CN111106373B - Zinc-bromine storage battery - Google Patents

Zinc-bromine storage battery Download PDF

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CN111106373B
CN111106373B CN201811249464.0A CN201811249464A CN111106373B CN 111106373 B CN111106373 B CN 111106373B CN 201811249464 A CN201811249464 A CN 201811249464A CN 111106373 B CN111106373 B CN 111106373B
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battery
zinc
positive electrode
bromine
negative electrode
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CN111106373A (en
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许鹏程
李先锋
张华民
赖勤志
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Dalian Institute of Chemical Physics of CAS
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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
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/431—Inorganic material
    • 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
    • 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

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Abstract

The invention relates to a zinc-bromine storage battery, which is formed by connecting two or more monocells in series or/and in parallel, wherein the electrodes of the battery are horizontally arranged, and the monocells comprise a positive electrode end plate, a positive electrode current collector, a positive electrode arranged at a through hole in the middle of a positive electrode frame, a battery diaphragm, a negative electrode arranged at a through hole in the middle of a negative electrode frame, a negative electrode current collector and a negative electrode end plate which are sequentially overlapped from bottom to top; the positive electrode and the negative electrode are soaked with electrolyte; the electrolyte is a mixed aqueous solution of zinc bromide and potassium chloride; when the battery is charged, free zinc ions in the negative electrode are directly deposited on the negative electrode in a zinc simple substance form, and bromine ions are oxidized into bromine simple substances in the positive electrode and adsorbed in the positive electrode; during discharging, the simple substance zinc is oxidized into zinc ions, and the simple substance bromine is reduced into bromine ions; the battery separator is a porous membrane.

Description

Zinc-bromine storage battery
Technical Field
The invention relates to the technical field of storage batteries, in particular to a zinc-bromine storage battery.
Background
The zinc bromine flow battery (ZBB) is a flow energy storage battery with high energy conversion efficiency, high energy density (theoretical energy density 435wh/kg) and low price of key materials (diaphragm and electrolyte), and is widely applied to the fields of power generation of renewable energy sources such as wind energy and solar energy, power grid peak regulation and frequency modulation, communication base stations and the like.
The zinc-bromine flow battery realizes the mutual conversion between electric energy and chemical energy through the oxidation-reduction reaction of active substances between a positive electrode and a negative electrode, and the positive electrode and the negative electrode both need a circulating pump to enable electrolyte to circularly flow in the working process of the zinc-bromine flow battery. The use of the circulating pump, the liquid storage tank and the pipeline increases the system cost of the zinc-bromine battery, reduces the overall energy conversion efficiency of the system, and also makes the system structure more complicated and is not beneficial to the miniaturization of the system. In addition, bromine has strong diffusivity, so that bromine generated in the charging process can diffuse to a negative electrode to directly react with zinc, the self-discharge of the battery is caused, and the capacity of the battery is reduced; the accumulation of zinc can cause the polarization of the battery to be increased, the performance of the battery is attenuated, the service life of the battery is influenced, and even dendritic crystals can be formed under severe conditions to cause short circuit failure of the battery.
Disclosure of Invention
In order to solve the technical problems, the invention provides a zinc-bromine storage battery, which reduces the self-discharge of the battery by Nafion modification of a diaphragm, improves the coulombic efficiency of the battery, ensures that bromine generated in the charging process is more uniformly distributed on an electrode in a mode that a battery anode is arranged on a lower cathode, reduces the influence of zinc accumulation on the battery performance of the cathode, and prolongs the service life of the battery.
In order to achieve the purpose, the specific technical scheme adopted by the branch is as follows:
a zinc bromine storage battery is composed of one or more than two monocells which are connected in series or/and in parallel, wherein the electrodes of the battery are horizontally arranged, and the monocells comprise a positive electrode end plate, a positive electrode current collector, a positive electrode frame, a positive electrode, a battery diaphragm, a negative electrode frame, a negative electrode current collector and a negative electrode end plate which are sequentially overlapped from bottom to top;
the positive electrode and the negative electrode are soaked with electrolyte;
when the battery is charged, free zinc ions in the negative electrode are directly deposited on the negative electrode in a zinc simple substance form, and bromine ions are oxidized into bromine simple substances in the positive electrode and adsorbed in the positive electrode; during discharging, the simple substance zinc is oxidized into zinc ions, and the simple substance bromine is reduced into bromine ions; the battery diaphragm is a porous membrane; and (3) coating a Nafion coating on the surface of the porous membrane close to the positive electrode, wherein the mass fraction of Nafion solution adopted by the coating is 1-5%, the coating thickness is 10-50um, preferably 20-40um, and the film thickness is 600-1000 um.
The positive electrode and the negative electrode are made of carbon felt or graphite felt and have the thickness of 3-8mm, the positive electrode frame and the negative electrode frame are made of PP and have the thickness of 1.5-6mm, the electrode thickness is larger than the electrode frame, and the electrode thickness compression ratio is 1.1-1.3.
In the battery assembling process, the anode and the cathode are completely soaked in the electrolyte and then assembled.
The battery electrolyte is a mixed aqueous solution of zinc bromide and potassium chloride; ZnBr in electrolyte2The content is 1-5mol/L, and the KCl content is 1-4 mol/L.
The battery diaphragm is a PE film, and the current collector is a graphite plate or a carbon composite plate.
The invention has the beneficial effects
1. By adopting the battery placing mode that the anode is arranged on the lower cathode, bromine generated in the charging process is more uniformly distributed on the anode, and the anode active substance is uniformly distributed, so that the discharging performance of the battery can be improved, the influence of zinc accumulation on the battery performance of the cathode is reduced, and the service life of the battery is prolonged.
2. Compared with the traditional zinc bromine storage battery, the battery provided by the invention adopts flexible carbon felt or graphite felt materials as the positive electrode and the negative electrode, so that the zinc deposition uniformity and the zinc deposition surface capacity are ensured, and the polarization can be obviously reduced. Higher surface capacity and higher energy density of the storage battery.
3. By blade-coating a Nafion coating on the surface of the porous membrane, the diffusion of bromine is reduced, and the coulombic efficiency of the zinc-bromine storage battery is improved by more than 2%.
4. Complexing agents are not required to be added into the electrolyte, so that the cost of the battery system is reduced.
5. Compared with a paste type electrode, the electrode is simpler to assemble in a dipping mode, and the electrolyte is more uniformly distributed.
6. The battery has high working current density, long cycle life, no need of a circulating pump, simpler system and lower cost.
Drawings
FIG. 1 comparative example 1 shows the current density at 20mA/cm for charging and discharging2The cell performance of (a).
Fig. 2 shows the charge and discharge curves of the battery of comparative example 2.
FIG. 3. example 1 at a charging/discharging current density of 20mA/cm2Battery performance of
FIG. 4 example 2 shows the current density at 20mA/cm in charge and discharge2Battery performance of
DETAILED DESCRIPTION OF EMBODIMENT (S) OF INVENTION
Comparative example 1
Soaking positive and negative carbon felt electrodes in 2mol/LZnBr2+3mol/LKCl +0.4m 1/L1-methyl 1-ethyl pyrrolidine bromide (MEP) for 10min, and assembling single cells with the electrode, wherein the single cells sequentially comprise a positive electrode end plate, a positive electrode and a negative electrodePole 6x6cm2Graphite plate, positive electrode frame, carbon felt, diaphragm, carbon felt, negative electrode frame, negative electrode 6x6cm2The graphite plate and the negative end plate are superposed. The membrane was not knife coated with Nafion, 900um thick.
The positive electrode and the negative electrode are made of carbon felts and have the thickness of 6mm, the thickness of the positive electrode frame and the negative electrode frame is 4mm, the thickness of the electrodes is larger than that of the electrode frames, and the thickness compression ratio of the electrodes is 1.2.
The battery is placed vertically, and the charging and discharging current density is 20mA/cm2；
As can be seen from fig. 1, the performance of the battery decreases significantly and the cycle performance is poor as the number of cycles increases when the battery is placed vertically. The bromine generated in the charging process is gathered at the bottom of an electrode due to the action of gravity, so that the discharging of the battery is uneven, and the service life of the battery is influenced.
Comparative example 2
The single cell comprises a positive electrode end plate and a positive electrode 6x6cm from bottom to top in sequence2Graphite plate, positive electrode frame, positive electrode, diaphragm, negative electrode frame, negative electrode 6x6cm2The graphite plate and the negative end plate are superposed. The battery adopts the mode that the anode is horizontally placed at the lower cathode and the diaphragm is not coated with Nafion, and the thickness of the diaphragm is 900 mu m.
The positive electrode and the negative electrode are made of carbon felts and have the thickness of 6mm, the thickness of the positive electrode frame and the negative electrode frame is 4mm, the thickness of the electrodes is larger than that of the electrode frames, and the thickness compression ratio of the electrodes is 1.2.
The charge-discharge current density is 20mA/cm2(ii) a The charge cut-off voltage was 2.1V.
The immersion type electrode is prepared by soaking positive and negative carbon felt electrodes in 3mol/LZnBr2+3mol/LKCl +0.4m1/LMEP for 10 min;
comparative example 3
Cell Assembly as in comparative example 2
The positive and negative electrodes are pasted electrodes, and the preparation method is as follows
1) Preparing extreme paste slurry: according to the weight portion, 1 portion of carbon powder, 1 portion of trimethyl ammonium bromide, 10 portions of zinc bromide, 1 portions of PTFE and 3 portions of distilled water are mechanically mixed and stirred into paste for standby;
2) by usingUniformly coating the extreme paste slurry on the upper surface and the lower surface of the carbon felt by a blade coating method; loading capacity: 10mg/cm2；
The paste type electrode is adopted, the charging voltage of the battery is higher than that of the battery adopting the immersion type electrode, the discharging voltage of the battery is lower than that of the battery adopting the immersion type electrode, and the surface capacity of the battery is 40mAh/cm2The charging voltage reaches the cut-off voltage of 2.1V, and the surface capacity of the electrode is 60mAh/cm2The charging voltage is only 1.99V. This is mainly due to the use of paste electrodes in the battery active material distribution, resulting in greater battery polarization, reduced active material utilization, and thus resulting in a battery surface capacity and energy density that are all lower than those of wet electrodes. The energy density of the battery adopting the paste type electrode is 50Wh/L, and the energy density of the battery adopting the immersion type electrode is 97 Wh/L.
Example 1
Soaking positive and negative carbon felt electrodes in 2mol/LZnBr2And assembling the single cells by using the electrode in the +3mol/LKCl for 10min, wherein the single cells sequentially comprise a positive electrode end plate and a positive electrode 6x6cm from bottom to top2Graphite plate, positive electrode frame, carbon felt, diaphragm, carbon felt, negative electrode frame, negative electrode 6x6cm2The graphite plate and the negative end plate are superposed. The battery adopts the mode that the anode is horizontally placed at the lower cathode and the diaphragm is not coated with Nafion, and the thickness of the diaphragm is 900 mu m.
The positive electrode and the negative electrode are made of carbon felts and have the thickness of 6mm, the thickness of the positive electrode frame and the negative electrode frame is 4mm, the thickness of the electrodes is larger than that of the electrode frames, and the thickness compression ratio of the electrodes is 1.2.
The charge-discharge current density is 20mA/cm2；
Example 2
Soaking positive and negative carbon felt electrodes in 2mol/LZnBr2And assembling the single cells by using the electrode in the +3mol/LKCl for 10min, wherein the single cells sequentially comprise a positive electrode end plate and a positive electrode 6x6cm from bottom to top2Graphite plate, positive electrode frame, carbon felt, diaphragm, carbon felt, negative electrode frame, negative electrode 6x6cm2The graphite plate and the negative end plate are superposed. The surface of the porous membrane close to the positive electrode side is coated with a Nafion coating, the mass fraction of Nafion solution adopted by the coating is 5%, the coating thickness is 30 mu m, and the film thickness is 900 mu m.
The positive electrode and the negative electrode are made of carbon felts and have the thickness of 6mm, the thickness of the positive electrode frame and the negative electrode frame is 4mm, the thickness of the electrodes is larger than that of the electrode frames, and the thickness compression ratio of the electrodes is 1.2.
The battery adopts a mode that the anode is horizontally arranged on the lower cathode and the upper cathode, and the charging and discharging current density is 20mA/cm2；
As can be seen from FIG. 3, the battery adopts the mode that the anode is horizontally arranged above the lower cathode, the cycle performance of the battery is not obviously attenuated, and compared with the battery adopting the vertical arrangement mode in the comparative example 1, the cycle performance of the battery is obviously improved.
Compared with fig. 2 and fig. 3, after the Nafion solution is scraped, the CE of the battery can reach 98%, and compared with the electrode without the Nafion solution, the CE of the battery is improved by more than 2%. The improvement of CE shows that Nafion modification is carried out on the diaphragm, and the self-discharge of the battery is effectively reduced.
Example 3
Soaking positive and negative carbon felt electrodes in 2mol/LZnBr2And assembling the single cells by using the electrode in the +3mol/LKCl for 10min, wherein the single cells sequentially comprise a positive electrode end plate and a positive electrode 6x6cm from bottom to top2Graphite plate, positive electrode frame, carbon felt, diaphragm, carbon felt, negative electrode frame, negative electrode 6x6cm2The graphite plate and the negative end plate are superposed. The battery adopts anodal negative pole under to put the mode at the upper level, and the diaphragm positive side adopts mass fraction 5% Nafion solution to carry out the knife coating, and the coating thickness is 10um, 20um, 30um, 40um, 50um, and the membrane is thick 900um, and anodal and negative pole material are the charcoal felt, thickness 6mm, and positive and negative electrode frame thickness 4mm, electrode thickness are greater than electrode frame thickness, and electrode thickness compression ratio is 1.2.
The charge-discharge current density is 20mA/cm2；
As the Nafion coating thickness increased, the cell CE increased and remained constant, and VE decreased, with the cell performance being optimal when the coating thickness was 30 um.
Example 4
Soaking positive and negative carbon felt electrodes in 2mol/LZnBr2And assembling the single cells by using the electrode in the +3mol/LKCl for 10min, wherein the single cells sequentially comprise a positive electrode end plate and a positive electrode 6x6cm from bottom to top2Graphite plate and positive electrode frameCarbon felt, diaphragm, carbon felt, negative electrode frame and negative electrode 6x6cm2The graphite plate and the negative end plate are superposed. The battery adopts a mode that the anode is horizontally arranged at the lower cathode and the upper cathode, the anode side of the diaphragm adopts Nafion solution with the mass fraction of 5 percent for blade coating, the thickness of the coating is 30 mu m, and the charge-discharge current density is 20mA/cm2(ii) a The membrane is thick 900um, and anodal and negative pole material are the charcoal felt, and charcoal felt thickness is 3mm, 4mm, 5mm, 6mm, 7mm, 8mm respectively. The electrode thickness compression ratio is 1.2.
Along with the increase of the thickness of the electrode carbon felt, the charging capacity of the battery is increased, the VE of the battery is reduced, the thickness of the electrode is within the range of 3-8mm, the energy efficiency of the battery can be ensured to be not less than 75%, and the actual use requirement of the battery is met.
TABLE 1 Battery Performance of Nafion coatings of varying thickness
Figure BDA0001841304340000051
TABLE 2 carbon felt Battery Performance in different thicknesses
Figure BDA0001841304340000052

Claims (4)

1. A zinc-bromine storage battery is characterized in that: the battery is formed by connecting one or more than two monocells in series or/and in parallel, the electrodes of the battery are horizontally arranged, and the monocells comprise a positive electrode end plate, a positive electrode current collector, a positive electrode arranged at a through hole in the middle of a positive electrode frame, a battery diaphragm, a negative electrode arranged at a through hole in the middle of a negative electrode frame, a negative electrode current collector and a negative electrode end plate which are sequentially overlapped from bottom to top;
the positive electrode and the negative electrode are soaked with electrolyte; the electrolyte is a mixed aqueous solution of zinc bromide and potassium chloride;
when the battery is charged, free zinc ions in the negative electrode are directly deposited on the negative electrode in a zinc simple substance form, and bromine ions are oxidized into bromine simple substances in the positive electrode and adsorbed in the positive electrode; during discharging, the simple substance zinc is oxidized into zinc ions, and the simple substance bromine is reduced into bromine ions; the battery diaphragm is a porous membrane;
the anode and cathode materials are respectively carbon felt or graphite felt, the thickness is 3-8mm, the thickness of the anode electrode frame and the cathode electrode frame is 1.5-6mm, the thickness of the electrodes is larger than that of the electrode frames, and the compression ratio of the thickness of the electrodes is 1.1-1.3;
the battery diaphragm is a porous membrane; the surface of the porous membrane close to the positive electrode side is coated with a Nafion coating, the mass fraction of Nafion solution adopted by the coating is 1-5%, the coating thickness is 10-50 mu m, and the membrane thickness is 600-;
in the battery assembling process, the anode and the cathode are completely soaked in the electrolyte and then assembled.
2. The zinc-bromine battery of claim 1 wherein the coating thickness is 20-40 um.
3. The zinc-bromine battery of claim 1 wherein the electrolyte concentration is: 0.5-3M zinc bromide and 1-4M potassium chloride.
4. The zinc-bromine battery of claim 1 wherein the positive and negative end plates are stainless steel plates and the current collector is a graphite plate or carbon composite plate.
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CN114497670B (en) * 2020-11-12 2023-10-13 中国科学院大连化学物理研究所 Zinc bromine single-liquid flow galvanic pile
CN114497660B (en) * 2020-11-12 2023-12-19 中国科学院大连化学物理研究所 Application of complexing agent in zinc-bromine storage battery electrolyte
CN114497616B (en) * 2020-11-12 2023-10-13 中国科学院大连化学物理研究所 Zinc-bromine storage battery
CN114628719B (en) * 2020-12-11 2023-12-22 中国科学院大连化学物理研究所 High-capacity zinc-bromine single flow battery

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