CN108270026B - High-energy gel static vanadium battery - Google Patents
High-energy gel static vanadium battery Download PDFInfo
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- CN108270026B CN108270026B CN201611252321.6A CN201611252321A CN108270026B CN 108270026 B CN108270026 B CN 108270026B CN 201611252321 A CN201611252321 A CN 201611252321A CN 108270026 B CN108270026 B CN 108270026B
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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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- 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
Abstract
The invention relates to a high-energy gel static vanadium battery, which uses positive gel state electrolyte and negative gel state electrolyte, wherein the positive gel state electrolyte and the negative gel state electrolyte respectively comprise vanadium active substances, acid and gelling agents, the concentration range of the vanadium active substances of the positive gel state electrolyte is 3.0-7.0M, and the acidity range of sulfuric acid of the positive gel state electrolyte is 3.0-6.0M; the concentration range of the vanadium active substance of the cathode gel state electrolyte is 3.0-7.0M, the concentration range of the sulfuric acid of the cathode gel state electrolyte is 3.0-5.7M, wherein the cathode gel state electrolyte contains 1-10 wt% of gelling agent, and the cathode gel state electrolyte contains 1-5 wt% of gelling agent. The invention improves the energy density of the battery, improves the crystallization phenomenon of the electrolyte, relieves the osmotic pressure difference generated between the anode and the cathode, and prolongs the service life of the battery.
Description
Technical Field
The invention relates to a high-energy gel static vanadium battery.
Background
The all-vanadium redox flow battery is a redox battery with active substances in a circularly flowing liquid state. The electric energy of the vanadium battery is stored in sulfuric acid electrolyte of vanadium ions with different valence states in a chemical energy mode, the electrolyte is pressed into a battery stack body through an external pump and circularly flows in closed loops of different liquid storage tanks and half batteries under the action of mechanical power, a proton exchange membrane is adopted as a diaphragm of a battery pack, the electrolyte solution parallelly flows through the surface of an electrode and generates electrochemical reaction, and current is collected and conducted through double electrode plates, so that the chemical energy stored in the solution is converted into electric energy. The reversible reaction process enables the vanadium battery to complete charging, discharging and recharging smoothly. The energy density of the all-vanadium redox flow battery is low, about 24Wh/kg, and the all-vanadium redox flow battery is large in occupied area and not suitable for moving due to the fact that the all-vanadium redox flow battery is a redox flow battery.
The high-energy gel static vanadium battery converts energy stored in electrolyte into electric energy by exchanging electrons between two groups of vanadium ions of different types and separated by a layer of diaphragm. Since this electrochemical reaction is reversible, high energy vanadium cells can be both charged and discharged. The electric energy and the chemical energy are mutually converted along with the change of the valence states of the two vanadium ions during charging and discharging. The nominal voltage of the high-energy gel static vanadium battery is 1.25V, the voltage is formed by connecting unit voltages in series, and the current is determined by the surface area of an electrode in a battery unit. Compared with the traditional vanadium redox flow battery, the high-energy gel static vanadium redox flow battery does not need additional pipelines, pumps, valves and storage tanks, so that the cost can be saved; the sealing is carried out in the plastic shell, so that the hidden trouble of liquid leakage and seepage is avoided; the structure is simple, and a complex flow channel design is not needed; the conversion efficiency is high, and no extra power consumption is caused.
The 'Xiaoyu jade article' patent in CN1319207C proposes a high-energy static vanadium battery, and the electrolyte of the high-energy static vanadium battery in the patent contains high-concentration vanadium ions and a stabilizer. The stabilizing agent can prevent the precipitation of high-concentration vanadium ions. However, this patent does not mention that during the charging and discharging processes, the volume of the two sides of the battery is inconsistent due to the internal heat generation of the battery and the easy migration of the electrolytes of the positive and negative electrodes, and the generated osmotic pressure is inconsistent, which leads to the attenuation of the battery capacity.
Patent 201080058340.X [ P ]]In the static vanadium battery, vanadium salt is adopted as an active substance for both the positive electrode and the negative electrode, the vanadium salt is dissolved in sulfuric acid, then excessive moisture is dried to form a solid active substance, the manufacturing process is complicated, vacuum drying is required, the internal resistance of the battery is high, and only 5mA/cm is adopted in a charge-discharge test2The current density of (2) does not allow large current charging and discharging. Meanwhile, the electrolyte is close to a solid state, so that dendritic crystals are easily generated in the charging and discharging processes, and the service life is influenced.
Disclosure of Invention
In order to overcome the problems that the osmotic pressure on two sides is inconsistent and the electrolyte is easy to crystallize to generate a dendritic crystal phenomenon caused by the migration of the positive and negative electrolytes in the charging and discharging processes of the battery in the prior art, the high-energy gel static vanadium battery is provided, wherein the positive gel state electrolyte and the negative gel state electrolyte are used, the positive gel state electrolyte and the negative gel state electrolyte respectively comprise a vanadium active substance, acid (sulfuric acid) and a gelling agent, the concentration range of the vanadium active substance of the positive gel state electrolyte is 3.0-7.0M, preferably 3.5-6.5M, more preferably 4-6M, and the acidity range of the sulfuric acid of the positive gel state electrolyte is 3.0-6.0M, preferably 3.5-5.5M; the concentration range of the vanadium active material of the cathode gel state electrolyte is 3.0-7.0M, preferably 3.5-6.5M, the concentration range of the sulfuric acid of the cathode gel state electrolyte is 3.0-5.7M, preferably 3.5-5.0M, wherein the cathode gel state electrolyte contains 1-10 wt%, preferably 2-8wt% of a gelling agent, and the cathode gel state electrolyte contains 1-5 wt%, preferably 2-4wt% of the gelling agent.
Further, the positive and negative electrode gel state electrolyte vanadium active material is 3.0-7.0M, preferably 4.0-6.0M of 3.5 valence state vanadium ion.
Preferably, the vanadium concentration and acidity of the positive gel state electrolyte are higher than those of the negative gel state electrolyte, more preferably the vanadium concentration of the positive gel state electrolyte is higher than that of the negative gel state electrolyte by more than 2%, preferably more than 5%, more preferably more than 10%, for example 10-20%; the acidity of the positive electrode gel-state electrolyte is higher than that of the negative electrode gel-state electrolyte by 1% or more, more preferably 2% or more, still more preferably 5% or more, for example 5 to 10%.
The gel is preferably one or more of polyvinyl alcohol, polyethylene glycol, polyacrylamide and carboxymethyl cellulose. The molecular weight of the polyvinyl alcohol is 25000-300000, usually 90000-250000, further 100000-200000, the molecular weight of the polyethylene glycol is 200-20000, for example 400-1500, and the molecular weight of the polyacrylamide is 400-2000, for example 400-1000.
Further, the battery comprises a battery tab (pole), a shell, a plate frame (namely an acid-proof liquid storage frame), a sealing element, a positive electrode, a current collector, a diaphragm (an ion exchange membrane or a porous membrane) and a negative electrode, wherein the positive gel electrolyte is adsorbed in the positive electrode, and the negative gel electrolyte is adsorbed in the negative electrode. The structure of the battery can be a static vanadium battery structure which is common in the field.
The invention is characterized in that the gel state electrolyte consists of vanadium active substances, acid and gelling agent. Preferably, the concentration and acidity of vanadium used in the anode and the cathode are different to balance the osmotic pressure difference between the anode and the cathode, and the concentration of the osmotic pressure at the low side is higher than that at the other side; the acidity of the anode and the cathode is different, and the crystallization phenomenon of the anode and the cathode is mainly inhibited according to the different solubility of the anode and the cathode electrolyte in sulfuric acid; wherein the gel state electrolyte vanadium active substance is 3.0-7.0M vanadium ion with 3.5 valence state; the acidity of the sulfuric acid is between 3.0 and 6.0M; the concentration range of vanadium active substances of the positive electrolyte is 3.0-7.0M, and the range of the sulfuric acid degree of the positive electrolyte is 3.0-6.0M; the concentration range of the vanadium active substance of the cathode electrolyte is 3.0-7.0M, and the concentration range of the sulfuric acid of the cathode electrolyte is 3.0-5.7M. The gel is 1-10% in the positive gel state electrolyte and 1-5% in the negative gel state electrolyte.
The high-energy gel static vanadium battery converts energy stored in electrolyte into electric energy by exchanging electrons between two groups of vanadium ions of different types and separated by a layer of diaphragm. The electrolyte is formed by mixing sulfuric acid, vanadium, a stabilizer and the like, and the electrochemical reaction is reversible, so that the high-energy gel static vanadium battery can be charged or discharged. And when the charge and discharge are carried out, the electric energy and the chemical energy are mutually converted along with the change of the valence states of the two vanadium ions. The nominal voltage of the high-energy gel static vanadium battery is 1.25V, the voltage is formed by connecting unit voltages in series, and the current is determined by the surface area of an electrode in a battery unit.
The electrochemical reaction formula of the battery in the charging and discharging processes is as follows:
positive electrode
Negative electrode
The high-energy gel static vanadium battery is a novel energy storage product, the electrolyte and the reaction site are tightly pressed and covered, and a conveying system, a storage tank and the like which are similar to those of the traditional redox flow vanadium battery are not needed. The high-energy gel static vanadium battery contains high-concentration vanadium ions and a stabilizer, has a simple structure, can be made into a square or cylindrical shape, and is convenient to move and transport. Compared with the traditional vanadium redox flow battery, the high-energy gel static vanadium battery has the advantages that the electrolyte is non-flowable, the potential safety hazard of electrolyte leakage of a galvanic pile is eliminated, a pump and a storage tank are omitted, the cost is reduced, a complex runner design and the like are not needed, the processing and the maintenance are simplified, the bypass current and the useless energy consumption loss are reduced, and the high-energy gel static vanadium battery can be used for replacing the fields of mobile phones, low-speed electric vehicles, solar energy storage, wind energy storage, UPS (uninterrupted power supply), communication base stations, power grid peak shaving and the like and the market application aspect of lead-acid batteries.
This patent has mainly solved among the prior art all vanadium redox flow battery (following vanadium dynamic battery for short) energy density low, about 24Wh/kg, and the structure is loaded down with trivial details, the transmission electrolyte pump needs extra consumption energy, the consumption of general pump accounts for 5-7% of entire system energy, and the liquid flow that lasts is sealed, requirements such as safety are higher, need install sensor such as pressure additional and monitor the system, to a great extent has increased the cost of system, make the volume of system great simultaneously. In some remote areas like islands, the use is greatly affected. The high-energy gel static vanadium battery adopts high-concentration vanadium electrolyte, so that the energy density of the battery is substantially improved, and the vanadium dynamic battery increases the capacity only by increasing the volume of the electrolyte, has a simple structure, is convenient to transport and move, does not need a conveying system, does not consume extra energy, improves the conversion efficiency, and reduces the cost of the whole system. The high-concentration vanadium positive electrolyte is easy to crystallize at high temperature, and the negative electrolyte is easy to crystallize at low temperature, so that the problem of crystallization of the high-concentration electrolyte is always a technical bottleneck. The invention solves the problem of crystallization by adding the gelling agent and adopting a mode of asymmetric concentration and acidity of the anode and the cathode, and simultaneously reduces the osmotic pressure difference formed by the anode and the cathode in the charging and discharging processes by the mode of asymmetric concentration and acidity of the anode and the cathode, although the addition of the gelling agent and the increase of the vanadium concentration can increase the viscosity of the electrolyte, the application of the gelling agent to the high-energy gel static vanadium static battery does not need a pump to drive the electrolyte, so that the adverse effect can not be generated.
The invention has the advantages that:
a: the gel static vanadium redox battery has the advantages of simple structure, low cost, high safety, convenience in movement, wide application range and high conversion efficiency, and in addition, the energy density of the gel static vanadium redox battery is improved by using high-concentration electrolyte;
b: the addition of the gelling agent can relieve the precipitation of high-concentration vanadium ions, and in addition, gel-state electrolyte is distributed on the electrode material, so that the electrolyte cannot be unevenly distributed on the electrode due to the action of gravity;
c: because the solubility of the vanadium ions of the positive electrode and the negative electrode in acid is different and the crystallization temperature is not used, the solubility of the vanadium ions can be increased by adopting the asymmetric vanadium concentration and the asymmetric acid concentration, the crystallization problem is relieved, and in addition, the osmotic pressure difference generated by the electrolyte of the positive electrode and the negative electrode in the charging and discharging processes can be relieved;
the invention improves the energy density of the battery, improves the crystallization phenomenon of the electrolyte, relieves the osmotic pressure difference generated between the anode and the cathode, and prolongs the service life of the battery.
Drawings
Fig. 1 is a schematic diagram of a high-energy gel static vanadium battery of the present invention, wherein fig. 1(a) is a schematic diagram of an overall structure of the high-energy gel static vanadium battery, and fig. 1(b) is a partially enlarged diagram.
1: a battery tab (a pole, the tab and the pole are the same words); 2: a housing; 3: plate frames (i.e., acid-resistant liquid storage frames); 4: a seal member; 5: a positive electrode (the gel state electrolyte is absorbed in the positive electrode); 6: a current collector; 7: a diaphragm; 8: and a negative electrode (the gel state electrolyte is absorbed in the negative electrode).
Fig. 2 is a plot of cycle number versus discharge capacity for three cases.
FIG. 3 is a cycle number versus energy efficiency map.
Detailed Description
The invention is further illustrated by the following specific examples, which, however, are to be construed as merely illustrative, and not limitative of the remainder of the disclosure in any way whatsoever.
Case 1:
high-energy gel static vanadium battery 1:
the number of battery sections: 1 is provided with
A diaphragm: ion exchange membrane (Zhejiang Qianqiu environmental protection water treatment Co., Ltd.)
Current collector: graphite block (Shanghai Dongyang carbon Co., Ltd.)
Electrode material: carbon felt (Liaoyang gold valley carbon fiber science and technology limited company)
Electrolyte No. 1: the mass fraction of the gel polyvinyl alcohol added into the positive electrode and the negative electrode is 2%, and the vanadium concentration and the acidity of the positive electrode electrolyte and the negative electrode electrolyte are consistent.
Gel positive and negative electrode electrolyte: the mass fraction of the additive polyvinyl alcohol is 2%, and the vanadium concentration and acidity of the positive and negative electrolyte are as follows: valence of 3.5 (3.5mol/L (V)) +4.6mol/L (H)2SO4) And (3) an electrolyte.
Preparing an electrode: uniformly coating the prepared gel electrolyte on positive and negative electrode felts, wherein the gel electrolyte on the positive and negative electrode sides is 80g respectively; placing the positive and negative electrodes in a positive and negative plastic liquid storage frame to form positive and negative electrodes;
manufacturing the battery: according to the schematic diagram of the battery, the pole, the current collector, the positive electrode, the sealing element, the diaphragm, the sealing element, the negative electrode, the current collector and the pole are sequentially placed in a battery shell and are compressed and packaged.
Case 2:
high-energy gel static vanadium battery 2:
the number and materials of the batteries were the same as those in case 1, and only the electrolyte was different;
electrolyte No. 2: the gel polyvinyl alcohol (analytically pure) added to the anode and the cathode accounts for 2% by mass, the vanadium concentration of the anode electrolyte is 10% higher than that of the cathode electrolyte, and the acidity is 5% higher;
gel positive electrode electrolyte: the mass fraction of the additive polyvinyl alcohol is 2%, and the vanadium concentration and acidity are as follows: valence of 3.5 (3.85mol/L (V)) +4.85mol/L (H)2SO4)；
Gel cathode electrolyte: the mass fraction of the additive polyvinyl alcohol is 2%, and the vanadium concentration and acidity are as follows: valence of 3.5 (3.5mol/L (V)) +4.6mol/L (H)2SO4)；
Preparing an electrode: uniformly coating the prepared gel electrolyte on positive and negative felts, wherein the weight of the gel electrolyte on the positive side is 95 g respectively; 80g of negative electrode electrolyte is placed in the positive and negative electrode plastic liquid storage frame to form positive and negative electrodes;
manufacturing the battery: according to the schematic diagram of the battery, the pole, the current collector, the positive electrode, the sealing element, the diaphragm, the sealing element, the negative electrode, the current collector and the pole are sequentially placed in a battery shell and are compressed and packaged.
Comparative example:
high-energy gel static vanadium battery 3:
the number and materials of the batteries were the same as those in case 1, and only the electrolyte was different;
electrolyte No. 3:
positive and negative electrode electrolytes: valence of 3.5 (3.5mol/L (V)) +4.6mol/L (H)2SO4) An electrolyte solution is added to the electrolyte solution,
preparing an electrode: dipping positive and negative felts in electrolyte to enable the positive and negative felts to fully absorb the electrolyte, wherein the mass of the positive and negative felts is 78.4g, and placing the positive and negative felts in a positive and negative plastic liquid storage frame to form positive and negative electrodes;
manufacturing the battery: according to the schematic diagram of the battery, the pole, the current collector, the positive electrode, the sealing element, the diaphragm, the sealing element, the negative electrode, the current collector and the pole are sequentially placed in a battery shell and are compressed and packaged.
6.2, Performance testing
The assembled battery was subjected to a charge and discharge test using a charge and discharge meter under the conditions that the battery was charged and discharged with a current density of 20mA/cm2, and the charge cut-off voltage was 1.7V and the discharge cut-off voltage was 0.9V, and the test results were shown in fig. 2, 3 and table 1:
TABLE 1 percent capacity reduction and comparative battery drainage liquid volume data
From the test results, the cycle life of the gel-state vanadium battery is far longer than that of the comparative case, and the precipitation amount of the electrolyte from the battery is obviously well inhibited.
Claims (4)
1. A high-energy gel static vanadium battery uses a positive gel state electrolyte and a negative gel state electrolyte, which respectively comprise a vanadium active substance, sulfuric acid and a gelling agent;
the concentration range of vanadium active substances of the positive gel electrolyte is 3.0-7.0M, and the concentration range of sulfuric acid of the positive gel electrolyte is 3.0-6.0M;
the concentration range of the vanadium active substance of the cathode gel state electrolyte is 3.0-7.0M, and the concentration range of the sulfuric acid of the cathode gel state electrolyte is 3.0-5.7M;
wherein the positive electrode gel state electrolyte contains 1-10 wt% of a gelling agent, and the negative electrode gel state electrolyte contains 1-5 wt% of the gelling agent;
the vanadium active substance concentration and the sulfuric acid concentration of the positive gel state electrolyte are higher than those of the negative gel state electrolyte, wherein the battery comprises a battery tab, a shell, a plate frame, a sealing piece, a positive electrode, a current collector, a diaphragm and a negative electrode, the positive gel state electrolyte is adsorbed in the positive electrode, and the negative gel state electrolyte is adsorbed in the negative electrode;
the concentration of the vanadium active substance of the positive gel state electrolyte is 10-20% higher than that of the vanadium active substance of the negative gel state electrolyte, and the concentration of the sulfuric acid of the positive gel state electrolyte is 5-10% higher than that of the sulfuric acid of the negative gel state electrolyte;
the gel is selected from one or more of polyvinyl alcohol, polyethylene glycol, polyacrylamide and carboxymethyl cellulose.
2. The high energy gel static vanadium battery of claim 1 wherein the positive gel state electrolyte has a vanadium active species concentration ranging from 3.5 to 6.5M, the positive gel state electrolyte has a sulfuric acid concentration ranging from 3.5 to 5.5M; the concentration range of the vanadium active substance of the cathode gel state electrolyte is 3.5-6.5M, and the concentration range of the sulfuric acid of the cathode gel state electrolyte is 3.5-5.0M;
wherein, the positive electrode gel state electrolyte contains 2-8wt% of gelling agent, and the negative electrode gel state electrolyte contains 2-4wt% of gelling agent.
3. The high energy gel static vanadium battery of claim 1 wherein the positive gel electrolyte has a vanadium active species concentration in the range of 4 to 6M.
4. The high energy gel static vanadium battery according to any one of claims 1 to 3, wherein the positive and negative gel state electrolyte vanadium active species is 3.0 to 7.0M vanadium ions in 3.5 valence state.
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| CN201611252321.6A CN108270026B (en) | 2016-12-30 | 2016-12-30 | High-energy gel static vanadium battery |
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| CN201611252321.6A CN108270026B (en) | 2016-12-30 | 2016-12-30 | High-energy gel static vanadium battery |
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| CN108270026B true CN108270026B (en) | 2021-06-18 |
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| CN113036156B (en) * | 2019-12-09 | 2022-05-31 | 中国科学院大连化学物理研究所 | Gel electrolyte and zinc-bromine or zinc-iodine single flow battery |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2003157882A (en) * | 2001-11-21 | 2003-05-30 | Sumitomo Electric Ind Ltd | Operation method of redox flow battery |
| CN1507103A (en) * | 2002-12-12 | 2004-06-23 | 肖玉璋 | High-energy static vanadium cell |
| CN103985892A (en) * | 2014-05-15 | 2014-08-13 | 大连融科储能技术发展有限公司 | All-vanadium redox flow battery |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2003157882A (en) * | 2001-11-21 | 2003-05-30 | Sumitomo Electric Ind Ltd | Operation method of redox flow battery |
| CN1507103A (en) * | 2002-12-12 | 2004-06-23 | 肖玉璋 | High-energy static vanadium cell |
| CN103985892A (en) * | 2014-05-15 | 2014-08-13 | 大连融科储能技术发展有限公司 | All-vanadium redox flow battery |
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