CN110534784A - A kind of preparation method of the alkaline flow battery system of high-energy density, low cost - Google Patents
A kind of preparation method of the alkaline flow battery system of high-energy density, low cost Download PDFInfo
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- CN110534784A CN110534784A CN201910716331.8A CN201910716331A CN110534784A CN 110534784 A CN110534784 A CN 110534784A CN 201910716331 A CN201910716331 A CN 201910716331A CN 110534784 A CN110534784 A CN 110534784A
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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
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- 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
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
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- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
- H01M8/184—Regeneration by electrochemical means
- H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
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Abstract
The present invention relates to alkaline oxygenated reduction flow battery energy storage field, the preparation method of the alkaline flow battery system of specifically a kind of high-energy density, low cost, to solve the problems such as existing all-vanadium flow battery energy density is low, expensive.Using carbon felt as flow battery positive electrode, zinc metal sheet or zine plate as flow battery negative electrode material.(such as: KMnO with permanganate4、NaMnO4Deng) alkaline aqueous solution as anode electrolyte, using the alkaline aqueous solution of highly basic (such as: KOH, NaOH) as electrolyte liquid, using ionized treated amberplex assembled battery of the perfluorosulfonic acid proton exchange film (such as: Nafion117, Nafion212) as flow battery.To obtain the alkaline oxygenated reduction flow battery system with low cost and high-energy density.The flow battery system tool energy density that the present invention is researched and developed is high, at low cost, the advantages that having extended cycle life, and can be widely applied for redox flow batteries energy storage field.
Description
Technical field:
The present invention relates to alkaline oxygenated reduction flow battery energy storage field, specifically a kind of high-energy density, inexpensive alkali
The preparation method of property flow battery system.
Background technique:
The growing property of the non-renewable and energy demand of fossil energy, so that there is an urgent need to a kind of new storages by the mankind
Can technology with Steady settlement new energy, such as: wind energy, solar energy etc..Because of its flexible structure, have extended cycle life, it is safe and reliable etc.
Advantage, flow battery are one of energy storage candidates of most prospect.In various traditional flow battery systems, all-vanadium flow battery
Ion cross-contamination issue effectively is avoided, but relatively low energy density (25Wh/L) and excessively high cost make its commercialization
Process is by huge obstacle.Although non-water system possesses higher open-circuit voltage and alternative active material abundant,
Lower solubility and solution conductivity make the maximum system energy density and power density by biggish limitation.In water system
In, active material solubility is higher, and ion diffusion velocity is very fast.Therefore it is close to be highly desirable to develop a kind of novel high-energy
Degree, inexpensive water system flow battery.
Summary of the invention:
For overcome the deficiencies in the prior art, the constraint of traditional flow battery system is broken through, it is an object of the invention to mention
For a kind of high-energy density, the preparation method of the alkaline flow battery system of low cost, existing flow battery energy density is solved
The problems such as low, at high cost.The energy-storage battery that cost is far below all-vanadium flow battery can get using this method, there is open circuit electricity
The advantages that pressure is high, energy density is high, at low cost, stability is good.
Technical scheme is as follows:
A kind of preparation method of the alkaline flow battery system of high-energy density, low cost, includes the following steps and technique item
Part:
(1) aqueous solution of strong acid, highly basic and oxidant is prepared respectively in beaker with deionized water;
(2) Nafion membrane is immersed in the aqueous oxidizing agent solution of step (1), carries out constant temperature cleaning;
(3) Nafion membrane for obtaining step (2) impregnates in deionized water, carries out water bath with thermostatic control;
(4) step (3) obtained Nafion membrane is immersed in the strong acid aqueous solution of step (1), carries out constant temperature proton
Change;
(5) the obtained Nafion membrane of step (4) is impregnated in deionized water, carries out water bath with thermostatic control;
(6) step (5) obtained Nafion membrane is immersed in the strong alkali aqueous solution of step (1), carries out constant temperature ion
Change;
(7) step (6) obtained Nafion membrane is cleaned into pH=6~7 with deionized water, then immersed in deionized water
It is spare as amberplex;
(8) zine plate of 3~6mm of thickness is polished on sand paper, with washes of absolute alcohol it is clean after, with hair dryer drying be used as
The negative electrode material of battery;
(9) carbon felt of 3~8mm of thickness is used as to the positive electrode of battery;
(10) above-mentioned steps (1) prepared strong alkali aqueous solution, the electrolyte liquid as battery are taken;
(11) it takes permanganate to be dissolved in above-mentioned steps (1) prepared strong alkali aqueous solution, is made into the alkali of permanganate
Property aqueous solution, the anode electrolyte as battery;
(12) step (7), (8), (9), (10), (11) resulting critical material are assembled into alkaline oxygenated reducing solution galvanic electricity
Pond body system, is tested with battery test system.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, it is prepared in step (1)
Strong acid aqueous solution molar concentration is 0.5~2M, and strong alkali aqueous solution molar concentration is 0.5~2M, aqueous oxidizing agent solution molar concentration
For 0.5~2M;Used strong acid is HCl, HNO3、H2SO4One of, used highly basic is one of KOH, NaOH,
Used oxidant is H2SO4/HNO3(V/V=3:1), H2O2、HNO3One of.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (2), cleaning temperature
It is 50~120 DEG C, the time is 30~80min.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (3), bath temperature
It is 60~100 DEG C, water bath time is 40~80min.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (4), protonation temperature
Degree is 50~120 DEG C, and the time is 30~80min.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (5), bath temperature
It is 60~100 DEG C, water bath time is 40~80min.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (6), ionization temperature
Degree is 50~120 DEG C, and the time is 30~80min.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (8), zine plate thickness 4~
5mm, the sand paper of 120 mesh, dehydrated alcohol mass fraction are 65~98%.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (10), electrolyte
Liquid molar concentration is 2~6M.
The preparation method of the alkaline flow battery system of the high-energy density, low cost, in step (11), anolyte
The active material of liquid is the high manganese ion to appraise at the current rate, and prepared permanganate alkaline aqueous solution molar concentration is 0.1~5M,
Permanganate is KMnO4Or NaMnO4。
Design philosophy of the invention is:
Compared with electrolyte of vanadium redox battery, permanganate active material has high solubility, suitable under alkaline condition
Current potential, lower cost, excellent invertibity and many advantages, such as chemical property.For monomer, has no this collaboration and make
Use mechanism.The present invention prepares that a kind of stability is preferable, lower-cost permanganate anode electricity by the way that a large amount of highly basic is added
Solve liquid.Compared to expensive electrolyte of vanadium redox battery, it is applied to the flow battery of alkaline permanganic acid object-zine plate system, it can
To obtain a kind of preparation method of alkaline flow battery system of low cost.Nafion membrane (perfluorosulfonic acid proton exchange film) is through water-bath
After ionization processing, Nafion-H+Diaphragm is transformed into Nafion-Na+Type diaphragm can guarantee the normal transmission structure of specific ion
At the closed circuit of inside battery.Meanwhile the preferable chemical stability of Nafion membrane can guarantee stable cycle performance, improve
Battery life.Under alkaline condition, the zinc compared with negative electricity electrode potential makes the battery possess high open-circuit voltage, in turn, can obtain
Obtain the energy density of a superelevation.Therefore, the alkaline system electrolyte economic advantages excellent chemical property in addition, is conducive to
The research and development for instructing inexpensive flow battery, are pushed further into the process of industrialization of flow battery field energy storage.
Compared with prior art, the present invention have the advantages that it is following significant and the utility model has the advantages that
1. the present invention selects carbon felt as positive electrode, zine plate as negative electrode material, using the water of permanganate and highly basic
Solution successfully assembles the alkaline flow battery system of a kind of high-energy density, low cost, the battery system as positive and negative anodes electrolyte
Have many advantages, such as that good cycle, energy density are high, at low cost.
2. raw material used in the present invention is easy to get, is low in cost, operation is simple, it is suitble to extensive development.
The works such as equipment price is cheap, raw material is easy to get 3. whole preparation process of the invention has, process is simple, operation is convenient
Industry functionization feature helps to promote flow battery commercialized development.
In short, the present invention uses carbon felt for cell positive material, zine plate is cell negative electrode material, with permanganate, highly basic
Positive and negative anodes electrolyte of the solution as battery proposes the alkaline flow battery system of a kind of high-energy density, low cost.Battery has
Open-circuit voltage is high, high-efficient, the advantages that having extended cycle life, is at low cost.Raw material used in this system is easy to get, low in cost and fit
Extensive industrialized development is closed, is expected to develop a kind of inexpensive, high-energy density alkaline flow battery.
Detailed description of the invention:
Fig. 1 is the cyclic voltammogram of permanganate-zine plate flow battery.
Fig. 2 is the performance map of molar concentration 0.5M permanganate-zine plate flow battery.
Fig. 3 is the charging and discharging curve figure of molar concentration 0.5M permanganate-zine plate flow battery.
Fig. 4 is the performance map of molar concentration 1M permanganate-zine plate flow battery.
Specific embodiment:
In the specific implementation process, the present invention is using carbon felt as flow battery positive electrode, and zinc metal sheet or zine plate are as liquid
Galvanic battery negative electrode material.(such as: KMnO with permanganate4、NaMnO4Deng) alkaline aqueous solution as anode electrolyte, with highly basic
The alkaline aqueous solution of (such as: KOH, NaOH) is as electrolyte liquid, and treated that perfluorinated sulfonic acid proton is handed over using ionized
Change amberplex of the film (such as: Nafion117, Nafion212) as flow battery.To, obtain have low cost and
The alkaline oxygenated reduction flow battery system of high-energy density.
In the following, being described further in conjunction with example to the present invention.
Embodiment 1:
In the present embodiment, alkaline flow battery system the preparation method is as follows:
The ionization treatment process of 1.Nafion film (the present embodiment uses Nafion212), comprising the following steps:
(1) Nafion membrane of long 7.5cm, width 5.5cm are placed in the H of molar concentration 1M2O2In aqueous solution, in 80 DEG C of constant temperature
Under the conditions of clean 1h;
(2) by treated, Nafion membrane is placed in deionized water, is handled 40min in 60 DEG C of constant temperature, is obtained clean
Nafion membrane;
(3) above-mentioned clean Nafion membrane is placed in the aqueous hydrochloric acid solution of molar concentration 1M the matter under 80 DEG C of constant temperatures
Sonization 1h;
(4) Nafion membrane after protonation is placed in deionized water, handles 40min in 60 DEG C of constant temperature, obtains clean
Nafion membrane;
(5) above-mentioned clean Nafion membrane is placed in the sodium hydrate aqueous solution of molar concentration 1M in 80 DEG C of constant temperatures
Lower ionization 1h;
(6) by the Nafion membrane after ionization, after being cooled to room temperature, rinsed with deionized water to neutrality, be immersed in from
In sub- water, the amberplex as battery is spare;
2. the preparation of electrode material:
(1) zine plate of thick 5mm is polished on the sand paper of 120 mesh, the washes of absolute alcohol with mass fraction 75% is clean
It is dried up afterwards with hair dryer, the negative electrode material as battery.
(2) by the carbon felt of thick 5mm, the negative electrode material as battery.
3. the preparation of electrolyte:
(1) potassium permanganate is dissolved in the sodium hydrate aqueous solution of molar concentration 1M, until completely dissolved, obtains molar concentration
The alkaline aqueous solution of the potassium permanganate of 0.5M is sealed in positive fluid reservoir, the anode electrolyte as battery.
(2) sodium hydroxide is dissolved in deionized water, until completely dissolved, the sodium hydroxide for obtaining molar concentration 1M is water-soluble
Liquid is sealed in cathode fluid reservoir, the electrolyte liquid as battery.
In the present embodiment, using carbon felt as flow battery positive electrode, zinc metal sheet as flow battery negative electrode material, using from
Nafion membrane after sonization assembles potassium permanganate-zine plate system flow battery.Using the alkaline aqueous solution conduct of potassium permanganate
Potassium permanganate-zine plate system flow battery of anode electrolyte assembling has high battery efficiency, excellent cyclical stability.
The performance indicator of the present embodiment is as follows: the height assembled using the alkaline aqueous solution of potassium permanganate as anode electrolyte
Basically no attenuation, coulombic efficiency is up to 100% to discharge capacity to potassium manganate-zine plate system flow battery, energy after the circle of circulation 100
Amount efficiency is up to 80.60% or so.
Embodiment 2:
Difference from Example 1 is, the preparation of electrolyte:
(1) sodium permanganate is dissolved in the sodium hydrate aqueous solution of molar concentration 1.5M, until completely dissolved, acquisition mole is dense
The alkaline aqueous solution for spending the sodium permanganate of 1M, is sealed in positive fluid reservoir, the anode electrolyte as battery.
(2) sodium hydroxide is dissolved in deionized water, until completely dissolved, obtains the sodium hydroxide water of molar concentration 1.5M
Solution is sealed in cathode fluid reservoir until completely dissolved, the electrolyte liquid as battery.
In the present embodiment, using carbon felt as flow battery positive electrode, zinc metal sheet as flow battery negative electrode material, using from
Nafion membrane after sonization assembles sodium permanganate-zine plate system flow battery.Using the alkaline aqueous solution conduct of sodium permanganate
Sodium permanganate-zine plate system flow battery of anode electrolyte assembling has high battery efficiency, excellent cyclical stability.
The performance indicator of the present embodiment is as follows: the height assembled using the alkaline aqueous solution of sodium permanganate as anode electrolyte
Basically no attenuation, coulombic efficiency is up to 100% to discharge capacity to sodium manganate-zine plate system flow battery, energy after the circle of circulation 115
Amount efficiency is up to 86.43% or so.
As shown in Figure 1, can be seen that from potassium permanganate-zine plate flow battery round-robin method peace voltammogram using permanganic acid
The potassium permanganate that the alkaline aqueous solution of potassium is assembled as anode electrolyte-zine plate system flow battery possesses the voltage of 1.94V,
High voltage favorably obtains the flow battery of high-energy density.
As shown in Fig. 2, can be seen that from molar concentration 0.5M potassium permanganate-zine plate flow battery performance map using high
The potassium permanganate that the alkaline aqueous solution of potassium manganate is assembled as anode electrolyte-zine plate system flow battery is enclosed in circulation 100
Basically no attenuation, coulombic efficiency is up to 100% to discharge capacity, and energy efficiency is up to 80.60% or so afterwards.
As shown in figure 3, can be seen that from molar concentration 0.5M potassium permanganate-zine plate flow battery charging and discharging curve figure
Potassium permanganate-zine plate system the flow battery assembled using the alkaline aqueous solution of potassium permanganate as anode electrolyte is being recycled
Discharge capacity of the cell only fails 15mAh after 100 circles, and capacity retention ratio is up to 94%.
As shown in figure 4, can be seen that from molar concentration 1M sodium permanganate-zine plate flow battery performance map using Gao Meng
The sodium permanganate that the alkaline aqueous solution of sour sodium is assembled as anode electrolyte-zine plate system flow battery is after the circle of circulation 115
Basically no attenuation, coulombic efficiency is up to 100% to discharge capacity, and energy efficiency is up to 86.43% or so.
From above-described embodiment it is known that the Gao Meng assembled using the alkaline aqueous solution of permanganate as anode electrolyte
It is hydrochlorate-zine plate system flow battery good cycling stability, high-efficient.The flow battery system tool energy that the present invention is researched and developed is close
High, at low cost, the advantages that having extended cycle life is spent, can be widely applied for redox flow batteries energy storage field.Therefore, low
The commercialized development of the advantageous alkaline flow battery of cost and excellent performance.
Claims (10)
1. a kind of preparation method of the alkaline flow battery system of high-energy density, low cost, which is characterized in that include the following steps
And process conditions:
(1) aqueous solution of strong acid, highly basic and oxidant is prepared respectively in beaker with deionized water;
(2) Nafion membrane is immersed in the aqueous oxidizing agent solution of step (1), carries out constant temperature cleaning;
(3) Nafion membrane for obtaining step (2) impregnates in deionized water, carries out water bath with thermostatic control;
(4) step (3) obtained Nafion membrane is immersed in the strong acid aqueous solution of step (1), carries out constant temperature protonation;
(5) the obtained Nafion membrane of step (4) is impregnated in deionized water, carries out water bath with thermostatic control;
(6) step (5) obtained Nafion membrane is immersed in the strong alkali aqueous solution of step (1), carries out constant temperature ionization;
(7) step (6) obtained Nafion membrane is cleaned into pH=6~7 with deionized water, then immerses conduct in deionized water
Amberplex is spare;
(8) zine plate of 3~6mm of thickness is polished on sand paper, with washes of absolute alcohol it is clean after, with hair dryer drying be used as battery
Negative electrode material;
(9) carbon felt of 3~8mm of thickness is used as to the positive electrode of battery;
(10) above-mentioned steps (1) prepared strong alkali aqueous solution, the electrolyte liquid as battery are taken;
(11) it takes permanganate to be dissolved in above-mentioned steps (1) prepared strong alkali aqueous solution, is made into the alkaline water of permanganate
Solution, the anode electrolyte as battery;
(12) step (7), (8), (9), (10), (11) resulting critical material are assembled into alkaline oxygenated reduction flow battery body
System, is tested with battery test system.
2. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In, in step (1), prepared strong acid aqueous solution molar concentration is 0.5~2M, and strong alkali aqueous solution molar concentration is 0.5~2M,
Aqueous oxidizing agent solution molar concentration is 0.5~2M;Used strong acid is HCl, HNO3、H2SO4One of, it is used strong
Alkali is one of KOH, NaOH, and used oxidant is H2SO4/HNO3(V/V=3:1), H2O2、HNO3One of.
3. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In in step (2), cleaning temperature is 50~120 DEG C, and the time is 30~80min.
4. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In in step (3), bath temperature is 60~100 DEG C, and water bath time is 40~80min.
5. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In in step (4), protonation temperature is 50~120 DEG C, and the time is 30~80min.
6. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In in step (5), bath temperature is 60~100 DEG C, and water bath time is 40~80min.
7. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In in step (6), ionization temperature is 50~120 DEG C, and the time is 30~80min.
8. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In in step (8), 4~5mm of zine plate thickness, the sand paper of 120 mesh, dehydrated alcohol mass fraction is 65~98%.
9. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature exist
In in step (10), electrolyte liquid molar concentration is 2~6M.
10. the preparation method of the alkaline flow battery system of high-energy density according to claim 1, low cost, feature
It is, in step (11), the active material of anode electrolyte is the high manganese ion to appraise at the current rate, prepared permanganate alkalinity
Aqueous solution molar concentration is 0.1~5M, permanganate KMnO4Or NaMnO4。
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