CN109802162A - Low-temperature solid oxide fuel cell based on zinc oxide-stannous oxide composite material - Google Patents
Low-temperature solid oxide fuel cell based on zinc oxide-stannous oxide composite material Download PDFInfo
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- CN109802162A CN109802162A CN201811631965.5A CN201811631965A CN109802162A CN 109802162 A CN109802162 A CN 109802162A CN 201811631965 A CN201811631965 A CN 201811631965A CN 109802162 A CN109802162 A CN 109802162A
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Abstract
The invention discloses a low-temperature solid oxide fuel cell based on a zinc oxide-stannous oxide composite material, wherein a cathode and an anode of the fuel cell are both foamed nickel with NCAL coated on the surfaces, and an electrolyte layer of the fuel cell is made of a SnO/ZnO/NCAL composite material. Namely, the fuel cell of the present invention has the structure: nickel foam// NCAL// SnO/ZnO/NCAL// NCAL// nickel foam. The low-temperature solid oxide fuel cell adopts the nickel-cobalt-aluminum-lithium and the SnO/ZnO composite material synthesized by the wet method as the electrolyte layer of the oxide fuel cell, thereby greatly reducing the electrode polarization loss in the electrochemical reaction process of the fuel cell; the electrolyte material has good output power at a low temperature section, so that the solid oxide fuel cell adopting the electrolyte material can efficiently and stably operate for a long time at the low temperature section (300-600 ℃).
Description
Technical field
The present invention relates to a kind of based on zinc oxide-stannous oxide 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.Nickel cobalt aluminium lithium (NCAL) is it is well known that it is answered
Electrode material is only used as in solid oxide fuel cell, not the report as electrolyte application.
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 semiconductor material Application of composite in the electrolyte of fuel cell, any short circuit phenomenon does not occur, and
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 zinc oxide-stannous oxide composite material low-temperature solid
Oxide body fuel cell, electrolyte in the fuel cell in low-temperature zone oxygen ion conduction ability with higher, from
And enable using the solid oxide fuel cell efficient operation of the electrolyte at 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 zinc oxide-stannous oxide 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 SnO/ZnO/NCAL composite material.
The structure of fuel cell of the present invention are as follows: nickel foam //NCAL//SnO/ZnO/NCAL//NCAL//nickel foam.
Wherein, the nickel foam that surface is coated with NCAL is prepared with the following method: by the desired amount of 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.
Wherein, the SnO/ZnO/NCAL composite material is to use SnO/ZnO powder made from wet process and NCAL powder
Dry mixed is ground and is made.
The preparation method of above-mentioned SnO/ZnO/NCAL composite material, specifically comprises the following steps:
Step 1, SnO/ZnO powder is prepared:
By SnCl2.2H2O and C4H6O4Zn 1: 1 mixing in molar ratio, obtains mixed material A；Mixed material A is dissolved in right amount
Deionized water in, under the conditions of 80 degree of constant temperature, stir 4 hours, be slowly added to citric acid into mixed material A in whipping process
(SnCl2.2H2O∶C4H6O4Zn: citric acid=1: 1: 3, molar ratio), mixed material B is obtained, mixed material B is by suction filtration, drying
After be sintered, after the completion of sintering, sinter is fully ground, obtains SnO/ZnO powder；
Step 2, SnO/ZnO+NCAL composite material is prepared:
SnO/ZnO powder made from step 1 is mixed with NCAL powder in mass ratio 1: 4, can be obtained after being fully ground
SnO/ZnO/NCAL composite material；NCAL substance is doped in SnO/ZnO by dry grinding.
Wherein, in step 1, sintering rises to 700 DEG C with the heating rate of 8 DEG C/min, from drying temperature, is sintered 2 hours,
Then cooled to room temperature.
Wherein, in step 1, in mixed material B, SnCl2∶C4H6O4Zn: the mixing molar ratio of citric acid is 1: 1: 3.
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 multiple
The both sides condensation material SnO/ZnO/NCAL are in symmetrical structure, i.e., the structure of fuel cell of the present invention are as follows: nickel foam //NCAL//SnO/
Piece of foam nickel //NCAL is put into compression mold bottom by ZnO/NCAL//NCAL//nickel foam structure, and surface is coated with NCAL's
On one side upward, it takes the SnO/ZnO/NCAL composite material of 0.35g to be put into compression mold, then another nickel foam //NCAL is put
Enter compression mold, be placed on above SnO/ZnO/NCAL composite material, surface be coated with NCAL one down, compression mold is put into
Tablet press machine is forced into 8Mpa, after pressure maintaining 5 seconds, takes out cell 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 prepares SnO/ZnO composite material using wet synthesis techniques, then
SnO/ZnO composite material is carried out dry grinding with NCAL to mix, compound electrolyte material of the invention is obtained after being fully ground
SnO/ZnO/NCAL, obtained electrolyte composite material can not only prevent the transmission of electronics, but also have high oxonium 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 be SnO/ZnO and NCAL different quality ratio fuel cell respectively the I-V when test temperature is 550 degree and
I-P characteristic curve；Under 550 degree of service condition, when the mass ratio of SnO/ZnO and NCAL is 1: 4, peak power output reaches
583mW/cm2；
Fuel cell when Fig. 3 is SnO/ZnO and the mass ratio of NCAL is 1: 4 respectively test temperature be 550,500,
I-V and I-P characteristic curve at 450 degree；Peak power output is respectively 583mW/cm2, 481 mW/cm2, 415mW/cm2；
The fuel cell of the fuel cell that Fig. 4 is SnO/ZnO and the mass ratio of NCAL is 1: 4 and pure SnO/ZnO is being tested
I-V and I-P characteristic curve when temperature is 550 degree；The fuel cell of pure SnO/ZnO is maximum defeated under 550 degree of service condition
Power is 247mW/cm out2；
Fig. 5 is ac impedance characteristic curve of the pure SnO/ZnO under hydrogen-oxygen atmosphere；
Fig. 6 is SnO/ZnO and the mass ratio of NCAL is 1: the 4 ac impedance characteristic curve under hydrogen-oxygen atmosphere.
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 the composite material of SnO/ZnO and NCAL, therefore the fuel cell
Structure are as follows: nickel foam //NCAL//SnO/ZnO/NCAL//NCAL//nickel foam；Wherein, NCAL is
Ni0.8Co0.15Al0.05LiO2-δMaterial, SnO/ZnO are the composite material prepared using Moist chemical synthesis；Nickel foam is commercially available
The nickel material of foam-like, NCAL powder are commercially available nickel cobalt aluminium lithium powder.
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；
SnO/ZnO/NCAL composite material (electrolyte layer-generating element as fuel cell) is prepared again:
Step 1, SnO/ZnO powder is prepared:
By SnCl2·2H2O and C4H6O4Zn 1: 1 mixing in molar ratio, obtains mixed material A；Mixed material A is dissolved in suitable
In the deionized water of amount, under the conditions of 80 degree of constant temperature, stirs 4 hours, be slowly added to lemon into mixed material A in whipping process
Acid (SnCl2·2H2O∶C4H6O4Zn: citric acid=1: 1: 3, molar ratio), obtain mixed material B, mixed material B by filtering,
It is sintered after drying, after the completion of sintering, sinter is fully ground, obtain SnO/ZnO powder；
Step 2, SnO/ZnO/NCAL composite material is prepared:
SnO/ZnO powder made from step 1 is mixed with NCAL powder in mass ratio 1: 4, obtains SnO/ after being fully ground
ZnO/NCAL 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 multiple
The both sides condensation material SnO/ZnO/NCAL are in symmetrical structure, i.e. nickel foam //NCAL//SnO/ZnO/NCAL//NCAL//nickel foam knot
Piece of foam nickel //NCAL is first put into compression mold bottom by structure, and surface is coated with the one side of NCAL upward, then takes 0.35g's
SnO/ZnO/NCAL composite material is put into compression mold, and another nickel foam //NCAL is finally put into compression mold, is put
On LNO/SDC composite material, surface be coated with NCAL one down, compression mold is put into tablet press machine, is forced into 8Mpa,
After pressure maintaining 5 seconds, cell piece is taken out, low-temperature solid oxide fuel cell of the invention is obtained.
It can be seen that from Fig. 2~4, pure SnO/ZnO can be used as the electrolyte of fuel cell, and under conditions of 550 degree, most
Big output power is 247mW/cm2, by SnO/ZnO material by different quality ratio and NCAL carry out it is compound after, when SnO/ZnO with
When the mass ratio of NCAL is 1: 4, chemical property reaches 583mW/cm2, change the mass ratio of SnO/ZnO and NCAL, it is cell performance
Apparent variation can occur.When SnO/ZnO and NCAL mass ratio are 1: 1, the maximum output power of fuel cell is 223mW/
cm2, when SnO/ZnO is 1: 2 with NCAL mass ratio, the maximum output power of fuel cell is 353mW/cm2, when SnO/ZnO with
When NCAL mass ratio is 1: 3, the maximum output power of fuel cell is 506mW/cm2, it is 1 with SnO/ZnO and NCAL mass ratio:
Output power is compared when 4, is declined slightly, if further increasing the quality accounting of NCAL in composite material, the property of composite material
Energy will be gradually close to pure NCAL, and cell output almost disappears at this time.When the matter for further increasing SnO/ZnO in composite material
Accounting is measured, performance is gradually intended to the output performance of pure SnO/ZnO.To sum up result of study is it is found that in pure SnO/ZnO material
Adulterate NCAL, be conducive to improve electrolyte catalytic activity, by experimental study show the two optimum proportioning be mass ratio be 1:
4.Electrolyte of the pure NCAL as fuel cell, under conditions of 550 degree, output power 0mW/cm2, i.e., its do not have oxygen from
Sub- conducting power.
ZnO and NCAL is the material with semiconductor property, if there is no SnO in compound electrolyte material, only ZnO with
If NCAL is compound, semiconductor property is still presented in material, only has electronics conduction function, without ionic conduction function
Energy.After SnO and ZnO is compound, SnO/ZnO nanocomposite has ion transfer function, oxygen ion conduction to hydrogen ion
, will be in conjunction with generation water when side, while electronics is released, to realize that conversion produces electricl energy, realize the electrochemistry of fuel cell
Reaction.
Experiment shows: SnO/ZnO nanocomposite can be used as the electrolyte of fuel cell, and open-circuit voltage is more than 1V, say
After bright SnO and ZnO are compound, short circuit phenomenon is not generated, although open-circuit voltage is higher, electric current is smaller, causes to export
The main reason for power is small, and electric current is small is that its oxygen ion conduction ability is inadequate.When adding one in SnO/ZnO nanocomposite
When quantitative NCAL material, the oxygen ion conduction ability of electrolyte can be significantly improved, improves electric current and power.
In Fig. 5, the ac impedance characteristic curve of pure SnO/ZnO and first intersection point of the imaginary axis represent ohmic loss, value
About 0.35 Ω cm2, second intersection point of ac impedance characteristic curve and the imaginary axis represent crystal boundary loss, value of about for
0.78Ω·cm2.It is special doped with the AC impedance of the SnO/ZnO (mass ratio of SnO/ZnO and NCAL are 1: 4) of NCAL in Fig. 6
Linearity curve and first intersection point of the imaginary axis represent ohmic loss, and value is about 0.12 Ω cm2, ac impedance characteristic curve and empty
Second intersection point of axis represents crystal boundary loss, and value is of about for 0.27 Ω cm2.By comparison diagram 5, Fig. 6 it is found that with pure SnO/
The impedance operator of ZnO is compared, and SnO/ZnO and the compound ohmic loss of NCAL and crystal boundary loss are substantially reduced, to prove to mix
The performance of compound electrolyte material after miscellaneous, which has, greatly to be promoted.
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 adulterates NCAL material in pure SnO/ZnO composite material, transports in low-temperature zone
When row (300~600 degree), compound electrolyte material has good oxygen ion conduction ability, to effectively improve fuel cell
In the efficiency of low-temperature zone operation.
Claims (7)
1. a kind of based on zinc oxide-stannous oxide composite material low-temperature solid oxide fuel cell, it is characterised in that: described
The electrolyte layer of fuel cell is SnO/ZnO/NCAL composite material.
2. it is according to claim 1 based on zinc oxide-stannous oxide 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 zinc oxide-stannous oxide 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 zinc oxide-stannous oxide composite material low-temperature solid oxide fuel cell,
It is characterized by: the SnO/ZnO/NCAL composite material is after mixing SnO/ZnO powder with NCAL powder, be fully ground and
It is made.
5. it is according to claim 4 based on zinc oxide-stannous oxide composite material low-temperature solid oxide fuel cell,
It is characterized by: the preparation method of the SnO/ZnO/NCAL composite material, specifically comprises the following steps:
Step 1, SnO/ZnO powder is prepared:
By SnCl2.2H2O and C4H6O4Zn 1: 1 mixing in molar ratio, obtains mixed material A；Mixed material A is dissolved in suitable go
In ionized water, under the conditions of 80 degree of constant temperature, stirs 4 hours, be slowly added to citric acid into mixed material A in whipping process, obtain
To mixed material B, mixed material B is sintered after filtering, drying, and after the completion of sintering, is carried out to sinter abundant
Grinding, obtains SnO/ZnO powder；
Step 2, SnO/ZnO/NCAL composite material is prepared:
SnO/ZnO powder made from step 1 is mixed with NCAL powder in mass ratio 1: 4, can be obtained SnO/ after being fully ground
ZnO/NCAL composite material.
6. it is according to claim 5 based on zinc oxide-stannous oxide composite material low-temperature solid oxide fuel cell,
It is characterized by: in step 1, sintering rises to 700 DEG C with the heating rate of 8 DEG C/min, from drying temperature, is sintered 2 hours, so
Cooled to room temperature afterwards.
7. low-temperature solid oxide fuel cell according to claim 5, it is characterised in that: in step 1, mixed material B
In, SnCl2∶C4H6O4Zn: the mixing molar ratio of citric acid is 1: 1: 3.
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