CN114551911A - Preparation and application of negative electrode structure for zinc-based flow battery - Google Patents
Preparation and application of negative electrode structure for zinc-based flow battery Download PDFInfo
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- CN114551911A CN114551911A CN202011340720.4A CN202011340720A CN114551911A CN 114551911 A CN114551911 A CN 114551911A CN 202011340720 A CN202011340720 A CN 202011340720A CN 114551911 A CN114551911 A CN 114551911A
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- 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
- H01M4/88—Processes of manufacture
- H01M4/8875—Methods for shaping the electrode into free-standing bodies, like sheets, films or grids, e.g. moulding, hot-pressing, casting without support, extrusion without support
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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
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- 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
- H01M2004/8684—Negative electrodes
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
A carbon felt electrode structure design capable of remarkably improving the capacity of a zinc negative electrode surface of a zinc-based flow battery. And cutting the surface of the carbon felt electrode to obtain a plurality of cuboid grooves, and embedding a three-dimensional porous insulating material with certain mechanical strength in the grooves to obtain the carbon felt electrode. Simple operation, stable process and low cost. The electrode designed by the invention greatly slows down the deposition pressure of zinc between the carbon felt and the membrane, provides a large amount of zinc deposition space, effectively improves the cycling stability of the zinc-based flow battery under the condition of high deposition surface capacity, and greatly prolongs the service life of the battery.
Description
Technical Field
The invention relates to the field of flow batteries, in particular to the field of zinc-based flow batteries.
Background
With the depletion of fossil energy and the increase of global warming, renewable energy plays an increasingly important role in energy structure. However, the fact that renewable energy sources such as wind energy and solar energy are discontinuous and unstable makes direct utilization of the renewable energy sources difficult, and therefore, the realization of continuous supply of renewable energy sources by using an energy storage technology becomes a key point for solving the problems. The zinc-based flow battery has the advantages of low cost, high theoretical energy density and strong safety, and becomes one of the most promising technologies in the large-scale energy storage market.
Unlike liquid-liquid type flow batteries (e.g., vanadium flow batteries, all-iron flow batteries) in which a redox couple exists in the liquid phase in the anolyte and catholyte, the zinc negative electrode of a zinc-based flow battery has a liquid-solid phase inversion process, i.e., the deposition/dissolution process of metallic zinc exists in the negative electrode. When the space for the cathode deposition is insufficient at high surface capacities, a series of consequences can occur, such as an increase in the overpotential for deposition, irreversible hydrogen evolution side reactions and short circuits caused by dendrite penetration of the separator. All of these problems will be reflected in battery performance, i.e., low battery capacity, low voltage efficiency, low coulombic efficiency, and short cycle life. Meanwhile, the high deposition surface capacity of the battery inevitably brings about the problem of aggravation of zinc dendrite growth. However, for zinc-based flow batteries, where the stored energy is directly related to the amount of metallic zinc plated on the negative electrode, it is necessary but very challenging to increase the zinc deposition surface capacity and solve the problem of zinc deposition under high surface capacity conditions.
Disclosure of Invention
A high surface capacity negative electrode structure design for a zinc-based flow battery. The manufacturing process of the electrode is simple and easy to implement, a plurality of cuboids are cut on the surface of the carbon felt, the cutting depth is 10-90% of the thickness of the carbon felt, preferably 50-80%, a three-dimensional porous insulating material (such as high-density sponge and the like) with certain mechanical strength is embedded in the cutting position, the upper surface of the embedded material is 0.5-3mm (preferably 1-1.5mm) higher than the upper surface of the carbon felt, and the electrode with high-low staggered distribution can be obtained. When the zinc-based flow battery is assembled, the negative electrode adopts an electrode structure with high-low staggered distribution, the positive electrode adopts an original carbon felt structure, the diaphragm adopts a porous membrane, and the electrolyte on the negative electrode side of the positive electrode circularly flows.
The negative electrode structure for the zinc-based flow battery comprises a carbon felt electrode body, wherein more than 2 strip-shaped bulges made of parallel porous insulating materials and spaced from left to right are sequentially arranged on the surface of one side of the carbon felt electrode body.
The height of the porous insulating material protrusions on the surface of the carbon felt (the distance from the plane of the protrusions away from the surface of the carbon felt to the surface of the carbon felt) is 0.5-2mm, preferably 1-1.2 mm; the distance between adjacent strip-like protrusions is 0.5-1.5cm, preferably 0.8-1 cm.
The distance between two ends (the upper end and the lower end in the figure 1) of the strip-shaped protruding strip and the upper edge and the lower edge of the adjacent carbon felt is 0.3-1cm, and preferably 0.5-0.8 cm; the distance between the strip-shaped protrusion at the leftmost side and the edge at the left side of the carbon felt is 0.3-1cm, preferably 0.5-0.8 cm; the distance between the rightmost strip-shaped protrusion and the right edge of the carbon felt is 0.3-1cm, and preferably 0.5-0.8 cm.
The width of the strip-shaped protrusion is 1-8mm, preferably 2-5 mm.
The carbon felt is in a rectangular flat plate shape, one side of the strip-shaped protrusion, which is close to the surface of the carbon felt, is embedded into the carbon felt, and the embedding depth is 10-90% of the thickness of the carbon felt, and is preferably 50-80%.
The porous insulating material is one or more than two kinds of high-density sponges, and the density of the porous insulating material is more than or equal to 45g/cm3The porosity is 90% or more.
The preparation method of the cathode structure comprises the following steps of,
bonding the strip-shaped porous insulating material on the surface of one side of the carbon felt to obtain an electrode with high-low staggered distribution; or more than 2 mutually spaced and parallel strip-shaped grooves are cut on the surface of one side of the carbon felt, and the cutting depth is 10-90% of the thickness of the carbon felt, preferably 50-80%; and (3) putting strip-shaped porous insulating materials with corresponding length (the length in the direction from top to bottom in the figure 1) and width (the width in the direction from left to right in the figure 1) in the groove, wherein the upper surface of the embedded strip-shaped porous insulating materials is 0.5-3mm (preferably 1-1.5mm) higher than the upper surface of the carbon felt, so as to obtain the electrode with staggered distribution.
The negative electrode structure is applied to a zinc-based flow battery.
The negative electrode structure is used as a negative electrode of the zinc-based flow battery, and when the zinc-based flow battery is assembled, the strip-shaped protrusions are placed on one side, facing the diaphragm.
The electrolyte flows into the negative side in the area among one end of the negative electrode of the zinc-based flow battery, the strip-shaped protrusions and the edge of the carbon felt, and the flowing direction of the electrolyte flowing into the negative side of the zinc-based flow battery is consistent with the length of the strip-shaped protrusions (the length of the direction from top to bottom in the figure 1).
A carbon felt electrode structure design which can obviously improve the capacity of the zinc negative electrode surface of a zinc-based flow battery; and cutting the surface of the carbon felt electrode to obtain a plurality of cuboid grooves, and embedding a three-dimensional porous insulating material with certain mechanical strength in the grooves to obtain the carbon felt electrode. The electrode designed by the invention greatly slows down the deposition pressure of zinc between the carbon felt and the membrane, provides a large amount of zinc deposition space, effectively improves the cycling stability of the zinc-based flow battery under the condition of high deposition surface capacity, and greatly prolongs the service life of the battery.
Simple operation, stable process and low cost. The electrode designed by the invention greatly slows down the deposition pressure of zinc between the carbon felt and the diaphragm, provides a large amount of zinc deposition space, effectively improves the cycling stability of the zinc-based flow battery under the condition of high deposition surface capacity, and greatly prolongs the service life of the battery.
The electrode made using the present method not only provides more space to accommodate the electrochemically reduced zinc than the original structure, but also creates a spatial barrier to dendrite growth. In addition, the macroscopic three-dimensional structure of the electrode optimizes the flow field distribution, so that the electrolyte can reach reaction parts more easily, and the concentration polarization is reduced.
The electrodes made using the method exhibit high coulombic efficiency and long cycle life at high area capacity. At 40mA cm-2When the zinc-iodine flow battery is operated, the capacity of a deposition surface can reach 160mAh cm-2The coulombic efficiency remained at 88%, and with the cells of the original structure, the coulombic efficiency suddenly dropped after 40 cycles.
Drawings
FIG. 1 is a schematic cross-sectional view of a staggered high and low electrode structure according to the present invention;
FIG. 2 is a schematic surface view of a staggered high and low electrode structure according to the present invention;
FIG. 3 is a graph of battery performance data for example 1;
FIG. 4 is a graph of cell performance data for example 2;
FIG. 5 is a graph of comparative example 1 cell performance data;
FIG. 6 is a graph of comparative example 2 cell performance data;
fig. 7 is a graph of comparative example 3 cell performance data.
Detailed Description
The performance of the electrode with the high-low misclassification distribution structure is tested by using the zinc-iodine flow battery, but the structure is not limited to the zinc-iodine flow battery and can be used in all zinc-based flow batteries. When testing, the negative electrode (examples 1 and 2) used carbon felt length × width × height dimensions 6cm × 06cm × 15mm, 5 parallel rectangular grooves cut on the upper surface, the cutting depth is 80% of the carbon felt thickness, the groove size length × width × height 5cm × 0.4cm × 4mm, the distance between the grooves is 0.8cm, the left-most and right-most grooves are respectively 0.4cm away from the left and right edges of the adjacent carbon felt, the upper and lower ends (as shown in fig. 1) of the groove are 0.5cm away from the upper and lower edges of the carbon felt, the high-density sponge size length × width × 5cm × 5mm, and the high-density sponge density is 48g/cm × 5mm3The porosity is 92%, and the upper surface of the sponge behind the high-density sponge is 1mm higher than the surface of the carbon felt. And (3) embedding the high-density sponge into the rectangular groove to obtain strip-shaped bulges with the dimensions of length multiplied by width multiplied by 5cm multiplied by 0.4cm multiplied by 4mm, wherein the distance between the strip-shaped bulges is 0.8cm, the strip-shaped bulges at the leftmost side and the rightmost side are respectively 0.4cm away from the left side edge and the right side edge of the adjacent carbon felt, and the upper end and the lower end (shown in figure 1) of the strip-shaped bulges are 0.5cm away from the upper edge and the lower edge of the carbon felt. The positive electrode used was a carbon felt having a size of 6cm × 6cm × 6mm in length × width × height. The assembly mode of the zinc-iodine flow battery is a conventional assembly mode, a high-low offset electrode is used at a negative electrode, an untreated original carbon felt electrode is used at a positive electrode, and a diaphragm is a commercial daramic porous membrane. The electrolyte is a conventional electrolyte corresponding to zinc iodine (the concentration of potassium iodide is 4mol/L, the concentration of zinc bromide is 2mol/L, and the concentration of potassium chloride is 2 mol/L).
Example 1
FIG. 3 shows a zinc-iodine flow battery assembled with a high-low miscella electrode (the high-low miscella electrode is used for the negative electrode, a 6 cm. times.6 mm carbon felt is used for the positive electrode), and a commercial daramic porous membrane is used for the separator, and the capacity of the membrane on the zinc deposition surface is 80 to 240mAh/cm2Coulombic efficiency data under conditions. The result shows that the battery can not only reach the given value of the surface capacity under the condition that the set surface capacity is continuously increased, but also has high coulombic efficiency. Zinc ions are preferentially deposited on the surface of the carbon felt close to one side of the diaphragm, the structure of the high-low staggered electrode greatly increases the depositable area and the depositable space of zinc close to the side of the diaphragm, the deposition pressure of zinc between the diaphragm and the carbon felt is relieved, the possibility of generation of dendritic crystals is reduced, and the carrying surface capacity of the zinc cathode is greatly expanded.
Example 2
FIG. 4 shows a zinc-iodine flow battery assembled using a high-low dislocation electrode (the high-low dislocation electrode is used for the negative electrode, and a 6 cm. times.6 mm-sized carbon felt is used for the positive electrode), and a commercial daramic porous membrane is used for the separator, and the capacity of the separator is 160/cm on the zinc deposition surface2Battery performance data under the conditions. The battery can stably circulate for 300 times at about 88% of coulombic efficiency, and the electrode design with a high-low staggered structure proves that the circulation stability of the zinc-based flow battery under high surface capacity is greatly improved.
Comparative example 1
FIG. 5 shows an assembly of a zinc-iodine flow battery using uncut carbon felt electrodes (positive and negative electrodes of 6 cm. times.6 mm) with a commercial porous membrane having a capacity of 80-240 mAh/cm on the zinc deposition surface2Coulombic efficiency data under conditions. In the process of increasing the surface capacity, the surface capacity of zinc which can be deposited by the original electrode structure is less than 80mAh/cm2And when the deposition amount is increased, the coulomb efficiency of the battery is reduced sharply, which indicates that the zinc dendrite is extruded and grows to pierce the diaphragm at the moment, and the internal micro short circuit of the battery is caused.
Comparative example 2
FIG. 6 shows an assembled zinc-iodine flow cell using uncut virgin carbon felt electrodes (positive and negative electrodes each 6 cm. times.6 mm) with a separator using a commercial porous membrane with a capacity of 160mAh/cm on the zinc deposition surface2Battery performance data under the conditions. The coulombic efficiency drops for less than 40 times after the battery is cycled, which shows that the excessive deposited zinc is continuously accumulated on the side close to the diaphragm to pierce the diaphragm, so that the battery is slightly short-circuited, and the service life of the battery is shortened.
Comparative example 3
FIG. 7 shows that the negative electrode uses a carbon felt with the length, width and height of 6cm, 5mm, and 5 parallel rectangular grooves are cut on the upper surface and the cutting depth is setThe degree is 80% of the thickness of the carbon felt, the size length of the grooves is multiplied by the width and multiplied by the height by 5cm and multiplied by 0.4cm and multiplied by 4mm, the distance between the grooves is 0.8cm, the left side and the right side of the grooves at the leftmost side and the rightmost side are respectively 0.4cm away from the edges of the left side and the right side of the adjacent carbon felt, the distance between the upper end and the lower end (shown in figure 1) of the grooves at the upper edge and the lower edge of the carbon felt is 0.5cm, and a high-density sponge supporting layer is not added; the positive electrode uses original carbon felt with the size of 6cm multiplied by 6mm to assemble the zinc-iodine flow battery, the diaphragm uses commercial porous membrane, and the capacity of the zinc deposition surface is 160mAh/cm2Battery performance data under the conditions. When the high-density sponge supporting layer is not added, the carbon felt is not tightly contacted with the current collector after being cut under the flushing of liquid flow, so that the performance of the battery is reduced and the battery fluctuates greatly.
Claims (10)
1. The negative electrode structure for the zinc-based flow battery comprises a carbon felt electrode body, wherein more than 2 strip-shaped bulges made of parallel porous insulating materials and spaced from left to right are sequentially arranged on the surface of one side of the carbon felt electrode body.
2. The negative electrode structure of claim 1, wherein: the height of the porous insulating material protrusions on the surface of the carbon felt (the distance from the plane of the protrusions away from the surface of the carbon felt to the surface of the carbon felt) is 0.5-2mm, preferably 1-1.2 mm; the distance between adjacent strip-shaped protrusions is 0.5-1.5cm, preferably 0.8-1 cm.
3. The negative electrode structure of claim 1 or 2, wherein: the distance between the two ends (the upper end and the lower end in the figure 1) of the strip-shaped protruding strip and the upper edge and the lower edge of the adjacent carbon felt is 0.3-1cm, and preferably 0.5-0.8 cm; the distance between the strip-shaped protrusion at the leftmost side and the edge at the left side of the carbon felt is 0.3-1cm, preferably 0.5-0.8 cm; the distance between the rightmost strip-shaped protrusion and the right edge of the carbon felt is 0.3-1cm, and preferably 0.5-0.8 cm.
4. The negative electrode structure of claim 1 or 2, wherein: the width of the strip-shaped protrusion is 1-8mm, preferably 2-5 mm.
5. The negative electrode structure of claim 1 or 2, wherein: the carbon felt is in a rectangular flat plate shape, one side of the strip-shaped protrusion, which is close to the surface of the carbon felt, is embedded into the carbon felt, and the embedding depth is 10-90% of the thickness of the carbon felt, and is preferably 50-80%.
6. The negative electrode structure of claim 1 or 2, wherein: the porous insulating material is one or more than two of high-density sponges, and the density of the porous insulating material is more than or equal to 45g/cm3The porosity is 90% or more.
7. A method of making the negative electrode structure of any of claims 1-6, characterized by:
bonding the strip-shaped porous insulating material on the surface of one side of the carbon felt to obtain an electrode with high-low staggered distribution; or more than 2 mutually spaced and parallel strip-shaped grooves are cut on the surface of one side of the carbon felt, and the cutting depth is 10-90% of the thickness of the carbon felt, preferably 50-80%; and (3) putting strip-shaped porous insulating materials with corresponding length (the length in the direction from top to bottom in the figure 1) and width (the width in the direction from left to right in the figure 1) in the groove, wherein the upper surface of the embedded strip-shaped porous insulating materials is 0.5-3mm (preferably 1-1.5mm) higher than the upper surface of the carbon felt, so as to obtain the electrode with staggered distribution.
8. Use of a negative electrode structure according to any of claims 1 to 6 in a zinc-based flow battery.
9. Use according to claim 8, characterized in that:
the negative electrode structure of any of claims 1-6 as a negative electrode of a zinc-based flow battery, wherein the protrusions are disposed facing a side of the separator when the zinc-based flow battery is assembled.
10. Use according to claim 8 or 9, characterized in that: the electrolyte flows into the negative side in the area among one end of the negative electrode of the zinc-based flow battery, the strip-shaped protrusions and the edge of the carbon felt, and the flowing direction of the electrolyte flowing into the negative side of the zinc-based flow battery is consistent with the length of the strip-shaped protrusions (the length of the direction from top to bottom in the figure 1).
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| CN111224115A (en) * | 2018-11-27 | 2020-06-02 | 中国科学院大连化学物理研究所 | Zinc-based battery negative electrode and preparation and application thereof |
| CN111244489A (en) * | 2018-11-28 | 2020-06-05 | 中国科学院大连化学物理研究所 | Application of electrode material in zinc-bromine single flow battery |
| CN111668508A (en) * | 2020-06-16 | 2020-09-15 | 氢源科技(赣州)有限公司 | Flow channel structure of bipolar plate of hydrogen fuel cell |
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- 2020-11-25 CN CN202011340720.4A patent/CN114551911B/en active Active
Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102299348A (en) * | 2010-06-25 | 2011-12-28 | 中国科学院大连化学物理研究所 | Porous electrode structure of redox flow battery and preparation method thereof |
| CN105322197A (en) * | 2014-08-01 | 2016-02-10 | 大连融科储能技术发展有限公司 | High specific surface area bipolar plate for flow battery and preparation method thereof |
| CN110970632A (en) * | 2018-09-29 | 2020-04-07 | 中国科学院大连化学物理研究所 | Bipolar plate suitable for trapezoidal flow battery and application |
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| CN109686995A (en) * | 2018-12-22 | 2019-04-26 | 一汽解放汽车有限公司 | A kind of interior bipolar plates with wedge-shaped protrusion of runner |
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