CN118156571A - Zinc-bromine flow battery performance recovery method - Google Patents
Zinc-bromine flow battery performance recovery method Download PDFInfo
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- CN118156571A CN118156571A CN202211550192.4A CN202211550192A CN118156571A CN 118156571 A CN118156571 A CN 118156571A CN 202211550192 A CN202211550192 A CN 202211550192A CN 118156571 A CN118156571 A CN 118156571A
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- ZRXYMHTYEQQBLN-UHFFFAOYSA-N [Br].[Zn] Chemical compound [Br].[Zn] ZRXYMHTYEQQBLN-UHFFFAOYSA-N 0.000 title claims abstract description 44
- 238000011084 recovery Methods 0.000 title claims abstract description 43
- 238000000034 method Methods 0.000 title claims abstract description 31
- 239000003792 electrolyte Substances 0.000 claims abstract description 67
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims abstract description 16
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 claims abstract description 15
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 claims abstract description 15
- 229910052794 bromium Inorganic materials 0.000 claims abstract description 15
- 239000007788 liquid Substances 0.000 claims description 35
- 238000002156 mixing Methods 0.000 claims description 20
- 239000000243 solution Substances 0.000 claims description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 8
- VNDYJBBGRKZCSX-UHFFFAOYSA-L zinc bromide Chemical compound Br[Zn]Br VNDYJBBGRKZCSX-UHFFFAOYSA-L 0.000 claims description 6
- 239000007864 aqueous solution Substances 0.000 claims description 3
- 229940102001 zinc bromide Drugs 0.000 claims description 3
- IDQXZLKEWHBPCA-UHFFFAOYSA-N 2-ethyl-1-methylpyrrolidine Chemical compound CCC1CCCN1C IDQXZLKEWHBPCA-UHFFFAOYSA-N 0.000 claims description 2
- CPELXLSAUQHCOX-UHFFFAOYSA-M Bromide Chemical compound [Br-] CPELXLSAUQHCOX-UHFFFAOYSA-M 0.000 claims description 2
- 239000000203 mixture Substances 0.000 claims description 2
- 239000008139 complexing agent Substances 0.000 claims 1
- 239000002904 solvent Substances 0.000 claims 1
- 239000003115 supporting electrolyte Substances 0.000 claims 1
- 239000011701 zinc Substances 0.000 description 7
- 229910052725 zinc Inorganic materials 0.000 description 7
- 238000009825 accumulation Methods 0.000 description 6
- 239000013543 active substance Substances 0.000 description 6
- 238000004146 energy storage Methods 0.000 description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 5
- 239000011149 active material Substances 0.000 description 5
- 229910052799 carbon Inorganic materials 0.000 description 5
- 238000002474 experimental method Methods 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 239000003795 chemical substances by application Substances 0.000 description 4
- 238000007599 discharging Methods 0.000 description 4
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 4
- 238000007086 side reaction Methods 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 239000008151 electrolyte solution Substances 0.000 description 3
- 229940021013 electrolyte solution Drugs 0.000 description 3
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- CPELXLSAUQHCOX-UHFFFAOYSA-N Hydrogen bromide Chemical compound Br CPELXLSAUQHCOX-UHFFFAOYSA-N 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 235000019253 formic acid Nutrition 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000005431 greenhouse gas Substances 0.000 description 2
- BMYNFMYTOJXKLE-UHFFFAOYSA-N 3-azaniumyl-2-hydroxypropanoate Chemical compound NCC(O)C(O)=O BMYNFMYTOJXKLE-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- PTFCDOFLOPIGGS-UHFFFAOYSA-N Zinc dication Chemical compound [Zn+2] PTFCDOFLOPIGGS-UHFFFAOYSA-N 0.000 description 1
- 125000003172 aldehyde group Chemical group 0.000 description 1
- 230000002238 attenuated effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
- 230000002860 competitive effect Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 239000007774 positive electrode material Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
Classifications
-
- 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
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04298—Processes for controlling fuel cells or fuel cell systems
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- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Hybrid Cells (AREA)
Abstract
The invention relates to the technical field of flow batteries, in particular to the field of zinc-bromine flow batteries. The invention provides a performance recovery method of a high-concentration zinc-bromine flow battery, namely when the battery needs to be recovered, firstly, battery electrolyte is mixed with each other, then zinc powder is added into the electrolyte, and accumulated bromine is eliminated. The method can fully recover the electrolyte of the zinc-bromine flow battery to an initial state, the first circle of the battery has higher coulombic efficiency after recovery, the recovery frequency of the battery is reduced, H 2 and CO 2 are not generated, the safety of the system is improved, and the environment is friendly.
Description
Technical Field
The invention relates to the technical field of flow batteries, in particular to the field of zinc-bromine flow batteries.
Background
Renewable energy sources such as wind energy and solar energy have the characteristics of discontinuity and instability, and the characteristic can cause impact on a power grid in the grid connection process, so that the safe and stable operation of the power grid is affected. The energy storage technology can ensure the high-efficiency stable operation of the renewable energy power generation grid connection. The energy storage technology is mainly divided into two main types of physical energy storage and chemical energy storage. Redox flow batteries suitable for large-scale and large-capacity energy storage in chemical energy storage are receiving attention because of the advantages of independent battery power and capacity, rapid response, simple structure, easy design and the like. The zinc-bromine flow battery, which is one of redox flow batteries, has the advantages of high open-circuit voltage (1.85V), high theoretical energy density (435 Wh/Kg), low price of electrolyte and diaphragm and the like besides the advantages. These advantages also make it more competitive with other flow batteries.
The zinc-bromine flow battery has the problem of accumulation of positive and negative active substances in the charge-discharge operation process, and the accumulation of the active substances can lead the polarization of the battery to become large, so that the performance of the battery is attenuated, and the service life of the battery is influenced. In the recovery method of the zinc-bromine flow battery in the prior art, after the running performance of the battery is reduced, a recovery agent is added into positive electrode electrolyte and/or negative electrode electrolyte, the recovery agent is an organic or inorganic substance which contains hydroxyl, aldehyde group and carboxyl and is mutually soluble with the zinc-bromine battery electrolyte and has reducibility, the recovery agent can be oxidized by a positive electrode bromine simple substance to generate protons and organic or inorganic micromolecular products, and the protons penetrate through a membrane to reach the negative electrode to react with the negative electrode zinc simple substance to generate zinc ions, so that the zinc-bromine or zinc-bromine single flow battery electrolyte is recovered to an initial state (ZL 201611089121.3); and the other is that after the battery is operated for a period of time, the positive electrode electrolyte in the positive electrode cavity is led into the negative electrode storage tank to be mixed with the negative electrode electrolyte, then part of the mixed liquid is filled into the positive electrode cavity again, and the performance of the battery is recovered through the mutual mixing of the positive electrode electrolyte and the negative electrode electrolyte (ZL 201711213349.3). The first recovery method can generate hydrogen after adding the recovery agent, so that the safe and stable operation of the system is affected, meanwhile, zinc generated in the first-circle charging process after the negative electrode is recovered and hydrobromic acid are subjected to chemical reaction, so that the charge-discharge coulomb efficiency of the first-circle battery is low, and in addition, greenhouse gas carbon dioxide is generated; in the second method, harmful gas is not generated when the battery performance is recovered by mixing the electrolyte, but the side reaction of the zinc anode is aggravated along with the increase of the concentration of the active material, so that the problem of accumulation of bromine of the active material of the positive electrode can exist after the electrolyte is mixed. The accumulation of bromine as the positive electrode active material causes the zinc generated by the charge of the negative electrode in the first-cycle charge-discharge cycle to react with bromine in the electrolyte first, so that the coulomb efficiency of the first-cycle battery is low.
Disclosure of Invention
The high-concentration zinc-bromine flow battery has the advantages that the side reaction of a zinc negative electrode is aggravated along with the increase of the concentration of an active substance, so that the problem of accumulation of bromine of an anode active substance exists after electrolyte is mixed, the accumulation of bromine of the anode active substance causes the zinc generated by charging the negative electrode in the first-cycle charge-discharge cycle process to react with bromine in the electrolyte at first, and the first-cycle coulomb efficiency of the battery is lower.
The invention provides a performance recovery method of a high-concentration zinc-bromine flow battery, namely when the battery needs to be recovered, firstly, battery electrolyte is mixed with each other, then zinc powder is added into the electrolyte, and accumulated bromine is eliminated. The method can fully recover the electrolyte of the zinc-bromine flow battery to an initial state, the first circle of the battery has higher coulombic efficiency after recovery, the recovery frequency of the battery is reduced, H 2 and CO 2 are not generated, the safety of the system is improved, and the environment is friendly.
The complete technical scheme provided by the invention is that the performance recovery method of the zinc-bromine flow battery is that when the battery needs to be recovered, the anode and cathode electrolyte is firstly mixed with the anode and cathode of the battery. When the voltage of the battery is reduced to 0V, zinc powder is respectively added into the positive and negative electrode liquid storage tanks until the electrolyte of the positive and negative electrode liquid storage tanks is colorless.
The positive and negative electrolyte of the zinc-bromine flow battery has the same initial composition.
The concentration of zinc bromide in the zinc-bromine flow battery electrolyte is 3-7M.
The technical proposal of the invention has the beneficial effects that
1. The recovery method can enable the first circle of the high-concentration zinc-bromine flow battery to have higher coulombic efficiency after recovery, and solves the problem of low coulombic efficiency of the first circle after recovery in the prior art.
2. And the battery recovery frequency is reduced by improving the coulomb efficiency of the first circle after recovery.
3. The recovery method is simple in operation, safe, reliable and environment-friendly, and dangerous gas (H 2) and greenhouse gas (CO 2) are not generated in the recovery process.
Detailed Description
Comprises a zinc bromine flow battery, an anode liquid storage tank filled with anode electrolyte, a cathode liquid storage tank filled with cathode electrolyte,
The positive electrolyte in the positive liquid storage tank is connected with the positive inlet of the zinc-bromine flow battery through a pump, and the positive outlet of the zinc-bromine flow battery is communicated with the positive liquid storage tank; the negative electrode electrolyte in the negative electrode liquid storage tank is connected with a negative electrode inlet of the zinc-bromine flow battery through a pump, and a negative electrode outlet of the zinc-bromine flow battery is communicated with the negative electrode liquid storage tank;
A first mixing branch pipeline is arranged on a pipeline which is communicated with the anode outlet and the anode liquid storage tank of the zinc-bromine flow battery, and a first mixing valve is arranged on the first mixing branch pipeline; a second mixing branch pipeline is arranged on a pipeline which is communicated with the negative electrode outlet of the zinc-bromine flow battery and the negative electrode liquid storage tank, and a second mixing valve is arranged on the second mixing branch pipeline;
When the positive and negative electrolyte are mixed, the first mixing valve and the second mixing valve are opened, the positive electrolyte flowing out of the positive outlet is led into the positive liquid storage tank and the negative liquid storage tank, and the negative electrolyte flowing out of the negative outlet is led into the positive liquid storage tank and the negative liquid storage tank;
When the voltage of the battery is reduced to 0V, zinc powder is respectively added into the positive and negative electrode liquid storage tanks until the electrolyte in the positive and negative electrode liquid storage tanks is colorless.
Example 1
The circulating performance experiment of the zinc-bromine flow battery is carried out by taking 3MZnBr 2 +0.5M KCl+0.8M MEP (N bromide, ethyl methyl pyrrolidine) aqueous solution as positive and negative electrolyte respectively, wherein the positive and negative electrodes are carbon felts, the flow rate of the electrolyte in positive and negative electrode cavities is 60ml/min, the current density is 40mA/cm 2, the effective area of the electrode is 36cm 2, the battery charging cut-off voltage is 2V, the discharging cut-off voltage is 0.5V, and the volumes of the positive and negative electrolyte are 80ml respectively. First circle coulomb efficiency CE97.1%, VE85.4%, EE82.9%;
After 800 cycles of cell operation, electrolyte intermixing occurs when the cell energy efficiency decays to 70%. After the voltage of the batteries is reduced to 0V, zinc powder is respectively added into the positive and negative electrode liquid storage tanks until the electrolyte of the positive and negative electrode liquid storage tanks is colorless. By adopting the recovery method, the batteries CE of the first circle after recovery are 97.2%, VE84.8% and EE82.4%.
The battery is operated for 500 cycles again for one recovery, and the first cycle of battery CE is 97.4%, VE is 84.2% and EE is 82.0% after recovery.
Example 2
The zinc-bromine flow battery cycle performance experiment is carried out by respectively taking 3MZnBr 2 +0.5M KCl+0.8MMEP water solution, 4MZnBr 2 +0.5M KCl+0.8MMEP water solution, 5MZnBr 2 +0.5M KCl+0.8MMEP water solution, 6MZnBr 2 +0.5M KCl+0.8MMEP water solution and 7MZnBr 2 +0.5M KCl+0.8MMEP water solution as positive and negative electrolyte solutions, wherein the electrodes are carbon felts, the flow rate of the electrolyte solution in positive and negative electrode cavities is 60ml/min, the current density is 40mA/cm 2, the effective area of the electrodes is 36cm 2, the battery charging cut-off voltage is 2V, the discharge cut-off voltage is 0.5V, and the volumes of the positive and negative electrolyte solutions are 80ml respectively. The battery performance after the first cycle and the 800 cycle of battery operation is recovered is as follows,
Both cells CE, VE decreased with increasing active material concentration, mainly due to the increased side reactions of the cells with increasing active material concentration leading to a decrease in cell CE; the decrease in electrolyte conductivity results in a decrease in battery VE. The initial level of the zinc bromide electrolyte CE with different concentrations can be reached after recovery.
Comparative example 1
The circulating performance experiment of the zinc-bromine flow battery is carried out by taking a water solution of 3MZnBr 2 +0.5MKCl+0.8MMEP as an electrolyte, wherein an electrode is made of carbon felt, the flow rate of the electrolyte is 60ml/min, the current density is 40mA/cm 2, the effective area of the electrode is 36cm 2, the charging cut-off voltage of the battery is 2V, the discharging cut-off voltage is 0.5V, and the volume of electrolyte of the anode and the cathode is 80ml respectively. After the first cycle of 97.1% of CE, 85.4% of VE and 800 cycles of running the battery with 82.9% of EE, electrolyte mixing is carried out when the energy efficiency of the battery is reduced to 70% of the energy efficiency of the battery. And after the voltage of the batteries is reduced to 0V, normal charge and discharge are carried out. By adopting the recovery method, the battery CE of the first circle after recovery is 90.1%, VE is 85.1%, and EE is 76.7%. This is mainly due to the presence of bromine in the electrolyte after the battery has been intermixed to 0V due to the presence of negative side reactions.
In addition, the battery is required to be recovered once after 200 cycles of running again by adopting the recovery method, and the first cycle of battery CE89.2%, VE84.2% and EE75.1% are recovered. Compared with the recovery method of adding zinc powder after mixing, the first-circle coulomb efficiency CE of the recovered battery is lower, and the recovery frequency of the battery is increased.
Comparative example 2
The circulating performance experiment of the zinc-bromine flow battery is carried out by taking a water solution of 3MZnBr 2 +0.5MKCl+0.8MMEP as an electrolyte, wherein an electrode is made of carbon felt, the flow rate of the electrolyte is 60ml/min, the current density is 40mA/cm 2, the effective area of the electrode is 36cm 2, the charging cut-off voltage of the battery is 2V, the discharging cut-off voltage is 0.5V, and the volumes of positive and negative electrolyte and electrolyte are 80ml respectively. First circle coulomb efficiency CE97.2%, VE85.1%, EE82.7%;
After 800 cycles of battery operation, formic acid is added into the electrolyte when the energy efficiency of the battery is reduced to 68 percent until the electrolyte turns from red to colorless, and normal charge and discharge are carried out. By adopting the recovery method, the batteries CE of the first circle after recovery is 92.1%, VE is 85.1% and EE is 78.4%. This is mainly due to the chemical reaction of the zinc formed during the first charge with HBr, which is formed by the reaction of formic acid with accumulated bromine to form HBr.
In addition, the battery is operated for 300 cycles again by adopting the recovery method, namely, one recovery is needed, and after the recovery, the first cycle of the battery CE is 91.8%, VE is 84.7% and EE is 77.8%. Compared with the recovery method by adding zinc powder, the recovery method has lower first-circle CE and increased battery recovery frequency.
Comparative example 3
The cycle performance experiment of the zinc-bromine flow battery is carried out by taking 2MZnBr 2 +0.5M KCl+0.8MMEP aqueous solution as positive and negative electrolyte, wherein an electrode is carbon felt, the flow rate of the electrolyte in a positive and negative electrode cavity is 60ml/min, the current density is 40mA/cm 2, the effective area of the electrode is 36cm 2, the battery charging cut-off voltage is 2V, the discharging cut-off voltage is 0.5V, and the volumes of the positive and negative electrolyte are 80ml respectively. After 800 cycles of cell operation, electrolyte intermixing occurs when the cell energy efficiency decays to 69%. After mixing to 0V the electrolyte became colorless, indicating the presence of bromine in the electrolyte.
When the active substance in the solution is 2M, the first circle CE98.4% VE86.1%
EE84.5%, first turn CE 98.2%, VE 86.2%, EE84.6% after intermixing recovery. This also means that when the active material concentration is 2M, the battery performance can be restored to the initial level by only the blending, and there are no problems that only the first-round CE of the blending is low and the restoration frequency is increased at a high concentration.
Claims (7)
1. A performance recovery method of a zinc-bromine flow battery is characterized by comprising the following steps:
When the battery needs to be recovered, firstly, the positive and negative electrolyte of the fully discharged zinc-bromine flow battery are mutually mixed, and then zinc powder is added into the mutually mixed positive and negative electrolyte to eliminate accumulated bromine.
2. A method according to claim 1, characterized in that: when the battery needs to be recovered, the recovery is started after the energy efficiency of the battery is reduced to 60% -70%.
3. A method according to claim 1, characterized in that: the miscible cut-off condition is a drop in cell or stack voltage to 0V.
4. A method according to claim 1, characterized in that: the device comprises a zinc-bromine flow battery, a positive electrode liquid storage tank filled with positive electrode electrolyte and a negative electrode liquid storage tank filled with negative electrode electrolyte, wherein the positive electrode electrolyte in the positive electrode liquid storage tank is connected with a positive electrode inlet of the zinc-bromine flow battery through a pump, and a positive electrode outlet of the zinc-bromine flow battery is communicated with the positive electrode liquid storage tank; the negative electrode electrolyte in the negative electrode liquid storage tank is connected with a negative electrode inlet of the zinc-bromine flow battery through a pump, and a negative electrode outlet of the zinc-bromine flow battery is communicated with the negative electrode liquid storage tank; a first mixing branch pipeline connected with the negative electrode liquid storage tank is arranged on a pipeline of the zinc bromine flow battery, wherein the positive electrode outlet of the zinc bromine flow battery is communicated with the positive electrode liquid storage tank, and a first mixing valve is arranged on the first mixing branch pipeline; a second intermixing branch pipeline connected with the positive electrode liquid storage tank is arranged on a pipeline which is communicated with the negative electrode outlet of the zinc-bromine flow battery and the negative electrode liquid storage tank, and a second intermixing valve is arranged on the second intermixing branch pipeline; when the positive and negative electrolyte are mixed, the first mixing valve and the second mixing valve are opened, the positive electrolyte flowing out of the positive outlet is led into the positive liquid storage tank and the negative liquid storage tank, and the negative electrolyte flowing out of the negative outlet is led into the positive liquid storage tank and the negative liquid storage tank;
When the voltage of the battery is reduced to 0V, zinc powder is respectively added into the positive and negative electrode liquid storage tanks until the electrolyte in the positive and negative electrode liquid storage tanks is colorless.
5. A method according to claim 1 or 4, characterized in that:
After eliminating accumulated bromine, the positive and negative electrolyte of the zinc-bromine flow battery is the same in initial composition, and then the charge and discharge operation of the zinc-bromine flow battery is carried out.
6. A method according to claim 1, characterized in that:
the positive solution and the negative solution of the zinc-bromine flow battery are the same, the concentration of zinc bromide is 3-7M (preferably 5-7M), and water is used as a solvent.
7. The method of claim 6, wherein: wherein, KCl aqueous solution with 0.4-0.8M of supporting electrolyte and bromine complexing agent MEP (N bromide, ethyl methyl pyrrolidine) with 0.6-1M are also added.
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| CN202211550192.4A CN118156571A (en) | 2022-12-05 | 2022-12-05 | Zinc-bromine flow battery performance recovery method |
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