CN110265694B - Pteridine water system organic redox flow battery - Google Patents
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Abstract
The invention discloses a pteridine water system organic redox flow battery, which takes organic molecules containing pteridine structural formulas as a negative electrode; taking potassium ferrocyanide, TEMPO or potassium benzoquinone sulfonate as a positive electrode; one or more of acid solution, alkali solution and salt water solution are mixed to be used as electrolyte; taking a perfluorinated sulfonic acid-polytetrafluoroethylene copolymer membrane as an ion exchange membrane diaphragm; two copper plates are used as current collectors of the battery; a graphite plate with a flow channel is used as a flow field plate of the anode and the cathode; carbon paper, graphite felt or metal electrode is used as the electrode of the battery; the pteridine water system organic redox flow battery has the advantages of flexibility in power energy design, low cost, large-scale assembly and application and the like, and is very suitable for large-scale energy storage application.
Description
Technical Field
The invention belongs to the field of large-scale energy storage, and particularly relates to a pteridine aqueous organic redox flow battery.
Background
Since the first industrial revolution, the consumption of non-renewable resources such as fossil energy, petroleum, coal, etc. has increased year by year, bringing about an increasingly severe energy crisis, and the environmental damage and greenhouse effect of the contained sulfides, nitrogen oxides and greenhouse gases to the earth have become the crises that people have to face. The utilization and collection of clean and renewable resources such as wind, tidal and solar energy is considered as a solution to this problem, however the intermittent and spatio-temporal uncertainty of these energy sources and the impact of the huge fluctuations of the current at the peaks and valleys on the power grid prevents the further development and utilization of these energy technologies. Redox flow batteries are considered as a solution to this problem, as a low-cost, safe, and efficient energy storage device that can store wind energy, solar energy at peak values and then release energy at valley values, thereby providing the possibility for these new energy technologies to be incorporated into smart integrated power grids.
A typical flow battery includes several major components: a reservoir, a stack and a pump. The active substances of the flow battery are stored in the liquid storage tank, the flow battery reaches the battery stack under the driving of the pump, the redox reaction is carried out on the battery stack, electrons flow to an external circuit through the current collector, and through the large-scale production of the flow battery, the energy of the battery pack of the flow battery can reach megawatt level, so that the flow battery is suitable for large-scale energy storage technology.
In the prior art of the flow battery, the commercial application level is mainly the all-vanadium flow battery and the zinc-bromine flow battery, but the shuttling effect of metal ions to the membrane causes the efficiency reduction and the capacity degradation of the battery, and in addition, the aqueous solution of the acid electrolyte and bromine used in the battery has a corrosion effect on a liquid storage tank and a pipeline, and the safety performance of the device is yet to be further improved.
For aqueous organic redox flow batteries, the advantages are: 1. the energy and power of the battery can be flexibly designed and adjusted. The energy density depends on the volume of the liquid storage tank, and the larger the volume is, the more the solution is contained, the more the energy is; the power density depends on the area of the cell stack, and the larger the area is, the larger the allowed current is, and the larger the output power is under the condition of fixed voltage. The cell stack and the liquid storage tank are independent, the cell structure can be flexibly designed according to actual conditions, and the requirements of power and energy are regulated and controlled. 2. Compared with the traditional noble metal ion flow batteries such as all-vanadium flow batteries and iron-cadmium flow batteries, the cost of the organic active substance can be greatly reduced because the elements of the organic active substance are derived from carbon, nitrogen, oxygen, sulfur and other elements which are abundant in nature, and the organic active substance is suitable for large-scale energy storage. 3. For the water-based flow battery, the electrolyte is an aqueous solution, so that the water-based flow battery is safer and more environment-friendly compared with an organic solvent. The organic molecule has a variety of structures, and the electrode potential and the solubility of the active material can be greatly improved by grafting a functional group on a core structure and modifying the functional group, so that the working voltage and the energy density of the battery are finally improved.
In recent years, benzoquinone, TEMPO, viologen, oxazine and ferrocene active substances are reported to be used in aqueous organic flow batteries and show good electrochemical performance.
The pteridine active molecules are not reported to be used as the negative electrode of the aqueous organic flow battery.
Disclosure of Invention
The pteridine water system organic redox flow battery provided by the invention solves the problem that the cost of the existing flow battery is too high, and meanwhile, the pteridine active substances are not utilized to assemble a high-voltage water system organic flow battery in the prior art.
In order to achieve the purpose, the invention adopts the technical scheme that:
the pteridine water system organic redox flow battery provided by the invention takes organic molecules containing pteridine structural formulas as a negative electrode; taking potassium ferrocyanide, TEMPO or potassium benzoquinone sulfonate as a positive electrode; one or more of acid solution, alkali solution and salt water solution are mixed to be used as electrolyte; taking a perfluorinated sulfonic acid-polytetrafluoroethylene copolymer membrane as an ion exchange membrane diaphragm; two copper plates are used as current collectors of the battery; a graphite plate with a flow channel is used as a flow field plate of the anode and the cathode; carbon paper, graphite felt or metal electrode is used as the electrode of the battery.
Preferably, the solubility of the organic molecule comprising the pteridine structure in the electrolyte is 0.1 to 10 mol/L.
Preferably, the organic molecule comprising a pteridine formula is a pteridine or a pteridine derivative.
Preferably, the pteridine derivatives include folic acid, anhydrous theophylline and pteroic acid.
Preferably, the acidic aqueous solution is sulfuric acid, nitric acid, phosphoric acid or hydrochloric acid.
Preferably, the neutral aqueous solution is sodium chloride, potassium nitrate, potassium phosphate, potassium sulfate, sodium nitrate, sodium sulfate or sodium phosphate.
Preferably, the aqueous alkaline solution is potassium hydroxide, sodium hydroxide, lithium hydroxide or barium hydroxide.
Preferably, when the electrolyte is an alkaline aqueous solution, the positive electrode of the flow battery is a potassium ferrocyanide aqueous solution; when the electrolyte is a neutral aqueous solution, the anode of the flow battery is a TEMPO aqueous solution; when the electrolyte is an acidic aqueous solution, the positive electrode of the flow battery is a benzoquinone potassium sulfonate aqueous solution.
The method for assembling the pteridine water system organic redox flow battery comprises the following steps of:
taking an organic molecule containing a pteridine structural formula as a negative electrode; taking potassium ferrocyanide, TEMPO or potassium benzoquinone sulfonate as a positive electrode; one or more of acid solution, alkali solution and salt water solution are mixed to be used as electrolyte; the battery is sequentially assembled by a copper current collector, a graphite plate flow channel, a carbon paper/graphite felt electrode, a perfluorinated sulfonic acid-polytetrafluoroethylene copolymer film, a carbon paper/graphite felt electrode, a graphite plate flow channel and a copper current collector.
Compared with the prior art, the invention has the beneficial effects that:
according to the pteridine water system organic redox flow battery provided by the invention, organic molecules containing a pteridine structural formula are used as a negative electrode of the water system aerobic redox flow battery, and the pteridine active molecules can perform reversible redox reaction and have better reversibility and excellent dynamic performance. Particularly, under the alkaline electrolyte condition, the pteridine active material can show a relatively negative potential, and can be matched with a proper positive electrode to form a high-voltage aqueous organic flow battery. In addition, the pteridine active substances are widely existed in nature, and as the main constituent elements of pteridine molecules are carbon, nitrogen and oxygen, and the element sources are cheap and abundant, the cost of the pteridine aqueous organic redox flow battery after large-scale production and manufacture is greatly reduced compared with the existing heavy metal ion flow battery such as vanadium, and the pteridine aqueous organic redox flow battery can be used for large-scale energy storage technology.
Drawings
FIG. 1 shows the results of cyclic voltammetry tests of the folic acid solution prepared in example 1 of the present invention, using silver/silver chloride as a reference electrode, at sweep rates of 25mV/s, 50mV/s, 80mV/s and 100 mV/s.
FIG. 2 is a linear fit of the peak current and square root of sweep rate for different sweep rates of the folic acid solution prepared in example 1 of the present invention in cyclic voltammetry tests.
FIG. 3 shows the cyclic voltammetry test results of the anhydrous theophylline solution prepared in example 2 of the present invention, using silver/silver chloride as a reference electrode, at sweep rates of 25mV/s, 50mV/s, 80mV/s and 100 mV/s.
FIG. 4 is a linear fit of the peak current and square root of sweep rate for different sweep rates of the anhydrous theophylline solution prepared in example 2 of the present invention under cyclic voltammetry.
FIG. 5 shows the results of cyclic voltammetry tests of the pteroic acid solution prepared in example 3 of the present invention, using silver/silver chloride as a reference electrode, at sweep rates of 25mV/s, 50mV/s, 80mV/s and 100 mV/s.
FIG. 6 shows the linear fit of the peak current and the square root of the sweep rate for different sweep rates of the pteroic acid solution prepared in example 3 of the present invention under cyclic voltammetry.
Fig. 7 is a current-capacity-coulombic efficiency chart for different current discharge conditions of the assembled battery in example 4 of the present invention.
Fig. 8 is a current-capacity-coulombic efficiency chart for different current charging situations of the assembled battery in example 4 of the present invention.
Fig. 9 is a time-voltage curve of a second cycle of the assembled battery of example 6 of the present invention charged and discharged at a current of 25 mA.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings.
According to the pteridine water system organic redox flow battery provided by the invention, the redox reaction is carried out on the pteridine and the pteridine derivatives serving as negative active materials in the redox flow battery for charging and discharging; taking potassium ferrocyanide, TEMPO or potassium benzoquinone sulfonate as a positive electrode; one or more of an acidic aqueous solution, a neutral aqueous solution and an alkaline aqueous solution are mixed to be used as an electrolyte; the perfluorinated sulfonic acid-polytetrafluoroethylene copolymer membrane is used as an ion exchange membrane diaphragm, two copper plates are used as current collectors of the battery, a graphite plate with a flow channel is used as a flow field plate of a positive electrode and a negative electrode, and carbon paper or a graphite felt is used as an electrode of the battery.
The pteridine has the structural formula:
wherein, four nitrogen atoms are contained in the two aromatic rings, and two asymmetric nitrogen atoms can play a role in stabilizing the structure.
The structural formula of the pteridine derivative is as follows:
wherein R is1、R2、R3And R4Are the same or different and are each-N (CH)3)2、–NH2、–OCH3、–OH、–SH、–CH3、–SiH3、–F、–Cl、–C2H3、–CHO、＝O、–COOCH3、–CF3、–CN、–COOH、–PO3H2、–SO3H、–NO2-alkyl chains or-halogens.
The pteridine derivatives include folic acid, anhydrous theophylline and pteroic acid.
The solubility of the pteridine active substance in the electrolyte is 0.1-10 mol/L.
Wherein the acidic aqueous solution is sulfuric acid aqueous solution, nitric acid aqueous solution, phosphoric acid aqueous solution or hydrochloric acid aqueous solution.
The neutral aqueous solution is sodium chloride aqueous solution, potassium nitrate aqueous solution, potassium phosphate aqueous solution, potassium sulfate aqueous solution, sodium nitrate aqueous solution, sodium sulfate aqueous solution or sodium phosphate aqueous solution.
The alkaline aqueous solution is potassium hydroxide aqueous solution, sodium hydroxide aqueous solution, lithium hydroxide aqueous solution or barium hydroxide aqueous solution.
The pteridine compound can be derived from molecules existing in nature and prepared through addition reaction, substitution reaction and cyclization reaction.
When the electrolyte is an alkaline aqueous solution, the positive electrode of the flow battery is a potassium ferrocyanide aqueous solution; when the electrolyte is a neutral aqueous solution, the anode of the flow battery is a TEMPO aqueous solution; when the electrolyte is an acidic aqueous solution, the positive electrode of the flow battery is a benzoquinone potassium sulfonate aqueous solution.
The electrode material is graphite felt, carbon paper or metal electrode which is subjected to high-temperature heat-preservation annealing treatment or acidification pretreatment; the metal motor is one or more of gold electrode, platinum electrode and silver electrode.
A method for assembling a pteridine water system organic redox flow battery comprises the following steps: taking an organic molecule containing a pteridine structural formula as a negative electrode; taking potassium ferrocyanide, TEMPO or potassium benzoquinone sulfonate as a positive electrode; one or more of acid solution, alkali solution and salt water solution are mixed to be used as electrolyte; the battery is sequentially assembled by a copper current collector, a graphite plate flow channel, a carbon paper/graphite felt electrode, a perfluorinated sulfonic acid-polytetrafluoroethylene copolymer film, a carbon paper/graphite felt electrode, a graphite plate flow channel and a copper current collector.
Example 1
Dissolving folic acid in 30 ml of 1mol/L potassium hydroxide solution, oscillating and stirring the solution to form a uniform solution, and preparing 0.001mol/L folic acid solution. And (3) performing cyclic voltammetry test on the prepared electrolyte by using a three-electrode system, wherein silver/silver chloride is used as a reference electrode, a platinum electrode is used as a counter electrode, and a glassy carbon electrode is used as a working electrode. The sweep rates were 25mV/s, 50mV/s, 80mV/s and 100 mV/s.
From the CV data in fig. 1, under alkaline conditions, there are a pair of significantly reversible redox peaks, which are good in electrochemical reversibility, and when silver/silver chloride is used as a reference electrode, the folic acid has an average potential of-1V or less, and shows a relatively negative potential as a negative electrode material.
In fig. 2, the slope of the linear fit between the oxidation-reduction peak potential and the square root of the sweep rate is on the same order of magnitude, which proves that the folic acid molecules have reversible electrochemical performance, and the diffusion coefficients of the oxidation reaction and the reduction reaction are approximately the same and on the same order of magnitude.
Example 2
Weighing anhydrous theophylline, dissolving in 30 ml of 1mol/L potassium hydroxide solution, shaking and stirring to obtain a uniform solution, and preparing into 0.001mol/L folic acid solution. And (3) performing cyclic voltammetry test on the prepared electrolyte by using a three-electrode system, wherein silver/silver chloride is used as a reference electrode, a platinum electrode is used as a counter electrode, and a glassy carbon electrode is used as a working electrode. The sweep rates were 25mV/s, 50mV/s, 80mV/s and 100 mV/s.
From the CV data in fig. 3, a pair of significantly reversible redox peaks was observed under alkaline conditions, the electrochemical reversibility was good, and when silver/silver chloride was used as a reference electrode, the folic acid showed a relatively negative potential when the average potential was-1V or less as a negative electrode material.
In fig. 4, the slope of the linear fit between the oxidation-reduction peak potential and the square root of the sweep rate is on the same order of magnitude, which proves that the anhydrous theophylline molecule has reversible electrochemical performance, and the diffusion coefficients of the oxidation reaction and the reduction reaction are approximately the same and on the same order of magnitude.
Example 3
Weighing and dissolving the pteroic acid in 30 ml of 1mol/L potassium hydroxide solution, oscillating and stirring the solution to form a uniform solution, and preparing the 0.001mol/L folic acid solution. And (3) performing cyclic voltammetry test on the prepared electrolyte by using a three-electrode system, wherein silver/silver chloride is used as a reference electrode, a platinum electrode is used as a counter electrode, and a glassy carbon electrode is used as a working electrode. The sweep rates were 25mV/s, 50mV/s, 80mV/s and 100 mV/s.
From the CV data in fig. 5, a pair of significantly reversible redox peaks was observed under alkaline conditions, the electrochemical reversibility was good, and when silver/silver chloride was used as a reference electrode, the folic acid showed a relatively negative potential as a negative electrode material with an average potential of-1V or less.
In fig. 6, the slope of the linear fit between the oxidation-reduction peak potential and the square root of the sweep rate is on the same order of magnitude, which proves that the anhydrous theophylline molecule has reversible electrochemical performance, and the diffusion coefficients of the oxidation reaction and the reduction reaction are approximately the same and on the same order of magnitude.
Example 4
0.331g of folic acid is weighed and dissolved in 7.5 ml of 1mol/L potassium hydroxide solution, the solution is shaken and stirred, and after the solution is formed into a uniform solution, 0.1 mol/L folic acid solution is prepared to be used as a negative electrode. 0.845g of potassium ferrocyanide is weighed out and dissolved in 40 ml of 1mol/L oxyhydrogenStirring the potassium cyanide solution by oscillation, and preparing 0.05 mol/L potassium ferrocyanide solution as a positive electrode after the potassium cyanide solution forms a uniform solution. And introducing nitrogen into the electrolyte to remove oxygen, and then introducing the electrolyte into a flow battery device as a positive electrode and a negative electrode. The method comprises the following steps of acidizing the graphite felt or the carbon paper, specifically putting the graphite felt into 300ml of 1mol/L dilute salt, stirring for 3-5 hours, taking out, washing with deionized water, and drying for use. Using copper current collector-graphite plate flow channel-carbon paper/graphite felt electrode (5 cm)2) -perfluorosulfonic acid-polytetrafluoroethylene copolymer membrane-carbon paper/graphite felt electrode-graphite plate flow channel-copper current collector in sequence and position to assemble the cell, with liquid drive charging and discharging with peristaltic pump.
The battery is subjected to charge and discharge performance tests, the battery is charged by adopting 100mA of current, and is discharged by adopting 25mA, 50mA, 100mA, 150mA and 200mA of current, so that a capacity-current diagram can be obtained.
As shown in fig. 7, the high capacity can still be maintained under the large current discharge, and the coulomb efficiency is maintained above ninety percent, which proves that the high capacity can be operated and high energy can be output. Meanwhile, the capacity voltage diagram can be obtained by charging the battery at the current values of 25mA, 50mA, 100mA, 150mA and 200mA and discharging the battery at the current value of 25mA, as shown in figure 8, the folic acid solution can still maintain higher capacity under the condition of large-current charging, and the coulomb efficiency is maintained above ninety percent when the battery is charged and discharged at the current value of below 150mA, so that the work and the higher energy output are proved.
Example 5
0.331g of folic acid is weighed and dissolved in 7.5 ml of 1mol/L potassium hydroxide solution, the solution is shaken and stirred, and after the solution is formed into a uniform solution, 0.1 mol/L folic acid solution is prepared to be used as a negative electrode. 0.845g of potassium ferrocyanide is weighed and dissolved in 40 ml of 1mol/L potassium hydroxide solution, and the solution is stirred by oscillation to form a uniform solution, and then 0.05 mol/L potassium ferrocyanide solution is prepared to be used as a positive electrode. And introducing nitrogen into the electrolyte to remove oxygen, and then introducing the electrolyte into a flow battery device as a positive electrode and a negative electrode. Heat treating graphite felt or carbon paper, and is prepared through heating graphite felt in muffle furnace at five hundred deg.c for ten hr, cooling to room temperature and taking outAnd then directly used. Using copper current collector-graphite plate flow channel-carbon paper/graphite felt electrode (5 cm)2) -perfluorosulfonic acid-polytetrafluoroethylene copolymer membrane-carbon paper/graphite felt electrode-graphite plate flow channel-copper current collector in sequence and position to assemble the cell, with liquid drive charging and discharging with peristaltic pump.
The battery is tested for charging and discharging performance, and the charging and discharging test is carried out at the current of 100mA constant current.
Example 6
0.331g of folic acid is weighed and dissolved in 7.5 ml of 3mol/L potassium hydroxide solution, the solution is shaken and stirred, and after the solution is formed into a uniform solution, 0.1 mol/L folic acid solution is prepared to be used as a negative electrode. 0.845g of potassium ferrocyanide is weighed and dissolved in 40 ml of 3mol/L potassium hydroxide solution, and the solution is stirred by oscillation to form a uniform solution, and then 0.05 mol/L potassium ferrocyanide solution is prepared to be used as a positive electrode. And introducing nitrogen into the electrolyte to remove oxygen, and then introducing the electrolyte into a flow battery device as a positive electrode and a negative electrode. The graphite felt or the carbon paper is subjected to heat treatment, and the specific operation is that the graphite felt is placed in a muffle furnace, heated for ten hours at five hundred ℃, cooled to room temperature, taken out and then directly used. Using copper current collector-graphite plate flow channel-carbon paper/graphite felt electrode (5 cm)2) -perfluorosulfonic acid-polytetrafluoroethylene copolymer membrane-carbon paper/graphite felt electrode-graphite plate flow channel-copper current collector in sequence and position to assemble the cell, with liquid drive charging and discharging with peristaltic pump. The battery is subjected to charge and discharge performance test, and the charge and discharge test is carried out by adopting the current of 25 mA.
Fig. 9 shows the time-voltage curve of the second turn of the battery, which shows that the battery can work normally and stably and maintain higher coulomb efficiency.
Claims (9)
1. A pteridine-based aqueous organic redox flow battery is characterized in that an organic molecule containing a pteridine structural formula is used as a negative electrode; taking potassium ferrocyanide, TEMPO or potassium benzoquinone sulfonate as a positive electrode; an acidic aqueous solution, an alkaline aqueous solution or a neutral aqueous solution as an electrolyte; taking a perfluorinated sulfonic acid-polytetrafluoroethylene copolymer membrane as an ion exchange membrane diaphragm; two copper plates are used as current collectors of the battery; a graphite plate with a flow channel is used as a flow field plate of the anode and the cathode; carbon paper, graphite felt or metal electrode is used as the electrode of the battery.
2. The pteridine-based aqueous organic redox flow battery of claim 1, wherein the solubility of the organic molecule comprising the pteridine structural formula in the electrolyte is 0.1-10 mol/L.
3. The pteridine-based aqueous-organic redox flow battery of claim 1, wherein the organic molecule comprising the pteridine structural formula is a pteridine or a pteridine-based derivative.
4. The pteridine-based aqueous-organic redox flow battery of claim 3, wherein the pteridine-based derivative comprises folic acid, anhydrous theophylline, and pteroic acid.
5. The pteridine-based aqueous organic redox flow battery of claim 1, wherein the acidic aqueous solution is sulfuric acid, nitric acid, phosphoric acid, or hydrochloric acid.
6. The pteridine-based water-based organic redox flow battery of claim 1, wherein the neutral aqueous solution is sodium chloride, potassium nitrate, potassium phosphate, potassium sulfate, sodium nitrate, sodium sulfate, or sodium phosphate.
7. The pteridine-based aqueous organic redox flow battery of claim 1, wherein the basic aqueous solution is potassium hydroxide, sodium hydroxide, lithium hydroxide, or barium hydroxide.
8. The pteridine-based aqueous organic redox flow battery of claim 1, wherein when the electrolyte is an alkaline aqueous solution, the positive electrode of the flow battery is an aqueous potassium ferrocyanide solution; when the electrolyte is a neutral aqueous solution, the anode of the flow battery is a TEMPO aqueous solution; when the electrolyte is an acidic aqueous solution, the positive electrode of the flow battery is a benzoquinone potassium sulfonate aqueous solution.
9. A method for assembling a pteridine-based water-based organic redox flow battery, the method being characterized in that the pteridine-based water-based organic redox flow battery according to any one of claims 1 to 8 comprises the steps of:
taking an organic molecule containing a pteridine structural formula as a negative electrode; taking potassium ferrocyanide, TEMPO or potassium benzoquinone sulfonate as a positive electrode; an acidic aqueous solution, an alkaline aqueous solution or a neutral aqueous solution as an electrolyte; the battery is sequentially assembled by a copper current collector, a graphite plate flow channel, a carbon paper/graphite felt electrode, a perfluorinated sulfonic acid-polytetrafluoroethylene copolymer film, a carbon paper/graphite felt electrode, a graphite plate flow channel and a copper current collector.
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