CN110429311A - A kind of anode chamber greatly improving MC-DCFC power density, method and battery - Google Patents
A kind of anode chamber greatly improving MC-DCFC power density, method and battery Download PDFInfo
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- CN110429311A CN110429311A CN201910641497.8A CN201910641497A CN110429311A CN 110429311 A CN110429311 A CN 110429311A CN 201910641497 A CN201910641497 A CN 201910641497A CN 110429311 A CN110429311 A CN 110429311A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/14—Fuel cells with fused electrolytes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/14—Fuel cells with fused electrolytes
- H01M8/143—Fuel cells with fused electrolytes with liquid, solid or electrolyte-charged reactants
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/14—Fuel cells with fused electrolytes
- H01M2008/147—Fuel cells with molten carbonates
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Abstract
The invention discloses a kind of anode chamber for greatly improving MC-DCFC power density, method and batteries, belong to the field MC-DCFC.Electrode assembly in the anode chamber can freely pick and place in heat-resisting hard tube, including pick and place stick, lower limit plate, high-temperature insulation conducting wire and current-collector；Lower limit plate, which is fixed on, picks and places stick lower end, and the periphery of lower limit plate and heat-resisting hard tube inner wall clearance fit；Current-collector, which is located at, to be picked and placed below stick；High-temperature insulation conducting wire one end connects current-collector, and the other end passes through the through-hole on lower limit plate to connect external equipment when in use；Lower limit plate and heat-resisting hard tube lower end surround the space for holding fuel powder, and current-collector is located in the space；Heat-resisting hard tube lower end offers recirculation hole, flows into heat-resisting hard tube for fused carbonate when in use and mixes with fuel powder.The present invention can guarantee that coal/carbon dust fuel and fused electrolyte come into full contact with, and improves reaction rate, greatly improves MC-DCFC power density.
Description
Technical field
The invention belongs to MC-DCFC (Molten Carbonate direct coal/carbon fuel cell, meltings
Direct coal/the carbon consuming cell of carbonate) field, it is related to a kind of anode chamber for greatly improving MC-DCFC power density, method and electricity
Pond, more particularly, to it is a kind of greatly improve the direct coal of fused carbonate/carbon consuming cell power density anode chamber design and
Method.
Background technique
Coal will not change within quite long period in the leading position in China's energy.Traditional coal-burning power plant's generating efficiency
Only 30-45%, and discharged a large amount of greenhouse gases and pollutant such as SO2, NOx, particulate matter etc..And directly coal/carbon fuel is electric
Coal/carbon chemical energy is converted into electric energy by pond (direct coal/carbon fuel cell, DCFC), and energy turns
Change improved efficiency by about one time, greatly reduces the discharge of energy loss and pollutant；And the very high CO of purity can be obtained2, convenient for storage
It deposits and utilizes.
Currently, the patent in relation to MC-DCFC is not that very much, domestic existing related patents are concentrated mainly on following a few sides
Face:
(1) with the MC-DCFC: Chinese patent CN201010207016.1 of reformer unit, in the patent, author is not straight
It connects with carbon fuel-feed, but gaseous fuel is translated by reformer unit；It is to close there are also some patents in reformer unit
In reforming catalyst, such as Chinese patent CN201780027891.1, Chinese patent CN201010206914.5.
(2) carbon fuel-feed mode aspect and carbon fuel processing method: Chinese patent CN201110257666.1, China
Patent CN201010287471.7, Chinese patent CN200810209833.3.
(3) in terms of electrolyte/electrolyte, there is following patent: Chinese patent CN201110304175.8.
(4) patent in terms of electrode material has: Chinese patent CN201510583169.9, Chinese patent
CN200610015494.6, Chinese patent CN100392894C.
(5) the domestic patent in terms of pile research has: Chinese patent CN203800125U, Chinese patent
CN202308175U。
Foreign countries are concentrated mainly on following aspect to the patent of MC-DCFC:
(1) there is the MC-DCFC of reformer unit, patent has: United States Patent (USP) US5348814A and US5100743A.
(2) pretreatment of the carbon fuel before charging, patent have: United States Patent (USP) US7981563B2.
(3) patent in terms of electrolyte has: United States Patent (USP) US6037076A.
(4) it is related to anode form, anode (such as resistant to sulfur) and anode material with some specific functions about the patent of anode
Material, patent are as follows: United States Patent (USP) US20060234098A1, United States Patent (USP) US4925745A, British patent GB2039131A and beauty
The special US5206095A of state.
It is (5) external that there are also patents in terms of pile, such as: Korean Patent KR101713344B1.
(6) in addition, there are also some patents associated with the types of fuel cells and other equipment: Japan Patent
JPH11312527A, United States Patent (USP) US9502728B1.
Although having done many electric performance tests using various carbon fuel in their MC-DCFC there are many scholar,
But the power density that they obtain is mostly relatively low, and above-mentioned document MPD usually under 600 DEG C~800 DEG C of reaction temperature is (maximum
Power density) there was only 17mW cm-2~141mW cm-2, as shown in table 1:
The performance of the MC-DCFC of the domestic and international different fuel of table 1
Note: fused carbonate, MC；Maximum power density, MPD；Open circuit potential, OCV.
Lower power density limits the development and commercialized running of MC-DCFC technology, therefore improves MC- as much as possible
The power density of DCFC is of great significance.
Summary of the invention
Aiming at the above defects or improvement requirements of the prior art, the present invention provides a kind of raising fused carbonate is direct
Coal/carbon consuming cell power density anode chamber enables carbon dust fuel it is intended that by the improvement of anode cell configuration
It is enough sufficiently to submerge in fused carbonate electrolyte, guarantee the carbon slurry of predetermined concentration, to come into full contact with and react, thus solves existing
There is in technology carbon dust fuel be easy to swim in above fused electrolyte and lead to carbon dust fuel and electrolyte insufficient contact, Yi Beikong
The technical issues of gas oxidation, reaction rate reduce.
To achieve the goals above, according to one aspect of the present invention, providing one kind, to greatly improve MC-DCFC power close
The anode chamber of degree, comprising: heat-resisting hard tube and electrode assembly；
Electrode assembly can freely pick and place in heat-resisting hard tube, including pick and place stick, lower limit plate, high-temperature insulation conducting wire with
And current-collector；Lower limit plate, which is fixed on, picks and places stick lower end, and the periphery of lower limit plate and heat-resisting hard tube inner wall clearance fit；
Current-collector, which is located at, to be picked and placed below stick；High-temperature insulation conducting wire one end connects current-collector, and the other end passes through lower limit
Through-hole on plate to connect external equipment when in use；
Lower limit plate and heat-resisting hard tube lower end surround the space for holding fuel powder, and current-collector is located at the space
It is interior；
Heat-resisting hard tube lower end offers recirculation hole, with when in use for fused carbonate flow into heat-resisting hard tube and with fuel powder
End mixing.
Further, heat-resisting hard tube material is stainless steel or corundum.
Further, the material for picking and placing stick is stainless steel or corundum.
Further, picking and placing stick and the material of lower limit plate is stainless steel, and is welded and fixed.
It further, further include top limit plate, the material of top limit plate is stainless steel, is located above lower limit plate
And it is welded and fixed with stick is picked and placed, the periphery of top limit plate and heat-resisting hard tube inner wall clearance fit；High-temperature insulation conducting wire is another
Hold the through-hole on the limit plate of top to connect external equipment when in use.
Further, current-collector is corrosion-and high-temp-resistant sheet metal.
It further, further include the fixing piece that electrode assembly is fixed on to specified location in heat-resisting hard tube.
In view of the above-mentioned drawbacks in the prior art, another object of the present invention is to provide one kind to greatly improve melting carbon
The direct coal of hydrochlorate/carbon consuming cell power density method, this method are based on above-mentioned anode chamber, strengthen coal/carbon fuel and electrolysis
The contact of matter, meanwhile, carbon fuel electric conductivity is improved by addition conductive carbon black and improves cell power density, to enhance sun
Pole electroxidation performance improves the overall performance of MC-DCFC, and then improves power density, promotes development and the quotient of MC-DCFC technology
The realization of industry.
To achieve the goals above, according to one aspect of the present invention, providing one kind, to greatly improve MC-DCFC power close
The method of degree, which is characterized in that the carbon dust fuel of partial size 0.08mm-0.25mm is added to any foregoing anode chamber, so
Carbon dust fuel is pressed into fused electrolyte by the anode chamber afterwards；Contain conductive black, conductive black matter in the carbon dust fuel
Amount accounts for the 10%~50% of carbon dust fuel gross mass.
The present invention also provides the MC-DCFC obtained based on the above method.
In general, the above technical scheme conceived by the present invention compared with prior art, can obtain following beneficial to effect
Fruit:
1) the configuration of the present invention is simple implements easily and effectively, is able to solve carbon dust fuel and fused carbonate electrolyte
The problem of coming into full contact with and improving reaction rate, while also assuring carbon dust fuel not oxidation by air, reduce waste of fuel；By
It prevents carbon dust fuel from floating in lower limit plate, forces carbon dust fuel to be sufficiently mixed with fused carbonate electrolyte, additionally it is possible to make
The concentration of anode chamber's carbon dust fuel keeps stable within a certain period of time；The electric conductivity of carbon dust fuel can be improved；Finally, it substantially mentions
The power density of the high direct coal/carbon consuming cell of fused carbonate.
2) anode chamber of stainless steel material, replacement carbon dust fuel ratio alundum tube will be more convenient, and improve testing efficiency, simultaneously also
Recoverable anode chamber, and greatly reduce the waste of fused electrolyte and carbon dust.
3) lower limit plate and heat-resisting hard tube inner wall clearance fit convenient for picking and placing, and can force pick-and-place stick lower end to be located at
Radial designated position in heat-resisting hard tube；Two structures are both designed as stainless steel material, are not only welded and fixed conveniently, prior
It is to be easy to steady operation under the high temperature conditions.
4) top, the cooperation of lower limit plate can prevent from picking and placing stick inclination, lower space volume avoided to change.
5) method of the invention constructs a kind of new structural anode chamber, can be on the basis of existing MC-DCFC battery
On, under conditions of not changing existing electrolyte Li/K carbonate molar ratio, Supplying gas condition and running temperature, by adding to anode chamber
Enter appropriate partial size, the coal of proper proportion and charcoal fuel combination, it is ensured that the fuel in electrolyte maintains certain concentration, both improves
The electrical conductance of electrolytic cell, ensure that coal/carbon dust fuel and fused electrolyte come into full contact with, improve reaction rate, while also keeping away
Coal/charcoal fuel pyrolysis evaporation escape and air oxidation are exempted from, several times promote the power density of MC-DCFC battery, should to realize
The commercialization of technology provides a kind of new technological approaches.And it may be constructed melting using the series and parallel structure of this monocell
The direct coal of carbonate/carbon fuel pile system, to realize required battery capacity.
Detailed description of the invention
Fig. 1 is the direct coal of fused carbonate/carbon consuming cell schematic diagram of the preferred embodiment of the present invention；
Fig. 2 is the anode cell configuration enlarged diagram in Fig. 1；
Fig. 3 is the direct coal of fused carbonate in the prior art/carbon consuming cell schematic diagram；
Fig. 4 is the anode cell configuration enlarged diagram in Fig. 3；
Fig. 5, Fig. 6 are that the power density for each carbon fuel that the anode chamber in Fig. 4, Fig. 2 measures under identical operating condition is bent respectively
Line.
In all the appended drawings, identical appended drawing reference is used to denote the same element or structure, in which:
1,1'- heating furnace, 2,2'- thermocouple, 3,3'-O2/CO2(1/2) gaseous mixture, 4,4'- electrochemical workstation, 5,5'-
Ar gas import, 6,6'-316 stainless steel tube, 7,7'- alundum tube I, 8,8'- gold thread, 9,9'- fused carbonate, 10,10'- fuel
Powder, 11,11'- corundum piece, 12,12'- gold plaque, 13,13'- cell body, 14,14'- alundum tube II, 15- lower limit plate,
16- high-temperature insulation conducting wire, 17,17'- current-collector, 18- recirculation hole, 19, the heat-resisting hard tube of 16'-, 20,18'- pick and place stick, on 21-
Portion's limit plate, 15'- stainless (steel) wire.
Specific embodiment
In order to make the objectives, technical solutions, and advantages of the present invention clearer, with reference to the accompanying drawings and embodiments, right
The present invention is further elaborated.It should be appreciated that the specific embodiments described herein are merely illustrative of the present invention, and
It is not used in the restriction present invention.As long as in addition, technical characteristic involved in the various embodiments of the present invention described below
Not constituting a conflict with each other can be combined with each other.
Fig. 1, Fig. 2 are the direct coal/carbon consuming cell of the fused carbonate of the preferred embodiment of the present invention and its anode cell configuration
Schematic diagram, battery specifically include that heating furnace 1, cell body 13, anode chamber 6.The structure of anode chamber 6 with lower component mainly by being constituted:
316 stainless steel tubes 6, bottom are provided with aperture 18, and gold plaque current-collector 17 is connected with refractory surfaces insulated conductor 16, and conducting wire passes through sun
The aperture 15 of pole room upper surface leads to top, is connected with electrochemical workstation 4, fuel powder 10 (the present embodiment is referred to as carbon dust)
It is uniformly distributed in the anode compartment.
A certain amount of two end number mixing carbonate powder is prepared, is added in cell body 13.By three electrode gold plaques 12, gold plaque 17
(current-collector 17 of the present embodiment is gold plaque, is also possible to other corrosion-and high-temp-resistant metals such as platinum) and the nitric acid treatment of spun gold 8,
It cleans, drying, it is right on battery then will to be inserted into respectively to the reference electrode in the electrode and alundum tube I 7 in alundum tube II 14
Position is answered, heating furnace 1 is started, temperature is detected by thermocouple 2.When heating, Ar gas is passed through from Ar gas import 5；Simultaneously respectively to yin
Pole air inlet 3 is passed through CO2.When furnace when target temperature is stablized, O is passed through to cathode inlet mouth 32/CO2Gaseous mixture.It will
Carbon dust 10 and a small amount of carbonate form carbon slurry after mixing, are added to anode chamber 6, are allowed to by the corundum piece 11 of battery bottom
Separate with metal wall surface, with their electrical property of the test of electrochemical workstation 4 under identical operating condition.
Below by taking five quasi-representative carbon dust fuel as an example, the direct coal/carbon consuming cell of the fused carbonate and its new knot are utilized
Structure anode chamber test result is as follows:
(1) it is respectively graphite, conductive carbon black, bamboo based activated carbon, Huangshi bituminous coal coke that five quasi-representative carbon dust fuel are selected in experiment
With Huangshi bituminous coal, particle size 0.08-0.25mm.Bamboo matrix activated carbon and bituminous coal coke are the heat by carbonization and bituminous coal to bamboo
It solves and prepares；Graphite powder and conductive carbon black are commercially available.The Industrial Analysis and elemental analysis of five kinds of carbon fuel are shown in Table 2,
Microstructure attributes are shown in Table 3.
(2) carbon dust fuel electric performance test is tested: preparing 664.42g proportion is 62mol%Li2CO3- 38mol%K2CO3
Two end number mixing carbonate is added in cell body.Nitric acid 30s is impregnated into the gold part of three electrodes, is cleaned with distilled water, drying,
It will be inserted into respectively corresponding position on battery to electrode and reference electrode, start heating furnace.Stove temperature-rise period is: room temperature~350
DEG C, 5 DEG C of min-1；350-600 DEG C, 10 DEG C of min-1.When heating, it is passed through Ar gas (50mL min-1, mark condition), the sky in battery is discharged
Gas；CO is passed through to cathode inlet mouth respectively simultaneously2(20mL min-1), so that cathode inlet gas-guide tube is had pressure, prevents in gas-guide tube
Fused salt liquid level rises under low pressure, final solidified and block gas-guide tube.When the target temperature is reached, Ar controlled atmosphere is 80mL min-1。
When furnace is stablized at 600 DEG C, 30mL min is passed through to cathode inlet mouth-1O2/CO2The gaseous mixture of (molar ratio 1/2).It will
2.0g carbon dust and a small amount of carbonate after mixing, are added to anode chamber, are allowed to by the corundum piece of battery bottom and metallic walls
Face partition, tests under identical operating condition with electrochemical workstation their electrical property.
The Industrial Analysis and elemental analysis result of each carbon fuel of table 2
Nitrogen adsorption feature (the N of each carbon fuel of table 32Absorption, 77K)
In experiment, general anode cell configuration is known as anode I by us, and the new construction anode chamber in this patent is known as anode
Ⅱ。
The general structure of anode I is shown in Fig. 3 and Fig. 4.Anode I is mainly characterized by carbon dust 10' and is directly appended to corundum tube anode
In, carbon dust 10' is likely to swim in above fused carbonate 9' at this time, because carbon dust 10' density is less than fused carbonate 9'；Bottom
Portion is opening, seals bottom with 316 stainless steel cloths of one piece of 325 mesh, prevents carbon dust from leaking, while guaranteeing anode chamber and pipe
Outer electrolyte connection.This anode chamber's construction carbon dust is also directly contacted with air, easy to oxidize that reaction rate is caused further to drop
It is low.
The power density curve of each carbon fuel measured in the anode chamber of two kinds of structures, under identical operating condition see Fig. 5 and
Fig. 6.In anode I, the maximum power density MPD of each carbon fuel by arranging from big to small are as follows: bituminous coal (36mW cm-2) > conductive charcoal
Black (28.2mW cm-2) > bituminous coal coke (18.9mW cm-2) ≈ graphite powder (18.6mW cm-2) > bamboo base carbon (13.8mW cm-2).With
Comparison, in new structure anode chamber II, the maximum power density MPD of each carbon fuel by arranging from big to small are as follows: bamboo base carbon
(144.9mW cm-2) > bituminous coal (136.8mW cm-2) > conductive carbon black (134.7mW cm-2) > bituminous coal coke (72.0mW cm-2) > stone
Ink powder (53.3mW cm-2).Maximum power density of each carbon fuel in MC-DCFC, each carbon fuel function greatly improved in anode II
The increased multiple of rate density is respectively as follows: bamboo base carbon, and 10.5 times；Conductive carbon black, 4.8 times；Bituminous coal, 3.8 times；Bituminous coal is burnt, and 3.8 times；
Graphite powder, 2.9 times.Wherein, anode II is most obvious to the improvement of bamboo base carbon.Anode II is just because of having well solved carbon
The problem of powder fuel and fused electrolyte come into full contact with and improve reaction rate, while also assuring carbon dust fuel not by air oxygen
Change, waste of fuel is reduced, and the carbon dust fuel concentration of anode chamber is made to keep stable within a certain period of time, to improve now
The power density of MC-DCFC.
In addition, we are added to the conductive carbon black of mass ratio 1:1 in bamboo base carbon and bituminous coal respectively, (i.e. conductive carbon black Zhan is total
The 50% of quality), i.e. fuel combination A and B.According to experimental result, the MPD value of A fuel is 163.6 (round up and take 164) mW
cm-2, the MPD value of B fuel is 170.5 (round up and take 171) mW cm-2.The two values are than being used alone bamboo base carbon or cigarette
It is much higher when coal.It can be seen that being conducive to improve the overall performance of battery using the electric conductivity that conductive carbon black improves carbon fuel.
Fig. 5, Fig. 6 are each carbon dust fuel in 600 DEG C of power density curves in anode I and anode II.Cathode gas is
O2/CO2(1/2,30mL min-1)；Carbon particle size, 0.08mm-0.25mm；In anode II, A expression fuel combination (bamboo base charcoal+
Conductive carbon black, mass ratio 1:1), B indicates fuel combination (bituminous coal+conductive carbon black, mass ratio 1:1)
For convenient for comparing with table 1, experimental results of the invention are as shown in table 4:
The performance of the MC-DCFC of the domestic and international different fuel of table 4
In short, a kind of method for greatly improving MC-DCFC power density according to the present invention, structure is simple, realizes
Easily and effectively to be able to solve flotation issue of the carbon dust fuel in molten salt electrolyte, contacts carbon dust and fused electrolyte and fill
Point, increase reaction rate, greatly improves the power density of battery.
As it will be easily appreciated by one skilled in the art that the foregoing is merely illustrative of the preferred embodiments of the present invention, not to
The limitation present invention, any modifications, equivalent substitutions and improvements made within the spirit and principles of the present invention should all include
Within protection scope of the present invention.
Claims (9)
1. a kind of anode chamber for greatly improving MC-DCFC power density characterized by comprising heat-resisting hard tube (19) and electrode
Component；
Electrode assembly can freely pick and place in heat-resisting hard tube (19), including to pick and place stick (20), lower limit plate (15), high temperature resistant exhausted
Edge conducting wire (16) and current-collector (17)；Lower limit plate (15), which is fixed on, picks and places stick (20) lower end, and lower limit plate (15)
Periphery and heat-resisting hard tube (19) inner wall clearance fit；
Current-collector (17), which is located at, to be picked and placed below stick (20)；High-temperature insulation conducting wire (16) one end connects current-collector (17), the other end
Through-hole on lower limit plate (15) to connect external equipment when in use；
Lower limit plate (15) and heat-resisting hard tube (19) lower end surround the space for holding fuel powder (10), current-collector (17)
In the space；
Heat-resisting hard tube (19) lower end offers recirculation hole (18), to flow into heat-resisting hard tube (19) simultaneously for fused carbonate when in use
It is mixed with fuel powder (10).
2. a kind of anode chamber for greatly improving MC-DCFC power density according to claim 1, which is characterized in that heat-resisting
Hard tube (19) material is stainless steel or corundum.
3. a kind of anode chamber for greatly improving MC-DCFC power density according to claim 1, which is characterized in that pick and place
The material of stick (20) is stainless steel or corundum.
4. a kind of anode chamber for greatly improving MC-DCFC power density according to claim 1, which is characterized in that pick and place
The material of stick (20) and lower limit plate (15) is stainless steel, and is welded and fixed.
5. a kind of anode chamber for greatly improving MC-DCFC power density according to claim 4, which is characterized in that also wrap
Include top limit plate (21), the material of top limit plate (21) is stainless steel, be located above lower limit plate (15) and with pick-and-place
Stick (20) is welded and fixed, the periphery and heat-resisting hard tube (19) inner wall clearance fit of top limit plate (21)；High-temperature insulation conducting wire
(16) other end passes through the through-hole on top limit plate (21) to connect external equipment when in use.
6. a kind of anode chamber for greatly improving MC-DCFC power density according to claim 1, which is characterized in that current collection
Device (17) is corrosion-and high-temp-resistant sheet metal.
7. a kind of anode chamber for greatly improving MC-DCFC power density described in any one according to claim 1~6, special
Sign is, further includes the fixing piece that electrode assembly is fixed on to specified location in heat-resisting hard tube (19).
8. a kind of method for greatly improving MC-DCFC power density, which is characterized in that described in claim 1~7 any one
Anode chamber be added partial size 0.08mm-0.25mm carbon dust fuel, then by the anode chamber by carbon dust fuel be pressed into melting electricity
Xie Zhizhong；Contain conductive black in the carbon dust fuel, conductive black quality accounts for the 10%~50% of carbon dust fuel gross mass.
9. the MC-DCFC that one kind obtains according to the method for claim 8.
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| CN114361533A (en) * | 2022-01-10 | 2022-04-15 | 华北科技学院(中国煤矿安全技术培训中心) | Test method of carbon fuel cell system with three-electrode structure |
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| CN114361533A (en) * | 2022-01-10 | 2022-04-15 | 华北科技学院(中国煤矿安全技术培训中心) | Test method of carbon fuel cell system with three-electrode structure |
| CN114361533B (en) * | 2022-01-10 | 2024-01-30 | 华北科技学院(中国煤矿安全技术培训中心) | Test method of carbon fuel cell system with three-electrode structure |
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