CN111416129B - Acid-base asymmetric electrolyte zinc-quinone battery - Google Patents
Acid-base asymmetric electrolyte zinc-quinone battery Download PDFInfo
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- CN111416129B CN111416129B CN201910008050.7A CN201910008050A CN111416129B CN 111416129 B CN111416129 B CN 111416129B CN 201910008050 A CN201910008050 A CN 201910008050A CN 111416129 B CN111416129 B CN 111416129B
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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
- H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
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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
- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
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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
- H01M4/9075—Catalytic material supported on carriers, e.g. powder carriers
- H01M4/9083—Catalytic material supported on carriers, e.g. powder carriers on carbon or graphite
Abstract
The application discloses a zinc-quinone battery, which comprises an anode, a cathode, a diaphragm, an anolyte and a catholyte; wherein the cathode contains a cathode catalyst selected from at least one of quinone reversible redox reaction catalysts; the anode is metallic zinc; the anolyte is an alkaline solution, and the catholyte is an acidic solution containing quinone; the anolyte and the catholyte are separated by the membrane. The open-circuit voltage of the zinc-quinone battery is 1.95V, and the maximum power density is 315mW cm‑2At 10mA cm‑2The voltage difference value of current density charge and discharge is 200mV, the problems of poor reversibility and poor stability of the traditional zinc-quinone battery are solved, the open-circuit voltage and the power density of the battery are improved, and the zinc-quinone battery has great potential and good application prospect in the development aspect of improving the performance of energy storage and conversion equipment.
Description
Technical Field
The application relates to a zinc-quinone battery, and belongs to the field of chargeable and dischargeable batteries.
Background
The energy crisis and environmental pollution problems caused by excessive consumption of fossil energy have greatly promoted the development of new environmentally friendly renewable energy sources including wind, tidal, and solar energy. Recently, zinc-based batteries, particularly zinc ion batteries, zinc flow batteries, and zinc-air batteries have attracted considerable research interest to scientific researchers. Because of low price, safety, high efficiency and environmental protection, the zinc-air battery has strong competitiveness in the development of new energy in the future. However, there are still some problems to be solved in zinc-air batteries. The first thing is that the dynamics of the cathode of the battery is slow and the reversibility of the battery is poor. When the battery is discharged, the cathode generates oxygen reduction reaction; when the battery is charged, the battery undergoes an oxygen evolution reaction. Therefore, researchers are working on developing high-activity and high-stability cathode catalysts to reduce the voltage difference during the charge and discharge process and enhance the reversibility of the battery. Although the current density is improved to a certain extent, the result is not satisfactory, and the current density is 10mA cm-2The voltage difference between charging and discharging is still 0.7V.
Therefore, some alternative reactions are used in zinc-air batteries to enhance the reversibility and energy efficiency of zinc-air batteries. The quinone compound has good reversibility, high specific capacity, rich source and wide application foreground in zinc-base cell. The zinc-quinone battery solves the reversibility problem of the traditional zinc-air battery to a certain extent, but the further improvement of the performance of the zinc-quinone battery is still a challenge. First, the voltage ratio of zinc-quinone cells is low; second, in zinc-quinone batteries, the development of catalysts for the reversible redox reaction of quinones remains challenging, resulting in limited overall cell performance. In addition, zinc anodes operate stably under alkaline conditions, while quinones react more rapidly under acidic conditions. Electrolyte mismatch between the zinc anode and the quinone cathode will impair cell performance.
Disclosure of Invention
According to one aspect of the application, the zinc-quinone battery constructed by the acid-base asymmetric electrolyte is provided, the open-circuit voltage of the zinc-quinone battery is 1.95V, and the maximum power density of the zinc-quinone battery is 315mW cm-2At 10mA cm-2The voltage difference value of current density charge and discharge is 200mV, so that the problems of reversibility and stable stability of the traditional zinc-quinone battery are solved, the open circuit and power density of the battery are improved, the practicability and durability of the device are improved, and the device has great potential and good application prospect in the aspect of promoting the development of energy storage and conversion equipment.
The zinc-quinone battery is characterized by comprising an anode, a cathode, a diaphragm, an anolyte and a catholyte;
wherein the cathode contains a cathode catalyst selected from at least one of quinone reversible redox reaction catalysts;
the anode is metallic zinc;
the anolyte is an alkaline solution, and the catholyte is an acidic solution containing quinone;
the anolyte and the catholyte are separated by the membrane.
Specifically, the zinc-quinone cell comprises an anode, a cathode, a diaphragm, an anode compartment electrolyte and a cathode compartment electrolyte; wherein the cathode is carbon paper loaded with a catalyst with excellent catalytic performance on quinone reversible reduction oxidation reaction; the anode is metallic zinc;
the anolyte is an alkaline solution, and the catholyte is an acidic solution;
the anolyte and the catholyte are separated by the membrane.
Optionally, the anolyte contains at least one of the bases; the alkali is at least one of sodium hydroxide and potassium hydroxide;
the catholyte is an acid solution containing quinone; the acid in the catholyte is at least one selected from sulfuric acid and hydrochloric acid.
Optionally, the concentration of the alkali in the anolyte is 3.0 mol/L-5.0 mol/L;
optionally, the concentration of the quinone in the catholyte is 0.01mol/L to 0.1mol/L, and the concentration of the acid in the catholyte is 1.0mol/L to 3.0 mol/L.
Optionally, the anolyte is a 4.0mol/L sodium hydroxide solution;
the catholyte is a 2.0mol/L sulfuric acid solution containing 0.1mol/L benzoquinone or a 4.0mol/L sulfuric acid solution containing 0.1mol/L benzoquinone.
Specifically, the electrolyte in the anode chamber contains at least one of sodium hydroxide and potassium hydroxide; the electrolyte in the cathode chamber contains sulfuric acid.
Specifically, the electrolyte in the anode chamber is sodium hydroxide solution; the electrolyte of the cathode chamber is a sulfuric acid solution containing 0.1mol/L benzoquinone.
Specifically, the concentration of the sodium hydroxide solution is 3.0 mol/L-5.0 mol/L; the concentration of the sulfuric acid solution is 1.0 mol/L-3.0 mol/L.
Specifically, the concentration of the sodium hydroxide solution is 4.0 mol/L; the concentration of the sulfuric acid solution is 2.0 mol/L.
Optionally, the quinone reversible reduction oxidation reaction catalyst is selected from at least one of an ultrathin carbon nanosheet-supported hollow nickel trisulfide composite material, a carbon nanosheet-supported nickel trisulfide composite material or a carbon nanosheet.
Specifically, the quinone catalyst is selected from at least one of an ultrathin carbon nanosheet-supported hollow nickel trisulfide composite material, a carbon nanosheet-supported nickel trisulfide composite material or a carbon nanosheet.
Optionally, the membrane is a bipolar membrane.
Optionally, the anion exchange membrane surface of the membrane is opposite to the anolyte, and the cation exchange membrane surface is opposite to the catholyte.
Specifically, the anion exchange membrane of the bipolar membrane faces the anolyte, and the cation exchange membrane faces the catholyte.
Optionally, the cathode is a carbon paper loaded with a cathode catalyst.
Optionally, the carbon paper has a size of 4cm × 4cm to 4cm × 5 cm.
Alternatively, the carbon paper has dimensions of 4cm × 4cm, and the area of the carbon paper coated with the cathode catalyst is 1cm × 1 cm.
Optionally, the load capacity of the catalyst with catalytic activity for the p-quinone reversible reduction oxidation reaction on the carbon paper of the cathode is 0.5-1.5 mg/cm2。
Optionally, the load of the catalyst with catalytic activity for the quinone reversible reduction oxidation reaction on the carbon paper of the cathode is 1.0mg/cm2。
Specifically, the cathode is formed by supporting the quinone catalyst on carbon paper; the diaphragm is a bipolar membrane.
Specifically, the carbon paper has a size of 4cm × 4cm, and the area of the catalyst is 1cm × 1 cm.
As a specific embodiment, the specific process of forming the cathode electrode by supporting the quinone catalyst on the carbon paper is as follows:
and dispersing the quinone catalyst in a water/ethanol/sodium perfluorosulfonate (Nafion) mixed solution, fully performing ultrasonic treatment, dripping the mixture on carbon paper, and removing the solvent to obtain the cathode electrode.
According to another aspect of the present application, there is provided a use of the zinc-quinone battery in an electrochemical energy storage and conversion system.
The beneficial effects that this application can produce include at least:
1) the zinc-quinone battery is a cheap, safe and efficient electrochemical energy storage and conversion device, and has the advantages of high efficiency, high power, good reversibility, strong stability and the like.
2) The zinc-quinone battery provided by the application is simple to assemble, high in practical value and easy for industrial production.
Drawings
Fig. 1 is a morphology of a zinc-quinone battery cathode catalyst prepared in the present application, wherein (a) is a scanning electron microscope image of an ultrathin carbon nanosheet-supported hollow nickel trisulfide composite material, and (b) is a transmission electron microscope image of an ultrathin carbon nanosheet-supported hollow nickel trisulfide composite material.
Fig. 2 is a schematic diagram of a zinc-quinone cell of the present application.
FIG. 3 shows a zinc-quinone cell 1 in examples 1 and 2 of the present application#，2#Open circuit voltage versus time.
FIG. 4 shows a zinc-quinone battery 1 in examples 1 and 2 of the present application#、2#Polarization curve and power density test results.
FIG. 5 shows a zinc-quinone cell 1 of example 1 of the present application#The stability test results of (1).
FIG. 6 shows the electrocatalytic redox activity of p-benzoquinone with different catalysts in example 4 of the present application.
Detailed Description
The present application will be described in detail with reference to examples, but the present application is not limited to these examples.
Unless otherwise specified, the raw materials in the examples of the present application were purchased commercially and used without treatment; the test conditions of the instrument all adopt the parameters recommended by the manufacturer.
In the examples, the anode zinc plates were purchased from Jane's laboratory (Taobao).
In the examples, bipolar membranes were purchased from Beijing Runfan technology development Ltd.
In the examples, an electrochemical workstation of model CHI760E from Chenghua, Shanghai was used for the electrochemical performance measurement, and a battery tester of model CT2001A from Wuhan blue electric company was used for the battery performance measurement.
In the embodiment, the morphology characterization of the ultrathin carbon nanosheet-supported hollow nickel trisulfide composite material adopts a SU8010 field emission scanning electron microscope (5kV) of Hitachi and a F20 transmission electron microscope (200kV) of FEI.
In the embodiment, the composite material of the ultrathin carbon nanosheet-supported hollow nickel trisulfide is obtained by the following method:
(1)2g of nickel sulfate heptahydrate, 1g of glucose, 0.5g of urea and 10g of sodium chloride are fully ground;
(2) ball-milling the mixture in a ball mill for 10 h;
(3) calcining the mixture in a high-temperature furnace at 750 ℃ for 2h, and then washing the mixture to obtain a sample.
An electron microscope image of the composite material of the ultrathin carbon nanosheet-supported hollow nickel trisulfide is shown in fig. 1, wherein (a) is a scanning electron microscope image, and (b) is a transmission electron microscope image. The graphs (a) and (b) of fig. 1 show that a plurality of hollow nanoparticles are grown on the ultrathin carbon nanosheets, and the nanoparticles have a particle size distribution of 30-50 nm.
A schematic diagram of one embodiment of a zinc-quinone cell as described herein is shown in fig. 2, corresponding to example 1. The zinc-quinone cell comprises an anode zinc plate, a cathode, a diaphragm, an anode chamber electrolyte and a cathode chamber electrolyte; the electrolyte of the cathode chamber is 2.0mol/L H containing 0.1mol/L benzoquinone2SO4The electrolyte in the anode chamber was 4.0mol/L NaOH solution, Ec was 0.735V, and Ea was-1.285V.
Example 1
Comprising an anode, a cathode, an anolyte, a catholyte, and a separator.
Anode: using a 1X 1cm2The zinc plate of (1).
Cathode: dispersing 5mg of the ultrathin carbon nanosheet-supported hollow nickel trisulfide composite material in 500uL of water/ethanol/Nafion mixed solution (the volume ratio of water/ethanol/Nafion is 5:5:1), performing ultrasonic treatment for half an hour to obtain slurry, and dropwise coating 100uL of the slurry on a liquid-transferring gun with the area of 4 multiplied by 4cm2On the carbon paper of (2), the coating area is 1X 1cm2And the loading capacity of the composite material of the ultrathin carbon nanosheet loaded hollow nickel trisulfide is 1.0mg, so that the cathode electrode is obtained. Placing the cathode air diffusion electrode under an infrared lamp for dryingAnd baking and drying the mixture for battery assembly.
A diaphragm: a bipolar membrane is used.
The anolyte in the anode chamber and the catholyte in the cathode chamber are separated by the bipolar membrane, so that the catholyte anolyte is prevented from mixing and a neutralization reaction occurs. The anion exchange membrane of the bipolar membrane faces the anolyte, and the cation exchange membrane faces the anion electrolyte.
Anolyte: 4.0mol/L NaOH solution.
And (3) cathode electrolyte: 2.0mol/L H containing 0.1mol/L benzoquinone2SO4And (3) solution.
After assembling the zinc-quinone battery, 4.0mol/L NaOH solution and 2.0mol/L H containing 0.1mol/L benzoquinone are added2SO4The solutions were injected into the anode and cathode compartments, respectively, to obtain the zinc-quinone cell, denoted as zinc-quinone cell 1#。
Example 2
Comprising an anode, a cathode, an anolyte, a catholyte, and a separator.
Anode: using a 1X 1cm2The zinc plate of (1).
Cathode: dispersing 5mg of the ultrathin carbon nanosheet-supported hollow nickel trisulfide composite material in 500uL of water/ethanol/Nafion mixed solution (the volume ratio of water/ethanol/Nafion is 5:5:1), performing ultrasonic treatment for half an hour to obtain slurry, and dropwise coating 100uL of the slurry on a liquid-transferring gun with the area of 4 multiplied by 4cm2On the carbon paper of (2), the coating area is 1X 1cm2And the loading capacity of the composite material of the ultrathin carbon nanosheet loaded hollow nickel trisulfide is 1.0mg, so that the cathode electrode is obtained. And (4) placing the cathode air diffusion electrode under an infrared lamp, baking and drying, and then using for battery assembly.
A diaphragm: a bipolar membrane is used.
The anolyte in the anode chamber and the catholyte in the cathode chamber are separated by the bipolar membrane, so that the catholyte anolyte is prevented from mixing and a neutralization reaction occurs. The anion exchange membrane of the bipolar membrane faces the anolyte, and the cation exchange membrane faces the anion electrolyte.
Anolyte: 4.0mol/L NaOH solution.
And (3) cathode electrolyte: a 4.0mol/L NaOH solution containing 0.1mol/L benzoquinone.
After the zinc-quinone battery is assembled, 4.0mol/L NaOH solution and 4.0mol/L NaOH solution containing 0.1mol/L benzoquinone are respectively injected into an anode chamber and a cathode chamber to obtain the zinc-quinone battery, which is marked as a zinc-quinone battery 2#。
Example 3 electrochemical Performance measurement
Respectively to zinc-quinone battery 1#～2#And carrying out electrochemical test to obtain the discharge polarization curve, power density and stability results of each battery.
Wherein the battery 1#、2#The open circuit voltage results of (1) are shown in FIG. 3. As can be seen from FIG. 3#Is 1.95V, and the battery 2#The open circuit voltage of the electrolyte is only 1.2V, which shows that the asymmetric electrolyte design is beneficial to improving the open circuit voltage of the zinc-quinone battery.
EXAMPLE 4 catalytic benzoquinone Redox Activity assay
The specific experimental steps are as follows: 6uL of dispersion (volume ratio water/ethanol/Nafion ═ 8:1:1) was dropped on a glassy carbon electrode having a diameter of 3mm, and the catalyst material was dried naturally with a loading of 0.8mg/cm-2. The catalyst materials are respectively a composite material of ultrathin carbon nanosheet loaded hollow nickel trisulfide, a composite material of carbon nanosheet loaded nickel trisulfide and a carbon nanosheet electrode, which is marked as No. 1, No. 2 and No. 3 and serves as a working electrode. The redox quinone of the material is tested by using a three-electrode system, and the ultrathin carbon nanosheet carries the hollow nickel trisulfide composite material, namely the carbon nanoThe meter-piece-carried nickel disulfide, carbon nanosheet electrode as working electrode, graphite rod as counter electrode, silver/silver chloride as reference electrode, and test solution 1.0M H containing 1.0mM benzoquinone2SO4And (3) solution. Cyclic voltammetry tests (1 #, 2#, 3#) were performed on the material with an electrochemical workstation (chenhua CHI 760E). The cyclic voltammetry test conditions were: the electrode modified by the catalyst is a working electrode, silver/silver chloride is a reference electrode, a platinum mesh is a counter electrode, the test electrochemical window is 0-0.8V (relative to a silver/silver chloride reference electrode), and the sweep rate is 50 millivolts per second.
The test result is shown in FIG. 6, and the result shows that the composite material of the ultrathin carbon nanosheet-supported hollow nickel trisulfide has the best oxidation-reduction catalytic activity on quinone, the oxidation-reduction peak potential difference is 39mV, and the peak potential difference is 2.46mA cm-2。
Although the present application has been described with reference to a few embodiments, it should be understood that various changes, substitutions and alterations can be made herein without departing from the spirit and scope of the application as defined by the appended claims.
Claims (12)
1. A zinc-quinone battery comprising an anode, a cathode, a separator, an anolyte, and a catholyte;
wherein the cathode contains a cathode catalyst selected from at least one of quinone reversible redox reaction catalysts;
the anode is metallic zinc;
the anolyte is an alkaline solution, and the catholyte is an acidic solution containing quinone;
the anolyte and the catholyte are separated by the membrane;
the quinone reversible reduction oxidation reaction catalyst is selected from a composite material of carbon nanosheet-supported nickelous trisulfide.
2. The zinc-quinone battery of claim 1, wherein the anolyte comprises at least one of a base; the alkali is at least one of sodium hydroxide and potassium hydroxide;
the catholyte is an acid solution containing quinone; the acid in the catholyte is at least one selected from sulfuric acid and hydrochloric acid.
3. The zinc-quinone battery of claim 2, wherein the concentration of base in the anolyte is 3.0mol/L to 5.0 mol/L;
the concentration of the quinone in the catholyte is 0.01mol/L to 0.1mol/L, and the concentration of the acid in the catholyte is 1.0mol/L to 3.0 mol/L.
4. The zinc-quinone cell of claim 1, wherein the anolyte is a 4.0mol/L sodium hydroxide solution;
the catholyte is a 2.0mol/L sulfuric acid solution containing 0.1mol/L benzoquinone or a 4.0mol/L sulfuric acid solution containing 0.1mol/L benzoquinone.
5. The zinc-quinone battery of claim 1, wherein the separator is a bipolar membrane.
6. The zinc-quinone cell of claim 1, wherein the membrane has an anion exchange membrane side opposite the anolyte and a cation exchange membrane side opposite the catholyte.
7. The zinc-quinone cell of claim 1, wherein the cathode is a carbon paper loaded with a cathode catalyst.
8. The zinc-quinone cell of claim 7, wherein the carbon paper has dimensions of 4cm x 4cm to 4cm x 5 cm.
9. The zinc-quinone cell of claim 7, wherein the carbon paper has dimensions of 4cm x 4cm, and the area of the carbon paper coated with the cathode catalyst is 1cm x 1 cm.
10. The Zn-quinone cell of claim 7, wherein the loading amount of the cathode catalyst on the carbon paper of the cathode is 0.5 to 1.5mg/cm2。
11. The zinc-quinone cell of claim 7, wherein the cathode catalyst is supported on the carbon paper of the cathode at a loading of 1.0mg/cm2。
12. Use of a zinc-quinone cell as claimed in any one of claims 1 to 11 in an electrochemical energy storage and conversion system.
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| CN112909269A (en) * | 2021-01-18 | 2021-06-04 | 东华大学 | Preparation method and application of cathode material of metal-air battery |
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