CN105762371A - Biomass alkaline fuel cell anode with electron transporter and preparation method - Google Patents
Biomass alkaline fuel cell anode with electron transporter and preparation method Download PDFInfo
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- CN105762371A CN105762371A CN201610237824.XA CN201610237824A CN105762371A CN 105762371 A CN105762371 A CN 105762371A CN 201610237824 A CN201610237824 A CN 201610237824A CN 105762371 A CN105762371 A CN 105762371A
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9008—Organic or organo-metallic compounds
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- 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
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Abstract
The invention discloses a biomass alkaline fuel cell anode with an electron transporter and a preparation method.The preparation method includes: (1), adding water into a graphene sheet and a carbon nano tube, ultrasonically dispersing, suction-filtering, and drying to obtain a mixed carrier GNPs-CNTs; (2), mixing the mixed carrier with 2-hydroxyl-1, 4 naphthoquinone water solution, adding ethylene glycol, ultrasonically dispersing, adjusting pH, ultrasonically dispersing, heating, standing, suction-filtering, washing, and drying to obtain a catalyst; (3), adding the catalyst into anhydrous alcohol, ultrasonically dispersing, adding PTFE emulsion, ultrasonically dispersing, stirring to obtain a thick product, flatly spreading and pressing the thick product on the surface of foamed nickel, rolling to form a thin layer to obtain the biomass alkaline fuel cell anode.2-hydroxyl-1, 4 naphthoquinone which is low in price, easy to get and good in performance is used to prepare the biomass alkaline fuel cell anode, so that power generating performance of a cell can be improved substantially; production cost can be lowered, and reaction time can be shortened.
Description
Technical field
The invention belongs to field of fuel cell technology, particularly relate to a kind of living beings basic fuel electricity with electron transit mediator
Pond anode and preparation method.
Background technology
Living beings alkaline fuel cell, is a kind of chemical energy being stored in biomass fuel and oxidant in alkaline environment
The device of electric energy it is converted into by the redox reaction of anode and negative electrode.It has energy conversion efficiency height, environmental pollution
Little, can power the most continuously, the plurality of advantages such as applied widely, be increasingly becoming the focus in energy research field, receive perhaps
The favor of many researchers.
Raising battery performance and stability, as the core component of living beings alkaline fuel cell, are had the heaviest by anode catalyst
The effect wanted.Along with the development of alkaline fuel cell, its catalyst being used for anode have also been obtained and is greatly enhanced, such as Pinchas
Schechner et al. (Schechner P, Kroll E, Bubis E, Chervinsky S, Zussman E.J Electrochem
Soc 2007;Silver spindle fiber 154:B942-B948.) is used to make anode;L.An et al. (An L, Zhao TS, Shen SY,
Wu QX,Chen R.J Power Sources 2011;196:186-190.) employ cheap anion-exchange membrane prevention oxygen
Gas is reacted therewith by negative electrode arrival anode and improves battery performance;Cindy X.Zhao et al. (Chen JY, Zhao CX,
Zhi MM,Wang KW,Deng LL,Xu G.Electrochim Acta 2012;66:133-138.) use and will not urge
The nickel foam of agent poisoning does anode and cathode makes battery performance improve 6 times;Debika Basu et al. (Basu D, Basu S.
Electrochim Acta 2010;55:5775-5779.) platinum, rubidium, activated carbon are made sun after ultrasonic vibration and heating water bath
Pole;Jinyao Chen et al. (Chen JY, Zhao CX, Zhi MM, Wang KW, Deng LL, Xu G.Electrochim
Acta 2012;66:133-138.) silver load is made anode in nickel foam;But the shortcoming that every kind of catalyst has himself.
First, although to make catalyst catalytic performance good for common noble metal such as gold, platinum etc., character is the most relatively stable, but it is expensive,
Cannot be used for large-scale industrialization to produce, additionally research shows these noble metals and easily by the intermediate product bag of course of reaction
Wrapping up in forfeiture catalytic site, and make catalysis activity reduce and even lose catalysis activity, this catalyst poisoning the most described is existing
As.Although current research shows that the noble metal such as palladium, ruthenium can avoid catalyst poisoning problem, improve battery performance but still deposit
In problem in price.And for the eelctro-catalyst nickel based on nano material received much concern in the last few years, nickel oxide, hydroxide
Nickel and the nano material of other metallic addition, urge as the materials such as CNT, Graphene and Ti/TiO2 are used for making anode
It is highly effective that agent improves battery performance, but its manufacture craft is more complicated.It is eager to explore one at present and can be used for alkaline environment
In non-precious metal catalyst.Therefore, study a kind of new electron transit mediator to be fixed on anode for catalysis biomass alkali
Property fuel cell will seem and be highly desirable to improving its performance.
Summary of the invention
It is an object of the invention to overcome the deficiencies in the prior art, it is provided that a kind of living beings alkaline fuel cell with electron transit mediator
Anode.
Second object of the present invention is to provide the preparation side of a kind of living beings alkaline fuel cell anode with electron transit mediator
Method.
Technical scheme is summarized as follows:
The preparation method of a kind of living beings alkaline fuel cell anode with electron transit mediator, comprises the steps:
(1) it is the ratio of 1:4 in mass ratio, weighs graphene film and CNT is placed in container, add distilled water, make steaming
Distilled water there was not graphene film and CNT, ultrasonic disperse 25~30min, suction filtration, in 110 DEG C of dry 1h, obtains mixing and carries
Body, described graphene film is referred to as GNPs, and described CNT is referred to as CNTs, and described mixed carrier is referred to as GNPs-CNTs;
(2) it is the ratio of 1:1~2 in mass ratio, by water-soluble to GNPs-CNTs and 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones that concentration is 30mM
Liquid mix, add ethylene glycol, described ethylene glycol is 1-2 times of 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones aqueous solution volume, ultrasonic disperse 15~
20min, regulates pH to 8.5, again ultrasonic disperse 15~20min with the NaOH aqueous solution, is subsequently placed in 700W micro-wave oven
5~10min are stood after heating 60s;Suction filtration also washs with distilled water, is dried, obtains 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones and be supported on GNPs-CNTs
On catalyst;
(3) catalyst that step (2) obtains is placed in container, adds absolute ethyl alcohol, make absolute ethyl alcohol not have described catalysis
Agent, ultrasonic disperse 25~30min, add ptfe emulsion, described graphene film and CNT sum and polytetrafluoroethyl-ne
The mass ratio of alkene emulsion is 1:0.5~0.8, ultrasonic disperse 25~30min;It is warming up to 70-75 DEG C of stirring, obtains dope;
Dope tiling is pressed into nickel foam surface, roll squeezer is rolled into 2~4mm thin layers, obtains the life with electron transit mediator
Material alkaline fuel cell anode.
A kind of living beings alkaline fuel cell anode with electron transit mediator prepared by said method.
Advantages of the present invention:
1. the present invention uses electron transit mediator 2-hydroxyl-1,4 naphthoquinones cheap and easy to get and of good performance preparation a kind of with electron transmission
The living beings alkaline fuel cell anode of body, can make the electricity generation performance of living beings alkaline fuel cell be greatly improved, it is adaptable to advise greatly
Mould produces;
2. comparing the method that more traditional noble metal catalyst improves electricity weak performance, galvanic anode used in the present invention can reduce life
Produce cost, and shorten the reaction time, improve battery performance.
Accompanying drawing explanation
Fig. 1 is the power density curve map of different living beings alkaline fuel cell corresponding to anode.
Fig. 2 is that the electron transmission liquid solution variable concentrations of two kinds of better performances is than corresponding power density curve.
Detailed description of the invention
Below in conjunction with specific embodiment, the present invention is further illustrated.
Graphene film guide number Ps in each embodiment, CNT is called for short CNTs, mixed carrier guide number Ps-CNTs;
Ptfe emulsion product introduction is pointed out: polytetrafluoroethylene solids content is in 60% (wt) left and right.
Embodiment 1
The preparation method of a kind of living beings alkaline fuel cell anode with electron transit mediator, comprises the steps:
(1) accurately weigh 0.2g GNPs and 0.8g CNTs to be placed in beaker, add distilled water, make distilled water not have GNPs
And CNTs, ultrasonic disperse 30min, suction filtration, 110 DEG C of dry 1h in baking oven, obtain mixed carrier GNPs-CNTs;
(2) it is that the 30mM electron transit mediator aqueous solution is placed in beaker mixing according to mass ratio 1:1 by GNPs-CNTs and concentration,
Adding ethylene glycol, ethylene glycol is 2 times of electron transit mediator aqueous solution volume, ultrasonic disperse 15min, adjusts with the NaOH aqueous solution
Joint pH to 8.5, again ultrasonic disperse 15min, stand 10min after being subsequently placed in 700W micro-wave oven heating 60s;Suction filtration is also
Wash with distilled water, be dried, obtain the catalyst that electron transit mediator is supported on GNPs-CNTs;
Electron transit mediator is respectively as follows:
Dimethyl diaminophenazine chloride, 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones, 1,5-dichloroanthraquinone, methylene blue, anthraquinone, methyl viologen,
It is abbreviated as: NR-dimethyl diaminophenazine chloride, NQ-2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones, DA-1,5-dichloroanthraquinone, MB-methylene blue, AQ-anthraquinone,
MV-methyl viologen, Bare-, without any electron transit mediator, replaces with the water of same volume;
(3) catalyst that step (2) obtains is placed in beaker, adds absolute ethyl alcohol, make absolute ethyl alcohol not have described catalyst,
Ultrasonic disperse 30min, adds the mass ratio of ptfe emulsion, described GNPs and CNTs sum and ptfe emulsion
For 1:0.5, ultrasonic disperse 30min;It is warming up to 75 DEG C of stirrings, obtains dope;The circle of one a diameter of about 2cm of cutting
Shape nickel foam, is pressed into nickel foam surface by dope tiling, is rolled into 3mm thin layer on roll squeezer, obtains passing with electronics
Pass the living beings alkaline fuel cell anode of body.
Embodiment 2
The power density curve of different alkaline fuel cells corresponding to anode
Fig. 1 show the power density curve of the battery corresponding to seven kinds of different anodes of embodiment 1 preparation.Wherein Bare curve
For the blank group without any electron transit mediator.For avoiding error, every kind of equal horizontal survey of anode 3 times, with the addition of
Error line, makes data more accurately and reliably.Battery used is dual chamber glucose fuel cell, and anode is respectively embodiment 1 to be prepared
Electrode, negative electrode is air diffusion electrode, and in battery, concentration of glucose is 1M, KOH concentration and is 3M.In Fig. 1 in NR-
Property is red, NQ-2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones, DA-1,5-dichloroanthraquinone, MB-methylene blue, AQ-anthraquinone, MV-methyl viologen, Bare-
Blank group)
Power density is followed successively by 7.39W/m2、9.95W/m2、7.07W/m2、9.37W/m2、6.70W/m2、10.05W/m2With
4.56W/m2.It can be seen that with compared with the blank group of any electron transit mediator, with the addition of the sun of electron transit mediator
Pole can increase substantially battery performance, and wherein better performances is to the addition of 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones and the anode of methyl viologen, its
Power density is respectively 9.95W/m2And 10.05W/m2.(MB-methylene blue is unstable).
Embodiment 3
The power density curve of different alkaline fuel cells corresponding to anode
Draw the electron transit mediator of two kinds of better performances from embodiment 2: 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones and methyl viologen, change they with
The mass ratio of GNPs-CNTs, the method also according to embodiment 1 prepares anode.Fig. 2 a is GNPs-CNTs and concentration is 30mM
Methyl viologen aqueous solution mass ratio be respectively 1:1,1:2,1;Cell power density curve corresponding to 3, Fig. 2 b is GNPs-CNTs
It is the cell power density song that 30mM2-hydroxyl-1,4 naphthoquinones aqueous solution mass ratio is respectively corresponding to 1:1,1:2,1:3 with concentration
Line.For avoiding error, every kind of equal horizontal survey of anode 3 times, with the addition of error line, make data more accurately and reliably.Used
Battery is identical with embodiment 2.From the test result of Fig. 2 it can be seen that GNPs-CNTs and concentration are that 30mM methyl viologen is water-soluble
Liquid mass ratio be respectively 1:1,1:2,1;Battery maximum power density corresponding to 3 is respectively 10.05W/m2、17.95W/m2With
18.01W/m2;GNPs-CNTs and concentration are that 30mM2-hydroxyl-1,4 naphthoquinones aqueous solution mass ratio is respectively 1:1,1:2,1:3 institute
Corresponding battery maximum power density 9.95W/m respectively2、16.10W/m2And 4.26W/m2。
Methyl viologen research shows, Viologen Compounds has toxicity, also has the biggest harmfulness to ecological environment, does not enters
Row protection.
2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones is a kind of ancient natural dye, can extract from plant, and in chemical constitution, it is one
Unique little molecule, without ionic group, defines according to the international convention of persistence chemicals, belongs to degradable organic in soil
Thing.
Embodiment 4
The preparation method of a kind of living beings alkaline fuel cell anode with electron transit mediator, comprises the steps:
(1) accurately weigh 0.2g GNPs and 0.8g CNTs to be placed in beaker, add distilled water, make distilled water not have GNPs
And CNTs, ultrasonic disperse 25min, suction filtration, 110 DEG C of dry 1h in baking oven, obtain mixed carrier GNPs-CNTs;
(2) by GNPs-CNTs and concentration, that to be 30mM2-hydroxyl-1,4 naphthoquinones aqueous solution be placed in beaker according to mass ratio 1:1 is mixed
Closing, add ethylene glycol, ethylene glycol is 1 times of 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones water volume, and ultrasonic disperse 18min is water-soluble with NaOH
Liquid regulation pH to 8.5, again ultrasonic disperse 18min, stand 5min after being subsequently placed in 700W micro-wave oven heating 60s;Take out
Filter is also washed with distilled water, is dried, obtains the catalyst that 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones is supported on GNPs-CNTs;
(3) catalyst that step (2) obtains is placed in beaker, adds absolute ethyl alcohol, make absolute ethyl alcohol not have described catalyst,
Ultrasonic disperse 25min, adds the mass ratio of ptfe emulsion, described GNPs and CNTs sum and ptfe emulsion
For 1:0.7, ultrasonic disperse 25min;It is warming up to 70 DEG C of stirrings, obtains dope;The circle of one a diameter of about 2cm of cutting
Shape nickel foam, is pressed into nickel foam surface by dope tiling, is rolled into 2mm thin layer on roll squeezer, obtains passing with electronics
Pass the living beings alkaline fuel cell anode of body.
Embodiment 5
The preparation method of a kind of living beings alkaline fuel cell anode with electron transit mediator, comprises the steps:
(1) accurately weigh 0.2g GNPs and 0.8g CNTs to be placed in beaker, add distilled water, make distilled water not have GNPs
And CNTs, ultrasonic disperse 28min, suction filtration, 110 DEG C of dry 1h in baking oven, obtain mixed carrier GNPs-CNTs;
(2) by GNPs-CNTs and concentration, that to be 30mM2-hydroxyl-1,4 naphthoquinones aqueous solution be placed in beaker according to mass ratio 1:1 is mixed
Closing, add ethylene glycol, ethylene glycol is 1.5 times of 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones water volume, and ultrasonic disperse 20min uses NaOH water
Solution regulation pH to 8.5, again ultrasonic disperse 20min, stand 8min after being subsequently placed in 700W micro-wave oven heating 60s;
Suction filtration also washs with distilled water, is dried, obtains the catalyst that 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones is supported on GNPs-CNTs;
(3) catalyst that step (2) obtains is placed in beaker, adds absolute ethyl alcohol, make absolute ethyl alcohol not have described catalysis
Agent, ultrasonic disperse 28min, add the matter of ptfe emulsion, described GNPs and CNTs sum and ptfe emulsion
Amount ratio is 1:0.8, ultrasonic disperse 28min;It is warming up to 73 DEG C of stirrings, obtains dope;One a diameter of about 2cm of cutting
Circular shaped foam nickel, by dope tiling be pressed into nickel foam surface, roll squeezer is rolled into 4mm thin layer, obtains with electricity
The living beings alkaline fuel cell anode of sub-carrier.
It is demonstrated experimentally that the power density of the living beings alkaline fuel cell anode with electron transit mediator of embodiment 4,5 and enforcement
The power of the living beings alkaline fuel cell anode with electron transit mediator (electron transit mediator is 2-hydroxyl-1,4 naphthoquinones) of example 1
Similar density.
Claims (2)
1., with the preparation method of living beings alkaline fuel cell anode for electron transit mediator, it is characterized in that comprising the steps:
(1) it is the ratio of 1:4 in mass ratio, weighs graphene film and CNT is placed in container, add distilled water, make steaming
Distilled water there was not graphene film and CNT, ultrasonic disperse 25~30min, suction filtration, is dried, obtains mixed carrier, described stone
Ink alkene sheet is referred to as GNPs, and described CNT is referred to as CNTs, and described mixed carrier is referred to as GNPs-CNTs;
(2) it is the ratio of 1:1~2 in mass ratio, by water-soluble to GNPs-CNTs and 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones that concentration is 30mM
Liquid mix, add ethylene glycol, described ethylene glycol is 1-2 times of 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones aqueous solution volume, ultrasonic disperse 15~
20min, regulates pH to 8.5, again ultrasonic disperse 15~20min, stands after being subsequently placed in 700W micro-wave oven heating 60s
5~10min;Suction filtration also washs with distilled water, is dried, obtains the catalyst that 2-hydroxyl-Isosorbide-5-Nitrae naphthoquinones is supported on GNPs-CNTs;
(3) catalyst that step (2) obtains is placed in container, adds absolute ethyl alcohol, make absolute ethyl alcohol not have described catalysis
Agent, ultrasonic disperse 25~30min, add ptfe emulsion, described graphene film and CNT sum and polytetrafluoroethyl-ne
The mass ratio of alkene emulsion is 1:0.5~0.8, ultrasonic disperse 25~30min;It is warming up to 70-75 DEG C of stirring, obtains dope;
Dope tiling is pressed into nickel foam surface, roll squeezer is rolled into 2~4mm thin layers, obtains the life with electron transit mediator
Material alkaline fuel cell anode.
2. a kind of living beings alkaline fuel cell anode with electron transit mediator that prepared by the method for claim 1.
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Cited By (2)
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CN107895800A (en) * | 2017-10-24 | 2018-04-10 | 天津大学 | The method that one-step method prepares electro-deposition cobalt activity carbon anode |
CN109585886A (en) * | 2018-10-10 | 2019-04-05 | 天津大学 | Organic waste treatment and the device and method to generate electricity for alkaline fuel cell |
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Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
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CN107895800A (en) * | 2017-10-24 | 2018-04-10 | 天津大学 | The method that one-step method prepares electro-deposition cobalt activity carbon anode |
CN107895800B (en) * | 2017-10-24 | 2020-08-25 | 天津大学 | Method for preparing electrodeposited cobalt activated carbon anode by one-step method |
CN109585886A (en) * | 2018-10-10 | 2019-04-05 | 天津大学 | Organic waste treatment and the device and method to generate electricity for alkaline fuel cell |
CN109585886B (en) * | 2018-10-10 | 2021-12-07 | 天津大学 | Device and method for treating organic waste and using organic waste for power generation of alkaline fuel cell |
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