CN103904352A - Zinc electrolyte for flow battery and preparation method thereof - Google Patents
Zinc electrolyte for flow battery and preparation method thereof Download PDFInfo
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- CN103904352A CN103904352A CN201410150815.8A CN201410150815A CN103904352A CN 103904352 A CN103904352 A CN 103904352A CN 201410150815 A CN201410150815 A CN 201410150815A CN 103904352 A CN103904352 A CN 103904352A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
The invention belongs to the large-scale energy storage flow battery technology in the field of electrochemical energy storage, and particularly relates to a zinc electrolyte for a flow battery and a preparation method thereof. The electrolyte consists of zinc sulfate, sodium acetate, acetic acid, water and an additive, wherein the additive is sodium methanesulfonate, and the mass ratio of the additive is 0.5-5% of the total weight of the electrolyte; the concentration of zinc sulfate in the zinc electrolyte is 1.0-2.5 mol/L, the concentration of sodium acetate is 1.0-3.0 mol/L, and the concentration of acetic acid is 1.0-3.0 mol/L; the optimum concentration ratio of sodium acetate to acetic acid is 1:1. A buffer solution can be formed by adding a large amount of acetic acid and sodium acetate, the initial state is faintly acid, the pH value of the zinc electrolyte in the operation process of the flow battery can be maintained between 2.0 and 6.0, the requirement of the zinc electrolyte in a faintly acid environment is met, and the energy efficiency of the battery can reach more than 70%.
Description
Technical Field
The invention belongs to the large-scale energy storage flow battery technology in the field of electrochemical energy storage, and particularly relates to a zinc electrolyte for a flow battery and a preparation method thereof.
Background
Zinc has the characteristics of low equilibrium potential, reversibility, aqueous electrolyte compatibility, low equivalent mass, high specific energy, high volumetric energy density, abundant resources, low cost, low toxicity, easy processing and the like, and is one of the most commonly used battery materials. Conventional batteries using zinc as a negative electrode include zinc-manganese batteries, zinc-carbon batteries, zinc-mercury oxide batteries, zinc-silver oxide batteries, zinc-air batteries, and the like.
A flow battery is an electrochemical system that can store energy on a large scale. It has a different battery structure from the conventional battery, with its active material not on the electrode but in the electrolyte; the structure features are similar to that of a fuel cell, but the production and manufacturing cost is lower than that of the fuel cell, and the production process is relatively simple compared with that of a lead-acid battery and the fuel cell. The flow battery can discharge deep heavy current, has high energy efficiency and megawatt power, has wide application field, can be used as an emergency standby power supply, a matched energy storage device of a new energy power generation system, a power grid peak regulation device and the like, and has the cost performance advantage exceeding that of a lithium ion battery and a nickel-hydrogen battery in the large-scale energy storage field.
Flow batteries using zinc as a negative active material include zinc-iron flow batteries, zinc-cerium flow batteries, zinc-vanadium flow batteries, and the like. Currently, the three kinds of flow battery negative electrolytes are generally zinc salt aqueous solutions or mixed solutions of zinc salt and strong acid, such as zinc sulfate solutions and mixed solutions of zinc sulfate and sulfuric acid. When the zinc sulfate aqueous solution is used as the negative electrolyte, the negative electrolyte is initially neutral, and the neutral environment can be rapidly damaged along with the charging process of the battery; because the protonic acid in the positive electrolyte enters the negative electrolyte through the ion exchange membrane. With the increase of the concentration of the protonic acid in the cathode electrolyte, the hydrogen evolution side reaction of the cathode is obviously enhanced, and the protonic acid and the electro-deposited zinc directly undergo a chemical reaction to release hydrogen. This not only destroys the initial composition of the positive and negative electrolytes, but also results in a more serious result in the inability to charge and discharge the battery. When a mixed solution of zinc sulfate and sulfuric acid is used as a negative electrode electrolyte, the deterioration of the battery performance is more rapid and severe. For this reason, some studies have been made to directly use an excessive amount of zinc sheet as a negative electrode, which temporarily solves the problem that the battery can be charged and cannot be discharged, but does not fundamentally solve the problems that the deposited zinc directly reacts with the protonic acid and the protonic acid releases hydrogen at the negative electrode. Therefore, the method of directly using the excessive zinc sheet as the cathode of the flow battery is not feasible in practical application. It is also attempted to use neutral aqueous solutions for both the electrolytes of the positive and negative electrodes, but this results in a sharp increase in the internal resistance of the cell, and the corresponding positive electrode pairs Fe (II)/Fe (III), ce (III)/Ce (IV) and V (IV)/V (V) of these three flow cells will not hydrolyze only in an acidic environment. Therefore, the problems that the electrolytes of the positive and negative electrodes both use neutral aqueous solutions cannot be solved fundamentally, and the electrolytes are unstable and the electrode reaction kinetics become slow are caused.
Disclosure of Invention
In order to solve the above problems, the present invention provides a zinc electrolyte for a flow battery and a method for preparing the same.
The technical scheme of the invention is as follows:
the zinc electrolyte for the flow battery consists of zinc sulfate, sodium acetate, acetic acid, water and an additive, wherein the additive is sodium methyl sulfonate, and the mass ratio of the additive to the total weight of the electrolyte is 0.5-5%.
The concentration of zinc sulfate in the zinc electrolyte is 1.0-2.5 mol/L, the concentration of sodium acetate is 1.0-3.0 mol/L, and the concentration of acetic acid is 1.0-3.0 mol/L.
The optimum concentration ratio of sodium acetate to acetic acid is 1:1.
A preparation method of a zinc electrolyte for a flow battery comprises the following steps:
firstly, weighing zinc carbonate with required amount, and putting the zinc carbonate into a beaker;
secondly, adding 6mol/L sulfuric acid solution into a beaker, fully stirring to ensure that the reaction is complete, and naturally cooling to room temperature;
then adding required amount of sodium acetate and acetic acid and additive, adding water to dilute to required concentration.
The zinc carbonate reacts with sulfuric acid to generate zinc sulfate, and the main components of the zinc electrolyte are zinc sulfate, sodium acetate, acetic acid and water. A buffer solution can be formed by adding a large amount of acetic acid and sodium acetate, the initial state is faintly acid, the pH value is 4.75, the pH value of the zinc electrolyte in the running process of the flow battery can be maintained between 2.0 and 6.0, and the requirement of the zinc electrolyte in a faintly acid environment is met.
In the zinc electrolyte of the present invention, an additive may be added to the solution in order to improve the conductivity and stability of the electrolyte. The additive is sodium methyl sulfonate, and the proportion of the additive is 0.5-5% of the total weight of the electrolyte.
The zinc electrolyte can be respectively matched with Fe (II)/Fe (III), ce (III)/Ce (IV) and V (IV)/V (V) under a strong acid environment to form a zinc-iron flow battery system, a zinc-cerium flow battery system and a zinc-vanadium flow battery system.
The key characteristic of the invention is that the zinc electrolyte contains a buffer system formed by acetic acid and sodium acetate. The buffer system is beneficial to the high concentration of zinc ions in the zinc electrolyte and can maintain the weak acidic environment required by the zinc electrolyte in the running process of the flow battery. The weak acidic environment is beneficial to slowing down the chemical corrosion rate of the metal zinc and the influence of hydrogen evolution side reaction on the performance of the battery. When the battery runs, when protons in the positive electrolyte penetrate through the cation exchange membrane and enter the zinc negative electrolyte, acetate and protonic acid are combined into acetic acid; when the battery runs reversely, the acetic acid can continuously release protons to permeate the cation exchange membrane to enter the electrolyte of the positive electrode. Thus, the contradiction between the difference requirement of the acidity environment of the positive and negative electrolyte when the battery runs and the requirement of proton conduction inside the battery is solved.
When the zinc electrolyte is applied to a zinc-iron flow battery, a zinc-cerium flow battery and a zinc-vanadium flow battery, the performance of the battery is obviously improved. The performance of the conventional zinc-iron flow battery is shown in figure 1, and the energy efficiency is 7.4%; the performance of the zinc-iron flow battery of the invention is shown in figure 2, and the energy efficiency is 83.4%. The performance of the conventional zinc-cerium flow battery is shown in fig. 3, and the energy efficiency is 7.3%; the performance of the zinc-cerium flow battery of the invention is shown in fig. 4, and the energy efficiency is 75.6%. The performance of the existing zinc-vanadium redox flow battery is shown in fig. 5, and the energy efficiency is 6.1%; the performance of the zinc-vanadium redox flow battery is shown in fig. 6, and the energy efficiency is 79.1%. The invention utilizes the buffer system formed by acetic acid and sodium acetate to effectively maintain the pH value of the zinc cathode electrolyte between 2.0 and 6.0 in the battery operation process, the pH value range enables the reaction of the electrodeposited zinc and the protonic acid to be very slow, and the hydrogen evolution side reaction of the protonic acid on the cathode is also effectively limited. (some research results also show that the energy efficiency of the battery can reach more than 70 percent if the negative electrode does not use carbon felt, but uses enough zinc sheets as the negative electrode, and the method is not feasible in practical application, because the method does not fundamentally solve the problems that the electro-deposited zinc directly reacts with protonic acid and the protonic acid is separated out from the negative electrode, the problem of the negative electrode is only temporarily covered and ignored, and the energy efficiency obtained by the method is not the same thing as the energy efficiency obtained by the invention.)
Drawings
Fig. 1 is a performance curve of a conventional zinc-iron flow battery.
Wherein the negative electrolyte is: 1.0mol/LZnSO 4 The positive electrolyte is: 1.0mol/LFeCl 2 +1mol/L H 2 SO 4 。
Fig. 2 is a graph of performance of a zinc-iron flow battery of the present invention.
Wherein the negative electrolyte is: 1.0mol/LZnSO 4 +1.0mol/L CH 3 COOH+1.0mol/L CH 3 COONa+0.5w%CH 3 SO 3 Na, positive electrolyte is: 1.0mol/LFeCl 2 +1mol/L H 2 SO 4 。
Fig. 3 is a performance curve of a conventional zinc-cerium flow battery.
Wherein the negative electrolyte is: 1.5mol/LZnSO 4 The positive electrolyte is: 1.0mol/LCe (CH) 3 SO 3 ) 3 +2mol/LCH 3 SO 3 H。
Fig. 4 is a performance curve of the zinc-cerium flow battery of the invention.
Wherein the negative electrolyte is: 1.5mol/LZnSO 4 +2.0mol/L CH 3 COOH+2.0mol/L CH 3 COONa+2.0w%CH 3 SO 3 Na, positive electrolyte is: 1.0mol/LCe (CH) 3 SO 3 ) 3 +2mol/L CH 3 SO 3 H。
Fig. 5 is a performance curve of a conventional zinc-vanadium flow battery.
The negative electrode electrolyte comprises: 2.5mol/LZnSO 4 The positive electrolyte is: 1.0mol/LVOSO 4 +2mol/LH 2 SO 4 。
Fig. 6 is a performance curve of the zinc-vanadium flow battery of the invention.
Wherein the negative electrolyte is: 2.5mol/LZnSO 4 +3.0mol/L CH 3 COOH+3.0mol/L CH 3 COONa+5.0w%CH 3 SO 3 Na, positive electrolyte is: 1.0mol/LVOSO 4 +2mol/L H 2 SO 4 。
Detailed Description
The invention mainly comprises zinc electrolyte taking sodium acetate and acetic acid buffer solution as supporting media, and a zinc-iron flow battery, a zinc-cerium flow battery and a zinc-vanadium flow battery taking the zinc electrolyte as negative electrolyte. The present invention is further described in the following detailed description with reference to specific examples, which should not be construed as limiting the invention, but rather as the technology described above may be modified, substituted or altered in many ways to achieve the desired results within the scope of the invention.
EXAMPLE 1 100mL1.0mol/LZnSO was prepared 4 +1.0mol/L CH 3 COOH+1.0mol/L CH 3 COONa+0.5w%CH 3 SO 3 Na zinc electrolyte.
Weighing 12.4 g of zinc carbonate, and transferring into a 250mL beaker;
adding 16.7mL6mol/LH into the beaker 2 SO 4 Fully reacting the solution;
adding 20mL of 5mol/LCH 3 COOH solution in the beaker;
8.2 g of CH are weighed 3 COONa is poured into the beaker, and stirred to be completely dissolved;
0.5 g of CH are weighed out 3 Pouring SONa into the beaker, and stirring to completely dissolve the SONa;
transferring the solution into a 100mL volumetric flask, and adding distilled water to a constant volume to obtain the solution required to be prepared.
EXAMPLE 2 preparation of 100mL1.5mol/LZnSO 4 +2.0mol/L CH 3 COOH+2.0mol/L CH 3 COONa+2.0w%CH 3 SO 3 Na zinc electrolyte.
Weighing 18.6 g of zinc carbonate, and transferring into a 250mL beaker;
25.0mL6mol/LH is added into the beaker 2 SO 4 Fully reacting the solution;
adding 20mL of 10mol/LCH 3 COOH solution in the beaker;
16.4 g CH are weighed 3 COONa is poured into the beaker, and stirred to be completely dissolved;
2.0 g of CH are weighed 3 Pouring SONa into the beaker, and stirring to completely dissolve the SONa;
transferring the solution into a 100mL volumetric flask, and adding distilled water to a constant volume to obtain the solution required to be prepared.
EXAMPLE 3 100mL2.5mol/LZnSO 4 +3.0mol/L CH 3 COOH+3.0mol/L CH 3 COONa+5.0w%CH 3 SO 3 Na zinc electrolyte.
Weighing 31.0 g of zinc carbonate, and transferring into a 250mL beaker;
41.7mL6mol/LH is added to the beaker 2 SO 4 Fully reacting the solution;
adding 30mL of 10mol/LCH 3 COOH solution in the beaker;
24.6 g CH are weighed 3 COONa is poured into the beaker, and stirred to be completely dissolved;
5.0 g of CH are weighed 3 SONa is poured into the beaker, and is stirred to be completely dissolved;
transferring the solution into a 100mL volumetric flask, and adding distilled water to a constant volume to obtain the solution required to be prepared.
Example 4 Performance testing of existing Zinc-iron flow batteries
The Nafion115 membrane separates the positive and negative electrode chambers of the zinc-iron flow battery; the carbon felt is used as a positive electrode and a negative electrode, and the apparent areas of the positive electrode and the negative electrode are both 5cm 2 . The electrolyte of the negative electrode is 100mL1.0mol/LZnSO 4 The positive electrode electrolyte is 100mL of 1mol/LFeCl 2 +1mol/LH 2 SO 4 . The charging and discharging current is 100mA, and the flow rate of the electrolyte is 20mL/min. The coulombic efficiency of the battery was 9.5%, the voltage efficiency was 77.6%, and the energy efficiency was 7.4%. The charge and discharge performance is shown in fig. 1.
Example 5 performance testing of a zinc-iron flow battery of the invention
The Nafion115 membrane separates the positive and negative electrode chambers of the zinc-iron flow battery; the carbon felt is used as a positive electrode and a negative electrode, and the apparent areas of the positive electrode and the negative electrode are both 5cm 2 . The electrolyte of the negative electrode is 100mL1.0mol/LZnSO 4 +1.0mol/L CH 3 COOH+1.0mol/L CH 3 COONa+0.5w%CH 3 SO 3 Na, positive electrode electrolyte 100mL1mol/LFeCl 2 +1mol/L H 2 SO 4 . The charging and discharging current is 100mA, and the flow rate of the electrolyte is 20mL/min. The coulombic efficiency of the battery is 99.2%, the voltage efficiency is 84.1%, and the energy efficiency is 83.4%. The charge and discharge performance is shown in fig. 2.
Example 6 testing of performance of a current zinc cerium flow battery.
The Nafion115 membrane separates the positive and negative electrode chambers of the zinc-cerium flow battery; the carbon felt is used as a positive electrode and a negative electrode, and the apparent areas of the positive electrode and the negative electrode are both 5cm 2 . The electrolyte of the negative electrode is 100mL1.5mol/LZnSO 4 The anode electrolyte is 100mL and 1mol/LCe (CH) 3 SO 3 ) 3 +2mol/L CH 3 SO 3 H. The charging and discharging current is 100mA, and the flow rate of the electrolyte is 20mL/min. The coulombic efficiency of the battery was 9.1%, the voltage efficiency was 80.1%, and the energy efficiency was 7.3%. The charge and discharge performance is shown in fig. 3.
Example 7 testing of the performance of zinc cerium flow batteries of the present invention.
The Nafion115 membrane separates the positive and negative electrode chambers of the zinc-cerium flow battery; the carbon felt is used as a positive material,A negative electrode having an apparent area of 5cm 2 . The electrolyte of the negative electrode is 100mL1.5mol/LZnSO 4 +2.0mol/L CH 3 COOH+2.0mol/L CH 3 COONa+2.0w%CH 3 SO 3 Na, positive electrode electrolyte 100mL1mol/LCe (CH) 3 SO 3 ) 3 +2mol/L CH 3 SO 3 H. The charging and discharging current is 100mA, and the flow rate of the electrolyte is 20mL/min. The coulombic efficiency of the cell was 90.3%, the voltage efficiency was 83.7%, and the energy efficiency was 75.6%. The charge and discharge performance is shown in fig. 4.
Example 8 testing of performance of existing zinc vanadium flow batteries.
The Nafion115 membrane separates the positive and negative electrode chambers of the zinc-vanadium flow battery; the carbon felt is used as a positive electrode and a negative electrode, and the apparent areas of the positive electrode and the negative electrode are both 5cm 2 . The electrolyte of the negative electrode is 100mL2.5mol/LZnSO 4 The anode electrolyte is 100mL and 1mol/LVOSO 4 +2mol/LH 2 SO 4 . The charging and discharging current is 100mA, the flow rate of the electrolyte is 20mL/min, the coulombic efficiency of the battery is 7.6%, the voltage efficiency is 80.4%, and the energy efficiency is 6.1%. The charge and discharge performance is shown in fig. 5.
Example 9 testing of the performance of zinc vanadium flow batteries of the invention.
The Nafion115 membrane separates the positive and negative electrode chambers of the zinc-vanadium flow battery; carbon felt is used as a positive electrode and a negative electrode, and the apparent areas of the positive electrode and the negative electrode are both 5cm 2 . The electrolyte of the negative electrode is 100mL2.5mol/LZnSO 4 +3.0mol/L CH 3 COOH+3.0mol/L CH 3 COONa+5.0w%CH 3 SO 3 Na, 100mL of 1mol/LVOSO as positive electrode electrolyte 4 +2mol/L H 2 SO 4 . The charging and discharging current is 100mA, the flow rate of the electrolyte is 20mL/min, the coulombic efficiency of the battery is 93.0%, the voltage efficiency is 85.1%, and the energy efficiency is 79.1%. The charge and discharge performance is shown in fig. 6.
Claims (4)
1. A zinc electrolyte for a flow battery is characterized in that: the electrolyte consists of zinc sulfate, sodium acetate, acetic acid, water and an additive, wherein the initial state of the electrolyte is weak acid, the pH value is 4.75, the pH value is maintained between 2.0 and 6.0 in the running process of the battery, the additive is sodium methanesulfonate, and the mass ratio of the additive is 0.5 to 5 percent of the total weight of the electrolyte.
2. The zinc electrolyte for a flow battery according to claim 1, wherein: the concentration of zinc sulfate in the zinc electrolyte is 1.0-2.5 mol/L, the concentration of sodium acetate is 1.0-3.0 mol/L, and the concentration of acetic acid is 1.0-3.0 mol/L.
3. The zinc electrolyte for a flow battery according to claim 1 or 2, characterized in that: the optimum concentration ratio of sodium acetate to acetic acid is 1:1.
4. A preparation method of a zinc electrolyte for a flow battery comprises the following steps:
firstly, weighing zinc carbonate with required amount, and putting the zinc carbonate into a beaker;
secondly, adding 6mol/L sulfuric acid solution into a beaker, fully stirring to ensure that the reaction is complete, and naturally cooling to room temperature;
then adding required amount of sodium acetate, acetic acid and additive, adding water to dilute to required concentration; wherein the concentration of zinc sulfate is 1.0-2.5 mol/L, the concentration of sodium acetate is 1.0-3.0 mol/L, the concentration of acetic acid is 1.0-3.0 mol/L, and the optimal concentration ratio of sodium acetate to acetic acid is 1:1; the zinc electrolyte is weakly acidic, and the pH value can be maintained between 2.0 and 6.0 when the battery operates.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105826587A (en) * | 2016-03-26 | 2016-08-03 | 江西理工大学 | Iron-based ionic liquid electrolyte for flow cell positive electrode and preparation method thereof |
| CN105914400A (en) * | 2016-05-04 | 2016-08-31 | 中国科学技术大学 | Electrolyte and sodium-ion battery |
| CN110770949A (en) * | 2017-05-01 | 2020-02-07 | 赛伦能源公司 | Electrolyte additive for zinc metal electrodes |
| CN113013460A (en) * | 2019-12-19 | 2021-06-22 | 中国科学院大连化学物理研究所 | Negative electrolyte for alkaline zinc-iron flow battery and zinc-iron flow battery |
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| CN101635363A (en) * | 2008-07-27 | 2010-01-27 | 比亚迪股份有限公司 | Vanadium ion redox flow battery electrolyte, preparation method thereof and battery thereof |
| CN102201590A (en) * | 2011-04-22 | 2011-09-28 | 北京化工大学 | Acidic zinc single liquid flow energy storage battery |
| CN103545578A (en) * | 2013-09-30 | 2014-01-29 | 刘甲祥 | Electrolyte of magnesium air battery |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101635363A (en) * | 2008-07-27 | 2010-01-27 | 比亚迪股份有限公司 | Vanadium ion redox flow battery electrolyte, preparation method thereof and battery thereof |
| CN102201590A (en) * | 2011-04-22 | 2011-09-28 | 北京化工大学 | Acidic zinc single liquid flow energy storage battery |
| CN103545578A (en) * | 2013-09-30 | 2014-01-29 | 刘甲祥 | Electrolyte of magnesium air battery |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105826587A (en) * | 2016-03-26 | 2016-08-03 | 江西理工大学 | Iron-based ionic liquid electrolyte for flow cell positive electrode and preparation method thereof |
| CN105826587B (en) * | 2016-03-26 | 2018-04-10 | 江西理工大学 | A kind of flow battery positive pole iron-based ionic liquid electrolyte and preparation method thereof |
| CN105914400A (en) * | 2016-05-04 | 2016-08-31 | 中国科学技术大学 | Electrolyte and sodium-ion battery |
| CN110770949A (en) * | 2017-05-01 | 2020-02-07 | 赛伦能源公司 | Electrolyte additive for zinc metal electrodes |
| CN113013460A (en) * | 2019-12-19 | 2021-06-22 | 中国科学院大连化学物理研究所 | Negative electrolyte for alkaline zinc-iron flow battery and zinc-iron flow battery |
| CN113013460B (en) * | 2019-12-19 | 2022-06-14 | 中国科学院大连化学物理研究所 | Negative electrolyte for alkaline zinc-iron flow battery and zinc-iron flow battery |
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