CN109687006A - It is a kind of based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell - Google Patents
It is a kind of based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell Download PDFInfo
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- CN109687006A CN109687006A CN201811631918.0A CN201811631918A CN109687006A CN 109687006 A CN109687006 A CN 109687006A CN 201811631918 A CN201811631918 A CN 201811631918A CN 109687006 A CN109687006 A CN 109687006A
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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
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
- H01M8/126—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing cerium oxide
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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
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M2008/1293—Fuel cells with solid oxide electrolytes
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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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- General Chemical & Material Sciences (AREA)
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- Fuel Cell (AREA)
Abstract
The invention discloses a kind of based on cerium oxide/nickel oxide 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 CeO2/ NiO composite material.The structure of fuel cell i.e. of the present invention are as follows: nickel foam //NCAL//CeO2/ NiO//NCAL//nickel foam.Low-temperature solid oxide fuel cell of the present invention uses CeO2/ NiO nanocomposite substantially reduces the electrode polarization loss during electrochemical reaction of fuel battery as its electrolyte layer；The electrolyte has high oxygen ion conduction ability 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 cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell, belongs to
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.
The widely used YSZ of the electrolyte of solid oxide fuel cell based on cathode-electrolyte-anode structure
(zirconium oxide of stabilized with yttrium oxide) completes the electrochemistry of fuel cell in 800 degree or so oxygen ion conduction abilities with higher
Reaction, electromotive power output.It is current most widely used electrolyte, but the material (YSZ) only just has at high temperature
Standby good oxygen ion transport ability, when temperature is reduced to 600 degree hereinafter, almost without oxygen ion conduction ability.Therefore, in recent years
Come, it is more and more about the technology for reducing solid oxide fuel cell, two technology paths are concentrated mainly on, first is that development is thin
Membrane technology, be thinned electrolyte YSZ thickness so that its middle-temperature section also can ion transport capability with higher, but by
To the limitation of technology, thickness can not be infinitely thinned, and thin film technique yield rate is also not very high；Second is that develop new material,
The new material of ion can be transmitted in low-temperature zone by finding.
Fuel cell is a typical electrochemical device, and the effect of intermediate electrolyte is transmission ion and prevention electronics
Transmission.The doped semiconductor in ion conductor, it is easy to allow people to associate the generation of short circuit phenomenon, just because of this, have half
The material of conductor nature is so far without using in a fuel cell.The a large amount of experimental study of the present invention shows in ion conductor material
The material of semiconductor property, the especially semiconductor with perovskite structure or perovskite-like structure are suitably doped in material
Any short circuit phenomenon does not occur, but produces enhancement effect for material, and output power obviously increases.
Summary of the invention
Technical problem to be solved by the invention is to provide a kind of based on cerium oxide/nickel oxide composite material low-temperature solid
Oxide fuel cell, the electrolyte in the fuel cell are the compound of nanoparticle material and nano semiconductor material,
Semiconductor-ion heterojunction structure is formed in compound electrolyte material, the semiconductor-ion heterojunction structure may advantageously facilitate ion
Transmission speed, make compound electrolyte material of the present invention low-temperature zone to oxonium ion have high conducting power, to make to use
The solid oxide fuel cell of the electrolyte can efficient operation 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 cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell, the yin of the fuel cell
Pole and anode are the nickel foam that surface is coated with NCAL, and the electrolyte layer of the fuel cell is CeO2/ NiO composite material.
The structure of fuel cell of the present invention are as follows: nickel foam //NCAL//CeO2/ NiO//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 CeO2/ NiO composite material is by CeO2Wet chemical one-step synthesis is used with NiO, through over cleaning, is taken out
It filters, dry, being sintered, being fully ground acquisition.
Above-mentioned CeO2The preparation method of/NiO composite material, specifically: by CeO2It mixes, obtains with NiO in mass ratio 3: 1
Mixed powder is put into 20mL deionized water by 4g mixed powder, and constant temperature stirs 4 hours, concentrated nitric acid is slowly added dropwise, until NiO
Powder completely disappears (NiO powder sufficiently dissolves), then suitable sodium carbonate liquor is added dropwise, and sufficiently after reaction, cleaning is filtered 4 times,
Then it is dried, sintering processes, is fully ground after sintering, obtains CeO2/ NiO powder.
Wherein, the concentration of the sodium carbonate liquor is 0.5mol/L.
Wherein, be sintered with the heating rate of 10 DEG C/min, rise to 700 degree from drying temperature, be sintered 4 hours, then from
So it is cooled to room temperature.
Wherein, drying temperature is 120 degree, and drying time is 12 hours.
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
Nano composite material CeO2The both sides /NiO are in symmetrical structure, i.e. nickel foam //NCAL//CCeO2/ NiONCAL//nickel foam structure, will
Piece of foam nickel //NCAL is put into compression mold bottom, and surface is coated with the one side of NCAL upward, takes the CeO of 0.35g2/ NiO is compound
Material is put into compression mold, then another nickel foam //NCAL is put into compression mold, is placed on CeO2On/NiO 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 prepares CeO using wet chemical one-step synthesis2/ NiO composite material,
Compound electrolyte material CeO of the invention is obtained after being fully ground2/ NiO, composite material can be improved the transmission speed of oxonium ion
Degree, therefore composite material has good output power in low-temperature zone, while compound electrolyte material can also reduce fuel cell
Electrode polarization loss in electrochemical reaction process；Therefore make using the solid oxide fuel cell of the electrolyte low
Temperature section (300-600 degree) being capable of long-term efficient stable operation.
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 two kinds of CeO2/ NiO synthetic composite material and pure CeO2The fuel cell of electrolyte is respectively in test temperature
I-V and I-P characteristic curve when degree is 550 degree；Under 550 degree of service condition, work as CeO2/ NiO preparation process uses NaCO3It is heavy
When shallow lake, peak power output reaches 530mW/cm2；
Fig. 3 is CeO2/ NiO synthetic composite material uses NaCO3Exchange resistance when depositing technology under hydrogen-oxygen atmosphere
Anti- characteristic curve；
Fig. 4 is CeO2/ NiO synthetic composite material is without NaCO3AC impedance when depositing technology under hydrogen-oxygen atmosphere
Characteristic curve；
Fig. 5 is pure CeO2Ac impedance characteristic curve under hydrogen-oxygen atmosphere；
Fig. 6 is CeO2The XRD diagram of/NiO composite material.
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
The nickel foam of NCAL is coated with using surface, core electrolyte layer is CeO2/ NiO composite material, therefore the structure of the fuel cell
Are as follows: nickel foam //NCAL//CeO2/ NiO//NCAL//nickel foam；Wherein, NCAL is the nickel cobalt aluminium lithium-of purchase
Ni0.8Co0.15Al0.05LiO2-δMaterial, CeO2/ NiO is composite material of the present invention using Moist chemical synthesis preparation；Nickel foam is quotient
The nickel material of the foam-like of industry purchase.
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；
CeO is prepared again2/ NiO composite material (electrolyte layer-generating element as fuel cell):
By CeO2It is mixed with NiO in mass ratio 3: 1, obtains 4g mixed powder, mixed powder is put into 20mL deionized water
In (CeO at this time2It is dissolved in the water, NiO is not dissolved in water), constant temperature stirs 4 hours, concentrated nitric acid is slowly added dropwise, until NiO powder
End completely disappears (i.e. NiO powder is completely dissolved), then suitable sodium carbonate liquor (concentration 0.5mol/L) is added dropwise, and works as reaction solution
In no longer generate new precipitating after, stop be added dropwise sodium carbonate liquor；Reaction solution is cleaned repeatedly, is filtered 4 times, by what is obtained
It filters object to dry 12 hours in 120 degree of drying box, places into muffle furnace and be sintered 4 hours under 700 °, naturally cooled to
Room temperature after being fully ground, obtains CeO2/ NiO composite material.
CeO2In/NiO composite material, CeO2In other than doped with NiO, also doped with micro sodium ion.
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
Nano composite material CeO2The both sides /NiO are in symmetrical structure, i.e. nickel foam //NCAL//CeO2/ NiO//NCAL//nickel foam structure, first
Piece of foam nickel //NCAL is put into compression mold bottom, surface is coated with the one side of NCAL upward, then takes the CeO of 0.35g2/NiO
Composite material is put into compression mold, and another nickel foam //NCAL is finally put into compression mold, is placed on CeO2/ NiO is multiple
Above condensation 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.
Fig. 2 can be seen that experimental study shows pure CeO2Can also be used as the electrolyte of fuel cell, but output performance compared with
Difference, under 550 degree of test temperature, peak power output is only 72mW/cm2, and it is unstable；It is closed using one step of wet chemical
At CeO2/ NiO composite material, by NiO and CeO2It carries out compound, prepares nanocomposite, i.e. CeO2/ NiO composite material, electricity
Chemical output performance is from 72mW/cm2Rise to 237mW/cm2, when NaCO is added dropwise in one-step synthesis technical process3Solution, output property
It can be obviously improved, reach 530mW/cm2。
In Fig. 3, CeO2NaCO is used in/NiO composite material synthesis process3When depositing technology under hydrogen-oxygen atmosphere
Ac impedance characteristic curve and first intersection point of the imaginary axis represent ohmic loss, and value is about 0.17 Ω cm2, AC impedance spy
Linearity curve and second intersection point of the imaginary axis represent crystal boundary loss, and value is of about for 0.48 Ω cm2。
In Fig. 4, CeO2Without NaCO in/NiO composite material synthesis process3Friendship when depositing technology under hydrogen-oxygen atmosphere
Flow impedance characteristic curve and first intersection point of the imaginary axis represent ohmic loss, and value is about 0.27 Ω cm2, ac impedance characteristic
Curve and second intersection point of the imaginary axis represent crystal boundary loss, and value is of about for 0.78 Ω cm2。
In Fig. 5, pure CeO2Ac impedance characteristic curve and first intersection point of the imaginary axis represent ohmic loss, value is about
0.39Ω·cm2, second intersection point of ac impedance characteristic curve and the imaginary axis represent crystal boundary loss, and value is of about for 1.6 Ω
cm2。
By comparison diagram 3, Fig. 4, Fig. 5 it is found that with pure CeO2Impedance operator compare, wet chemical preparation CeO2/NiO
The ohmic loss of composite material and crystal boundary loss all substantially reduce, to prove that the performance of the composite material after doping has significantly
Promotion.
NiO is p-type semiconductor material, and the NiO that wet chemical is prepared not is stringent atomic ratio 1-1, there is many lack
Falling into leads to intrinsically p-type；With ion conductor CeO2It is compound, i.e., electronics phase is adulterated in ion phase, is formed heterojunction structure, i.e., is partly led
Body-ion heterojunction structure；By CeO2The electrolyte layer of ion conductor, which becomes one, has the electrolysis of semiconductor-ion heterojunction structure
There is matter layer semiconductor-ion heterojunction structure electrolyte can reinforce the transmittability to oxonium ion, therefore electrolyte
Composite material also has good output power in low-temperature zone (300-600 °).
Material prepared by the present invention is nano material, i.e., nanoparticle material and nano semiconductor material is compound, then passes through
It crosses grinding, forms the nano combined of ionic material and semiconductor material, it is different to form semiconductor-ion in this two-phase composite material
Matter structure forms the interface of nanoelectronic phase with nanoparticle phase, nanoelectronic phase and nanoparticle in electrolyte layer
The interface of phase can reinforcement material to the transmittability of oxonium ion so that the output power of fuel cell dramatically increases.
As shown in fig. 6, comparison blue CeO2Standard diagram, it can be seen that pure CeO2There is also in mixed-powder, compare
Red NiO standard diagram, it can be seen that pure NiO is there is also in mixed-powder, therefore, CeO2With NiO it is that two-phase is compound, and
There is no reaction, also not new mutually appearance；A peak value is found 30 degree of positions, is compared by analysis, the peak value and Na
The peak value of standard PDF card is corresponding.
By XRD analysis it is found that CeO2It is two-phase composite nano materials with NiO, there is no chemical reaction, CeO for itself2Belong to
In ionic conductor material, but ionic conductivity be not it is very high, NiO is doped into CeO2Afterwards, NiO first is a kind of with catalysis
The material of effect further improves the ionic conductivity of composite material, and simultaneous oxidation nickel internal structure, which is tangled, leads to current-carrying
Son can not flow, and leading to nickel oxide is insulator, non-conductive；In composite material, a small amount of Na ion occurs in the composite,
The catalytic activity of composite material is further improved, because of Na catalytic activity with higher.
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 in pure CeO2It is middle to adulterate NiO material using wet chemical, it is transported in low-temperature zone
When row, composite material has high oxygen ion conduction ability, to effectively increase the efficiency that fuel cell is run in low-temperature zone.
Claims (8)
1. a kind of based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell, it is characterised in that: the combustion
The electrolyte layer for expecting battery is CeO2/ NiO composite material.
2. it is according to claim 1 based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell,
Be characterized in that: the cathode and anode of the fuel cell are the nickel foam that surface is coated with NCAL.
3. it is according to claim 2 based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell,
Be characterized in that: the nickel foam that surface is coated with NCAL is prepared with the following method: the desired amount of NCAL powder is added to pine
In oleyl alcohol, starchy mixture is obtained, starchy mixture is uniformly applied in nickel foam, table can be obtained after drying
Face is coated with the nickel foam of NCAL.
4. it is according to claim 1 based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell,
It is characterized in that: the CeO2/ NiO composite material is to prepare CeO by one step of wet chemical2After/NiO, it is fully ground and is made.
5. it is according to claim 4 based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell,
It is characterized in that: CeO2The preparation method of/NiO composite material, specifically: by CeO2It is mixed with NiO in mass ratio 3: 1, it is mixed to obtain 4g
Powder is closed, mixed powder is put into 20mL deionized water, constant temperature stirs 4 hours, concentrated nitric acid is slowly added dropwise, until NiO powder
It completely disappears, then suitable sodium carbonate liquor is added dropwise, sufficiently after reaction, cleaning is filtered 4 times, is then dried, at sintering
Reason, is fully ground after sintering, obtains CeO2/ NiO powder.
6. it is according to claim 5 based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell,
Be characterized in that: the concentration of the sodium carbonate liquor is 0.5mol/L.
7. it is according to claim 5 based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell,
Be characterized in that: sintering rises to 700 degree with the heating rate of 10 DEG C/min, from drying temperature, is sintered 4 hours, then naturally cold
But to room temperature.
8. it is according to claim 5 based on cerium oxide/nickel oxide composite material low-temperature solid oxide fuel cell,
Be characterized in that: drying temperature is 120 degree, and drying time is 12 hours.
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| CN114068958A (en) * | 2021-11-16 | 2022-02-18 | 东南大学 | Method for preparing carbon nano tube by catalytic pyrolysis of waste plastics and applying carbon nano tube to low-temperature fuel cell |
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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 |
| CN114068958A (en) * | 2021-11-16 | 2022-02-18 | 东南大学 | Method for preparing carbon nano tube by catalytic pyrolysis of waste plastics and applying carbon nano tube to low-temperature fuel cell |
| CN114068958B (en) * | 2021-11-16 | 2023-12-08 | 东南大学 | Method for preparing carbon nano tube by catalytic pyrolysis of waste plastics and applying carbon nano tube to low-temperature fuel cell |
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Effective date of registration: 20211028 Address after: A213, Kechuang building, National Science and Technology Park, Southeast University, 271 Heyan Road, Qixia District, Nanjing, Jiangsu 210028 Patentee after: NANJING SUOLEYOU ENERGY SAVING TECHNOLOGY Co.,Ltd. Address before: No. 3601 Jiangning Road, Nanjing District hirokage 211171 cities in Jiangsu Province Patentee before: NANJING XIAOZHUANG University |
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