CN102760898B - Linear-carbon fuel cell device with porous ceramic material as support - Google Patents

Linear-carbon fuel cell device with porous ceramic material as support Download PDF

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CN102760898B
CN102760898B CN201210197627.1A CN201210197627A CN102760898B CN 102760898 B CN102760898 B CN 102760898B CN 201210197627 A CN201210197627 A CN 201210197627A CN 102760898 B CN102760898 B CN 102760898B
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anode
carbon fuel
fuel cell
cathode
porous ceramic
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CN102760898A (en
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弭永利
郝文斌
何晓瑾
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Jiangsu Huachang Aluminum Factory Co., Ltd.
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DONGYING JIEDA CHEMICAL TECHNOLOGY CO LTD
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

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Abstract

The invention relates a linear-carbon fuel cell device with a porous ceramic material as a support. The linear-carbon fuel cell device comprises an anode gas outlet pipe, a gas pump, a cathode gas inlet pipe, a cylindrical container, a heat-conducting pad, an anode gas inlet pipe, a cathode gas outlet pipe, a single cell and a heating coil, wherein the single cell sequentially comprises a porous ceramic sheet, a cell cathode, a cathode electrolyte transition layer and an electrolyte layer from the top down, which are stuck and sealed with a carbon fuel bin through high-temperature sealing adhesive; carbon fuel is filled in the single cell and taken as an anode; and the single cell is connected with an external load through a cathode current collector wire and an anode current collector wire. The linear-carbon fuel cell device has the advantages as follows: by adopting a fuel cell structure that the porous ceramic material, instead of the anode, the electrolyte or the cathode as in the prior art, is taken as the support, the mechanical strength of the cell is improved, the electrodes and the electrolyte material are saved, the consumption of the impedance inside the cell is reduced; and according to the novel structure, a large-power linear-carbon fuel cell pile can be researched and developed.

Description

A kind ofly take the straight carbon fuel cell device of porous ceramic film material as supporting
Technical field
The present invention relates to straight carbon consuming cell field, particularly a kind ofly take the straight carbon fuel cell device of porous ceramic film material as supporting.
Background technology
In recent years, owing to take the sustainable growth of the fossil energy prices of raw and semifnished materials that oil is representative, national governments all heightened awareness to the height to fossil energy, to rely on be a kind of non-sustainability strategy, these resources not only will be developed totally, it is as the CO of fuel generation 2more constantly aggravating the greenhouse effect of global climate.For this reason, many countries drop into a large amount of research fundings, study the method that novel regenerative resource or exploitation more efficiently utilize existing energy resources.With regard to the Chinese fundamental realities of the country, coal in China reserves rank third place in the world, it is mainly used in thermal power generation as primary energy.But owing to there is this process of coal burning, not only efficiency is limited to cause this energy utilization patterns, and can produce a large amount of greenhouse gas CO 2.Therefore, people are necessary to study the new way of coal generating.
Straight carbon consuming cell is a kind of electrochemical energy battery.It take carbon as raw material, directly the chemical energy of carbon is converted into electric energy; Rather than apply traditional technique: the burning by carbon is converted into heat energy by its chemical energy, then by steam turbine, heat energy is converted into mechanical energy, and then drive generator generating electric energy.Because do not experience the conversion of heat energy, therefore there is no the constraint of Carnot cycle to the efficiency upper limit.In theory, the generating efficiency of straight carbon consuming cell can reach 100%, and this compares with the efficiency of existing thermal power generation 30% left and right, can be described as revolutionary raising.In addition, because coal is solid, oxidation product is CO 2gas, straight carbon consuming cell be designed with separation and the CO that is beneficial to both 2the recovery of gas, reduces discharging even zero discharge CO thereby reach 2the effect of greenhouse gas.
Since entering the new century, along with solar energy, biomass energy, the novel energies such as wind energy and regenerative resource research popular, fuel cell also enters people's the visual field.Along with going deep into of research, the kind of fuel cell is also increasingly extensive, develops the polytypes such as alkaline fuel cell (AFC), phosphoric acid fuel cell (PAFC), molten carbonate fuel cell (MCFC), Proton Exchange Membrane Fuel Cells (PEMFC), Solid Oxide Fuel Cell (SOFC), direct methanol fuel cell (DMFC).These fuel cells are fuel mainly with gas and liquid, utilize solid carbon to compare for fuel with straight carbon consuming cell, and in the storage of fuel with carry and all has larger inferior position, therefore directly carbon consuming cell becomes the focus of fuel cell studies.
Straight carbon consuming cell is mainly divided into and has two kinds of plate and tubular types by structure.In order to reach the object of continuous operation, within carbon fuel is placed in to cell panel top or battery socket, make its because of Action of Gravity Field all the time with galvanic anode close contact, realize carbon fuel and be converted into CO 2electrochemical reaction is carried out continuously.This just makes anode, among these three layers, electrolyte and negative electrode, has more thick and heavy processed in order to support of one deck at least.The existing plate or straight carbon consuming cell of tubular type is all to make by electrode layer or dielectric substrate the structure supporting.
On the other hand, for the consideration that reduces internal resistance consumption and save electrode material, the thickness of electrode and dielectric substrate is but the more Bao Yuehao of processing.This just has higher requirement to electrode and the electrolytical strength of materials and structural design.If do not solved, will hinder the development of straight carbon consuming cell technology.Therefore, guaranteeing, under the prerequisite of battery machine intensity, how to be made to obtain the frivolous large technical barrier that becomes straight carbon consuming cell of structure.
Summary of the invention
Object of the present invention is exactly in view of the foregoing defects the prior art has, and a kind of straight carbon fuel cell device of porous ceramic film material as supporting of take is provided.
Its technical scheme is: mainly anode escape pipe, air pump, cathode inlet conduit, cylindrical pressure vessel, heat-conducting pad, anode air inlet pipe, negative electrode outtake tube, seal washer, battery cell, heating collar, consist of, the top of described cylindrical pressure vessel is provided with lid, outside is provided with heating collar parcel, cylindrical pressure vessel inner bottom part has heat-conducting pad, battery cell is placed on it, reserve the runner that cathode gas flows through, the duct that negative electrode gas is seen through on pottery contacts with negative electrode, by seal washer, cylindrical pressure vessel is separated into cathodic region and anode region; Cylindrical pressure vessel bottom is cathodic region, by air pump, through cathode inlet conduit, negative electrode conductance is entered, and cathode exhaust gas is derived by negative electrode outtake tube; On cylindrical pressure vessel top, be anode region, anode carrier gas imports through anode air inlet pipe, by anode escape pipe, is derived;
Above-mentioned battery cell is followed successively by porous ceramics piece from top to bottom, cell cathode, catholyte transition zone, dielectric substrate, with high-temperature seal adhesive and carbon Bunker adhesion sealing, pack carbon fuel within it into, be anode, each parts formation battery cell of combining closely, is connected external loading by cathode collector wire with anode current collector wire.
Above-mentioned battery cell can be four layers to six layers structure: wherein, four-layer structure refers to it is porous ceramics piece from top to bottom successively, negative electrode, negative electrode-electrolyte transition zone and dielectric substrate; Five-layer structure is on four layers of basis, adds one deck fused mass or liquid anode on electrolyte again; Six layers of structure are on five-layer structure basis, in the middle of anode and electrolyte, add anode-electrolyte transition zone.
Above-mentioned porous ceramics piece is by being aluminium oxide, zirconia, and magnesium oxide etc. or wherein a kind of, two kinds or two or more porcelain powder sinterings form; Its pore size is 1mm to 10nm, and the porous ceramics piece of its application can be plate, can be also tubular type, comprises two types of both ends open and ports.
Above-mentioned dielectric substrate is by transition metal oxide, the composite electrolyte that rare earth oxide and carbonate are mixed and processed, concrete the is cerium oxide that samarium oxide mixes, zirconia and the aluminium oxide Al 2O3 of scandia stabilized, lithium carbonate Li2CO3, potash K2CO3, sodium carbonate Na2CO3 two kinds or the two or more compound electrolyte material of pressing certain mass formation than mixing wherein.
Above-mentioned carbon Bunker is earthenware, and described heat-conducting pad is potsherd, and described seal washer is alumina fibre plate, and described cylindrical pressure vessel is stainless steel still, and described heating collar is ceramic heat circle.
Above-mentioned carbon fuel is amorphous carbon, carbon black, coal, coke or other fuel containing carbon rich.
Above-mentioned anode gas is nitrogen, and described negative electrode gas is air, oxygen or both gaseous mixtures.
The invention has the beneficial effects as follows: this straight carbon consuming cell monomer be take porous ceramic sheet material as support, but not existing with anode, electrolyte or the negative electrode fuel cell structure for supporting, when improving battery machine intensity, save electrode and electrolyte, and reduced the consumption of internal battery impedance.Meanwhile, can carry out according to this new construction the research and development of high-power straight carbon fuel cell stack.
Accompanying drawing explanation
Fig. 1 is structural representation of the present invention;
Fig. 2 is the structural representation of battery cell of the present invention;
In upper figure: cathode collector wire 1, carbon fuel 2, dielectric substrate 3, cell cathode 4, anode current collector wire 5, carbon Bunker 6, catholyte transition zone 7, porous ceramics piece 8; Anode escape pipe 9, air pump 10, cathode inlet conduit 11, cylindrical pressure vessel 12, heat-conducting pad 13, anode air inlet pipe 14, negative electrode outtake tube 15, seal washer 16, battery cell 17, heating collar 18.
Embodiment
The present invention mentions, and to take porous ceramic film material be that the straight carbon fuel cell device that supports is mainly by anode escape pipe 9, air pump 10, cathode inlet conduit 11, cylindrical pressure vessel 12, heat-conducting pad 13, anode air inlet pipe 14, negative electrode outtake tube 15, seal washer 16, battery cell 17, heating collar 18 forms, the top of described cylindrical pressure vessel 12 is provided with lid, outside is provided with heating collar 18 parcels, cylindrical pressure vessel 12 inner bottom parts have heat-conducting pad 13, battery cell 17 is placed on it, reserve the runner that cathode gas flows through, the duct that negative electrode gas is seen through on pottery contacts with negative electrode, by seal washer 16, cylindrical pressure vessel 12 is separated into cathodic region and anode region, cylindrical pressure vessel 12 bottoms are cathodic region, by air pump 10, through cathode inlet conduit 11, negative electrode conductance are entered, and cathode exhaust gas is derived by negative electrode outtake tube 15, on cylindrical pressure vessel 12 tops, be anode region, anode carrier gas imports through anode air inlet pipe 14, by anode escape pipe 9, is derived.
Wherein, battery cell 17 is followed successively by porous ceramics piece 8 from top to bottom, cell cathode 4, catholyte transition zone 7, dielectric substrate 3, with high-temperature seal adhesive and the 6 adhesion sealings of carbon Bunker, pack carbon fuel 2 within it into, for anode, each parts formation battery cell of combining closely, is connected external loading by cathode collector wire 1 with anode current collector wire 5.
It should be noted that: battery cell 17 can be four layers to six layers structure: wherein, four-layer structure refers to it is porous ceramics piece from top to bottom successively, negative electrode, negative electrode-electrolyte transition zone and dielectric substrate; Five-layer structure is on four layers of basis, adds one deck fused mass or liquid anode on electrolyte again; Six layers of structure are on five-layer structure basis, in the middle of anode and electrolyte, add anode-electrolyte transition zone.
Wherein, porous ceramics piece 8 is by being aluminium oxide, zirconia, and magnesium oxide etc. or wherein a kind of, two kinds or two or more porcelain powder sinterings form, and proportioning is well known to those skilled in the art; Its pore size is 1mm to 10nm, and the porous ceramics piece of its application can be plate, can be also tubular type, comprises two types of both ends open and ports.
Above-mentioned dielectric substrate 3 is by transition metal oxide, the composite electrolyte that rare earth oxide and carbonate are mixed and processed, concrete the is cerium oxide that samarium oxide mixes, zirconia and the aluminium oxide Al 2O3 of scandia stabilized, lithium carbonate Li2CO3, potash K2CO3, sodium carbonate Na2CO3 two kinds or the two or more compound electrolyte material that certain mass forms than mixing, the prior art that this mass ratio is well known to those skilled in the art of pressing wherein.
Above-mentioned carbon Bunker 6 is earthenware, and described heat-conducting pad 13 is potsherd, and described seal washer 16 is alumina fibre plate, and described cylindrical pressure vessel 12 is stainless steel still, and described heating collar 18 is ceramic heat circle.
Above-mentioned carbon fuel 2 is amorphous carbon, carbon black, coal, coke or other fuel containing carbon rich, above-mentioned anode gas is nitrogen, described negative electrode gas is air, and oxygen or both gaseous mixtures above-mentioned be take the straight carbon fuel cell device of porous ceramic film material as supporting, its operating temperature range is 500 to 1000 ℃, above-mentioned straight carbon fuel cell device can be according to actual conditions, and the supply of carbon fuel can adopt intermittent feeding working method, can attempt continuous feed mode and transform.
Adopt plate and design tubular type type, different from traditional plate shaped battery, at anode, electrolyte, on the basis of negative electrode three layer function material structures, added one deck porous ceramic plate as backing material, make that plate shaped battery needn't to take certain one deck be the structure (as anode-supported, electrolyte-supported) supporting making because of the consideration of mechanical strength, saved electrode material, more reduce the internal resistance of battery, thereby reduced the in-fighting of battery.Utilize its intensity significantly improving, can carry out the trial of high power battery heap exploitation.
The example of the technology of the present invention generating is as follows:
Embodiment 1
Using carbon black as carbon fuel, and 10:3 adds glass putty and carbon fuel, good seal cell apparatus to take in the fuel cavity that porous ceramic is the straight carbon consuming cell monomer that supports successively in mass ratio.At normal temperatures, anode passes into nitrogen, gets rid of the air in anode cavities.Heater, while being warmed up to 500 ℃, passes into air to cathode cavity, and air pressure is 0.5Mpa, records battery operating mode, now enumerates the battery performance situation at 600 ℃, sees attached list one.
Embodiment 2
Using carbon black as carbon fuel, and 20:3 adds glass putty and carbon fuel, good seal cell apparatus to take in the fuel cavity that porous ceramic is the straight carbon consuming cell monomer that supports successively in mass ratio.At normal temperatures, anode passes into nitrogen, gets rid of the air in anode cavities.Heater, while being warmed up to 500 ℃, passes into air to cathode cavity, and air pressure is 0.5Mpa, records battery operating mode, now enumerates the battery performance situation at 700 ℃, sees attached list one.
Embodiment 3
Using carbon black as carbon fuel, and 5:2 adds glass putty and carbon fuel, good seal cell apparatus to take in the fuel cavity that porous ceramic is the straight carbon consuming cell monomer that supports successively in mass ratio.At normal temperatures, anode passes into nitrogen, gets rid of the air in anode cavities.Heater, while being warmed up to 500 ℃, passes into air to cathode cavity, and air pressure is 0.5Mpa, records battery operating mode, now enumerates the battery performance situation at 750 ℃, sees attached list one.
Embodiment 4
Using carbon black as carbon fuel, and 20:3 adds glass putty and carbon fuel, good seal cell apparatus to take in the fuel cavity that porous ceramic is the straight carbon consuming cell monomer that supports successively in mass ratio.At normal temperatures, anode passes into nitrogen, gets rid of the air in anode cavities.Heater, while being warmed up to 500 ℃, flow passes into air to cathode cavity, and air pressure is 0.5Mpa, records battery operating mode, now enumerates the battery performance situation at 800 ℃, sees attached list one.
Embodiment 5
Using carbon black as carbon fuel, and 10:1 adds glass putty and carbon fuel, good seal cell apparatus to take in the fuel cavity that porous ceramic is the straight carbon consuming cell monomer that supports successively in mass ratio.At normal temperatures, anode passes into nitrogen, gets rid of the air in anode cavities.Heater, while being warmed up to 500 ℃, passes into air to cathode cavity, and air pressure is 0.5Mpa, records battery operating mode, now enumerates the battery performance situation at 850 ℃, sees attached list one.
Subordinate list one is as follows:
Embodiment Tin: carbon (mass ratio) Temperature Maximum current density Maximum power density Average power density
1 10:3 600 4.44mA/cm 2 2.57mW/cm 2 2.32mW/cm 2
2 20:3 700 4.01mA/cm 2 3.64mW/cm 2 3.08mW/cm 2
3 5:2 750 8.45mA/cm 2 10.00mW/cm 2 8.31mW/cm 2
4 20:3 800 9.93mA/cm 2 12.53mW/cm 2 11.43mW/cm 2
5 10:1 850 54.33mA/cm 2 42.79mW/cm 2 34.12mW/cm 2

Claims (8)

1. take the straight carbon fuel cell device of porous ceramic film material as supporting for one kind, it is characterized in that: mainly by anode escape pipe (9), air pump (10), cathode inlet conduit (11), cylindrical pressure vessel (12), heat-conducting pad (13), anode air inlet pipe (14), negative electrode outtake tube (15), seal washer (16), battery cell (17), heating collar (18) forms, the top of described cylindrical pressure vessel (12) is provided with lid, outside is provided with heating collar (18) parcel, cylindrical pressure vessel (12) inner bottom part has heat-conducting pad (13), battery cell (17) is placed on it, reserve the runner that cathode gas flows through, the duct that negative electrode gas is seen through on pottery contacts with negative electrode, by seal washer (16), cylindrical pressure vessel (12) is separated into cathodic region and anode region, cylindrical pressure vessel (12) bottom is cathodic region, by air pump (10), through cathode inlet conduit (11), negative electrode conductance is entered, and cathode exhaust gas is derived by negative electrode outtake tube (15), on cylindrical pressure vessel (12) top, be anode region, anode carrier gas imports through anode air inlet pipe (14), by anode escape pipe (9), is derived,
Described battery cell (17) is followed successively by porous ceramics piece (8) from top to bottom, cell cathode (4), catholyte transition zone (7), dielectric substrate (3), with high-temperature seal adhesive, by dielectric substrate (3) and carbon Bunker (6) adhesion sealing, packing glass putty and carbon fuel (2) within it into, is anode, each parts formation battery cell of combining closely, is connected external loading by cathode collector wire (1) with anode current collector wire (5).
2. according to claim 1ly take the straight carbon fuel cell device of porous ceramic film material as supporting, it is characterized in that: described battery cell (17) can be four layers to six layers structure: wherein, four-layer structure refers to it is porous ceramics piece from top to bottom successively, negative electrode, negative electrode-electrolyte transition zone and dielectric substrate; Five-layer structure is on four layers of basis, adds one deck fused mass or liquid anode on electrolyte again; Six layers of structure are on five-layer structure basis, in the middle of anode and electrolyte, add anode-electrolyte transition zone.
3. according to claim 1ly take the straight carbon fuel cell device of porous ceramic film material as supporting, it is characterized in that: described porous ceramics piece (8) is by aluminium oxide, zirconia, magnesium oxide or wherein a kind of, two kinds or two or more porcelain powder sinterings form; Its pore size is 1mm to 10nm.
4. according to claim 1ly take the straight carbon fuel cell device that porous ceramic film material be to support, it is characterized in that: described dielectric substrate (3) is by transition metal oxide, the composite electrolyte that rare earth oxide and carbonate are mixed and processed.
5. according to claim 1ly take the straight carbon fuel cell device of porous ceramic film material as supporting, it is characterized in that: described carbon Bunker (6) is earthenware, described heat-conducting pad (13) is potsherd, described seal washer (16) is alumina fibre plate, described cylindrical pressure vessel (12) is stainless steel still, and described heating collar (18) is ceramic heat circle.
6. according to claim 1ly take the straight carbon fuel cell device that porous ceramic film material be to support, it is characterized in that: described carbon fuel (2) be carbon black, coal, coke or other contain the fuel of carbon rich.
7. according to claim 1ly take the straight carbon fuel cell device that porous ceramic film material be to support, it is characterized in that: described anode gas is nitrogen.
8. according to claim 1ly take the straight carbon fuel cell device that porous ceramic film material be to support, it is characterized in that: described negative electrode gas is air or oxygen.
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Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101800326A (en) * 2010-04-17 2010-08-11 上海交通大学 Two-electrolyte direct carbon fuel cell and assembling method thereof

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US7438987B2 (en) * 2003-05-15 2008-10-21 Lawrence Livermore National Security, Llc Carbon fuel particles used in direct carbon conversion fuel cells

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101800326A (en) * 2010-04-17 2010-08-11 上海交通大学 Two-electrolyte direct carbon fuel cell and assembling method thereof

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