CN101476132A - Bioelectrochemical hydrogen production plant, method for preparing hydrogen by using the same - Google Patents
Bioelectrochemical hydrogen production plant, method for preparing hydrogen by using the same Download PDFInfo
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- CN101476132A CN101476132A CNA2009100004302A CN200910000430A CN101476132A CN 101476132 A CN101476132 A CN 101476132A CN A2009100004302 A CNA2009100004302 A CN A2009100004302A CN 200910000430 A CN200910000430 A CN 200910000430A CN 101476132 A CN101476132 A CN 101476132A
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Images
Abstract
The invention discloses a bioelectrochemistry hydrogen production unit which includes a reactor, an anode, a cathode, a first gas outlet and an external power source, wherein, the reactor is opened a mouth as the first gas outlet; the anode and the cathode are placed in the reactor; the reactor is installed with reacting liquid for preparing hydrogen; the anode connects with the positive pole of the external power source through lead, the cathode connects with negative pole of the external power source through lead. The bioelectrochemistry hydrogen production unit can reduce cost for preparing hydrogen greatly, increas preparing efficiency. The invention also discloses a method for preparing hydrogenon by using the bioelectrochemistry hydrogen production unit.
Description
Technical field
The present invention relates to hydrogen preparation field, relate in particular to a kind of bioelectrochemistry device for producing hydrogen and utilize described device for producing hydrogen to produce the method for hydrogen.
Background technology
Because fossil energy is exhausted day by day, the substitute energy of seeking cleaning has become the active demand of social development.Hydrogen has been subjected to extensive concern as the most potential new forms of energy.At present, the hydrogen in the whole world about 96% is from fossil oil, and as natural gas hydrogen preparation, water-gas reforming hydrogen manufacturing, solar hydrogen making etc., remaining hydrogen comes from water electrolysis hydrogen producing mostly.
Along with the development of process for making hydrogen, fermentative hydrogen production has also obtained people's attention.With glucose as the biological hydrogen production raw material be example carry out fermentative hydrogen production reaction equation suc as formula shown in (1) and the formula (2):
Through type (1) and formula (2) as can be seen, if having only acetate in the product, 1mol glucose can be produced 4mol hydrogen, if having only butyric acid in the product, 1mol glucose can be produced 2mol hydrogen.Present fermentation technique can make 1mol glucose produce 2～3mol hydrogen.
Because in the fermentative hydrogen production technology, most of organic substance can not thoroughly be converted into hydrogen, slatterns with acetate or butyro-form, makes that the productive rate of fermentative hydrogen production technology is lower.Though can improve productive rate by photosynthesis or pure enzyme in the technology of fermentative hydrogen production, these methods realize that cost is higher, and industrialization is difficult.
Another kind of hydrogen production process---bioelectrochemistry hydrogen producing technology has also been proposed in the prior art, the bioelectrochemistry hydrogen producing technology can not only utilize the raw material (as sewage, glucose etc.) of biological hydrogen production to carry out fermentative hydrogen production, can also further utilize the tunning hydrogen manufacturing behind the fermentative hydrogen production.
Tunning acetate with formula (1) is example, and by reaction equation formula (3) and formula (4), the bioelectrochemistry hydrogen producing technology can further utilize tunning hydrogen manufacturing.
Anode:
Negative electrode:
By reaction equation (1), (3) and (4) as can be seen, with glucose is hydrogen feedstock, utilize in the method for acetic acid type ferment for hydrogen production, 1mol glucose can be produced 2～3mol hydrogen, further, utilizes the bioelectrochemistry hydrogen producing technology, can from 1mol tunning acetate, obtain 3mol hydrogen, the hydrogen manufacturing of then whole process bioelectrochemistry can use 1mol glucose to obtain 8～9mol hydrogen, compares with traditional biological ferment for hydrogen production technology, and productive rate significantly improves.
In the bioelectrochemistry hydrogen producing technology, the microbiological oxidation organic substrates generates carbonic acid gas, proton and electronics near the anode, electronics is transferred to anode by close anode bacterium, is accepted the back by anode and transfers to negative electrode by lead, and proton sees through proton exchange membrane and is diffused into cathode compartment from the anolyte compartment.Cathode reaction chambers is airtight, keeps oxygen-free environment, utilizes external power to strengthen the electromotive force of negative electrode in the microbiological fuel cell circuit, provides the parts of fine bacteria growing required energy on the one hand, provides electronics to negative electrode on the other hand.And directly be used as electron acceptor(EA) at negative electrode at the negative electrode proton, produce hydrogen.
But, proton exchange membrane can be disturbed the smooth transfer of the proton that produces during anolyte compartment's microorganism metabolism, a large amount of protons that the anolyte compartment is produced can't in time be transferred to cathode compartment, make that the pH value is lower in the anolyte compartment, and in cathode compartment, can not in time replenish owing to proton, the pH value is higher in the cathode compartment, has reduced the efficient that produces hydrogen; In addition, because the existence of proton exchange membrane makes that the production cost of bioelectrochemistry hydrogen producing technology is higher, limited its application at hydrogen preparation field.
Summary of the invention
The embodiment of the invention provides a kind of bioelectrochemistry device for producing hydrogen and utilizes described device for producing hydrogen to produce the method for hydrogen, greatly reduces the hydrogen manufacturing cost, has improved hydrogen generation efficiency.
A kind of bioelectrochemistry device for producing hydrogen, described bioelectrochemistry device for producing hydrogen comprises reactor, anode, negative electrode, first pneumatic outlet and external source, wherein:
Described first pneumatic outlet is positioned at reactor top;
Described anode and negative electrode place reactor;
Having only packs in the described reactor of a cavity is used for the reaction solution of hydrogen manufacturing;
Anode links to each other with the positive pole of external source by lead, and negative electrode links to each other with the negative pole of external source by lead.
A kind ofly utilize described bioelectrochemistry device for producing hydrogen to produce the method for hydrogen, said method comprising the steps of:
The reaction solution that will be used for hydrogen manufacturing imports reactor;
Utilize external source between anode and negative electrode, to apply voltage;
Produce electronics and proton around the described anode, described electronics is transferred to negative electrode by lead, and described prototropy is to negative electrode;
Electronics on negative electrode and proton produce hydrogen and derive by first pneumatic outlet.
Bioelectrochemistry device for producing hydrogen and hydrogen production process that the embodiment of the invention provides, cancelled proton exchange membrane, realize that by placing anode and negative electrode in the reactor that communicates at the fast and stable of proton shifts, reduced the Preparation of Hydrogen cost, improved Preparation of Hydrogen efficient.
Description of drawings
Fig. 1 (a) is the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 1 in the embodiment of the invention one;
Fig. 1 (b) is for to utilize bioelectrochemistry device for producing hydrogen 1 to produce the method steps synoptic diagram of hydrogen;
Fig. 2 (a) and Fig. 2 (b) are the longitudinal sectional drawing and the transverse cross-sectional view of bioelectrochemistry device for producing hydrogen 2 in the embodiment of the invention two;
Fig. 3 (a) and Fig. 3 (b) are the longitudinal sectional drawing and the transverse cross-sectional view of bioelectrochemistry device for producing hydrogen 3 in the embodiment of the invention three;
Fig. 4 (a) and Fig. 4 (b) are the stereographic map and the transverse cross-sectional view of bioelectrochemistry device for producing hydrogen 4 in the embodiment of the invention four;
Fig. 5 is the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 5 in the embodiment of the invention five;
Fig. 6 is the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 6 in the embodiment of the invention six;
Fig. 7 (a) and Fig. 7 (b) are the stereographic map and the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 7 in the embodiment of the invention seven;
Fig. 8 (a) and 8 (b) are the stereographic map and the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 8 in the embodiment of the invention eight;
Fig. 9 (a) and Fig. 9 (b) are the stereographic map and the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 9 in the embodiment of the invention nine;
Figure 10 is the structural representation of cathode cavity in the embodiment of the invention ten.
Embodiment
Below in conjunction with Figure of description various embodiments of the present invention are described in detail.
Embodiment one:
Shown in Fig. 1 (a), be the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 1 in the embodiment of the invention one, as can be seen from the figure, this bioelectrochemistry device for producing hydrogen 1 comprises: reactor 11, anode 12, negative electrode 13, pneumatic outlet 14 and external source 15.
The annexation of each several part is in the bioelectrochemistry device for producing hydrogen 1:
Pneumatic outlet 14 is positioned at the top of reactor 11; Anode 12 and negative electrode 13 place reactor 11; Having only packs in the reactor 11 of a cavity is used for the reaction solution of hydrogen manufacturing, and liquid communicates in the reactor; Anode 12 links to each other with the positive pole of external source by lead, and negative electrode 13 links to each other with the negative pole of external source by lead.
In present embodiment one, fully to work in order to make anode and negative electrode, the top that can make the top of anode 12 and negative electrode 13 is all below the reaction solution liquid level.
The anode shape that relates in the embodiment of the invention one and follow-up each embodiment is sheet, trellis, spherical or fan-shaped etc., and anode can be the entity of dense packing, also can be the entity that hollow out is piled up.The anodic electrode materials is carbon felt, carbon paper, carbon cloth or graphite, is electrogenesis electricity bacterium at the catalyzer of plate load.Negative electrode be shaped as sheet, trellis, spherical or fan-shaped etc., similarly, negative electrode can be the entity of dense packing, also can be the entity that hollow out is piled up.The electrode materials of negative electrode is carbon felt, carbon paper, carbon cloth or graphite, is C-Pt, nickel, nanometer MoS at the catalyzer of cathode load
2, raney nickel or Pt and Cu, Ni, Co alloy etc.
The reaction solution that relates in the various embodiments of the present invention is meant the raw material that is used for hydrogen manufacturing, can be the mixing liquid of sewage and bacterium liquid, also can be the mixing liquid of glucose and bacterium liquid, and the present invention also is not limited to other raw materials that is used for hydrogen manufacturing.Can comprise in corrupt Shiva Salmonella, mud bacterium, rhodospirillum, Aeromonas, the clostridium one or more in the described bacterium liquid, described sewage can be meant organic sewage.If reaction solution is the mixing liquid of sewage and bacterium liquid, then the span of the volume ratio of bacterium liquid and sewage is 1:100～60:100.
The voltage of supply scope that the external source that relates in the various embodiments of the present invention can provide is 250mV～1200mV.
In the anode that in various embodiments of the present invention, relates to, each anodic shape and surface-area can be the same or different, similarly, the shape and the surface-area of negative electrode can be the same or different, and the ratio range of the surface-area sum of anodic surface-area sum and negative electrode is 1:5～50:1.
In the scheme of the embodiment of the invention one, can regard the part below reactor 11 liquid levels as two class chambers: anolyte compartment and cathode compartment, place anode 12 in the anolyte compartment, place negative electrode 13 in the cathode compartment.
Utilize bioelectrochemistry device for producing hydrogen 1 is produced hydrogen among the embodiment one method steps synoptic diagram shown in Fig. 1 (b), this method of producing hydrogen may further comprise the steps:
Step 101: the reaction solution that will be used for hydrogen manufacturing places reactor 11.
In the present embodiment, the volume ratio of bacterium liquid and sewage can further be set to 5:100～50:100.
Step 102: external source 15 anode 12 and negative electrode 13 provide power supply.
External source 15 provides the anode portion of energy of bacterial growth on every side can on the one hand anode 12, and the negatron that produces around the anode 12 is transferred to negative electrode 13 by lead, can also provide negatron to negative electrode 13 on the other hand, the negatron that external source 15 provides and all be used to produce hydrogen from the negatron that anode 12 is transferred to negative electrode 13.
Step 103: produce proton and negatron around the anode 12, described negatron is transferred to negative electrode 13 by the lead of external source 15, and described prototropy is to negative electrode 13.
Owing to do not have proton exchange membrane in the bioelectrochemistry device for producing hydrogen 1 in the embodiment of the invention one, in the liquid that communicates, proton can be easily by transferring to negative electrode 13 around the anode 12, and the pH value of reaction solution keeps constant in the reactor 11, and the scope of pH value is 6～8.
Step 104: under the effect of the catalyzer of negative electrode 13, proton and negatron be in conjunction with producing hydrogen, and the hydrogen that produces is derived by pneumatic outlet 14.
Owing in step 103, except producing proton and negatron, also produce by-product gas around the anode 12, therefore, described by-product gas is also derived by pneumatic outlet 14.
Described by-product gas can be CO
2, also can be CH
4, can also be CO
2And CH
4Mixed gas, the embodiment of the invention also is not limited to the by-product gas of other non-hydrogen.
Along with the prolongation of working time, the continuous execution of step 103 and step 104, hydrogen output can be stablized gradually, and the voltage that external source 15 provides is when 500mV～1000mV, and the purity that obtains hydrogen is 80%～92%; Hydrogen-producing speed is 0.4～1.3 cubic metre of (0.4～1.3m of every cubic metre of reactor hydrogen producing every day
3D
-1M
-3), current consumption is every cubic metre of reactor power consumption every day 1.5～2.5 kilowatt-hour (1.5～2.5kWhd
-1M
-3), COD (Chemical Oxygen Demand, chemical oxygen demand (COD)) clearance is 80%～98%.
Anode 12 in the embodiment of the invention one can be different with the number of negative electrode 13, and the position relation is unfixing yet.For example can be that the anodic number is one, the number of negative electrode be a plurality of; Also can be that the anodic number is a plurality of, the number of negative electrode be one, illustrates by embodiment two and embodiment three respectively below.
When the bioelectrochemistry device for producing hydrogen 1 in utilizing the embodiment of the invention one was produced hydrogen, owing to do not use proton exchange membrane, the proton that produces around the anode can be transferred to negative electrode reposefully, kept the pH value in the reactor constant, improved the productive rate of hydrogen; Simultaneously, the reaction solution that uses in the present embodiment can be the mixed solution of sewage and bacterium liquid, therefore, can dispose of sewage continuously, and depleted sewage is well utilized, and has reduced cost of sewage disposal.
Embodiment two:
The embodiment of the invention two also provides a kind of bioelectrochemistry device for producing hydrogen 2, is the special case of bioelectrochemistry device for producing hydrogen 1, shown in Fig. 2 (a) and 2 (b), is respectively the longitudinal sectional drawing and the transverse cross-sectional view of bioelectrochemistry device for producing hydrogen 2.
The parts that parts that bioelectrochemistry device for producing hydrogen 2 comprises and bioelectrochemistry device for producing hydrogen 1 comprise are roughly the same, mainly comprise: reactor 21, anode 22, a plurality of negative electrode 23, pneumatic outlet 24 and an external source 25, in the bioelectrochemistry device for producing hydrogen 2 of the embodiment of the invention two, the container shapes of assumed response device 21 is that volume is the square of 25L, and the number of negative electrode 23 is 4.Bioelectrochemistry device for producing hydrogen 2 in the present embodiment two also is not limited to the negative electrode 23 of other quantity, and it is the square of 25L that the volume of reactor 21 and container shapes also are not limited to.
The positive pole of external source 25 links to each other with anode 22 by lead, and the negative pole of external source 25 links to each other with 4 negative electrodes 23 respectively by lead.Anode 22 closes with the position of negative electrode 23: 4 negative electrodes 23 distribute around the anode 22.The negatron that anode 22 produces is transferred to each negative electrode 23 by lead, and the prototropy that anode 22 produces is to each negative electrode 23, and under the effect of the catalyzer of negative electrode 23, proton and negatron are in conjunction with producing hydrogen.
In the present embodiment, the pneumatic outlet 24 at reactor 21 tops can for one also can be for a plurality of.
In the bioelectrochemistry device for producing hydrogen 2 shown in present embodiment Fig. 2 (a) and 2 (b), 4 negative electrodes 23 are placed on the four sides, all directions of reactor 21, anode 22 is placed on the centre of 4 negative electrodes 23, and present embodiment two also is not limited to other negative electrodes and anodic position relation.
Embodiment three:
Bioelectrochemistry device for producing hydrogen 3 in the embodiment of the invention three is a plurality of anodic situations of negative electrode, also is the special case of bioelectrochemistry device for producing hydrogen 1.Shown in Fig. 3 (a) and 3 (b), be respectively the longitudinal sectional drawing and the transverse cross-sectional view of bioelectrochemistry device for producing hydrogen 3.
Bioelectrochemistry device for producing hydrogen 3 comprises: reactor 31, a plurality of anode 32, negative electrode 33, pneumatic outlet 34 and an external source 35.Because in the bioelectrochemistry device for producing hydrogen 3 of the embodiment of the invention three, the container shapes of reactor 21 is identical with embodiment two, all is the square of 25L, the number of therefore setting anode 32 is 4.Bioelectrochemistry device for producing hydrogen 3 in the present embodiment three also is not limited to the anode 32 of other quantity, and it is the square of 25L that the volume of reactor 31 and container shapes also are not limited to.
The positive pole of external source 35 links to each other with 4 anodes 32 respectively by lead, and the negative pole of external source 35 links to each other by lead negative electrode 33.
4 anodes 32 that distribute around the negative electrode 33, negative electrode 33 respectively with each anode 32 cooperating to produce hydrogen, promptly the negatron that produces of each anode 32 all is transferred to negative electrode 33 by lead, the proton that each anode 32 produces all is transferred to negative electrode 33.
In the present embodiment, the pneumatic outlet 34 at reactor 31 tops can for one also can be for a plurality of.
In the bioelectrochemistry device for producing hydrogen 3 shown in present embodiment Fig. 3 (a) and 3 (b), it is four sides, all directions with 4 anodes, 32 placing response devices 31, negative electrode 33 is placed on the centre of 4 anodes 32, and present embodiment three also is not limited to other negative electrodes and anodic position relation.
For further improving hydrogen generation efficiency, can on the basis of embodiment one, a plurality of bioelectrochemistry device for producing hydrogen 1 be combined, constitute new bioelectrochemistry device for producing hydrogen, a plurality of anodes and a plurality of negative electrode promptly are set in new bioelectrochemistry device for producing hydrogen.Because the array mode difference of bioelectrochemistry device for producing hydrogen 1, new bioelectrochemistry device for producing hydrogen are also different, describe respectively below by embodiment four and embodiment five.
Embodiment four:
Shown in Fig. 4 (a) and Fig. 4 (b), be respectively the stereographic map and the transverse cross-sectional view of bioelectrochemistry device for producing hydrogen 4 in the embodiment of the invention four.
Bioelectrochemistry device for producing hydrogen 4 comprises: reactor 41, a plurality of anode 42, a plurality of negative electrode 43, pneumatic outlet 44 and external source 45, the number of the number of anode 42 and negative electrode 43 can be the same or different.
A plurality of anodes 42 and a plurality of negative electrode 43 all are placed in the reactor 41, and anode 42 and alternately placement of negative electrode 43.The quantity span of anode 42 is 3～100, and the quantity span of negative electrode 43 also can be 3～100.The positive pole of external source 45 links to each other with each anode 42 by lead, and the negative pole of external source 45 links to each other with each negative pole 43 by lead, in the open top of reactor 41 a plurality of pneumatic outlets 44 is set.
The bioelectrochemistry device for producing hydrogen 4 of embodiment four is described below by a concrete example.
Reactor 41 is cylindrical vessels, its cross-sectional diameter is 30cm, and height is 45cm, and the upper limb of anode 42 is lower than the top 2～10cm of reactor 41, the upper limb of negative electrode 43 is lower than the upper limb 2～10cm of anode 42, and the surface-area sum of anode 42 is identical with the surface-area sum of negative electrode 43.
Utilize process that bioelectrochemistry device for producing hydrogen 4 produces hydrogen and to utilize bioelectrochemistry device for producing hydrogen 1 to produce the process of hydrogen similar, only a plurality of anodes 42 and a plurality of negative electrode 43 are worked simultaneously, when the power supply that provides when external source 45 was 400mV～800mV, the purity that obtains hydrogen was 85%～90%; Hydrogen-producing speed is 0.4～1.2m
3D
-1M
-3If initial COD is 2500mgL
-1, the COD clearance is 87.2%.
In the bioelectrochemistry device for producing hydrogen 4 shown in Fig. 4 (a) and Fig. 4 (b), be with anode 42 and negative electrode 43 alternately arrange constitute with the similar circle of reactor 41 be that example is represented, the present invention also is not limited to other arrangement modes, as long as can guarantee that distance between adjacent anode 42 and the negative electrode 43 is less than 10cm.Further, adjacent anode 42 and the distance between the negative electrode 43 are less than 5cm.
Embodiment five:
The scheme of embodiment four is a situation about combining after the inside conducting with a plurality of bioelectrochemistry device for producing hydrogen 1, and the embodiment of the invention five is a plurality of independently bioelectrochemistry device for producing hydrogen 1 to be combined become bioelectrochemistry device for producing hydrogen 5.As shown in Figure 5, be the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 5 in the embodiment of the invention five, in the present embodiment, negative electrode and anodic position relation is to be arranged above and below, can be negative electrode last, anode under Rankine-Hugoniot relations.
Bioelectrochemistry device for producing hydrogen 5 comprises: reactor 51, anode 52, negative electrode 53, pneumatic outlet 54, external source 55, reaction solution inlet 56 and reaction solution outlet 57.
More than one of the quantity of reactor 51 has all been placed an anode 52 and a negative electrode 53 in each reactor 51, external source 55 links to each other by lead with each anode 52 and each negative electrode 53 respectively.After external source 55 pressurization, the gas that produces around anode 52 in reactor 51 and the negative electrode 53 is derived by pneumatic outlet 54, and the reaction solution of this reactor 51 flows to the reaction solutions inlet 56 of next reactor 51 by reaction solution outlet 57 simultaneously.
Bioelectrochemistry device for producing hydrogen 5 can also comprise the liquid treatment parts, before reaction solution enters reactor 51 by reaction solution inlet 56, removes the oxygen in the reaction solution, and makes reaction solution flow into described reactor 51.
The liquid treatment parts can comprise: anaerobism reservoir and peristaltic pump, the anaerobism reservoir is removed oxygen to the logical nitrogen of reaction solution, is made in the reaction solution inflow reactor 51 by the peristaltic pump pressurization then.In addition, a liquid uniform distribution device can be set in the bottom of each reactor 51, make reaction solution equably in the inflow reactor 51, and in reactor 51, evenly flow through.
Liquid treatment parts and liquid uniform distribution device not only can be applied to embodiment five, can also be applied in the other embodiments of the invention.
The bioelectrochemistry device for producing hydrogen 5 of embodiment five is described below by a concrete example.
Suppose that the single reactor 51 in the bioelectrochemistry device for producing hydrogen 5 is cylindrical vessel, its external diameter is 80cm, highly is 120cm.When the power supply that provides when external source 55 was 400mV～800mV, the purity that obtains hydrogen was 85%～90%; Hydrogen-producing speed is 0.4～1.3m
3D
-1M
-3If initial COD is 2500mgL
-1, then the COD clearance is 88%.
The embodiment of the invention four and embodiment five combine a plurality of bioelectrochemistry device for producing hydrogen 1, further, also be not limited to scheme that a plurality of bioelectrochemistry device for producing hydrogen 2 are combined, or the scheme that a plurality of bioelectrochemistry device for producing hydrogen 3 are combined.
To produce the method for hydrogen identical for bioelectrochemistry device for producing hydrogen 1 in utilizing method that the embodiment of the invention two, three, four and the bioelectrochemistry device for producing hydrogen in five produce hydrogen and utilizing embodiment one.
In the scheme of the embodiment of the invention one to embodiment five, the gas that obtains by pneumatic outlet is the mixed gas of hydrogen and by-product gas.In order directly to obtain the higher hydrogen of purity, can in the reactor of bioelectrochemistry device for producing hydrogen, baffle plate be set, the hydrogen that is used for producing on the by-product gas that produces around will anode and the negative electrode is kept apart, simultaneously, at least two pneumatic outlets are set in reactor, a pneumatic outlet is used to derive hydrogen, and another pneumatic outlet is used to derive by-product gas.
Embodiment six:
The bioelectrochemistry device for producing hydrogen 6 that the embodiment of the invention six provides is to increase by one to be used for the isolated baffle plate of hydrogen that produces around the by-product gas that produces around will anode and the negative electrode on the basis of embodiment one, as shown in Figure 6, be the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 6 in the embodiment of the invention six.
Bioelectrochemistry device for producing hydrogen 6 comprises: reactor 61, anode 62, negative electrode 63, baffle plate 64, first pneumatic outlet 65, second pneumatic outlet 66 and external source 67, further, bioelectrochemistry device for producing hydrogen 6 can also comprise the hydrogen collecting device.
The annexation of each several part is in the bioelectrochemistry device for producing hydrogen 6:
Anode 62 and negative electrode 63 place reactor 61, and the top of the top of anode 62 and negative electrode 63 is under the liquid level of reaction solution; Anode 62 is by lead and 67 anodal linking to each other of external source, and negative electrode 63 links to each other by the negative pole of lead with external source 67; Space more than reactor 61 liquid levels is provided with baffle plate 64, and being used for the separated by spaces more than the liquid level in the reactor 61 is two portions, and baffle plate 64 can go deep into the following 0.5cm～4cm of reactor liquid level, and the following liquid level in baffle plate 64 bottoms communicates fully.Further, to be arranged in baffle plate 64 be that anode 62 is positioned under the second section space under the first part space of two portions with the separated by spaces more than the liquid level to negative electrode 63; At first part's top of space opening as first pneumatic outlet 65, at second section top of space opening as second pneumatic outlet 66.Owing to produce hydrogen on the negative electrode, therefore, the gas that the hydrogen collecting device is collected from first pneumatic outlet 66 is exactly the hydrogen that needs.
In the embodiment of the invention six, the sheet that is shaped as of baffle plate 64 can be set, and the placement form is as shown in Figure 6, be vertical placement, vertical is two portions with the separated by spaces of reactor liquid level more than 61.Here " vertically " not exclusively is vertical in the geometry, also comprises tilted-putted at a certain angle situation.
The method of utilizing bioelectrochemistry device for producing hydrogen 6 to produce to utilize bioelectrochemistry device for producing hydrogen 1 to produce hydrogen among the method for hydrogen and the embodiment one is similar, different is, utilize bioelectrochemistry device for producing hydrogen 6 to produce in the process of hydrogen, the hydrogen that produces on the negative electrode 63 is derived by first pneumatic outlet 65, the hydrogen purity that obtains is 90%～96%, and the by-product gas that produces around the anode is derived by second pneumatic outlet 66.And utilizing bioelectrochemistry device for producing hydrogen 1 to produce in the process of hydrogen, the gas of deriving from pneumatic outlet 14 is the mixed gas of hydrogen and by-product gas.
Embodiment seven:
The bioelectrochemistry device for producing hydrogen 7 of the embodiment of the invention seven is the further improvement to the bioelectrochemistry device for producing hydrogen 2 in the embodiment of the invention two, directly obtains the hydrogen that produces by baffle plate is set.Shown in Fig. 7 (a) and Fig. 7 (b), be the stereographic map and the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 7.Bioelectrochemistry device for producing hydrogen 7 comprises: reactor 71, anode 72, negative electrode 73, baffle plate 74, first pneumatic outlet 75, second pneumatic outlet 76 and external source 77.
Zone more than reactor 71 liquid levels is provided with baffle plate 74, baffle plate 64 among the shape of this baffle plate 74 and the embodiment six is incomplete same, baffle plate 74 can be made up of 4 sheet baffle plates, 4 sheet baffle plates join end to end (ring structure), with the region separation more than reactor 71 liquid levels is two parts, wherein: 4 negative electrodes 73 are positioned under the first part space, and anode 72 is positioned under the second section space, and 4 negative electrodes 73 lay respectively at anode 72 around; 4 first pneumatic outlets 75 are positioned at directly over first part's spatial, and second pneumatic outlet 76 is positioned at directly over the second section spatial, and the gas of deriving by first pneumatic outlet 75 is hydrogen.
Embodiment eight:
The bioelectrochemistry device for producing hydrogen 8 of the embodiment of the invention eight is the further improvement to the bioelectrochemistry device for producing hydrogen 3 in the embodiment of the invention three, shown in Fig. 8 (a) and 8 (b), is respectively the stereographic map and the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 8.Bioelectrochemistry device for producing hydrogen 8 comprises: reactor 81, anode 82, negative electrode 83, baffle plate 84, first pneumatic outlet 85, second pneumatic outlet 86 and external source 87.
With embodiment seven similarly, zone more than reactor 81 liquid levels of embodiment eight is provided with baffle plate 84, the shape of this baffle plate 84 is identical with baffle plate 74 among the embodiment seven, baffle plate 84 is two parts with the region separation more than reactor 81 liquid levels, wherein: negative electrode 83 is positioned under the first part space, 4 anodes 82 lay respectively under the second section space, and negative electrode 83 placed around 4 anodes 82; First pneumatic outlet 85 is positioned at directly over first part's spatial, and second pneumatic outlet 86 is positioned at directly over the second section spatial, and the gas of deriving by first pneumatic outlet 86 is hydrogen.
Embodiment nine:
The bioelectrochemistry device for producing hydrogen 9 of the embodiment of the invention nine is the further improvement to the bioelectrochemistry device for producing hydrogen 4 in the embodiment of the invention four, is two portions by baffle plate with the separated by spaces more than the liquid level in the reactor, derives hydrogen and the by-product gas that produces respectively.Shown in Fig. 9 (a) and Fig. 9 (b), be respectively the stereographic map and the longitudinal sectional drawing of bioelectrochemistry device for producing hydrogen 9 in the embodiment of the invention nine.
Bioelectrochemistry device for producing hydrogen 9 comprises: reactor 91, anode 92, negative electrode 93, baffle plate 94, first pneumatic outlet 95, second pneumatic outlet 96, external source 97, reaction solution inlet 98 and reaction solution outlet 99.
Reaction solution inlet 98 and reaction solution outlet 99 lay respectively at the two ends of reactor 91, and the effect of reaction solution inlet 98 is that the effect of reaction solution outlet 99 is to discharge reacted reaction solution as the passage that injects reaction solution to reactor 91.
Baffle plate 94 comprises a plurality of sheet baffle plates, is a plurality of parts with the separated by spaces more than the liquid level in the reactor 91 respectively, places an anode 92 or negative electrode 93 under each part.Under place anode 92 part, one first pneumatic outlet 95 is set directly over it, under place negative electrode 93 part, one second pneumatic outlet 96 is set directly over it, therefore, the gas that second pneumatic outlet 96 is derived is hydrogen, and hydrogen purity is about 93%.
In embodiment two, three, four, seven, eight and nine relation of the position of related anode and negative electrode, the embodiment of the invention ten also proposes a kind of bioelectrochemistry device for producing hydrogen 10, in bioelectrochemistry device for producing hydrogen 10, a slot is set in anode, negative electrode is inserted (being that negative electrode inserts in the anode) in the described slot of anodic, and the top of negative electrode is higher than the anodic top, the positive pole of external source links to each other with anode by lead, and the negative pole of external source links to each other with negative electrode by lead.
In the bioelectrochemistry device for producing hydrogen 10 of embodiment ten, in order to maintain a certain distance between the negative electrode that makes anode and insertion, avoid the distance of anode and negative electrode excessive again (as greater than 10cm), the embodiment of the invention ten has proposed a kind of cathode cavity, as shown in figure 10, this cathode cavity has bottom surface 101, bracing frame 102, and further, this cathode cavity can also comprise baffle plate 103 and pneumatic outlet 104.
Negative electrode is placed on the bottom surface 101 of cathode cavity, the described cathode cavity that will comprise negative electrode then inserts in the anodic slot.Because cathode cavity has bottom surface 101 and bracing frame 102, therefore, anode and negative electrode do not contact, and simultaneously owing to the bigger side of area among Figure 10 is empty, therefore, liquid around the anode and the liquid around the negative electrode can communicate.The hydrogen that produces on negative electrode is owing to there is baffle plate 103 to isolate, and therefore, hydrogen can be derived by pneumatic outlet 104, and the by-product gas that produces around the anode can be derived by other pneumatic outlets that are provided with.
When the bioelectrochemistry device for producing hydrogen that utilizes the embodiment of the invention to provide is produced hydrogen, can reduce hydrogen and produce cost, improve hydrogen and produce efficient; Because the hydrogen and the by-product gas that produce are isolated, can directly obtain the higher hydrogen of purity, and hydrogen output is stable; And,, can when producing hydrogen, dispose of sewage the reduction cost of sewage disposal owing to produce reaction solution that hydrogen uses mixed gas as sewage and bacterium liquid.
Obviously, those skilled in the art can carry out various changes and modification to the present invention and not break away from the spirit and scope of the present invention.Like this, if of the present invention these are revised and modification belongs within the scope of claim of the present invention and equivalent technologies thereof, then the present invention also is intended to comprise these changes and modification interior.
Claims (21)
1, a kind of bioelectrochemistry device for producing hydrogen is characterized in that, described bioelectrochemistry device for producing hydrogen comprises reactor, anode, negative electrode, first pneumatic outlet and external source, wherein:
Described first pneumatic outlet is positioned at the top of reactor;
Described anode and negative electrode place reactor;
Having only packs in the described reactor of a cavity is used for the reaction solution of hydrogen manufacturing;
Anode links to each other with the positive pole of external source by lead, and negative electrode links to each other with the negative pole of external source by lead.
2, bioelectrochemistry device for producing hydrogen as claimed in claim 1 is characterized in that, described bioelectrochemistry device for producing hydrogen also comprises: the baffle plate and second pneumatic outlet;
The hydrogen that described baffle plate is used for producing around the by-product gas that produces around will anode and the negative electrode is isolated;
Described first pneumatic outlet is used to derive the hydrogen that produces on the negative electrode, and described second pneumatic outlet is used to derive the by-product gas that produces around the anode.
3, bioelectrochemistry device for producing hydrogen as claimed in claim 2 is characterized in that,
It is two portions that described baffle plate is used for the separated by spaces more than the reactor liquid level, and baffle plate gos deep into the following 0.5cm～4cm of reactor liquid level, and the following liquid level in baffle plate bottom communicates.
4, bioelectrochemistry device for producing hydrogen as claimed in claim 1 is characterized in that,
The top of described anodic top and negative electrode is below the liquid level of reaction solution.
5, as the arbitrary described bioelectrochemistry device for producing hydrogen of claim 1-4, it is characterized in that,
A plurality of negative electrodes that distribute around the described anode, the positive pole of external source links to each other with anode by lead, and the negative pole of external source links to each other with each negative electrode by lead; Perhaps,
A plurality of anodes that distribute around the described negative electrode, the positive pole of external source links to each other with each anode by lead, and the negative pole of external source links to each other with negative electrode by lead.
6, as the arbitrary described bioelectrochemistry device for producing hydrogen of claim 1-4, it is characterized in that,
Described anodic and negative electrode be a plurality of, and anode and negative electrode alternately place, the positive pole of external source links to each other with each anode by lead, the negative pole of external source links to each other with each negative electrode by lead.
7, as the arbitrary described bioelectrochemistry device for producing hydrogen of claim 1-4, it is characterized in that,
Described anode is provided with a slot, and described negative electrode inserts in the described slot of anodic, and the top of negative electrode is higher than the anodic top; And
The positive pole of described external source links to each other with anode by lead, and the negative pole of external source links to each other with negative electrode by lead.
8, bioelectrochemistry device for producing hydrogen as claimed in claim 7 is characterized in that,
Described negative electrode is arranged in cathode cavity, and the described cathode cavity that comprises negative electrode inserts in the described slot of anodic; Described cathode cavity is used to make negative electrode and anode not to contact, and anode liquid and negative electrode liquid on every side on every side communicates.
9, as claim 1 or 8 described bioelectrochemistry device for producing hydrogen, it is characterized in that,
Described negative electrode and positive interpolar distance are less than 10cm.
10, bioelectrochemistry device for producing hydrogen as claimed in claim 7 is characterized in that,
The scope that described negative electrode top exceeds anode top is 0～6cm.
11, bioelectrochemistry device for producing hydrogen according to claim 1 is characterized in that,
Described reaction solution is the mixing liquid of sewage and bacterium liquid, and perhaps, described reaction solution is the mixing liquid of glucose and bacterium liquid.
12, as bioelectrochemistry device for producing hydrogen as described in the claim 11, it is characterized in that,
Comprise in corrupt Shiva Salmonella, mud bacterium, rhodospirillum, Aeromonas, the clostridium one or more in the described bacterium liquid.
13, as bioelectrochemistry device for producing hydrogen as described in the claim 11, it is characterized in that,
The scope of the volume ratio of bacterium liquid and sewage is 1:100～60:100.
14, bioelectrochemistry device for producing hydrogen as claimed in claim 1 is characterized in that, described bioelectrochemistry device for producing hydrogen also comprises:
The liquid treatment parts are used for removing the oxygen of reaction solution, and reaction solution is fed described reactor.
15, bioelectrochemistry device for producing hydrogen as claimed in claim 1 is characterized in that,
The ratio range of the surface-area sum of anodic surface-area sum and negative electrode is 1:5～50:1.
16, as claim 1,2,3,4,8,10,11,12,13,14 or 15 described bioelectrochemistry device for producing hydrogen, it is characterized in that,
Described anodic is shaped as sheet, trellis, spherical or fan-shaped, and described anode is the entity of dense packing or the entity that hollow out is piled up;
Described negative electrode be shaped as sheet, trellis, spherical or fan-shaped, described negative electrode is the entity of dense packing or the entity that hollow out is piled up.
17, as claim 1,2,3,4,8,10,11,12,13,14 or 15 described bioelectrochemistry device for producing hydrogen, it is characterized in that,
The anodic electrode materials is carbon felt, carbon paper, carbon cloth or graphite, and the catalyzer of plate load is an electrogenesis electricity bacterium;
The electrode materials of negative electrode is carbon felt, carbon paper, carbon cloth or graphite, and the catalyzer of cathode load is C-Pt, nickel, nanometer MoS
2, raney nickel or Pt and Cu, Ni, Co alloy.
18, as claim 1,2,3,4,8,10,11,12,13,14 or 15 described bioelectrochemistry device for producing hydrogen, it is characterized in that,
The voltage of supply scope that described external source provides is 250mV～1200mV.
19, a kind of method of utilizing the described bioelectrochemistry device for producing hydrogen of claim 1 to produce hydrogen is characterized in that, said method comprising the steps of:
The reaction solution that will be used for hydrogen manufacturing imports reactor;
Utilize external source between anode and negative electrode, to apply voltage;
Produce electronics and proton around the described anode, described electronics is transferred to negative electrode by lead, and described prototropy is to negative electrode;
Electronics on negative electrode and proton produce hydrogen and derive by first pneumatic outlet.
20, the method for producing hydrogen as claimed in claim 19 is characterized in that,
When the baffle plate in the bioelectrochemistry device for producing hydrogen was two portions with the separated by spaces more than the reactor liquid level, electronics around the described negative electrode and proton produced hydrogen and derive by first pneumatic outlet;
Also produce by-product gas around the described anode, described by-product gas is derived by second pneumatic outlet.
As claim 19 or the 20 described methods of producing hydrogen, it is characterized in that 21, the reaction solution that will be used for hydrogen manufacturing imports before the reactor, the described method of producing hydrogen is further comprising the steps of:
Described liquid treatment parts are removed the oxygen in the reaction solution, and reaction solution is fed described reactor.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102555817A (en) * | 2012-01-18 | 2012-07-11 | 原国平 | Petroleum substituted new energy vehicle |
| CN103864201A (en) * | 2012-12-18 | 2014-06-18 | 中国科学院生态环境研究中心 | Method for microbial electrolytic preparation of hydrogen by use of source separated urine |
| CN104674297A (en) * | 2015-01-30 | 2015-06-03 | 湘潭大学 | Method for preparing hydrogen evolution electrode of transition metal chalcogenide compound |
| CN113106017A (en) * | 2021-04-30 | 2021-07-13 | 成都理工大学 | Controllable rotating disc electrode reinforced microorganism hydrogen production system |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102555817A (en) * | 2012-01-18 | 2012-07-11 | 原国平 | Petroleum substituted new energy vehicle |
| CN103864201A (en) * | 2012-12-18 | 2014-06-18 | 中国科学院生态环境研究中心 | Method for microbial electrolytic preparation of hydrogen by use of source separated urine |
| CN104674297A (en) * | 2015-01-30 | 2015-06-03 | 湘潭大学 | Method for preparing hydrogen evolution electrode of transition metal chalcogenide compound |
| CN104674297B (en) * | 2015-01-30 | 2017-04-26 | 湘潭大学 | Method for preparing hydrogen evolution electrode of transition metal chalcogenide compound |
| CN113106017A (en) * | 2021-04-30 | 2021-07-13 | 成都理工大学 | Controllable rotating disc electrode reinforced microorganism hydrogen production system |
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