CN106328976A - Full-vanadium oxidation reduction flow battery - Google Patents
Full-vanadium oxidation reduction flow battery Download PDFInfo
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- CN106328976A CN106328976A CN201610993954.6A CN201610993954A CN106328976A CN 106328976 A CN106328976 A CN 106328976A CN 201610993954 A CN201610993954 A CN 201610993954A CN 106328976 A CN106328976 A CN 106328976A
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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
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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
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Abstract
The invention provides a full-vanadium oxidation reduction flow battery which comprises an electrode, a membrane, a positive electrode electrolyte and a negative electrode electrolyte, wherein the positive electrode electrolyte contains vanadium ion, sulfuric acid, water and super-acid; the concentration of the super-acid is 0-0.15mol/L; the negative electrode electrolyte contains vanadium ion, sulfuric acid, water and additive containing functional group -NH2 and/or -COOH; the concentration of the additive is 0.05-5% of the concentration of the vanadium ion in the negative electrode electrolyte. The positive electrode electrolyte of the full-vanadium oxidation reduction flow battery provided by the invention can restrain the hydrolysis of pentavalent vanadium ion. The full-vanadium oxidation reduction flow battery has the advantages of high stability of the positive electrode electrolyte, low viscosity of the negative electrode electrolyte and high electrochemical performance.
Description
Technical field
The present invention relates to vanadium chemical field, more particularly, relate to a kind of vanadium redox battery.
Background technology
In the sulfuric acid solution of the vanadium ion that electric energy is stored in different valence state by vanadium cell with the line of chemical energy, will by pump
Electrolyte is pressed in battery so that it is can circulate respectively in cathode chamber and anode chamber, complete charge and discharge at electrode surface
Electric process.Anode electrolyte is by V (IV) and V (V) solution composition, and electrolyte liquid is by V (II) and V (III) solution composition.But
Different valence state V electrolyte stability difference at different temperatures is very big, and V (V) solution is high temperature (> 40 DEG C) under heat stability
Difference, easily generates V2O5Precipitation, and V (II), V (III) and V (IV) solution (< 0 DEG C) at low temperatures easily separate out precipitation, this is greatly
Limit the temperature range of battery operation and the concentration of electrolyte.The acidity and the reduction temperature that increase electrolyte can improve V (V)
The stability of ion, but owing to common-ion effect can accelerate V (II), V (III) and the precipitation of V (IV), meanwhile, improve solution acid
Degree also implies that increase cost.In electrolyte, add a small amount of additive can improve its stability, be a kind of economically feasible
Method.At present the additive of research mainly has two classes: (1) inorganic additive, (2) organic additive.Patent
CN102110836A discloses a kind of interpolation alkaline metal salt, hydroxyl material and cation surface activating in V electrolyte
Agent, its objective is " making vanadium ion electrolyte keep liquid or microemulsion state, to prevent precipitation or the precipitation of vanadium ion ", but
Pentavalent vanadium has strong oxidizing property, and organic additive can be oxidized, it is impossible to plays the effect of stable electrolyte, and changes electrolysis
The state-of-charge of liquid, reduces the efficiency of electrolyte.
In vanadium cell charge and discharge process, the viscosity of electrolyte has great impact to the performance of battery.Electrolyte viscosity
The big diffusion process that not only have impact on vanadium ion, reduces the electro-chemical activity of electrolyte；Also reduce in running and be electrolysed
The flow velocity of liquid, increases pump consumption；More seriously the pressure difference between pile electrolyte entrance and outlet increases, and adds pile leakage
The risk of liquid.
Summary of the invention
For the deficiencies in the prior art, an object of the present invention is to solve present in above-mentioned prior art
One or more problems.Such as, an object of the present invention is to provide a kind of vanadium redox battery, and this battery is just
Pole electrolyte stability is strong, and electrolyte fluid viscosity is low.
To achieve these goals, the invention provides a kind of vanadium redox battery, described battery includes electricity
Pole, barrier film and anode electrolyte and electrolyte liquid, it is characterised in that described anode electrolyte include vanadium ion, sulphuric acid,
Water and super acids, the concentration of described super acids is 0～0.15mol/L, described electrolyte liquid include vanadium ion, sulphuric acid, water and
Containing functional group-NH2And/or the additive of-COOH, the molar concentration of described additive is vanadium ion in described electrolyte liquid
The 0.05%～5% of molar concentration.
One embodiment of the vanadium redox battery according to the present invention, described super acids includes or is trifluoro
One or more in pyrovinic acid, chlorosulfonic acid and fluorine antimony sulfonic acid.
One embodiment of the vanadium redox battery according to the present invention, described super acids is trifluoromethyl sulphur
Acid, the concentration of trifluoromethane sulfonic acid is no more than 0.15mol/L.
One embodiment of the vanadium redox battery according to the present invention, vanadium ion in described anode electrolyte
Concentration is 1.5～3.0mol/L, and sulfuric acid concentration is 2～5mol/L.
One embodiment of the vanadium redox battery according to the present invention, in described electrolyte liquid, additive is
The combination of at least two in organic carboxyl acid, aminoacid and high molecular polymer.
One embodiment of the vanadium redox battery according to the present invention, described organic carboxyl acid includes or is second
One or more in acid, oxalic acid, succinic acid, acrylic acid, citric acid and malic acid.
One embodiment of the vanadium redox battery according to the present invention, described aminoacid includes or is the third ammonia
Acid, valine, leucine, isoleucine, proline, phenylalanine, tryptophan, methionine, glycine, serine, threonine,
In cysteine, tyrosine, agedoite, glutamine, lysine, arginine, histidine, aspartic acid and glutamic acid one
Plant or multiple.
One embodiment of the vanadium redox battery according to the present invention, described high molecular polymer include or
For one or more in polyvinyl alcohol, polyacrylic acid, polyacrylamide and polyvinylpyrrolidone.
One embodiment of the vanadium redox battery according to the present invention, the concentration of vanadium ion in electrolyte liquid
Being 1.5～3mol/L, sulfuric acid concentration is 2～5mol/L.
Compared with prior art, the anode electrolyte of the vanadium redox battery of the present invention can suppress pentavalent vanadium
The hydrolysis of ion, the stability of anode electrolyte is high, and the viscosity of electrolyte liquid is low, chemical property is high.
Detailed description of the invention
Hereinafter, the vanadium redox electricity according to the present invention is described in detail by combining exemplary embodiment
Pond.
The invention provides a kind of vanadium redox battery (also referred to as vanadium cell or battery), the positive electrical of battery
Solving liquid and contain super acids, the acidity of super acids, much stronger than sulphuric acid, adds a small amount of super acids and can improve the acidity of electrolyte, suppress five
The hydrolysis of valency vanadium ion, improves the stability of anode electrolyte；In the electrolyte liquid of battery, additive contains functional group-NH2
And/or-COOH, it can be adsorbed in vanadium ion surface, make more to disperse between vanadium ion by electrostatic repulsion, reduces collision several
Rate, suppression vanadium ion generation condensation reaction forms oligomer.
In one exemplary embodiment of the present invention, vanadium redox battery includes electrode, barrier film, Yi Jizheng
Pole electrolyte and electrolyte liquid, anode electrolyte includes vanadium ion, sulphuric acid, water and super acids, the concentration of super acids be 0～
0.15mol/L, electrolyte liquid includes vanadium ion, sulphuric acid, water and contains functional group-NH2And/or the additive of-COOH, add
The molar concentration of agent is 0.05%～5% of vanadium ion molar concentration in electrolyte liquid.
Additive too much in electrolyte liquid can destroy the hydrated sheath on vanadium ion surface, large volume of additive molecule
Replacement small volume of water Molecular Adsorption, on vanadium ion surface, can make vanadium ion volume increase, cause viscosity to raise, therefore electrolyte
During in liquid, additive concentration should control electrolyte liquid within the 5% of vanadium ion concentration.
In the present example embodiment, in anode electrolyte, the concentration of vanadium ion is 1.5～3.0mol/L, and sulphuric acid is dense
Degree is 2～5mol/L；Super acids includes one or more in trifluoromethane sulfonic acid, chlorosulfonic acid and fluorine antimony sulfonic acid；Preferably, super
Strong acid is trifluoromethane sulfonic acid, and trifluoromethane sulfonic acid concentration is no more than 0.15mol/L.
In the present example embodiment, in electrolyte liquid, the concentration of total vanadium ion is 1.5～3mol/L, and sulfuric acid concentration is
2～5mol/L；Additive be organic carboxyl acid, aminoacid and and high molecular polymer in the combination of at least two, wherein macromolecule
Polymer contains functional group-NH2And/or-COOH.Organic carboxyl acid includes or is acetic acid, oxalic acid, succinic acid, acrylic acid, Fructus Citri Limoniae
One or more in acid and malic acid.Aminoacid includes or is alanine, valine, leucine, isoleucine, dried meat ammonia
Acid, phenylalanine, tryptophan, methionine, glycine, serine, threonine, cysteine, tyrosine, agedoite, paddy ammonia
One or more in amide, lysine, arginine, histidine, aspartic acid and glutamic acid.High molecular polymer contains sense
Group-NH2And/or-COOH, high molecular polymer includes or is polyvinyl alcohol, polyacrylic acid, polyacrylamide and polyethylene pyrrole
One or more in pyrrolidone.
In order to be more fully understood that the above-mentioned exemplary embodiment of the present invention, below in conjunction with concrete example, it is carried out further
Explanation.
Example 1
The anode electrolyte of vanadium redox battery is placed in constant temperature in water-bath stand, tests the steady of electrolyte
Qualitative.Be 2.0mol/L by 150mL total V density, sulfuric acid concentration be the pentavalent vanadium anode electrolyte of 3mol/L be five equal portions, point
Not being placed in the water-bath that temperature is 10 DEG C, 20 DEG C, 30 DEG C, 40 DEG C and 50 DEG C, constant temperature is static until there is precipitation, experimental result
As blank, it is shown in Table 1.
A, being 2.0mol/L by 150mL vanadium ion concentration, sulfuric acid concentration is 3mol/L, and containing 0.75ml trifluoromethyl sulphur
The pentavalent vanadium anode electrolyte of acid is divided into five equal portions, and being respectively placed in temperature is 10 DEG C, 20 DEG C, 30 DEG C, 40 DEG C and the water-bath of 50 DEG C
In Guo, constant temperature is static until there is precipitation, and experimental result is shown in Table 1.
B, being 2.0mol/L by 150mL vanadium ion concentration, sulfuric acid concentration is 3mol/L, and containing 1.5ml trifluoromethyl sulphur
The pentavalent vanadium anode electrolyte of acid is divided into five equal portions, and being respectively placed in temperature is 10 DEG C, 20 DEG C, 30 DEG C, 40 DEG C and the water-bath of 50 DEG C
In Guo, constant temperature is static until there is precipitation, and experimental result is shown in Table 1.
C, being 2.0mol/L by 150mL vanadium ion concentration, sulfuric acid concentration is 3mol/L, and containing 3.0ml trifluoromethyl sulphur
The pentavalent vanadium anode electrolyte of acid is divided into five equal portions, and being respectively placed in temperature is 10 DEG C, 20 DEG C, 30 DEG C, 40 DEG C and the water-bath of 50 DEG C
In Guo, constant temperature is static until there is precipitation, and experimental result is shown in Table 1.
Example 2
Taking 150ml vanadium ion concentration is 2.0mol/L, and sulfuric acid concentration is the trivalent vanadium electrolyte liquid of 3mol/L, at 30 DEG C
Under the conditions of with Ubbelohde viscometer detection electrolyte viscosity, testing result, as blank, is shown in Table 2.
A, to take 150ml vanadium ion concentration be 2.0mol/L, and sulfuric acid concentration is 3mol/L, and containing 0.006mol citric acid,
The trivalent vanadium electrolyte liquid of 0.003mol glutamic acid, by the viscosity of Ubbelohde viscometer detection electrolyte under the conditions of 30 DEG C, real
Test and the results are shown in Table 2.
B, to take 150ml vanadium ion concentration be 2.0mol/L, and sulfuric acid concentration is 3mol/L, and oxalic acid containing 0.002mol,
The polyacrylic trivalent vanadium electrolyte liquid of 0.9g, by the viscosity of Ubbelohde viscometer detection electrolyte under the conditions of 30 DEG C, real
Test and the results are shown in Table 2.
C, to take 150ml vanadium ion concentration be 2.0mol/L, and sulfuric acid concentration is 3mol/L, and containing 0.009mol succinic acid,
The trivalent vanadium electrolyte liquid of 0.009mol glutamic acid, by the viscosity of Ubbelohde viscometer detection electrolyte under the conditions of 30 DEG C, real
Test and the results are shown in Table 2.
D, to take 150ml vanadium ion concentration be 2.0mol/L, and sulfuric acid concentration is 3mol/L, and containing 0.012mol lysine,
The trivalent vanadium electrolyte liquid of 0.5g polyvinylpyrrolidone, gluing with Ubbelohde viscometer detection electrolyte under the conditions of 30 DEG C
Degree, experimental result is shown in Table 2.
E, to take 150ml vanadium ion concentration be 2.0mol/L, and sulfuric acid concentration is 3mol/L, and containing 0.015mol citric acid,
The trivalent vanadium electrolyte liquid of 0.009mol aspartic acid, by the viscosity of Ubbelohde viscometer detection electrolyte under the conditions of 30 DEG C,
Experimental result is shown in Table 1.
F, to take 150ml vanadium ion concentration be 2.0mol/L, and sulfuric acid concentration is 3mol/L, and containing 0.0015mol acrylic acid,
The trivalent vanadium electrolyte liquid of 0.0015mol serine and 0.6g polyacrylic acid amide, uses Ubbelohde viscometer under the conditions of 30 DEG C
The viscosity of detection electrolyte, experimental result is shown in Table 2.
The stability of table 1 pentavalent anode electrolyte of vanadium battery
(in table 1, d1 represents sky, h representative hour.)
As it can be seen from table 1 at relatively high temperatures, the stability that anode electrolyte of vanadium battery contains trifluoromethane sulfonic acid is bright
Aobvious enhancing.Under the conditions of 30 DEG C, in A, B, C, vanadic anhydride (V2O5) the time ＞ 30 days of Precipitation；Under the conditions of 40 DEG C,
In A, B, C, vanadic anhydride (V2O5) time >=36h of Precipitation；Under the conditions of 50 DEG C, in A, B, C, vanadic anhydride
(V2O5) time >=4h of Precipitation.
The viscosity of table 2 trivalent vanadium electrolyte liquid
| Numbering | Viscosity (mm2/s) |
| Blank | 6.85 |
| a | 6.63 |
| b | 6.70 |
| c | 6.56 |
| d | 6.66 |
| e | 6.52 |
| f | 6.45 |
From table 2 it can be seen that after addition additive, the viscosity≤6.70mm of vanadium redox battery negative pole electrolyte2/ s, is respectively less than not
Add the viscosity number of the trivalent vanadium battery electrolyte of additive.
In sum, the stability of the anode electrolyte of the vanadium redox battery of the present invention is remarkably reinforced, negative
The viscosity of pole electrolyte substantially reduces, and the chemical property of electrolyte is good.
Although the most describing the present invention by combining exemplary embodiment, but those skilled in the art should be clear
Chu, in the case of the spirit and scope limited without departing from claim, can be carried out respectively the exemplary embodiment of the present invention
Plant modifications and changes.
Claims (9)
1. a vanadium redox battery, described battery includes electrode, barrier film and anode electrolyte and electrolyte
Liquid, it is characterised in that described anode electrolyte include vanadium ion, sulphuric acid, water and super acids, the concentration of described super acids be 0～
0.15mol/L, described electrolyte liquid includes vanadium ion, sulphuric acid, water and contains functional group-NH2And/or the additive of-COOH,
The molar concentration of described additive is in described electrolyte liquid the 0.05%～5% of vanadium ion molar concentration.
Vanadium redox battery the most according to claim 1, it is characterised in that described super acids includes fluoroform
One or more in base sulfonic acid, chlorosulfonic acid and fluorine antimony sulfonic acid.
Vanadium redox battery the most according to claim 2, it is characterised in that described super acids is trifluoromethyl
Sulfonic acid, the concentration of trifluoromethane sulfonic acid is no more than 0.15mol/L.
Vanadium redox battery the most according to claim 1, it is characterised in that in described anode electrolyte vanadium from
The concentration of son is 1.5～3.0mol/L, and sulfuric acid concentration is 2～5mol/L.
Vanadium redox battery the most according to claim 1, it is characterised in that add in described electrolyte liquid
Agent is the combination of at least two in organic carboxyl acid, aminoacid and high molecular polymer.
Vanadium redox battery the most according to claim 5, it is characterised in that described organic carboxyl acid includes second
One or more in acid, oxalic acid, succinic acid, acrylic acid, citric acid and malic acid.
Vanadium redox battery the most according to claim 5, it is characterised in that described aminoacid includes the third ammonia
Acid, valine, leucine, isoleucine, proline, phenylalanine, tryptophan, methionine, glycine, serine, threonine,
In cysteine, tyrosine, agedoite, glutamine, lysine, arginine, histidine, aspartic acid and glutamic acid one
Plant or multiple.
Vanadium redox battery the most according to claim 5, it is characterised in that described high molecular polymer includes
One or more in polyvinyl alcohol, polyacrylic acid, polyacrylamide and polyvinylpyrrolidone.
Vanadium redox battery the most according to claim 1, it is characterised in that vanadium ion in electrolyte liquid
Concentration is 1.5～3mol/L, and sulfuric acid concentration is 2～5mol/L.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110970646A (en) * | 2018-09-29 | 2020-04-07 | 中国科学院大连化学物理研究所 | Application of additive in negative electrode electrolyte of all-vanadium redox flow battery |
| CN111200150A (en) * | 2018-11-19 | 2020-05-26 | 大连融科储能技术发展有限公司 | All-vanadium redox flow battery electrolyte formula and process for maintaining high performance of electrolyte |
| CN111244519A (en) * | 2020-01-21 | 2020-06-05 | 西安理工大学 | Reducible and renewable electrolyte suitable for single flow battery and preparation method thereof |
| CN111313071A (en) * | 2018-12-11 | 2020-06-19 | 中国科学院大连化学物理研究所 | All-vanadium redox flow battery negative electrode electrolyte and method for reducing negative electrode vanadium ion migration |
| WO2022014195A1 (en) * | 2020-07-17 | 2022-01-20 | 住友電気工業株式会社 | Electrolytic solution and redox flow cell |
| CN115498232A (en) * | 2022-11-18 | 2022-12-20 | 苏州融科储能技术有限公司 | Electrolyte and all-vanadium redox flow battery |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110970646A (en) * | 2018-09-29 | 2020-04-07 | 中国科学院大连化学物理研究所 | Application of additive in negative electrode electrolyte of all-vanadium redox flow battery |
| CN110970646B (en) * | 2018-09-29 | 2021-06-25 | 中国科学院大连化学物理研究所 | Application of additive in negative electrode electrolyte of all-vanadium redox flow battery |
| CN111200150A (en) * | 2018-11-19 | 2020-05-26 | 大连融科储能技术发展有限公司 | All-vanadium redox flow battery electrolyte formula and process for maintaining high performance of electrolyte |
| CN111200150B (en) * | 2018-11-19 | 2021-10-26 | 大连融科储能技术发展有限公司 | All-vanadium redox flow battery electrolyte formula and process for maintaining high performance of electrolyte |
| CN111313071A (en) * | 2018-12-11 | 2020-06-19 | 中国科学院大连化学物理研究所 | All-vanadium redox flow battery negative electrode electrolyte and method for reducing negative electrode vanadium ion migration |
| CN111244519A (en) * | 2020-01-21 | 2020-06-05 | 西安理工大学 | Reducible and renewable electrolyte suitable for single flow battery and preparation method thereof |
| CN111244519B (en) * | 2020-01-21 | 2023-01-24 | 西安理工大学 | Reducible regenerative electrolyte suitable for single flow battery and preparation method thereof |
| WO2022014195A1 (en) * | 2020-07-17 | 2022-01-20 | 住友電気工業株式会社 | Electrolytic solution and redox flow cell |
| CN115498232A (en) * | 2022-11-18 | 2022-12-20 | 苏州融科储能技术有限公司 | Electrolyte and all-vanadium redox flow battery |
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