CN109786795A - It is a kind of based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell - Google Patents
It is a kind of based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell Download PDFInfo
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- CN109786795A CN109786795A CN201811547182.9A CN201811547182A CN109786795A CN 109786795 A CN109786795 A CN 109786795A CN 201811547182 A CN201811547182 A CN 201811547182A CN 109786795 A CN109786795 A CN 109786795A
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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
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- 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
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Abstract
The invention discloses a kind of based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell, and the cathode and anode of the fuel cell are the nickel foam that surface is coated with NCAL, and the electrolyte layer of the fuel cell is SSO/LSCF composite material.The structure of fuel cell i.e. of the present invention are as follows: nickel foam //NCAL//SSO/LSCF//NCAL//nickel foam.Low-temperature solid oxide fuel cell of the present invention, as its electrolyte layer, substantially reduces the electrode polarization loss during electrochemical reaction of fuel battery using the stronitum stannate of perovskite structure and the composite material of lanthanum-strontium ferro-cobalt；The electrolyte has good output power in low-temperature zone, to make efficient stable to run for a long time using the solid oxide fuel cell of the electrolyte in low-temperature zone (300-600 degree).
Description
Technical field
The present invention relates to a kind of based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell, belongs to
In field of new energy technologies.
Background technique
Chemical energy in fuel (such as hydrogen, methane) can be efficiently converted to electric energy by solid oxide fuel cell.
Transfer efficiency is not limited by Carnot cycle, and efficiency is much higher than thermal power generation unit.Fuel cell is electrolysed qualitative classification by it can
It is divided into Proton Exchange Membrane Fuel Cells, solid oxide fuel cell, alkaline fuel cell, molten carbonate fuel cell, phosphorus
Hydrochlorate fuel cell, wherein solid oxide fuel does not need that noble metal catalyst, material selection range be wide, high conversion efficiency
The advantages that, it receives significant attention.But current solid oxide fuel cell mainly uses yttria-stabilized zirconia
(YSZ) it is used as electrolyte, YSZ needs that higher catalytic activity could be obtained in high temperature (900 degree or so).Therefore traditional solid
Oxide fuel cell generally all operates in the condition of high temperature.Hot operation all proposes that harshness is wanted to battery material, connecting material
It asks, in addition, hot operation proposes challenge to solid oxide fuel cell long-time stability.Therefore research low-temperature zone (300-
600 degree) solid oxide fuel cell in recent years, cause extensive concern.
Currently, the electrolyte of the solid oxide fuel cell based on cathode-electrolyte-anode structure is using relatively broad
YSZ (zirconium oxide of stabilized with yttrium oxide) complete fuel cell in 900 degree or so oxygen ion conduction abilities with higher
Electrochemical reaction, electromotive power output.But the material (YSZ) only just has good oxygen ion transport ability at high temperature,
When temperature is reduced to 600 degree hereinafter, almost without oxygen ion conduction ability.Therefore, in recent years, about reduction soild oxide combustion
Expect that the technology of battery is more and more, be concentrated mainly on two technology paths, first is that developing thin film technique, is thinned electrolyte YSZ's
Thickness so that its middle-temperature section also can ion transport capability with higher, but due to technical limitations, thickness can not
It is unlimited to be thinned, and thin film technique yield rate is also not very high；Second is that developing new material, ion can be transmitted in low-temperature zone by finding
New material.
Fuel cell is a typical electrochemical device, and the effect of intermediate electrolyte is transmission ion and prevention electronics
Transmission.Electrolyte according to semiconductor material as fuel cell, it is easy to people be allowed to associate the hair of short circuit phenomenon
Raw, just because of this, the material with semiconductor property is so far without using in a fuel cell.The a large amount of experimental study of the present invention
Show by the semiconductor material Application of composite with perovskite structure or perovskite-like structure fuel cell electrolysis material
In material, any short circuit phenomenon does not occur, and electrolyte composite material also has good output power in low-temperature zone.
Summary of the invention
Technical problem to be solved by the invention is to provide a kind of based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid
Oxide body fuel cell, the electrolyte in the fuel cell use the N-type semiconductor material tin with perovskite structure
Sour strontium (SrSnO3) and p-type semiconductor material lanthanum-strontium ferro-cobalt (LSCF) with perovskite structure it is compound, obtained electrolyte is multiple
Condensation material can not only prevent the transmission of electronics, but also have high ionic conductivity, therefore the electrolyte composite material
There is good output power in low-temperature zone, to enable efficient using the solid oxide fuel cell of the electrolyte
Operate in low-temperature zone (300-600 degree).
In order to solve the above technical problems, the technical scheme adopted by the invention is as follows:
It is a kind of based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell, the fuel cell
Cathode and anode are the nickel foam that surface is coated with NCAL, and the electrolyte layer of the fuel cell is SSO/LSCF composite material.
The structure of fuel cell of the present invention are as follows: nickel foam //NCAL//SSO/LSCF//NCAL//nickel foam.
Wherein, the nickel foam that surface is coated with nickel cobalt aluminium lithium (NCAL) is prepared with the following method: will be the desired amount of
NCAL(Ni0.8Co0.15Al0.05LiO2-δ) powder is gradually added into terpinol, until mixture is starchiness, starchy will mix
It closes object to be uniformly applied in nickel foam, the nickel foam after smearing is put into baking oven drying 2 hours at 200 DEG C, can be obtained
Surface is coated with the nickel foam of NCAL.
Wherein, the SSO/LSCF composite material is to mix SSO powder by certain mass ratio with nanometer LSCF powder, is filled
Grinding is divided to obtain.
The preparation method of above-mentioned SSO/LSCF composite material, specifically comprises the following steps:
Step 1, the SSO powder (SrSnO of perovskite structure is prepared3Powder):
The tin tetrachloride of 0.025mol is dissolved in the ethylene glycol of 1mol, obtains mixed solution A, is added into mixed solution A
0.25mol citric acid stirs 2 hours under 60 degree, after completely dissolution, obtains mixed solution B, be added into mixed solution B
The SrCO of 0.025mol3, under 80 degree of constant temperature, stirs 6 hours, obtains mixed solution C, mixed solution C is heated to 135 degree,
Heating 12 hours or more, the gel of amber transparent is obtained, gel is heated 3 hours under 350 degree, obtains xerogel, then will contain
There is the xerogel of Sr to be put into heating furnace and heat 700 degree, is sintered 4 hours, cooled to room temperature, after the completion of sintering, to sintering
Object is fully ground, and obtains SSO powder；
Step 2, SSO/LSCF composite material is prepared:
SSO powder made from step 1 is mixed with LSCF powder in mass ratio 1: 2, can be obtained SSO/ after being fully ground
LSCF composite material.
Wherein, in step 1, the heating of gel is divided into two processes: firstly, with the heating rate of 5 DEG C/min, from room temperature
350 degree are risen to, is sintered 3 hours, then rises to 700 DEG C from 350 temperature, is sintered 4 hours, cooled to room temperature.
The preparation of low-temperature solid oxide fuel cell of the present invention:
The nickel foam that surface is coated with NCAL is fabricated to electrode, electrode size is circle, and diameter D=13mm, electrode is being received
It the both sides nano composite material SSO/LSCF, will in symmetrical structure, i.e. nickel foam //NCAL//SSO/LSCF/NCAL//nickel foam structure
Piece of foam nickel //NCAL is put into compression mold bottom, and surface is coated with the one side of NCAL upward, takes the SSO/LSCF of 0.35g compound
Material is put into compression mold, then another nickel foam //NCAL is put into compression mold, is placed on SSO/LSCF composite material
Face, surface be coated with NCAL one down, compression mold is put into tablet press machine, is forced into 8Mpa, after pressure maintaining 5 seconds, take out battery
Piece obtains low-temperature solid oxide fuel cell of the invention.
Compared with the prior art, technical solution of the present invention has the beneficial effect that
Low-temperature solid oxide fuel cell of the present invention has the SSO material of perovskite structure using Moist chemical synthesis, then
The LSCF of SSO material obtained and perovskite structure is subjected to dry mixed, combined electrolysis of the invention is obtained after being fully ground
Material SSO/LSCF, obtained electrolyte composite material can not only prevent the transmission of electronics, but also have high ion
Conducting power, therefore the electrolyte composite material has good output power in low-temperature zone, while composite material also subtracts significantly
Electrode polarization loss during small electrochemical reaction of fuel battery；Therefore make the solid oxygen using the electrolyte composite material
Compound fuel cell being capable of long-term efficient stable operation in low-temperature zone (300-600 degree).
Detailed description of the invention
Fig. 1 is the structural schematic diagram of low-temperature solid oxide fuel cell of the present invention；
Fig. 2 is that the I-V when test temperature is 550 degree and I-P is special respectively for the fuel cell of SSO and LSCF different quality ratio
Linearity curve；Under 550 degree of service condition, when the mass ratio of SSO/LSCF is 1: 2, peak power output reaches 656mW/cm2；
Fuel cell when Fig. 3 is SSO and the mass ratio of LSCF is 1: 2 is respectively 550,525,500 degree in test temperature
When I-V and I-P characteristic curve；Peak power output is respectively 656mW/cm2, 535mW/cm2, 399mW/cm2；
Ac impedance characteristic curve when Fig. 4 is SSO and the mass ratio of LSCF is 1: 2 under hydrogen-oxygen atmosphere；
Fig. 5 is ac impedance characteristic curve of the pure SSO under hydrogen-oxygen atmosphere；
Fig. 6 is the space-charge region formed after electrolyte composite material combines.
Specific embodiment
According to following embodiments, the present invention may be better understood.However, as it will be easily appreciated by one skilled in the art that real
It applies content described in example and is merely to illustrate the present invention, without sheet described in detail in claims should will not be limited
Invention.
As shown in Figure 1, the nickel foam that surface is coated with NCAL constitutes symmetry electrode, fuel battery negative pole of the present invention and anode are equal
It is coated with the nickel foam of NCAL using surface, core electrolyte layer is SSO and LSCF composite material, therefore the structure of the fuel cell
Are as follows: nickel foam //NCAL//SSO/LSCF//NCAL//nickel foam；Wherein, NCAL Ni0.8Co0.15Al0.05LiO2-aMaterial (can
Purchase is prepared using disclosed method), SSO is commercially available or is made using the method for the present invention that LSCF is commercially available；Nickel foam
For the nickel material of commercially available foam-like.
The preparation method of fuel cell of the present invention:
First prepare the nickel foam (anode and cathode as fuel cell) that surface is coated with NCAL: by NCAL
(Ni0.8Co0.15Al0.05LiO2-δ) powder is gradually added into terpinol, until mixture is starchiness, by starchy mixture
It is uniformly applied in nickel foam, the nickel foam after smearing is put into baking oven drying 2 hours at 200 DEG C, surface can be obtained
It is coated with the nickel foam of NCAL；
SSO/LSCF composite material (electrolyte layer-generating element as fuel cell) is prepared again:
Step 1, the SSO powder (SrSnO of perovskite structure is prepared3Powder):
The tin tetrachloride of 0.025mol is dissolved in the ethylene glycol of 1mol, obtains mixed solution A, is added again into mixed solution A
Enter 0.25mol citric acid, is stirred 2 hours under 60 degree, after completely dissolution, obtain mixed solution B, be added into mixed solution B
The SrCO of 0.025mol3, under 80 degree of constant temperature, stirs 6 hours, obtains mixed solution C, mixed solution C is heated to 135 degree,
Heating 12 hours or more, the gel of amber transparent is obtained, gel is heated 3 hours under 350 degree, obtains xerogel, then will contain
There is the xerogel of Sr to be put into heating furnace and heat 700 degree, is sintered 4 hours, cooled to room temperature, after the completion of sintering, to sintering
Object is fully ground, and obtains SSO powder；Has perovskite structure using SSO prepared by sol-gel method；
Step 2, SSO/LSCF composite material is prepared:
SSO powder made from step 1 is mixed with the LSCF powder in mass ratio 1: 2 of purchase, can be obtained after being fully ground
Obtain SSO/LSCF composite material；
Finally, combining electrode material obtained with electrolyte, low-temperature solid oxide fuel of the invention is obtained
Battery:
The nickel foam that surface is coated with NCAL is fabricated to electrode, electrode size is circle, and diameter D=13mm, electrode is being received
The both sides nano composite material SSO/LSCF are in symmetrical structure, i.e. nickel foam //NCAL//SSO/LSCF//NCAL//nickel foam structure,
Piece of foam nickel //NCAL is first put into compression mold bottom, surface is coated with the one side of NCAL upward, then takes the SSO/ of 0.35g
LSCF composite material is put into compression mold, and another nickel foam //NCAL is finally put into compression mold, is placed on SSO/
Above LSCF composite material, surface be coated with NCAL one down, compression mold is put into tablet press machine, is forced into 8Mpa, pressure maintaining 5
After second, cell piece is taken out, low-temperature solid oxide fuel cell of the invention is obtained.
Experimental study shows that pure SSO can also be used as the electrolyte of fuel cell, but output performance is poor, and unstable
It is fixed, can be seen that from Fig. 2, Fig. 3, by SSO material by different quality ratio and LSCF carry out it is compound after, when the mass ratio of SSO and LSCF
When being 1: 2, chemical property reaches 656mW/cm2, changing the mass ratio of SSO and LSCF, there is apparent variation in battery performance,
When SSO and LSCF mass ratio are 1: 1, the maximum output power of fuel cell is 415mW/cm2, when SSO and LSCF mass ratio are 1
: when 2, the maximum output power of fuel cell is 656mW/cm2, when SSO is 1: 3 with LSCF mass ratio, fuel cell is maximum
Output power be 146mW/cm2, when SSO is 2: 1 with LSCF mass ratio, the maximum output power of fuel cell is 199mW/
cm2.It can be seen from the experiment that if further increasing the quality accounting of LSCF in composite material, the performance of composite material will be to pure
LSCF is close, gradually reduces, and when LSCF accounting is close to 1 (being almost pure LSCF in composite material), cell output is several
It disappears.When the quality accounting for further increasing SSO in composite material, performance is gradually intended to the output performance of pure SSO.It is comprehensive
For upper result of study it is found that SSO and LSCF is compound according to a certain percentage, obtained composite material has high ion in low-temperature zone
Conducting power shows that the two optimum quality ratio is 1: 2 by experimental study to have big output power.
In Fig. 4, first intersection point of ac impedance characteristic curve and the imaginary axis when SSO and LSCF mass ratio are 1: 2 is represented
Ohmic loss, value are about 0.12 Ω cm2, second intersection point of ac impedance characteristic curve and the imaginary axis represent crystal boundary loss,
Its value is of about for 0.2 Ω cm2.In Fig. 5, the ac impedance characteristic curve of pure SSO and first intersection point of the imaginary axis represent ohm
Loss, value is about 0.52 Ω cm2, second intersection point of ac impedance characteristic curve and the imaginary axis represent crystal boundary loss, value
Of about for 1.7 Ω cm2。
Through comparison diagram 4, Fig. 5 it is found that compared with the impedance operator of pure SSO, ohm of the composite material of SSO and LSCF is damaged
It loses and crystal boundary loss all substantially reduces, greatly promoted to prove that the performance of composite material has.
The structure of fuel cell of the present invention, nickel foam are respectively used to anode and cathode to promote the redox reaction at the two poles of the earth
Process and play the role of electronics collection.The present invention is by the N-type semiconductor material SSO with perovskite structure and has calcium titanium
The p-type semiconductor material LSCF of mine structure is compound, as shown in fig. 6, can be formed in electrolyte layer by nanostructure P-type material and
The space-charge region that n type material is established, space-charge region can cause band curvature to establish strong built in field at the interface (P-N),
And then accelerate the conduction of velocity (ion is accelerated in space-charge region) of oxonium ion, while the space-charge region can prevent electricity
The transmission of son；Traditional electrolyte is to transmit ion in the electrolyte, i.e. left side oxygen ion concentration
It is continuously increased, so that the oxygen ion concentration of bath surface is continuously increased, at high temperature, oxonium ion is spread into electrolyte, gradually
Another side is gradually reached to react with hydrogen ion, and compound electrolyte material of the present invention does not need to be can be realized at high temperature by oxonium ion
It is quickly transmitted to hydrogen ion side, therefore electrolyte composite material of the present invention has good output power in low-temperature zone.
Claims (6)
1. a kind of based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell, it is characterised in that: described
The electrolyte layer of fuel cell is SSO/LSCF composite material.
2. it is according to claim 1 based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell,
It is characterized by: the cathode of the fuel cell and anode are the nickel foam that surface is coated with NCAL.
3. it is according to claim 2 based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell,
It is characterized by: the nickel foam that surface is coated with NCAL is prepared with the following method: the desired amount of NCAL powder is added to
In terpinol, starchy mixture is obtained, starchy mixture is uniformly applied in nickel foam, can be obtained after drying
Surface is coated with the nickel foam of NCAL.
4. it is according to claim 1 based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell,
It is characterized by: the SSO/LSCF composite material is after being mixed by the SSO powder for preparing wet process with LSCF powder, sufficiently
It grinds and is made.
5. it is according to claim 4 based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell,
It is characterized by: the preparation method of the SSO/LSCF composite material, specifically comprises the following steps:
Step 1, SSO powder is prepared:
The tin tetrachloride of 0.025mol is dissolved in the ethylene glycol of 1mol, obtains mixed solution A, is added into mixed solution A
0.25mol citric acid stirs 2 hours under 60 degree, after completely dissolution, obtains mixed solution B, be added into mixed solution B
The SrCO of 0.025mol3, under 80 degree of constant temperature, stirs 6 hours, obtains mixed solution C, mixed solution C is heated to 135 degree,
Heating 12 hours or more, the gel of amber transparent is obtained, gel is heated 3 hours under 350 degree, obtains xerogel, then will contain
There is the xerogel of Sr to be put into heating furnace and heat 700 degree, is sintered 4 hours, cooled to room temperature, after the completion of sintering, to sintering
Object is fully ground, and obtains SSO powder；
Step 2, SSO/LSCF composite material is prepared:
SSO powder made from step 1 is mixed with LSCF powder in mass ratio 1: 2, can be obtained SSO/LSCF after being fully ground
Composite material.
6. it is according to claim 5 based on stronitum stannate/lanthanum-strontium ferro-cobalt composite material low-temperature solid oxide fuel cell,
It is characterized by: the heating of gel is divided into two processes in step 1: firstly, being risen with the heating rate of 5 DEG C/min from room temperature
It to 350 degree, is sintered 3 hours, then rises to 700 DEG C from 350 temperature, be sintered 4 hours, cooled to room temperature.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112048735A (en) * | 2020-09-14 | 2020-12-08 | 湖北大学 | Solid oxide electrolytic cell and preparation method thereof |
| CN113725468A (en) * | 2021-08-13 | 2021-11-30 | 南京晓庄学院 | Application of lithium lanthanum zirconium tantalum oxygen as solid oxide fuel cell electrolyte material |
| CN113782794A (en) * | 2021-08-30 | 2021-12-10 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
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| CN107660318A (en) * | 2015-06-30 | 2018-02-02 | 株式会社Lg化学 | Manufacture method, electrolyte for solid oxide fuel cell film, SOFC and the fuel cell module of electrolyte for solid oxide fuel cell film |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112048735A (en) * | 2020-09-14 | 2020-12-08 | 湖北大学 | Solid oxide electrolytic cell and preparation method thereof |
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| CN113782794A (en) * | 2021-08-30 | 2021-12-10 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
| CN113782794B (en) * | 2021-08-30 | 2024-03-08 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
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