e., the contact time and contact surface between these two phases, can thus be increased.

[0143] The gas mixture located above the liquid surface 128 in the gas separation device 110 during the operation of the device 100 contains the product gas and, depending on the efficiency of the conversion, small to vanishingly slight residues of unreacted substrate gas. This gas mixture can be drained off entirely or partially at the first outlet 114 from the device 100 and optionally recirculated by means of the first return branch 118 to the reactor 108. In other words, a gaseous phase of identical composition is drained off at the first outlet 112 and at the second outlet (belonging to the optional first return branch 118).

[0144] Equilibrium generally obtains for a particular H.sub.2/CO.sub.2 ratio in the reactor 108 or in the gas separation device 110: a CO.sub.2 concentration in the gas corresponds to a CO.sub.2 concentration in the aqueous medium 116. If the entire CO.sub.2 is converted, the pH value in the aqueous medium 116 will rise, which may be undesirable. Therefore, the feeding of the substrate gas at the inlet line 102 can be adjusted so that both in the gas phase drained off at the first outlet 114 and thus also at the second outlet a residue of CO.sub.2 always remains, for example around 1% to around 2%. A total conversion of H.sub.2 on the other hand does not result in shifting of the pH value. In order to stabilize the pH value it can thus be beneficial to supply the substrate gas to the device 100 by means of the inlet line 102 in a ratio of around 4:1 (H.sub.2 to CO.sub.2) or less.

[0145] The introducing of the substrate gas into the reactor 108 by means of the nozzle 106, resulting in the mixing of the aqueous medium 116 with the substrate gas, ensures that a much larger number of the methanogenic organisms per unit of time come into contact with the substrate gas in the dynamic case and therefore a larger number of the methanogenic organisms can produce methane per unit of time than in the static case. Approximately speaking, the reaction or contact surface between an aqueous medium 116 present in the reactor and the substrate gas corresponds in the static case to the surface of the medium. In the dynamic case, however, or according to the teaching of the invention as explained in this specification, this surface is much larger, since there must be added to the already roughened and thus larger surface of the aqueous medium 116 in the reactor 108 (indicated by the wavy line inside the reactor 108) the sum of the surfaces of the gas bubbles permeating the aqueous medium 116, wherein the gas bubbles at the beginning of the tube reactor 108 tend to have only substrate gas, and at its end the gas bubbles ideally can have only the end product methane and in between the gas forming the bubbles can have any given mix ratio of substrate gas and methane.

[0146] Moreover, for further increasing of the contact surface between the substrate gas and the aqueous medium 116 the reactor 108 can optionally have at least one mixing element 124. The at least one mixing element 124 can be at least one element which is suitable to mix the substrate gas present in the reactor 108 with the aqueous medium 116. The at least one mixing element 124 can be, for example, a mechanically dynamic element and be designed for example as a rotating water wheel, a jet stream mixer, a turbine stirrer, a propeller stirrer, or perhaps an in-line mixer, this being by no means considered to be an exhaustive listing of possible mixing elements. But the at least one mixing element 124 can also be a mechanically static element, such as an atomization screen, which converts larger substrate gas bubbles into smaller substrate gas bubbles. The at least one mixing element 124 can also have at least one of both a mechanically dynamic and a mechanically static element.

[0147] As shown moreover in FIG. 1, the sample device 100 for the production of methane by means of methanogenic microorganisms has at least two valves, namely, the first valve 104 and the second valve 112. Clearly, as needed, additional fluidic elements can be provided in the device 100, such as further valves, flow meters and compressors. By means of the first valve 104 and the second valve 112 the part of the sample device 100 between the inlet line 102 supplying the substrate gas and the first outlet 114 of the gas separation device 110 draining off the gaseous phase containing the methane gas can be exposed to a pressure gradient, which makes possible the charging of the reactor 108 and creates a fluid flow from the reactor 108 to the gas separation device 110. The lower pressure level (i.e., the pressure at the second valve 112) of the pressure gradient can be at ambient pressure (atmospheric pressure). But if need be, the lower pressure level can also be at a pressure higher than ambient pressure, for example, around 50 mbar, for example 100 mbar, for example 200 mbar, for example 500 mbar or more above ambient pressure. This may prove to be beneficial, as one can thus effectively prevent oxygen from getting into the device 100, which usually can have negative impact on the lifetime and/or number of the methanogenic microorganisms. The first valve 104 furthermore can also be used to control the quantity of substrate gas supplied to the reactor 108 per unit of time and its mix ratio. The latter can also be adjusted by providing separate feeds for H.sub.2 and CO.sub.2 and two corresponding first valves.

[0148] The effective conversion of the substrate gas by means of the methanogenic microorganisms into the product gas methane is based on a highly turbulent gas/water/bacteria mixing inside the tube reactor 108 with an adequate flow rate of the aqueous medium 116, which when using static in-line mixers can be for example in the range of around 3 m/s to around 10 m/s, for example in the range of around 3 m/s to around 5 m/s. When using dynamic in-line mixers with independent motor drive unit, no flow rate is dictated.

[0149] The boosted reaction rate inside the reactor 108 can be accomplished by a highly turbulent mixing of the aqueous medium 116 with the substrate gas. Preferably, the gas volume introduced into the reactor 108 per hour is greater than the volume capacity of the tube reactor 108 itself. The ratio of the gas volume introduced into the reactor 108 per hour to its volume capacity can be for example around 5:1 or more, for example around 10:1, for example around 25:1, for example 50:1 or more. These values pertain to the gas feed at the feed mechanism 102.

[0150] Based on these figures, a little mathematical estimate shall be made to demonstrate the possible capability of the concept presented here. If one starts from a ratio of the gas volume introduced into the reactor 108 per hour to its volume capacity of 5:1, for each cubic meter of reactor volume with an almost complete conversion of the substrate gas according to the teaching of this specification 1 m.sup.3 of methane can be formed per hour. 1 m.sup.3 of methane has an energy content of around 10 kWh. It follows from the development of 1 m.sup.3 methane per hour per 1 m.sup.3 of reactor volume, at complete conversion of the substrate gases to methane, that a corresponding reactor will have a power of around 10 kW per cubic meter. Thus, a reactor 100 m.sup.3 in size would have a power of 1 MW. If one increases the gas throughput ratio to 25:1 per hour, with complete conversion of the substrate gases to methane one can realize a reactor plant with 1 MW power with only 20 m.sup.3 of reactor volume. However, it must be stressed that this is a sample calculation, which is meant to illustrate quantitatively a possible operating scenario of the device for production of methane by means of methanogenic microorganisms as an estimation and should in no way be taken as limiting the power spectrum of the concept presented here.

[0151] The highly turbulent mixing of the aqueous medium 116 with the substrate gas inside the reactor 116by whatever means this is brought aboutensures a distinct increasing of the contact surface between the aqueous medium 116 with the methanogenic microorganisms and the substrate gas, which in turn ensures a distinctly higher reaction rate inside the reactor 108 as compared to the static case mentioned above. In view of the intense mixing of the aqueous medium 116, one can speak in the present case of a rather atypical operation of the tube reactor 108 of the sample device 100 for the production of methane by means of methanogenic microorganisms, since tube reactors of this kind used in chemistry usually have a negligible axial mixing in operation. But in the case presented here of the production method for methane by means of the 100 from FIG. 1 as a sample embodiment it is this mixing which ensures a boosted reaction rate inside the reactor and thus a distinctly increased methane yield as compared to customary production conditions. In this context, the nozzle 106 in FIG. 1 can be seen in terms of its function as a reaction boosting device, since the driving jet produced by it brings about a recirculation of the aqueous medium 116 in the reactor 108 and thus the increased reaction rate can be achieved by said increasing of the contact surface. The mixing element 124 optionally provided in the reactor 108 also contributes to the recirculation of the aqueous medium 116 inside the tube reactor 108 and should thus also be assigned functionally to the reaction boosting device.

[0152] The sample embodiment of the device 100 for production of methane described thus far and represented in FIG. 1 embodies one possibility of obtaining a highly efficient conversion of the substrate gas into methane, according to the teaching presented here. In the following, on the basis of the device from FIG. 1, further sample embodiments shall be described. Starting from FIG. 1, functionally identical elements shall be given the same reference number and will not be described again in greater detail.

[0153] Another sample embodiment of a device 200 for the production of methane by means of methanogenic microorganisms is represented in FIG. 2. The device 200, in contrast with the embodiment represented in FIG. 1, is based on a stirred tank 202 (STR, stirred tank reactor or CSTR, continuous stirred tank reactor), in which the aqueous medium 116 is present, the stirred tank 202 being classified in the category of the submerse reactors. The stirred tank 202 has a stirrer 204, which acts functionally as a mixing element. In the stirrer 204, for example on the surface of its rotor blades, openings can be provided, from which gas can emerge. As in the device 100 shown in FIG. 1, here as well the substrate gas is supplied by means of the inlet line 102 to the reactor. The substrate gas can then emerge, as shown in FIG. 2, from the stirrer 204 itself, for example from its rotor blades during its rotation (stirring motion) or alternatively be introduced into the aqueous medium 116 by means of a separate channeling device independent of the stirrer 204. Such a channeling device can be arranged for example on the bottom of the stirred tank 202 and can introduce the substrate gas into the aqueous medium 116 through a plurality of openings. In either case, an optimal mixing of the substrate gas with the aqueous medium 116 is achieved. Thanks to the rotation of the stirrer 204 or the interaction of the stirrer 204 with the channeling device arranged below it (not shown in FIG. 2), an optimal mixing of the substrate gas with the aqueous medium 116 can be achieved, as illustrated by the gas bubbles rising in the aqueous medium 116, shown in FIG. 2. A strong formation of gas bubbles may be desirable, since this can significantly increase the reaction surface between the substrate gas introduced into the stirred tank 202 and the aqueous medium 116. From this standpoint, the formation of many small gas bubbles may be better than the formation of a few larger gas bubbles. Moreover, a large gas recirculation may be beneficial, which can bring about an increased contact time and contact surface between the aqueous medium and the substrate gas. The methanogenic microorganisms in the aqueous medium 116in addition to the supplying at the interface boundary between aqueous medium 116 and the gas phase above it inside the stirred tank 202can be supplied through the surface of each gas bubble with the product gases H.sub.2 and CO.sub.2, so that in a first approximation the entire volume of the liquid medium 116 can be utilized for the formation of methane. In order to promote the formation of small gas bubbles, the stirrer 204 can have corresponding elements, such as screens or other fine-mesh structures on its surface.

[0154] By means of the first return branch 118 the gaseous phase, possibly containing unreacted substrate gas which collects above the surface of the aqueous medium 116 inside the stirred tank 202, can be taken away and mixed in with the substrate gas supplied at the inlet line 102 by means of a compressor 206 and thus ensure a boosted turbulent mixing of the phases inside the stirred tank 202.

[0155] A further sample embodiment of a device 300 for the production of methane by means of methanogenic microorganisms is shown in FIG. 3. The device 300 is based on a submerse reactor 302. On the floor of the submerse reactors 302 is arranged the nozzle 106, for example a driving jet nozzle, by means of which a driving jet is created and can be directed from the floor of the submerse reactor 302 into the aqueous medium 116. With the nozzle 106, one can accomplish on the one hand a forced convection of the aqueous medium 116 under energy input, and on the other hand the aqueous medium 116 can be turbulently mixed with the substrate gas. In functional terms, the nozzle 106 thus corresponds to the reaction boosting device, while of course at least one mixing element 124 can be additionally provided in the submerse reactor 302, which has been described further above in conjunction with the device shown in FIG. 1. The nozzle 106 is provided with fluids in the same way as already described in conjunction with the device 100 shown in FIG. 1, namely, with the substrate gas, with the aqueous medium 116 via the second return branch 122 and optionally with the gaseous phase from the inside of the submerse reactor 302.

[0156] Yet another sample embodiment of a device 400 for the production of methane by means of methanogenic microorganisms is shown in FIG. 4, in which a spray tower 402 is used as the reactor. The substrate gas is introduced by means of the first valve 104 into the interior of the spray tower 402. By means of the second return branch 122 the aqueous medium 116 is transported upward to a dispersion device 404, such as an atomization nozzle. In this sample embodiment, the aqueous medium 116 is atomized into tiny droplets 406 and sprayed into the spray tower 402 at its ceiling. Thus, in functional terms, the dispersion device 404 is a reaction boosting device. The tinier the droplets 406 produced by the dispersion device 404, the greater the contact surface between the aqueous medium 116 and the substrate gas and the greater the reaction rate of the conversion. The introducing of the substrate gas via the inlet line 102 can also occur, in departure from the representation in FIG. 4, beneath the surface of the aqueous medium 116 in the spray tower 402, for example, via an outlet opening or a corresponding arrangement of closely spaced outlet openings, so that the substrate gas can at first pass through the aqueous medium 116 present in the spray tower 402 as a liquid column and a methane gas production can also occur already in this liquid column. Generally speaking, the reaction boosting devices presented in this application can be combined with each other in any expedient manner in order to maximize the contact surface between the substrate gas and the aqueous medium 116 and thus the methanogenic microorganisms in order to maximize the reaction rate of the methane production.

[0157] FIG. 5 shows another embodiment of the device for the production of methane by means of methanogenic microorganisms, in which a trickling-bed reactor 502 is used. The device 500 resembles the layout of the device shown in FIG. 4. In addition, however, there is provided inside it a porous or honeycomb matrix 504, on which the liquid medium 116 sprayed in from above can trickle down. The interior surface of the matrix 504, for example the size of the pores or honeycombs inside it, defines the reaction surface here. The matrix 504 can be coated with or consist of a material such as glass, plastic, lava ash which ensures a uniform and continuous wetting of the matrix 504 and/or prevents too fast a seepage of the aqueous medium 116 through the matrix 504. In the device 500 shown in FIG. 5 for the production of methane, the reaction boosting device is formed from the matrix 504 and the dispersion device 404, since the interplay of these two devices enables a much increased reaction surface between the aqueous medium 116 and the substrate gas as compared to the static case.

[0158] Yet another embodiment of the device for the production of methane by means of methanogenic microorganisms is shown in FIG. 6, in which a driving jet reactor 602 is used. The substrate gas and the aqueous medium 116 are supplied from the outside to the nozzle 106, such as a driving jet nozzle, arranged on the ceiling or in the upper section of the jet reactor 602. The nozzle 106 moreover can directly aspirate the gaseous phase from the inside of the jet reactor 602, which corresponds to the optional first return branch 118. The driving jet produced by the nozzle 106 can be introduced into or be directed into the aqueous medium 116, resulting in its turbulent mixing with the substrate gas. For example, the driving jet can be introduced by means of a pipe 604 into the aqueous medium 116, while fine openings can be provided on the sides of the pipe 604, through which already a portion of the substrate gas flowing downward can be introduced into the aqueous medium 116. It may be beneficial for the end of the elongated pipe 604 to be situated near the bottom of the jet reactor 602, so that the driving jet passes through a relatively large portion of the aqueous medium 116.

[0159] FIG. 7 shows a sample embodiment of a device for the production of methane (formula symbol CH.sub.4) by means of methanogenic microorganisms by conversion of hydrogen (formula symbol H.sub.2) and carbon dioxide (formula symbol CO.sub.2). This device is a submerse reactor. According to the invention, methanogenic macrocolonies, so-called pellets, are added in high densities to a submerse bioreactor predominantly filled with nutrient liquid. The supplying of the organisms with their substrate, a hydrogen/carbon dioxide mixture, is done by an intensive gasification of the nutrient liquid in which the organisms are present. This is accomplished in that the reactor is operated under greater than atmospheric pressure (12), in order to increase the solubility of the hydrogen. Furthermore, the reactor is mixed by an internal gas recirculation (4). The reactor has a gasified upstream part (A) and nongasified downstream part (B). The gas from the gas phase lying on top of the liquid phase is introduced under pressure into the gasified part and thus produces an upward flow of a gas/liquid/pellet mixture. In the upper part of the reactor, the gas is given off to the gas phase, so that a pellet/nutrient medium mixture can flow back down in the nongasified part (B). The recirculated gas quantity (4) here per unit of time is much greater than the quantity of the gas mixture (3) supplied to the reactor.

[0160] Several such submerse reactors (R.sub.1 to R.sub.n) can be operated in series as a cascade one after another (see FIGS. 8, 9 and 10). A particular gas quantity flows from the front reactor to the one behind it. If the reactors are operated with different gas pressures, different conditions and a plug flow will be established in the reactors. In this way, the gaseous substrate can be extensively converted to methane. This method can make a contribution to utilizing unusable peak production of electricity in order to convert it into a storable form: energy-rich methane. The method consumes carbon dioxide, which need not be provided in pure form. As compared to chemical methods, the method of biomethanization according to the invention takes place under natural conditions. Methane bacteria can survive without nutrition for lengthy periods of time. Thus, they can respond in flexible manner to the demand.

In all the embodiments presented here of the device for production of methane by means of methanogenic microorganisms the CO.sub.2 can be obtained from a smoke gas, such as a trash incinerator or a power plant, such as a coal-fired power plant. For this, the device according to the invention can have a concentration device, having for example a pressurized tank filled with water, through which smoke gas is taken. Since CO.sub.2 has better solubility as compared to N.sub.2 and O.sub.2, the water can become enriched with CO.sub.2 under pressure. Then, by reducing the pressure, the smoke gas can at first be removed from the concentration device. By a further pressure reduction the CO.sub.2 can then be released from the water and supplied as substrate gas to the nozzle 106 and used, for example, together with the recirculated aqueous medium 116 to form the driving jet. Oxygen residues can be removed chemically or biologically before feeding to the nozzle 106.

[0161] As compared to chemical methods using catalysis, the method according to the invention can also be carried out with gases that are not pure. Steps to purify the gases are done away with. As compared to other methods of biomethanization, defined biomass densities can be established here and reproduced as needed. Furthermore, a good gas supply of the organisms is assured by the internal recirculation of the gas.

Sample Embodiment 1

[0162] Load water in reactor with nutrient salts for freshwater medium per Widdel (1980) as well as permillage trace elements per Immhoff-Stuckle et al. (1983). Heat water in the reactor to around 60-70 C., drive out the atmosphere with N.sub.2. Close reactor. Let water cool down under N.sub.2 atmosphere to around 40 C. and add N.sub.2 up to a pressure of around 0.2 bar. Add a permillage vitamin solution per Balch et al. (1979). Reduce with NaS to <0.2 V. Add active methanogenic bacterial macrocolonies, so-called pellets, from an anaerobic industrial wastewater treatment plant (such as a pulp plant or the food industry) in sufficient concentration (around 1% dry substance). Adjust temperature from 35 to 38 C. and pH to around 7. Start mixing of the reactor. Charge reactor with a defined quantity of substrate gases (H.sub.2/CO.sub.2) per unit of time in a ratio of around 4:1 with a pressure of 0.2 bar. Maintain a pressure in the reactor of 0.2-0.1 bar. Release the resulting gas mixture from the reactor at a pressure of >0.2-0.1 bar.

LITERATURE

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