CN112599828B - Novel titanium-manganese single flow battery - Google Patents
Novel titanium-manganese single flow battery Download PDFInfo
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- CN112599828B CN112599828B CN202011482443.0A CN202011482443A CN112599828B CN 112599828 B CN112599828 B CN 112599828B CN 202011482443 A CN202011482443 A CN 202011482443A CN 112599828 B CN112599828 B CN 112599828B
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- MECMQNITHCOSAF-UHFFFAOYSA-N manganese titanium Chemical compound [Ti].[Mn] MECMQNITHCOSAF-UHFFFAOYSA-N 0.000 title claims abstract description 30
- 239000003792 electrolyte Substances 0.000 claims abstract description 64
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Inorganic materials O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 claims abstract description 15
- 238000003860 storage Methods 0.000 claims abstract description 11
- WAEMQWOKJMHJLA-UHFFFAOYSA-N Manganese(2+) Chemical group [Mn+2] WAEMQWOKJMHJLA-UHFFFAOYSA-N 0.000 claims abstract description 10
- 229910001437 manganese ion Inorganic materials 0.000 claims description 27
- 239000010936 titanium Substances 0.000 claims description 15
- 239000011148 porous material Substances 0.000 claims description 11
- 239000007774 positive electrode material Substances 0.000 claims description 10
- 229910052719 titanium Inorganic materials 0.000 claims description 10
- -1 titanium ions Chemical class 0.000 claims description 10
- 238000006243 chemical reaction Methods 0.000 claims description 9
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 7
- 229910052799 carbon Inorganic materials 0.000 claims description 6
- 239000003575 carbonaceous material Substances 0.000 claims description 4
- 238000000151 deposition Methods 0.000 claims description 3
- 239000013618 particulate matter Substances 0.000 claims description 3
- 239000011248 coating agent Substances 0.000 claims description 2
- 238000000576 coating method Methods 0.000 claims description 2
- 230000008021 deposition Effects 0.000 claims description 2
- 239000004744 fabric Substances 0.000 claims description 2
- 239000003014 ion exchange membrane Substances 0.000 claims description 2
- 239000012528 membrane Substances 0.000 claims description 2
- 229910052751 metal Inorganic materials 0.000 claims description 2
- 239000007769 metal material Substances 0.000 claims description 2
- 239000000758 substrate Substances 0.000 claims description 2
- 239000000463 material Substances 0.000 claims 2
- 238000004519 manufacturing process Methods 0.000 abstract description 2
- 238000001556 precipitation Methods 0.000 abstract 1
- 238000011161 development Methods 0.000 description 4
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 description 3
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 description 3
- 229910052794 bromium Inorganic materials 0.000 description 3
- 230000007613 environmental effect Effects 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- 239000007773 negative electrode material Substances 0.000 description 3
- ZRXYMHTYEQQBLN-UHFFFAOYSA-N [Br].[Zn] Chemical compound [Br].[Zn] ZRXYMHTYEQQBLN-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000004146 energy storage Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 239000013049 sediment Substances 0.000 description 2
- HYHCSLBZRBJJCH-UHFFFAOYSA-N sodium polysulfide Chemical compound [Na+].S HYHCSLBZRBJJCH-UHFFFAOYSA-N 0.000 description 2
- 229910052720 vanadium Inorganic materials 0.000 description 2
- LCKIEQZJEYYRIY-UHFFFAOYSA-N Titanium ion Chemical compound [Ti+4] LCKIEQZJEYYRIY-UHFFFAOYSA-N 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 238000012864 cross contamination Methods 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000007323 disproportionation reaction Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- XLYOFNOQVPJJNP-ZSJDYOACSA-N heavy water Substances [2H]O[2H] XLYOFNOQVPJJNP-ZSJDYOACSA-N 0.000 description 1
- 239000011702 manganese sulphate Substances 0.000 description 1
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 1
- 239000012982 microporous membrane Substances 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000011236 particulate material Substances 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000027756 respiratory electron transport chain Effects 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 229910000349 titanium oxysulfate Inorganic materials 0.000 description 1
- 238000006276 transfer reaction Methods 0.000 description 1
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Classifications
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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
-
- 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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- Fuel Cell (AREA)
- 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)
Abstract
The invention discloses a single flow battery, which comprises a titanium-manganese battery module, a circulating pump, a negative electrolyte storage tank, a negative electrolyte input pipeline and a negative electrolyte output pipeline, wherein the titanium-manganese battery module is connected with the circulating pump through the negative electrolyte storage tank; the titanium-manganese battery module comprises a positive electrode, a diaphragm and a negative electrode; the redox couple of the negative electrode is Ti3+/Ti4+The redox couple of the positive electrode is Mn2+/MnO2Solves the problem of anode MnO2The problem that the anode is easy to block due to precipitation is solved, the battery cost is greatly reduced, the popularization and the application of the flow battery are facilitated, and the flow battery has the characteristics of long cycle life and simple structure and manufacturing process.
Description
Technical Field
The invention belongs to the field of batteries, and particularly relates to a novel titanium-manganese single flow battery.
Background
With the development of economy, the demand for energy is increasing, and environmental problems caused by the large consumption of fossil energy are becoming more prominent. The method utilizes renewable energy resources on a large scale, and realizes energy diversification as an important strategy for energy safety and sustainable development of countries in the world. However, the discontinuity and instability of renewable energy sources such as wind energy and solar energy make their direct utilization difficult, so that the continuous supply of renewable energy sources by using energy storage technology becomes the key to solve the above problems. The flow battery has good safety and long service life due to flexible design (energy and power separated design), and has become one of the technologies with the best prospect in the large-scale energy storage market.
The current developed and mature liquid flow systems comprise all-vanadium liquid flow batteries, zinc-bromine liquid flow batteries, sodium polysulfide bromine and other systems. However, the all-vanadium redox flow battery has the problems of high cost and strong acidity and corrosivity of electrolyte; in addition, zinc bromine flow battery systems and sodium polysulfide bromine systems face the problems of volatility and corrosiveness of bromine, and the environmental pollution is serious. Therefore, the development of a novel flow battery with low cost, environmental friendliness and high reliability becomes important.
The titanium-manganese flow battery is a novel flow battery with low cost and environmental friendliness, and is gradually paid the attention of researchers, but the positive trivalent manganese ion is disproportionated to generate MnO2Deposit, easily cause the blockage of the anode and the damage of the galvanic pile, and generally avoid the generation of MnO by methods such as controlling the concentration of trivalent manganese ions and the like2The development of the titanium-manganese flow battery is seriously hindered by the sediment which is difficult to completely avoid the fault and only can utilize the single electron transfer reaction from the divalent manganese ions to the trivalent manganese ions.
Disclosure of Invention
Aiming at the problems, the application provides a novel titanium-manganese single flow battery, the electrolyte of a positive electrode does not flow, and the disproportionation reaction of trivalent manganese ions is fully utilized to generate MnO2And the sediment widens the reaction process from the divalent manganese ions to the trivalent manganese ions to the reaction process from the divalent manganese ions to the tetravalent manganese ions, so that the energy density of the anode electrolyte is improved, the potential risk that the anode of the titanium-manganese flow battery is easily blocked is solved, and the popularization and the application of the titanium-manganese flow battery are facilitated.
In order to achieve the purpose, the specific technical scheme of the invention is as follows:
the invention provides a single flow battery, which comprises a titanium-manganese battery module, a circulating pump, a negative electrolyte storage tank, a negative electrolyte input pipeline and a negative electrolyte output pipeline, wherein the titanium-manganese battery module is connected with the circulating pump through the negative electrolyte input pipeline;
the titanium manganese battery module comprises a single battery or a galvanic pile formed by connecting two or more single batteries in series;
the single cell comprises a positive electrode end plate, a negative electrode end plate, a current collecting plate, a positive electrode bipolar plate, a positive electrode material, a cell diaphragm, a negative electrode material and a negative electrode bipolar plate, wherein the positive electrode bipolar plate, the positive electrode material, the cell diaphragm, the negative electrode material and the negative electrode bipolar plate are sequentially overlapped between the positive electrode end plate and the current collecting plate;
the galvanic pile comprises a positive electrode end plate, a negative electrode end plate, a current collecting plate, N positive electrode bipolar plates which are sequentially overlapped between the positive electrode end plate and the current collecting plate, a positive electrode material arranged in a cavity of a positive electrode frame, a battery diaphragm, a negative electrode material arranged in a cavity of a negative electrode frame and a negative electrode bipolar plate; the N combinations are connected in series; n is more than or equal to 2, and N is an integer;
the negative electrolyte storage tank is communicated with the negative electrode through a negative electrolyte input pipeline and a negative electrolyte output pipeline, and the circulating pump is arranged on the negative electrolyte input pipeline;
the single flow battery also comprises a positive electrolyte, and the positive electrolyte is the same as the negative electrolyte; a cavity is arranged between the positive electrode and the diaphragm; the positive electrode electrolyte does not flow and is sealed in the cavity;
the redox couple of the negative electrode is Ti3+/Ti4+The redox couple of the positive electrode is Mn2+/MnO2。
Negative electrode: 2Ti3++2H2O-2e-＝2TiO2++4H+(ii) a And (3) positive electrode: MnO2+4H++2e-＝Mn2++2H2O
Based on the technical scheme, preferably, the positive electrode material in the cavity of the positive electrode frame between the positive bipolar plate and the battery diaphragm is a porous material, the positive electrolyte is sealed in the pores of the porous material, and the positive electrode MnO is2The particle substances are deposited on the surface of the porous material, and the specific surface area of the porous material is more than 0.2-1000 m2(ii) a porosity of 1-60%.
Based on the above technical scheme, preferably, seal structure is adopted to the positive pole side, need not to dispose anodal electrolyte storage tank, circulating pump and circulating line alone, the positive pole is equipped with anodal electrolyte and advances, exports for the filling of anodal electrolyte before the battery operation.
Based on the above technical solution, preferably, the negative electrode electrolyte contains manganese ions (Mn)2+) And titanium ions (including Ti)3+And Ti4+) Sulfuric acid solution of (2), ratio of two ionsBy way of example and not limitation, the total concentration of titanium ions is in the range of 1mol dm-3～5mol·dm-3The total concentration of manganese ions is 0-5 mol/dm-3。
Based on the technical scheme, preferably, the positive electrolyte contains manganese ions (including Mn)2+，Mn3+) And titanium ion (Ti)4+) Sulfuric acid solution of (2) having a total manganese ion concentration of 1mol dm-3～5mol·dm-3MnO formed by the reaction of the positive electrode2The particulate matter is deposited on the surface of the porous material with a deposition amount of 0.1g/cm2～100g/cm2(ii) a The total concentration of titanium ions is 0-5 mol dm-3。
Based on the above technical solution, preferably, the positive electrode and the negative electrode both use a plate-shaped or porous metal or carbon material; the positive electrode is used as a substrate to be coated with a positive active material; the positive active material is MnO2A particulate material.
Based on the technical scheme, preferably, the carbon material is carbon felt, carbon cloth or carbon paper.
Based on the above technical solution, preferably, the coating amount of the positive electrode active material on the positive electrode is 0.1g/cm2～100g/cm2。
Based on the above technical scheme, preferably, the titanium-manganese battery module further comprises a negative electrode frame and a positive electrode frame; the positive electrode is positioned in the positive electrode frame, and the negative electrode is positioned in the negative electrode frame; the thickness of the negative electrode frame is 0.1-4mm, and the thickness of the negative electrode is 0.05-5 mm; the thickness of the positive electrode frame is 1-20mm, and the thickness of the positive electrode is 1-30 mm.
Based on the technical scheme, preferably, the diaphragm is an ion exchange membrane, a porous membrane or a microporous membrane.
Advantageous effects
1. The application provides a novel titanium-manganese single flow battery, and positive and negative electrolytes all contain manganese ions and titanium ions, so that cross contamination of the positive and negative electrolytes is avoided.
2. The application solves the problem of anode MnO by sealing the anode electrolyte2The precipitate is easy to block in the flowing processThe positive pole and the conveying pipeline, greatly reduces the cost of the battery, is beneficial to the popularization and the application of the flow battery, and has the characteristics of long cycle life, simple structure and simple manufacturing process.
3. The electrolyte of the anode contains manganese ions, and in the reaction process of the anode, the existence of titanium ions can delay Mn3+To MnO2So that MnO is formed2Can be dispersed in the electrolyte to avoid the instant generation of large amount of MnO2Agglomeration causes clogging of electrode pores and increases battery life.
4. Compared with the conventional reaction process of utilizing the divalent manganese ions to the trivalent manganese ions, the reaction process of utilizing the divalent manganese ions to the tetravalent manganese ions greatly improves the energy density of the anode electrolyte.
Drawings
FIG. 1 is a schematic diagram of a single cell of the titanium manganese single flow battery of example 1;
FIG. 2 is a graph of the cycling efficiency of the titanium manganese single flow battery in example 1;
in the figure; 1. a positive electrode terminal plate; 2. a negative terminal plate; 3. a positive electrode; 4. a negative electrode; 5. a diaphragm; 6. a circulation pump; 7. a negative electrolyte storage tank.
Detailed Description
The raw materials used in the examples are all conventional products which are commercially available.
Example 1
1. Electrolyte preparation:
the positive and negative electrodes were the same, and 40ml of each electrolyte was prepared, and the electrolyte content was 1mol dm-3Manganese sulfate and 1mol dm-3Titanyl sulfate.
2. Assembling the battery:
the single cell is arranged according to the positive electrode end plate and the positive electrode (3 multiplied by 3 cm)2Graphite felt, a diaphragm (Nafion211), and a negative electrode (3X 3 cm)2Sequentially assembling the graphite felt) and the negative end plate;
assembling the single battery with a circulating pump, a negative electrolyte storage tank, a negative electrolyte input pipeline and a negative electrolyte output pipeline; the negative electrolyte storage tank is communicated with the negative electrode through a negative electrolyte input pipeline and a negative electrolyte output pipeline, the circulating pump is arranged on the negative electrolyte input pipeline, and the positive electrolyte is sealed in a cavity between the positive electrode and the diaphragm; the assembled cell structure and system are shown in fig. 1.
3. And (3) testing the battery:
when the flow rate of the electrolyte at the negative electrode is 5ml/min, the charge-discharge current density is 80-100mA/cm2As shown in fig. 2, the average energy efficiency of the battery is about 80%, and the cycle life is 2000 or more.
Comparative example 1
The difference from example 1 is that: the anode electrolyte circularly flows, and specifically comprises the following steps: the anode electrolyte is communicated with the anode through an anode electrolyte storage tank input pipeline and an anode electrolyte output pipeline, and the circulating pump is arranged on the anode electrolyte input pipeline.
TABLE 1 comparison of the performance of the titanium-manganese double flow cell of comparative example 1 with that of the titanium-manganese single flow cell of example 1
| Running electric density (mA cm)-2) | Average energy efficiency | Cycle life (circle) | Energy density (Wh. L)-1) | Cost (Yuan/kWh) | |
| Titanium manganese |
100 | 82％ | ＞2000 | 35 | 1500 |
| Titanium-manganese double- |
100 | 75％ | ≈200 | 20 | 2600 |
In table 1, the single cell performances of the titanium-manganese single flow battery and the double flow battery are compared, and the comparison shows that the selected titanium-manganese single flow battery has a current density of 100mA · cm-2The energy efficiency is more than 80 percent and is higher than that of a titanium-manganese double-flow battery. The cycle life of the battery and the cost per kilowatt-hour are obvious and beneficial effects are achieved by the single-flow battery. Most importantly, the titanium manganese single flow battery can broaden the reaction process from the divalent manganese ion to the trivalent manganese ion to the reaction process from the divalent manganese ion to the tetravalent manganese ion, so the energy density is close to twice that of the titanium manganese double flow battery.
Claims (9)
1. A single flow battery, characterized by: the single flow battery comprises a titanium-manganese battery module, a circulating pump, a negative electrolyte storage tank, a negative electrolyte input pipeline and a negative electrolyte output pipeline;
the titanium manganese battery module comprises a single battery or a galvanic pile formed by connecting more than two single batteries in series;
the single cell comprises a positive electrode end plate, a negative electrode end plate, and a positive electrode, a diaphragm and a negative electrode which are sequentially overlapped between the positive electrode end plate and the negative electrode end plate;
the galvanic pile comprises a positive electrode end plate, a negative electrode end plate and a combination of N positive electrodes, diaphragms and negative electrodes which are sequentially overlapped between the positive electrode end plate and the negative electrode end plate; the N combinations are connected in series; n is more than or equal to 2, and N is an integer;
the negative electrolyte storage tank is communicated with the negative electrode through a negative electrolyte input pipeline and a negative electrolyte output pipeline, and the circulating pump is arranged on the negative electrolyte input pipeline;
the single flow battery also comprises positive electrolyte, and a cavity is arranged between the positive electrode and the diaphragm; the positive electrode electrolyte does not flow and is sealed in the cavity;
the redox couple of the negative electrode is Ti3+/Ti4+The redox couple of the positive electrode is Mn2+/MnO2；
The positive electrode and the negative electrode both adopt porous metal or carbon materials; the positive electrode is used as a substrate to be coated with a positive active material; the positive active material is MnO2(ii) particulate matter.
2. The single flow battery as claimed in claim 1, wherein: be equipped with anodal material in the anodal electrode frame cavity between anodal bipolar plate and the battery diaphragm, anodal material is porous material, anodal electrolyte seal in porous material's hole, the MnO that the anodal reaction generated2Depositing the particulate matter on the surface of the porous material; the deposition amount was 0.1g/cm2～100g/cm2(ii) a The specific surface area of the porous material is more than 0.2-1000 m2(ii) a porosity of 1-60%.
3. The single flow battery as claimed in claim 1, wherein: the positive electrolyte is a sulfuric acid solution containing divalent and trivalent manganese ions and tetravalent titanium ions, and the total concentration of the manganese ions is 1mol dm-3～5mol·dm-3The total concentration of the titanium ions is 0-5 mol dm-3。
4. The single flow battery as claimed in claim 1, wherein: the negative electrode electrolyte is a sulfuric acid solution containing trivalent titanium ions, tetravalent titanium ions and divalent manganese ions, and the total concentration of the titanium ions is 1 to5mol·dm-3The total concentration of the manganese ions is 0-5 mol dm-3。
5. The single flow battery as claimed in claim 1, wherein: the positive electrode is provided with a positive electrolyte inlet and a positive electrolyte outlet and is used for filling the positive electrolyte before the battery operates.
6. The single flow battery of claim 1, wherein: the carbon material is carbon felt, carbon cloth or carbon paper.
7. The single flow battery as claimed in claim 1, wherein: the coating amount of the positive electrode active material on the positive electrode is 0.1g/cm2～100g/cm2。
8. The single flow battery as claimed in claim 1, wherein: the titanium-manganese battery module also comprises a negative electrode frame and a positive electrode frame; the positive electrode is positioned in the positive electrode frame, and the negative electrode is positioned in the negative electrode frame; the thickness of the negative electrode frame is 0.1-4mm, and the thickness of the negative electrode is 0.05-5 mm; the thickness of the positive electrode frame is 1-20mm, and the thickness of the positive electrode is 1-30 mm.
9. The single flow battery of claim 1, wherein: the diaphragm is an ion exchange membrane or a porous membrane.
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Inventor after: Qiao Lin Inventor after: Li Haixia Inventor after: Liu Shumin Inventor after: Liu Yuqin Inventor after: Ma Xiangkun Inventor before: Qiao Lin Inventor before: Li Haixia Inventor before: Liu Shumin Inventor before: Liu Yuqin |