CN113036233B - Zinc-based single cell electrode structure and application - Google Patents
Zinc-based single cell electrode structure and application Download PDFInfo
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- CN113036233B CN113036233B CN201911250090.9A CN201911250090A CN113036233B CN 113036233 B CN113036233 B CN 113036233B CN 201911250090 A CN201911250090 A CN 201911250090A CN 113036233 B CN113036233 B CN 113036233B
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/36—Accumulators not provided for in groups H01M10/05-H01M10/34
- H01M10/38—Construction or manufacture
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/36—Accumulators not provided for in groups H01M10/05-H01M10/34
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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
- Y02E60/10—Energy storage using batteries
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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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
A zinc-based battery electrode structure is characterized in that the surface of an electrode is designed into a concave-convex structure, and the structure can be independently applied to a battery anode or a battery cathode; the structure can also be simultaneously applied to the cross coupling of the positive electrode and the negative electrode. The design method of the electrode surface structure enables the charge and discharge surface capacity, the energy density and the cycle life of the battery to be obviously improved. The electrode has the advantages of simple structure and simple processing and manufacturing process.
Description
Technical Field
The invention relates to a novel zinc-based battery electrode.
Technical Field
The zinc-based battery system is an energy storage system with low cost, high energy density, long service life, environmental friendliness and high safety, and is mainly applied to the fields of power grid peak shaving, power generation of renewable energy sources such as wind energy and solar energy, electric automobiles and the like. The zinc-based battery system mainly comprises a zinc ion battery, a zinc ion capacitor, a zinc-nickel battery, a zinc-air battery and a zinc-based flow battery system (a zinc-nickel flow battery, a zinc-iron flow battery, a zinc-iodine flow battery, a zinc-bromine flow battery and the like) thereof. The method is characterized in that the negative electrode part utilizes the deposition and dissolution reaction of zinc, so the electrode structure of the zinc-based battery plays a very critical role in the performance of the battery.
The structural design of the novel zinc-based battery aims at the problems of low surface capacity, poor circulation stability, easy formation of dendrite and the like of the zinc-based battery, combines the working characteristics of the zinc-based battery, increases the specific surface area of a macroscopic structure by changing the surface structure of a macroscopic electrode, and adjusts the deposition mode of zinc. The structure can effectively increase the deposition amount of zinc and improve the energy density; the influence of the zinc dendrite on the cycling stability of the battery can be effectively reduced, and the coulomb efficiency and the cycle life of the battery are improved.
Compared with the microcosmic and chemical structural design of other electrode structures, the method has more remarkable effect of improving the battery performance, is simple in operation process and can be realized only by using a mechanical processing method; the usage amount of the electrode material can be reduced, and the economic benefit is improved.
Disclosure of Invention
According to the invention, the working principle of the zinc-based battery and the structural characteristics of the battery are combined, the rugged macrostructure design is carried out on the surface of the electrode, and the macroscopical three-dimensional surface is constructed, so that the deposition behavior of zinc on the electrode is effectively adjusted, and further, the energy density, the coulombic efficiency and the cycle life of the battery are improved.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
the electrode surface macrostructure is shown in fig. 6. The concave-convex structure on the surface of the electrode has the characteristic of uniform size. The convex structures and the concave structures have the characteristic of being capable of being coupled in a staggered mode (namely, if the positive electrode and the negative electrode are coupled in a staggered mode, the relative positions of the convex structures or the concave structures are consistent and symmetrical). Fig. 7 shows a method for coupling the positive electrode and the negative electrode in a staggered manner.
The invention has the beneficial effects that:
aiming at the problems of low surface capacity, poor circulation stability and the like of the water system zinc-based battery, the invention increases the surface area of the electrode by designing a macroscopic uneven structure on the surface of the electrode, so that the deposition amount of zinc of the negative electrode is increased, and the active area effectively utilized by the positive electrode is increased. The energy density, the coulomb efficiency and the cycle life of the battery can be effectively improved. The electrode is simple in structural design and processing, can be produced in batches, can improve the cycling stability of the zinc-based battery, and promotes the development of the zinc-based battery.
Drawings
Fig. 1 general dimensions of each of the electrode structure designs described.
FIG. 2 is a schematic diagram of the electrode structure design.
FIG. 3 is a schematic view of the structure of the method for using the positive and negative electrodes
Figure 4. Cycling performance of untreated carbon felt.
Figure 5 is a first charge and discharge curve for untreated carbon felt.
Fig. 6 shows the cycling performance of positive and negative electrodes using carbon felt with a concave-convex design.
Fig. 7 shows the first charge-discharge curves of positive and negative electrodes using carbon felt with a concave-convex design.
Detailed Description
A zinc-based single cell electrode structure comprises a positive electrode, a diaphragm and a negative electrode which are sequentially stacked, wherein the positive electrode and the negative electrode are provided with groove structures.
Defining two directions of an X axis and a Y axis which are vertical to each other on a reference plane by taking a contact surface of the electrode and the diaphragm as the reference plane; defining a direction perpendicular to the surface of the electrode and away from the diaphragm as a Z-axis direction; wherein the electrodes comprise a positive electrode and a negative electrode.
More than two groups of groove rows which are spaced are uniformly arranged on the surface of the positive electrode facing the diaphragm along the X-axis direction, each X-axis groove row comprises more than 2 grooves which are sequentially spaced along the Y-axis direction, except the grooves, the original surface of the electrode facing the diaphragm is reserved to form an island surface A, and the geometric center of the island surface is AC; the groove bottom surface forms a new electrode surface B, the geometric center of which is BC.
More than two groups of groove rows which are spaced are uniformly arranged on the surface of the negative electrode facing the diaphragm along the X-axis direction, each X-axis groove row comprises more than 2 grooves which are sequentially spaced along the Y-axis direction, except the grooves, the original surface of the electrode facing the diaphragm is reserved to form an island surface D, and the geometric center of the island surface is DC; the trench floor forms a new electrode surface E, with EC being the geometric center of the trench floor.
The using method is that the anode and the cathode are oppositely arranged at two sides of the diaphragm and are sequentially the anode, the diaphragm and the cathode when viewed from top to bottom; the positive electrode and the negative electrode are respectively projected to the surface of one side of the diaphragm, and the surfaces of the positive electrode islands and the negative electrode islands are uniformly distributed in a staggered manner one by one in each row of projection, namely the geometric center AC of the surfaces of the positive electrode islands is superposed with the geometric center EC of the bottom surface of the negative electrode groove; the geometric center DC of the surface of the negative island is coincided with the geometric center BC of the bottom surface of the positive groove.
Viewed from the direction of an X axis or a Y axis, the positive island AC projection lines and the negative island DC projection lines are sequentially and alternately arranged.
The structure according to claim 1, wherein a cross-sectional shape of the groove perpendicular to the X-axis or Y-axis direction is a rectangle, a trapezoid, or a profile, as viewed in the X-axis or Y-axis direction.
The depth dimension of the groove along the Z-axis direction is 3mm.
Defining four directions on the periphery of the surface of the diaphragm as left, right, upper and lower directions respectively; the left and right directions are opposite, the up and down directions are opposite, and the left and right directions are respectively vertical to the up and down directions;
comparative example
3 x 3cm positive and negative electrode effective areas of assembled zinc-bromine redox flow battery 2 (ii) a The electrode current collector is made of graphite, and is made of original 6mm carbon felt with positive and negative electrodes without any treatment, and the electrolyte comprises 0.8M MEP and 2M ZnBr 2 And 3M KCl assembling the double-flow battery. The charging current density is 40mA/cm 2 Charging for 2.5h and charging cut-off voltage of 2.5V; discharge current density 40mA/cm 2 And a cut-off voltage of 0.4V. As can be seen from fig. 4, at the end of each charge, a large polarization is produced, and the charge voltage rapidly jumps to 2.5V; fig. 5 can show that the charging is stopped due to the voltage protection without being performed for a predetermined charging time of 2.5 h.
Example 1
The effective areas of the positive electrode and the negative electrode of the zinc-bromine redox flow battery assembled by the electrode structure are 3X 3cm 2 (ii) a The material of the polar current collector is graphite; the positive and negative electrodes are carbon felts with special-shaped groove structures observed in the X-axis or Y-axis direction, the special-shaped structures are specifically described as that two sides of a semicircle with the diameter of 3mm are connected with 1/4 of an arc (not forming a whole circle) with the diameter of 3mm, the end points of the arc tail ends are linearly connected, the semicircle end points point to the Z-axis direction, and the structure of the felt is shown in FIGS. 1a,2a and 3a; the electrolyte composition is 0.8M MEP and 2M ZnBr 2 And 3M KCl assembling the double-flow battery. The charging current density is 40mA/cm 2 Charging for 2.5h and charging cut-off voltage of 2.5V; discharge current density 40mA/cm 2 And a cut-off voltage of 0.4V. No large polarization is generated at the end of each charging, the charging voltage is not increased to 2.5V, and the battery is stable in circulation (more than 30 stable cycles); the charging can be carried out for 2.5h, and the charging voltage curve is stable. The embodiment can fully show that the performance of the positive and negative carbon felts is superior to that of carbon felts without any treatment under the condition of high surface capacity by adopting the structural design and assembly method.
Example 2
The effective areas of the positive electrode and the negative electrode of the zinc-bromine redox flow battery assembled by the electrode structure are 3X 3cm 2 (ii) a The material of the polar current collector is graphite; the positive and negative electrodes are carbon felts with special-shaped groove structure observed from X-axis direction or Y-axis direction, and two 1/4 circles with diameter of 3mm are symmetrically connected with side length of 3mOn a square of m, the 3mm side length of the formed special shape is far away from the island area direction, and the electrode structure is shown in FIGS. 1b,2b and 3b; the electrolyte composition is 0.8M MEP and 2M ZnBr 2 And 3M KCl assembling the double-flow battery. The charging current density is 40mA/cm 2 Charging for 2.5h and charging cut-off voltage of 2.5V; discharge current density 40mA/cm 2 And cutoff voltage 0.4V. No large polarization is generated at the end of each charge, the battery is cycled stably (more than 30 stable cycles), and the charge voltage is not increased to 2.5V in a surge way; the charging can be carried out for 2.5h, and the charging voltage curve is stable. The implementation of the pair can be fully explained, and the performance of the positive and negative carbon felts is superior to that of carbon felts without any treatment under the condition of high surface capacity by adopting the structural design and assembly method.
Example 3
The effective area of the positive electrode and the negative electrode of the zinc-bromine redox flow battery assembled by the electrode structure is 3 x 3cm 2 (ii) a The material of the polar current collector is graphite; observing the carbon felt with an isosceles trapezoid groove structure from the X-axis direction or the Y-axis direction, wherein the isosceles trapezoid is specifically described as the distance between parallel sides being 3mm, the short side of the parallel sides being 3mm, the long side being 9mm, the parallel short sides being far away from the island area, and the electrode structure is shown in FIGS. 1c,2c and 3c; the electrolyte composition is 0.8M MEP and 2M ZnBr 2 And 3M KCl assembling the double-flow battery. The charging current density is 40mA/cm 2 Charging for 2.5h and the charge cut-off voltage is 2.5V; discharge current density 40mA/cm 2 And a cut-off voltage of 0.4V. No large polarization is generated at the end of each charging, the charging voltage is not increased to 2.5V, and the battery is stable in circulation (more than 30 stable cycles); the charging can be carried out for 2.5h, and the charging voltage curve is stable. The embodiment can fully show that the performance of the positive and negative carbon felts is superior to that of carbon felts without any treatment under the condition of high surface volume by adopting the structural design and assembly method.
Example 4
The effective areas of the positive electrode and the negative electrode of the zinc-bromine redox flow battery assembled by the electrode structure are 3X 3cm 2 (ii) a The material of the polar current collector is graphite; the positive and negative electrodes are carbon felts with rectangular groove structures observed from the X-axis direction or the Y-axis direction,the long side of the rectangle is 9mm, the short side is 3mm, wherein the long side is parallel to the original surface of the electrode, and the electrode structure is shown in FIGS. 1d,2d and 3d; the electrolyte composition is 0.8M MEP and 2M ZnBr 2 And 3M KCl assembling the double-flow battery. The charging current density is 40mA/cm 2 Charging for 2.5h and charging cut-off voltage of 2.5V; discharge current density 40mA/cm 2 And cutoff voltage 0.4V. As can be seen from fig. 6, no significant polarization is produced at the end of each charge, and the cell cycles stable (greater than 30 stable cycles); fig. 7 can show that the charging can be performed for 2.5h, and the charging voltage curve is smooth. The embodiment can fully show that the performance of the positive and negative carbon felts is superior to that of carbon felts without any treatment under the condition of high surface volume by adopting the design and assembly method.
Example 5
The effective areas of the positive electrode and the negative electrode of the zinc-bromine redox flow battery assembled by the electrode structure are 3X 3cm 2 (ii) a The material of the polar current collector is graphite; only the positive electrode uses a carbon felt with a rectangular groove structure, the long side of the rectangle is 9mm, the short side of the rectangle is 3mm, and the long side is parallel to the original surface of the electrode, and the electrode structure is shown in FIGS. 1d and 2d; the electrolyte composition is 0.8M MEP and 2M ZnBr 2 And 3M KCl assembling the double-flow battery. The charging current density is 40mA/cm 2 Charging for 2.5h and charging cut-off voltage of 2.5V; discharge current density 40mA/cm 2 And a cut-off voltage of 0.4V. The results show that at the end of each charge, a large polarization was produced, the charge could not be carried out for 2.5h, the voltage rapidly climbed to 2.5V, and the cell cycling was unstable. The embodiment can fully illustrate that the performance of the positive carbon felt is not obviously superior to that of the positive and negative carbon felts which are all original carbon felts under the condition of high surface capacity only by adopting the design and assembly method, and the performance is also not superior to that of the positive and negative carbon felts which are all observed from the X-axis direction or the Y-axis direction and provided with rectangular groove structures.
Example 6
The effective areas of the positive electrode and the negative electrode of the zinc-bromine redox flow battery assembled by the electrode structure are 3X 3cm 2 (ii) a The material of the polar current collector is graphite; only the negative electrode uses the carbon felt with a rectangular groove structure observed from the X-axis direction or the Y-axis directionThe long side of the rectangle is 9mm, the short side is 3mm, wherein the long side is parallel to the original surface of the electrode, and the electrode structure is shown in fig. 1d and 2d; the electrolyte composition is 0.8M MEP and 2M ZnBr 2 And 3M KCl assembling the double-flow battery. The charging current density is 40mA/cm 2 Charging for 2.5h and the charge cut-off voltage is 2.5V; discharge current density 40mA/cm 2 And cutoff voltage 0.4V. The results show that no significant polarization is produced at the end of each charge; the charging can be carried out for 2.5h, the charging voltage curve is stable, but the cycling stability (less than 30 times of stable cycling) is not superior to that of a carbon felt with a rectangular groove structure observed from the X-axis direction or the Y-axis direction. The embodiment can fully explain that the performance of the carbon felt with the rectangular groove structure observed from the X-axis direction or the Y-axis direction is not better than that of the carbon felt with the rectangular groove structure observed from the X-axis direction or the Y-axis direction under the condition of high surface capacity only by adopting the design and assembly method for the cathode carbon felt.
Claims (5)
1. The utility model provides a zinc bromine redox flow battery electrode structure, zinc-based monocell includes positive pole, diaphragm, the negative pole that stacks gradually which characterized in that:
defining two directions of an X axis and a Y axis which are vertical to each other on a reference plane by taking a contact surface of the electrode and the diaphragm as the reference plane; defining the direction which is vertical to the surface of the electrode and far away from the diaphragm as the Z-axis direction; wherein the electrode comprises a positive electrode and a negative electrode;
more than two groups of spaced groove rows are uniformly arranged on the surface of the positive electrode facing the diaphragm along the X-axis direction, each X-axis groove row comprises more than 2 grooves sequentially arranged at intervals along the Y-axis direction, except the grooves, the original surface of the electrode facing the diaphragm is reserved to form an island surface A, and the geometric center of the island surface is AC; forming a new electrode surface B on the bottom surface of the groove, wherein the geometric center of the bottom surface of the groove is BC; the sum of the projected areas of all the grooves on the surface of the positive electrode is 80 to less than 100 percent of the surface area of one side of the positive electrode;
more than two groups of groove rows which are spaced are uniformly arranged on the surface of the negative electrode facing the diaphragm along the X-axis direction, each X-axis groove row comprises more than 2 grooves which are sequentially spaced along the Y-axis direction, except the grooves, the original surface of the electrode facing the diaphragm is reserved to form an island surface D, and the geometric center of the island surface is DC; forming a new electrode surface E on the bottom surface of the groove, wherein the geometric center of the bottom surface of the groove is EC; the sum of the projected areas of all the grooves on the surface of the negative electrode is 80 to less than 100 percent of the surface area of one side of the negative electrode;
the positive electrode and the negative electrode are oppositely arranged at two sides of the diaphragm, and viewed from top to bottom, the positive electrode, the diaphragm and the negative electrode are sequentially arranged; the positive electrode and the negative electrode respectively project towards the surface of one side of the diaphragm, and the surfaces of the positive electrode islands and the negative electrode islands in each row of projection are uniformly distributed in a staggered manner one by one, namely the geometric center AC of the surface of the positive electrode island is superposed with the geometric center EC of the bottom surface of the negative electrode groove; the geometric center DC of the surface of the negative island is superposed with the geometric center BC of the bottom surface of the positive groove;
viewed from the direction of an X axis or a Y axis, the positive island AC projection lines and the negative island DC projection lines are sequentially and alternately arranged;
the depth dimension of the groove along the Z-axis direction ranges from 0.5 mm to 6mm.
2. The structure of claim 1, wherein the sum of the projected areas of all the grooves on the surface of the positive electrode is 90-95% of the surface area of the positive electrode side;
the sum of the projected areas of all the grooves on the surface of the negative electrode is 90-95% of the surface area of one side of the negative electrode.
3. The structure according to claim 1, wherein the cross-sectional shape of the groove perpendicular to the X-axis or Y-axis direction is a rectangle, an ellipse, a trapezoid, or a profile, as viewed in the X-axis or Y-axis direction.
4. The structure as claimed in claim 1, wherein the corner part with the line segment edge in the groove can be processed into a circular arc chamfer with the diameter of 0.5-6 mm.
5. The use of the electrode structure of a zinc-bromine flow battery as defined in any one of claims 1 to 4 as an anode and a cathode, respectively, in a zinc-bromine flow battery.
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