CN102916202A - Fuel cell anode and in situ preparation method thereof - Google Patents
Fuel cell anode and in situ preparation method thereof Download PDFInfo
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- CN102916202A CN102916202A CN2012104249103A CN201210424910A CN102916202A CN 102916202 A CN102916202 A CN 102916202A CN 2012104249103 A CN2012104249103 A CN 2012104249103A CN 201210424910 A CN201210424910 A CN 201210424910A CN 102916202 A CN102916202 A CN 102916202A
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Abstract
一种直接硼氢化钠燃料电池阳极，以泡沫镍为集流体，泡沫镍的表面分布有Pd纳米短棒，该Pd纳米短棒作为燃料电池的阳极催化剂。阳极的原位制备方法包括：以泡沫镍作为阳极催化剂的载体和集流体装在阳极极板的一侧；以Pt/C催化剂为阴极装配成直接硼氢化钠燃料电池，将电池升温到80oC；在阳极一侧先通入混合液并保持在阳极流场内，向阳极流场缓慢通入抗坏血酸溶液或者硼氢化钠溶液，混合液与抗坏血酸或者硼氢化钠溶液反应使得阳极流场内的Pd离子还原并依附于泡沫镍表面生长形成Pd纳米短棒；通入去离子水清洗阳极流场，获取燃料电池阳极。本发明具有阳极的电子传导稳定、结合力好、催化空间利用率高的优点。
A direct sodium borohydride fuel cell anode uses nickel foam as a current collector, Pd nano short rods are distributed on the surface of the foam nickel, and the Pd nano short rods are used as an anode catalyst of the fuel cell. The in-situ preparation method of the anode includes: using nickel foam as the carrier of the anode catalyst and the current collector on one side of the anode plate; using the Pt/C catalyst as the cathode to assemble a direct sodium borohydride fuel cell, and heating the battery to 80 o C: On the anode side, the mixed solution is first introduced and kept in the anode flow field, and the ascorbic acid solution or sodium borohydride solution is slowly introduced into the anode flow field, and the mixed solution reacts with ascorbic acid or sodium borohydride solution to make the anode flow field Pd ions are reduced and attached to the surface of nickel foam to grow to form short Pd nanorods; the anode flow field is cleaned by passing through deionized water to obtain the anode of the fuel cell. The invention has the advantages of stable electron conduction of the anode, good binding force and high catalytic space utilization rate.
Description
Technical field
Present technique relates to a kind of anode of fuel cell and preparation method thereof.
Background technology
Fuel cell is the generation technology that a kind of chemical energy that directly will be stored in the fuel is converted into electric energy, because it has the advantages such as the high and low discharging of energy conversion efficiency, pollution-free and noiselessness, the 4th kind of electricity-generating method outside be considered to continue firepower, waterpower, the nuclear energy.
Direct sodium borohydride fuel cell is take proton exchange membrane as electrolyte, the direct liquid fuel battery take sodium borohydride as fuel a kind of.It also has original advantage except having the common advantage of other fuel cells.For example: it is convenient that normal temperature uses, simple in structure, fuel carries supply, has good mobility, is suitable as very much small-sized movable and compact power.And because used fuel sodium borohydride has good reducing activity, so the anode catalyst of catalytic oxidation sodium borohydride often need not to adopt expensive rare Pt catalyst.Its cathod catalyst also can be without Pt simultaneously, but with cheap Co/N/C[H.Y. Qin, Z.X. Liu, W.X. Yin, J.K. Zhu, Z.P. Li. A cobalt polypyrrole composite catalyzed cathode for the direct borohydride fuel cell. Journal of Power Sources, 185 (2008) 909-912], perhaps MnO
2[A. Verma, A.K. Jha, S. Basu. Manganese dioxide as a cathode catalyst for direct alcohol or sodium borohydride fuel cell with a flowing alkaline electrolyte. Journal of Power Sources, 141 (2005) 30-34], Ag[B.H. Liu, S. Suda. Influences of fuel crossover on cathode performance in a micro borohydride fuel cell. Journal of Power Sources, 164 (2007) 100-104] etc. catalyst.So that comparing with other fuel cells, direct sodium borohydride fuel cell has flexibility that larger catalyst selects and the possibility of cost.
It is catalyst [L.B. Wang that the anode of direct sodium borohydride fuel cell adopts hydrogen bearing alloy usually, C.A. Ma, X.B. Mao, J.F. Sheng, F.Z. Bai, F. Tang. Rare earth hydrogen storage alloy used in borohydride fuel cells. Electrochemistry Communication, 7 (2005) 1477-1481.], the conventional preparation process of its anode is: with the carbon dust of hydrogen storing alloy powder and proper proportion, Nafion solution hybrid modulation is slurry, is coated on the nickel foam dry tack free and namely can be used as anode.The main purpose of adding carbon dust is to strengthen conductivity, and the electronic energy that produces when making hydrogen bearing alloy catalytic oxidation sodium borohydride is led toward negative electrode by carbon dust and nickel foam smoothly; The main purpose of adding Nafion is the caking property that strengthens catalyst granules and nickel foam, prevents from that catalyst granules is washed to peel off the disengaging nickel foam when liberation of hydrogen generation bubble hydrogen.
Although conductivity and life-span that many researchs can improve anode by the ratio of regulating carbon dust and Nafion solution, obtain preferably cell output.Yet there is unavoidable congenital deficiency in this technique.At first, because hydrogen bearing alloy contacts with nickel foam by carbon dust, there are at least two interfaces of hydrogen bearing alloy-carbon dust and carbon dust-nickel foam, the stability of electrical conductivity is brought very large uncertainty.Secondly, hydrogen bearing alloy and carbon dust all are to be bonded in the nickel foam surface by Nafion, and this combination is fragile unsettled, when fuel flow rate quickening and the aggravation of liberation of hydrogen generation bubble hydrogen, under the continuous erosion effect, thereby hydrogen bearing alloy and carbon dust probably are stripped from the nickel foam inactivation.Again, if hydrogen bearing alloy overwhelming majority surface is lived by carbon dust or Nafion embedding, then can't contact fuel, can't play catalytic action, also be that its space availability ratio is low.
Summary of the invention
The present invention the invention provides a kind of a kind of anode of fuel cell and in-situ preparation method thereof that electrical conductivity is stable, adhesion is good, the catalysis space availability ratio is high of anode for the problem that electrical conductivity is unstable, adhesion is poor and the catalyst space utilance is low that the anode that overcomes prior art exists.
A kind of anode of fuel cell, take nickel foam as collector, the surface distributed of nickel foam has Pd nanometer stub, the act as a fuel anode catalyst of battery of this Pd nanometer stub.
Further, non-overlapping copies between the Pd nanometer stub; Non-overlapping copies between the Pd nano particle.
The in-situ preparation method of described anode of fuel cell may further comprise the steps:
1) side that, is contained in plate with nickel foam as carrier and the collector of anode catalyst; Be assembled into direct sodium borohydride fuel cell take the Pt/C catalyst as negative electrode, battery is warmed up to 80
oC;
2), passing into first the mixed liquor that is comprised of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol in anode one side also remains on this mixed liquor in the anode flow field, then the anode flow field slowly passes into ascorbic acid solution or sodium borohydride solution, and mixed liquor and ascorbic acid or sodium borohydride solution reaction form Pd nanometer stub so that the Pd ion in the anode flow field reduces and depends on the nickel foam superficial growth;
3) wait for that Pd nanometer stub is covered with the nickel foam surface;
4), pass into the washed with de-ionized water anode flow field,
5), obtain anode of fuel cell, Pd nanometer stub is as anode catalyst, nickel foam is as anode collector.
Further, step 2) in, the mass ratio of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol is 1:2:20:50 in the described mixed liquor; The time of mixed liquor and ascorbic acid or sodium borohydride solution reaction is 0.1 ~ 5 hour.
The diameter of the Pd nanometer stub further, step 2) is 5 ~ 20 nm, and length is 20 ~ 500 nm, and the average headway between the Pd nanometer stub is 50 ~ 200 nm, and Pd nanometer stub spatial shape all is cuboid, and four sides are { 100}
PdCrystal face.
Further, step 2) in, non-overlapping copies between the Pd nanometer stub.
Use the nickel foam that is covered with Pd nanometer stub to be anode, Pt/C passes into fuel as the direct sodium borohydride fuel cell of negative electrode and oxygen can obtain 200 mW/cm
2Above power density, continuous discharge 120 h, the performance degradation amount is less than 5%.
The present invention has advantage:
1, Pd nanometer stub growth in situ is on the nickel foam surface, be combined firmly with nickel foam, thereby so that the bubbling that this catalyst can stand washing away for a long time of fuel and sodium borohydride liberation of hydrogen when producing bubble hydrogen impacts and do not come off, guaranteed namely that also this catalyst has good stability and useful life.
2, Pd nanometer stub is grown directly upon the nickel foam surface, and both ensure preferably electronic conduction direct the connection.So that the electronic energy that fuel produces during by catalytic reduction conducts to rapidly nickel foam and further is transferred to negative electrode by anode, ensured the high conductivity of anode.
3, Pd nanometer stub is grown in the nickel foam surface and forms the structure of similar mace so that every Pd nanometer stub non-overlapping copies can both trigger with fuel joint and give birth to catalytic reaction, also namely has great real space utilance.
4, four sides of this Pd nanometer stub are the main positions that catalytic reaction occurs much larger than bottom surface and end face.And these four sides are (100)
PdCrystal face, experimental study show that the sodium borohydride molecule is in (100)
PdCrystal face can be realized line absorption, thereby has guaranteed that these four sides have good catalytic reduction to sodium borohydride.
Description of drawings
Accompanying drawing 1 Pd nanometer stub is grown in the schematic diagram that the nickel foam surface forms similar mace structure.
Accompanying drawing 2 Pd nanometer stub crystal face characteristic scalar diagrams.
Accompanying drawing 3 is with the typical I-V curve chart of the sodium borohydride fuel cell of anode assembling of the present invention.
Embodiment
Embodiment 1
A kind of anode of fuel cell, take nickel foam as collector, the surface distributed of nickel foam has Pd nanometer stub, the act as a fuel anode catalyst of battery of this Pd nanometer stub.Non-overlapping copies between the Pd nanometer stub; Non-overlapping copies between the Pd nano particle, as shown in Figure 1.The number of Pd nanometer stub is numerous.
A kind of in-situ preparation method of anode of fuel cell may further comprise the steps:
1) side that, is contained in plate with nickel foam as carrier and the collector of anode catalyst; Be assembled into direct sodium borohydride fuel cell take the Pt/C catalyst as negative electrode, battery is warmed up to 80
oC;
2), passing into first the mixed liquor that is comprised of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol in anode one side also remains on this mixed liquor in the anode flow field, then the anode flow field slowly passes into ascorbic acid solution or sodium borohydride solution, and mixed liquor and ascorbic acid or sodium borohydride solution reaction form Pd nanometer stub so that the Pd ion in the anode flow field reduces and depends on the nickel foam superficial growth;
3) wait for that Pd nanometer stub is covered with the nickel foam surface;
4), pass into the washed with de-ionized water anode flow field,
5), obtain anode of fuel cell, Pd nanometer stub is as anode catalyst, nickel foam is as anode collector.
Step 2) in, the mass ratio of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol is 1:2:20:50 in the mixed liquor of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol; The time of mixed liquor and ascorbic acid or sodium borohydride solution reaction is 0.1 ~ 5 hour.
The diameter of the Pd nanometer stub step 2) is 5 ~ 20 nm, and length is 20 ~ 500 nm, and the average headway between the Pd nanometer stub is 50 ~ 200 nm, and Pd nanometer stub spatial shape all is cuboid, and four sides are { 100}
PdCrystal face.
Step 2) in, non-overlapping copies between the Pd nanometer stub.
Use the nickel foam that is covered with Pd nanometer stub to be anode, Pt/C passes into fuel as the direct sodium borohydride fuel cell of negative electrode and oxygen can obtain 200 mW/cm
2Above power density, continuous discharge 120 h, the performance degradation amount is less than 5%.
The present invention has advantage:
1, Pd nanometer stub growth in situ is on the nickel foam surface, be combined firmly with nickel foam, thereby so that the bubbling that this catalyst can stand washing away for a long time of fuel and sodium borohydride liberation of hydrogen when producing bubble hydrogen impacts and do not come off, guaranteed namely that also this catalyst has good stability and useful life.
2, Pd nanometer stub is grown directly upon the nickel foam surface, and both ensure preferably electronic conduction direct the connection.So that the electronic energy that fuel produces during by catalytic reduction conducts to rapidly nickel foam and further is transferred to negative electrode by anode, ensured the high conductivity of anode.
3, Pd nanometer stub is grown in the nickel foam surface and forms the structure of similar mace so that every Pd nanometer stub non-overlapping copies can both trigger with fuel joint and give birth to catalytic reaction, also namely has great real space utilance.
4, four sides of this Pd nanometer stub are the main positions that catalytic reaction occurs much larger than bottom surface and end face.And these four sides are (100)
PdCrystal face, experimental study show that the sodium borohydride molecule is in (100)
PdCrystal face can be realized line absorption, thereby has guaranteed that these four sides have good catalytic reduction to sodium borohydride.
In conjunction with actual tests, further specify the present invention:
Embodiment 2:
Take Pt/C as negative electrode, take the N117 film as dielectric film, take nickel foam as anode collector with catalyst matrix, the assembling direct sodium borohydride fuel cell.Battery is warming up to 80
oC and insulation.Pass into the mixed liquor of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol and remain in the anode flow field from anode one side direction inside battery anode flow field, slowly pass into afterwards ascorbic acid solution, keep reaction approximately to clean anode flow field with deionized water behind 1 h.So that the nickel foam superficial growth goes out Pd nanometer stub, form similar mace structure.Pd nanometer stub diameter 5 nm, length is 20 nm approximately, and average headway is 50 nm, and four sides are { 100}
PdCrystal face.Anode passes into the sodium borohydride basic fuel afterwards, and negative electrode passes into oxygen, and the battery discharge test result shows that battery has good electric output performance, and peak power output density surpasses 180 mW/cm
2Continuous discharge 100 h, the battery performance attenuation is less than 3%.
Embodiment 3:
Take Co/N/C as negative electrode, take the N117 film as dielectric film, take nickel foam as anode collector with catalyst matrix, the assembling direct sodium borohydride fuel cell.Battery is warming up to 80
oC and insulation.Pass into the mixed liquor of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol and remain in the anode flow field from anode one side direction inside battery anode flow field, slowly pass into afterwards rare sodium borohydride solution, keep reaction approximately to clean anode flow field with deionized water behind 0.5 h.So that the nickel foam superficial growth goes out Pd nanometer stub, form similar mace structure.Pd nanometer stub diameter 20 nm, length is 500 nm approximately, and average headway is 200 nm, and four sides are { 100}
PdCrystal face.Anode passes into the sodium borohydride basic fuel afterwards, and negative electrode passes into oxygen, and the battery discharge test result shows that battery has good electric output performance, and peak power output density surpasses 200 mW/cm
2Continuous discharge 120 h, the battery performance attenuation is less than 5%.
Embodiment 4:
Take Ag/C as negative electrode, take the N117 film as dielectric film, take nickel foam as anode collector with catalyst matrix, the assembling direct sodium borohydride fuel cell.Battery is warming up to 80
oC and insulation.Pass into the mixed liquor of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr, ethanol and ascorbic acid and remain in the anode flow field from anode one side direction inside battery anode flow field, keep reaction approximately to clean anode flow field with deionized water behind 4 h.So that the nickel foam superficial growth goes out Pd nanometer stub, form similar mace structure.Pd nanometer stub diameter 10 nm, length is 100 nm approximately, and average headway is 80 nm, and four sides are { 100}
PdCrystal face.Anode passes into the sodium borohydride basic fuel afterwards, and negative electrode passes into oxygen, and the battery discharge test result shows that battery has good electric output performance, and peak power output density surpasses 200 mW/cm
2Continuous discharge 100 h, the battery performance attenuation is less than 4%.
Do not depart from the scope of the present invention and principle, different changes of the present invention and variation are apparent for those of ordinary skills, are to be understood that to the invention is not restricted in illustrative embodiments proposed above.
Claims (6)
1. anode of fuel cell, take nickel foam as collector, it is characterized in that: the surface distributed of nickel foam has Pd nanometer stub, the act as a fuel anode catalyst of battery of this Pd nanometer stub.
2. a kind of anode of fuel cell as claimed in claim 1 is characterized in that: non-overlapping copies between the Pd nanometer stub; Perhaps non-overlapping copies between the Pd nano particle.
3. the in-situ preparation method of anode of fuel cell as claimed in claim 2 may further comprise the steps:
1) side that, is contained in plate with nickel foam as carrier and the collector of anode catalyst; Be assembled into direct sodium borohydride fuel cell take the Pt/C catalyst as negative electrode, battery is warmed up to 80
oC;
2), passing into first the mixed liquor that is comprised of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol in anode one side also remains on this mixed liquor in the anode flow field, then the anode flow field slowly passes into ascorbic acid solution or sodium borohydride solution, and mixed liquor and ascorbic acid or sodium borohydride solution reaction form Pd nanometer stub so that the Pd ion in the anode flow field reduces and depends on the nickel foam superficial growth;
3), wait for that Pd nanometer stub is covered with the nickel foam surface;
4), pass into the washed with de-ionized water anode flow field,
5), obtain anode of fuel cell, Pd nanometer stub is as anode catalyst, nickel foam is as anode collector.
4. the in-situ preparation method of a kind of anode of fuel cell as claimed in claim 3 is characterized in that: step 2) in, the mass ratio of polyvinylpyrrolidone, chlorine palladium acid sodium, KBr and ethanol is 1:2:20:50 in the described mixed liquor; The time of mixed liquor and ascorbic acid or sodium borohydride solution reaction is 0.1 ~ 5 hour.
5. such as the in-situ preparation method of claim 3 or 4 described a kind of anode of fuel cell, it is characterized in that: step 2) in the diameter of Pd nanometer stub be 5 ~ 20 nm, length is 20 ~ 500 nm, average headway between the Pd nanometer stub is 50 ~ 200 nm, Pd nanometer stub spatial shape all is cuboid, and four sides are { 100}
PdCrystal face.
6. the in-situ preparation method of a kind of anode of fuel cell as claimed in claim 5 is characterized in that: step 2) in, non-overlapping copies between the Pd nanometer stub.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104638272A (en) * | 2013-11-14 | 2015-05-20 | 北汽福田汽车股份有限公司 | Positive pole piece for sodium borohydride fuel cell and preparation method of positive pole piece |
| CN110153410A (en) * | 2019-06-06 | 2019-08-23 | 安徽师范大学 | Method for growing ordered Pd array rod-shaped nanoparticles on the surface of Au triangular plate and its application |
| CN114122419A (en) * | 2021-03-24 | 2022-03-01 | 包头稀土研究院 | Direct sodium borohydride fuel cell DBFC anode and preparation method thereof |
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| CN102544532A (en) * | 2012-03-06 | 2012-07-04 | 杭州电子科技大学 | Nanowire network structure catalyst and preparation method thereof |
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| CN102544532A (en) * | 2012-03-06 | 2012-07-04 | 杭州电子科技大学 | Nanowire network structure catalyst and preparation method thereof |
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| BYUNGKWON LIMET.AL: "Shape-Controlled Synthesis of Pd Nanocrystals in Aqueous Solutions", 《ADV. FUNCT. MATER.》 * |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104638272A (en) * | 2013-11-14 | 2015-05-20 | 北汽福田汽车股份有限公司 | Positive pole piece for sodium borohydride fuel cell and preparation method of positive pole piece |
| CN104638272B (en) * | 2013-11-14 | 2017-10-13 | 北汽福田汽车股份有限公司 | Sodium borohydride fuel cell anode pole piece and preparation method thereof |
| CN110153410A (en) * | 2019-06-06 | 2019-08-23 | 安徽师范大学 | Method for growing ordered Pd array rod-shaped nanoparticles on the surface of Au triangular plate and its application |
| CN110153410B (en) * | 2019-06-06 | 2021-07-30 | 安徽师范大学 | Method for growing ordered Pd array rod-like nanoparticles on the surface of Au triangular plate and its application |
| CN114122419A (en) * | 2021-03-24 | 2022-03-01 | 包头稀土研究院 | Direct sodium borohydride fuel cell DBFC anode and preparation method thereof |
| CN114122419B (en) * | 2021-03-24 | 2023-12-12 | 包头稀土研究院 | Direct sodium borohydride fuel cell DBFC anode and preparation method thereof |
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