CN113659150A - Composite dual-functional electrode for eutectic solvent electrolyte flow battery - Google Patents
Composite dual-functional electrode for eutectic solvent electrolyte flow battery Download PDFInfo
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- CN113659150A CN113659150A CN202110779237.4A CN202110779237A CN113659150A CN 113659150 A CN113659150 A CN 113659150A CN 202110779237 A CN202110779237 A CN 202110779237A CN 113659150 A CN113659150 A CN 113659150A
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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
- H01M4/96—Carbon-based electrodes
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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
- H01M4/8652—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites as mixture
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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
- 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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- 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
- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
- H01M2004/8694—Bipolar electrodes
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
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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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
The invention belongs to the technical field of flow batteries in electrochemical energy storage, and discloses a composite dual-function electrode for a eutectic solvent flow battery and application thereof. The dual-function electrode is a composite electrode consisting of an oxygen-enriched carbon material electrode and a metal-doped electrode, and integrates high electrocatalytic activity and high electrical conductivity. The oxygen-rich carbon material electrode is close to a diaphragm of the battery, and the metal doped electrode is close to a current collector of the battery; the two electrodes are vertically stacked and arranged to be used as a battery cathode, and the graphite felt, the graphite fiber or the carbon fiber is used as a battery anode. The electrode can effectively promote the oxidation-reduction reaction of the active material, accelerate the electron transfer process, further reduce the polarization of the battery and improve the power density and energy efficiency of the flow battery.
Description
Technical Field
The invention belongs to the technical field of flow batteries in electrochemical energy storage, and particularly relates to a composite dual-function electrode for a eutectic solvent electrolyte flow battery and application thereof.
Background
The large consumption of fossil energy causes resource shortage and environmental pollution, and renewable energy sources such as wind energy and solar energy are developed to alleviate this problem. In view of the defects of discontinuous and unstable power output and poor grid-connection performance of renewable energy sources, the development of an efficient and low-cost energy storage system is very important for the application of the renewable energy sources.
Among various energy storage technologies, the flow battery technology is considered to be the most promising technology in the large-scale energy storage technology due to the advantages of adjustable output power and energy storage capacity, environmental friendliness and the like. Flow batteries can be classified into aqueous and nonaqueous ones according to the electrolyte. The commercial development of the water-based flow battery is limited to a certain extent due to the low energy density and the narrow electrochemical window. The electrolyte of the nonaqueous flow battery not only can provide a wider electrochemical window, but also can improve the energy density of the battery.
The electrode is used as a key component of the flow battery, and the electrochemical activity of the electrode also has a certain influence on the performance of the battery. However, the energy efficiency and power density of the flow battery are limited by the defects of low electrochemical activity, poor kinetic reversibility, poor hydrophilicity and the like of the conventional graphite felt or carbon felt electrode. In order to improve the operation performance of the battery, it is necessary to improve the electrochemical activity of the electrode. In addition, the ionic conduction and electron transfer resistance in the battery is large due to the large viscosity of the battery electrolyte. Therefore, in order to promote the oxidation-reduction reaction and the electron transfer process on the surface of the electrode, the concept of the composite bifunctional electrode is utilized to improve the overall performance of the planar electrode.
In the deposition type flow battery disclosed in chinese patent application with publication No. CN 111509234a, which is mainly used in the currently published patent application, a gradient electrode is made with the porosity and deposition site of the electrode as the research objects to promote the uniform deposition of the active material and inhibit the growth of dendrites. For another example, in chinese patent No. CN 106558704B, graphite fibers with different bulk densities are used as research objects in an all-vanadium redox flow battery, and a needle punching method is used to reduce the bulk resistance of the electrode. The main difference of the invention is that electrochemical modification at different electrode parts is taken as a technical means, and different electrochemical modification methods are implemented according to the performance improvement requirements of different positions of the electrode. It is contemplated to combine a highly electrocatalytically active electrode on the proximal membrane side with a highly conductive electrode on the proximal current collector side to improve cell performance.
Disclosure of Invention
The invention aims to provide a composite dual-function electrode for a eutectic solvent flow battery and application thereof, which are used for improving the electrocatalytic activity and the conductivity of the electrode and obtaining a planar electrode with higher overall performance, thereby improving the power density and the energy efficiency of the battery. The invention can effectively improve the reaction rate of the electrode surface active material, can improve the electron transfer process in the reaction process and can improve the battery performance.
In order to achieve the purpose, the technical scheme of the invention is as follows:
a composite dual-function electrode for a eutectic solvent electrolyte flow battery comprises an oxygen-rich carbon material electrode and a metal doped electrode which are vertically arranged; the oxygen-rich carbon material electrode has high catalytic activity, the metal-doped electrode has high conductivity, and the composite dual-function electrode integrates high electrocatalytic activity and high conductivity.
The oxygen-enriched carbon material electrode is as follows: the graphite felt, the carbon paper, the graphite fiber or the carbon fiber are used as substrate materials and are obtained by one of high-temperature heat treatment, concentrated sulfuric acid treatment and hydrothermal oxidation;
the metal doped electrode is as follows: the material is obtained by taking graphite felt, carbon paper, graphite fiber or carbon fiber as a substrate material and carrying one of silver, copper and gold through electrodeposition.
Further, the electrodeposition method is one of direct current electrodeposition, pulsed electrodeposition, ultrasonic electrodeposition or jet electrodeposition; the plating solution selected in the electrodeposition process is single salt plating solution or complex plating solution; wherein the complex plating solution is any one of cyanide plating solution, hydroxide plating solution, pyrophosphate plating solution, lemon manganate plating solution and tartrate plating solution.
The composite dual-function electrode prepared by the invention is applied to a eutectic solvent electrolyte flow battery, and graphite felt, graphite fiber or carbon fiber is used as the anode of the battery; the composite bifunctional electrode is used as the cathode of the battery, wherein the oxygen-rich carbon material electrode of the composite bifunctional electrode is close to the diaphragm of the battery, and the metal-doped electrode is close to the current collector of the battery.
In the eutectic solvent electrolyte flow battery, the electrolyte comprises a eutectic solvent and an active material;
the eutectic solvent is a liquid formed by mixing organic salt and a hydrogen bond donor at the temperature of 80-100 ℃; wherein the organic salt is one of choline chloride, diethyl hydrochloride and aminoethanol; the hydrogen bond donor is one of ethylene glycol, urea, malonic acid and oxalic acid; the molar ratio of organic salt to hydrogen bond donor is 1: 2.
The positive active material added on the positive electrode side of the battery is one of bivalent manganese ions, tetravalent vanadium ions, bivalent iron ions and monovalent copper ions;
the negative electrode active material added on the negative electrode side of the battery is one of trivalent vanadium ions, trivalent chromium ions, divalent zinc ions, divalent copper ions and trivalent iron ions.
The diaphragm is an ion exchange membrane, preferably a perfluorinated sulfonic acid ion exchange membrane.
The invention mainly has the following positive and beneficial effects:
(1) the composite electrode with high electrocatalytic activity and high conductivity is adopted, the electrode structure is simple, the assembly is convenient, the composite electrode is safe and applicable, the effect is obvious, the dynamic polarization of the battery is reduced, the redox reaction of active ions is promoted, and the electron transmission rate in the reaction process is accelerated.
(2) The flow battery selects the eutectic solvent as the electrolyte, and can provide a wider electrochemical window, thereby being beneficial to further improving the energy density of the battery.
Drawings
FIG. 1 is a schematic structural view of a composite dual-function electrode of the eutectic solvent electrolyte flow battery of the present invention;
FIG. 2 is a graphical representation of the polarization curves and power densities for the single flow battery tests of example 1 and comparative example 1;
Detailed Description
The present invention will be described in detail below, but it should be understood that the practice of the invention is not limited to the following embodiments.
The electrode for the eutectic solvent flow battery is formed by compounding electrodes with high electrocatalytic activity and high conductivity, and comprises an oxygen-rich base carbon material electrode and a metal-doped electrode which are vertically arranged, and is shown in figure 1. Namely: the electrode which is close to the diaphragm side and made of oxygen-enriched carbon material has high catalytic activity, and the electrode which is close to the current collector side and made of high-conductivity metal is doped. The composite dual-function electrode is used as the negative electrode of the eutectic solvent flow battery, and the graphite felt is used as the positive electrode material, so that the redox reaction of active ions is promoted, the internal electron transmission performance is accelerated, and the electrode polarization is reduced.
The oxygen-rich base carbon material electrode is prepared with graphite felt, carbon paper, graphite fiber or carbon fiber as base material and through one of high temperature heat treatment, concentrated sulfuric acid treatment and hydrothermal oxidation.
The metal doped electrode is as follows: the high-conductivity electrode is obtained by depositing one of silver, copper and gold loaded by taking graphite felt, carbon paper, graphite fiber or carbon fiber as a substrate material in an electrodeposition mode.
When the battery is assembled, an oxygen-rich carbon-based material electrode is arranged on the side close to the diaphragm, and a metal-doped electrode is arranged on the side close to the current collector. The eutectic solvent formed by mixing organic salt and hydrogen bond donor at room temperature is used, and the battery positive active substance added at the positive side is one of bivalent manganese ions, tetravalent vanadium ions, bivalent iron ions and monovalent copper ions; the battery negative electrode active substance added at the negative electrode side is one of trivalent vanadium ions, trivalent chromium ions, divalent zinc ions, divalent copper ions and trivalent iron ions; the ion exchange membrane is a perfluorinated sulfonic acid ion exchange membrane.
Example 1
Graphite felt and carbon paper are used as electrode substrate materials, the thickness of the graphite felt electrode is 3mm, and the thickness of the carbon paper electrode is 0.19 mm. And washing the electrode with absolute ethyl alcohol and deionized water. And (3) placing the carbon paper electrode in a muffle furnace for heat treatment, raising the temperature to 500 ℃ at the heating rate of 5 ℃/min, and preserving the heat for 5 hours to obtain the carbon paper electrode modified by the heat treatment, wherein the treated carbon paper electrode has more oxygen-containing functional groups through X-ray photoelectron spectroscopy test, so that the oxygen-enriched carbon-based material electrode is obtained. The graphite felt electrode is used as a working electrode and a traditional three-electrode system is adopted for constant voltage deposition. The volume of the plating solution is 60ml, and the plating solution comprises 0.005M of copper sulfate and 0.004M of sodium citrate dihydrate to obtain the metal doped electrode. The deposition voltage was-1.0V. The electrochemical impedance spectrum test result shows that the charge transfer resistance of the deposited graphite felt electrode is 10.02 omega, and the charge transfer resistance of the original graphite felt electrode is 18.69 omega, which shows that electrons have faster transfer rate on the surface of the electrode.
A deposited graphite felt electrode with the size of 1cm multiplied by 1cm, namely a metal doped electrode, is placed on one side close to a current collector, and a heat-treated carbon paper electrode with the same size, namely an oxygen-enriched base carbon material electrode, is placed on one side close to a diaphragm close to the graphite felt. The composite electrode is used as the negative electrode of a flow battery. The positive electrode material is graphite felt.
The choline chloride and the ethylene glycol are selected according to a molar ratio of 1: the eutectic solvent which is uniformly mixed at the temperature of 2,100 ℃ is used as the electrolyte of the battery. The concentration of the positive electrode active material of the battery is 0.1mol-1Fe (b) of2+Adding into 50ml of eutectic solvent, mixing and preparing. The concentration of the battery negative electrode active material is 0.1mol-1V of3+Adding into 50ml of eutectic solvent, mixing and preparing. The ion exchange membrane of the cell is selected from Naffinion 212 diaphragm.
As shown in figure 2, the eutectic solvent iron vanadium redox flow battery adopting the composite dual-function electrode of the invention is at 2mA/cm2The power density of the battery reaches 12.71mW/cm2The limiting current density reaches 60mA/cm2。
Comparative example 1
Two cleaned and pretreated graphite felts with the thickness of 3mm and the size of 1cm multiplied by 1cm are respectively used as anode and cathode materials to be assembled in the eutectic solvent flow battery. The electrolyte selected by the battery is choline chloride and ethylene glycolAccording to a molar ratio of 1:2 a uniformly mixed eutectic solvent. The concentration of the positive electrode active material of the battery is 0.1mol-1Fe (b) of2+Adding into 50ml of eutectic solvent, mixing and preparing. The concentration of the battery negative electrode active material is 0.1mol-1V of3+Adding into 50ml of eutectic solvent, mixing and preparing. The ion exchange membrane of the cell is selected from Naffinion 212 diaphragm. As shown in figure 2, the eutectic solvent iron vanadium redox flow battery adopting the composite dual-function electrode of the invention is at 2mA/cm2The power density of the battery reaches 9.76mW/cm2The limiting current density reaches 45mA/cm2。
The results of the examples and the comparative examples show that the composite bifunctional electrode provided by the invention integrates high electrocatalytic activity and high electrical conductivity. By placing the electrode with rich oxygen and high catalytic activity close to the diaphragm side and placing the electrode with high conductivity close to the current collector side, the redox reaction of active substances is improved, the transfer rate of internal electrons is increased, the polarization of the electrode is reduced, and finally the performance of the battery is improved.
Finally, it should be noted that: the above examples are only for illustrating the technical solutions of the present invention, but not for limiting the same, i.e. it is not meant that the present invention must rely on the above detailed features and methods to be implemented. It will be apparent to those skilled in the art that any modifications, equivalent substitutions of materials and steps used in the present invention, as well as additions of auxiliary materials and steps, selection of specific means, etc., are within the scope and disclosure of the present invention.
Claims (8)
1. A composite dual-function electrode for a eutectic solvent electrolyte flow battery is characterized by comprising an oxygen-rich carbon material electrode and a metal-doped electrode which are vertically arranged;
the oxygen-enriched carbon material electrode is as follows: the graphite felt, the carbon paper, the graphite fiber or the carbon fiber are used as substrate materials and are obtained by one of high-temperature heat treatment, concentrated sulfuric acid treatment and hydrothermal oxidation;
the metal doped electrode is as follows: the material is obtained by taking graphite felt, carbon paper, graphite fiber or carbon fiber as a substrate material and carrying one of silver, copper and gold through electrodeposition.
2. A composite bifunctional electrode according to claim 1 wherein the electrodeposition method is one of galvanic electrodeposition, pulsed electrodeposition, ultrasonic electrodeposition or jet electrodeposition; the plating solution selected in the electrodeposition process is single salt plating solution or complex plating solution.
3. The composite bifunctional electrode as defined in claim 2 wherein the complex bath is any one of a cyanide bath, a hydroxide bath, a pyrophosphate bath, a lemon manganate bath, and a tartrate bath.
4. The composite bifunctional electrode of any one of claims 1 to 3 is applied to a eutectic solvent electrolyte flow battery, and is characterized in that graphite felt, graphite fibers or carbon fibers are used as a positive electrode of the battery; the composite dual-function electrode is used as a negative electrode of a battery, and the electrolyte comprises a eutectic solvent and an active substance;
wherein, the oxygen-rich carbon material electrode of the composite dual-function electrode is close to the diaphragm of the battery, and the metal doped electrode is close to the current collector of the battery.
5. The use according to claim 4, wherein the eutectic solvent is a liquid obtained by mixing an organic salt and a hydrogen bond donor at 80-100 ℃; wherein the organic salt is one of choline chloride, diethyl hydrochloride and aminoethanol; the hydrogen bond donor is one of ethylene glycol, urea, malonic acid and oxalic acid; the molar ratio of organic salt to hydrogen bond donor is 1: 2.
6. The use of claim 4, wherein the active materials comprise a positive electrode active material and a negative electrode active material,
the positive active material added on the positive electrode side of the battery is one of bivalent manganese ions, tetravalent vanadium ions, bivalent iron ions and monovalent copper ions;
the negative electrode active material added on the negative electrode side of the battery is one of trivalent vanadium ions, trivalent chromium ions, divalent zinc ions, divalent copper ions and trivalent iron ions.
7. The use of claim 4, wherein the membrane is an ion exchange membrane.
8. The use of claim 7, wherein the ion exchange membrane is a perfluorosulfonic acid ion exchange membrane.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2023169600A1 (en) * | 2022-03-11 | 2023-09-14 | 上海朗雄能源科技有限公司 | Flow battery stack or battery cell, electrode-diaphragm composite assembly and composite electrode structure thereof |
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Application publication date: 20211116 |