CN106328975A - Full-vanadium oxidation reduction flow battery - Google Patents
Full-vanadium oxidation reduction flow battery Download PDFInfo
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- CN106328975A CN106328975A CN201610992633.4A CN201610992633A CN106328975A CN 106328975 A CN106328975 A CN 106328975A CN 201610992633 A CN201610992633 A CN 201610992633A CN 106328975 A CN106328975 A CN 106328975A
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- electrolyte
- vanadium
- battery
- carbon materials
- redox battery
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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
-
- 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 provides a full-vanadium oxidation reduction flow battery which comprises a positive electrode, a negative electrode, a membrane, a positive electrode electrolyte and a negative electrode electrolyte, wherein the negative electrode comprises a carbon material substrate and a Sn-containing electro-catalyst combining with the carbon material surface; the negative electrode electrolyte comprises 1.0mol/L-1.8mol/L of vanadium ion, 2.0mol/L-5.0mol/L of sulfuric acid, and 0.01mol/L-0.3mol/L of Sn phosphate. According to the invention, the Sn-containing electro-catalyst is combined with the carbon material surface, so that the carbon material surface has higher catalytic activity; the electro-catalytic activity of the electrode material for V(III)/V(II) electron pair reaction is increased; the electrochemical polarization is reduced; the voltage efficiency and the energy efficiency of the battery are increased; according to the invention, Sn ion is introduced into the electrolyte, so that the electrochemical activity of the vanadium battery electrolyte is increased; the capacity fading of the vanadium battery is reduced; the use ratio of the electrolyte is increased when the battery is charged/discharged under a high-current density condition; the energy efficiency of the vanadium battery is increased.
Description
Technical field
The invention belongs to flow battery field, specifically, relate to a kind of vanadium redox battery.
Background technology
Common, socioeconomic fast development, the energy of needs is increasing, meanwhile, fast along with fossil energy
The exhausted ecological deterioration problem brought with the combusts fossil energy of speed becomes increasingly conspicuous.In order to reduce the utilization of fossil energy, Ren Menyue
More pay close attention to the exploitation of regenerative resource (such as wind energy, solar energy etc.).But regenerative resource is by the condition such as region, meteorology
Impact, has unstability and discontinuity.In order to better profit from new forms of energy, it is necessary to develop large-scale energy storage technology.Entirely
Vanadium oxide reduction flow battery (referred to as " vanadium cell ") is separate because of its output and capacity, has power and capacity
Greatly, service life cycle is long, and energy efficiency is high, and degree of depth charge-discharge performance is good, and security performance advantages of higher is it is considered to be most should
With the extensive energy-storage battery of one of prospect, increasingly paid close attention to by people.
Vanadium cell is a kind of redox cell with different valence state vanadium ion as active substance, and V (V) and V (IV) electricity is right
As positive active material, V (III) and V (II) electricity is to as negative electrode active material.Vanadium cell mainly by electrode, electrolyte and
Barrier film forms.
Electrolyte, as the key components of vanadium cell, is the carrier of active substance, and the quality of its performance directly affects
The performance of vanadium cell.At present, owing to the electro-chemical activity ratio of electrolyte of vanadium redox battery is relatively low, cause vanadium cell under high current density
When carrying out discharge and recharge, the utilization rate of electrolyte is the highest, and the energy efficiency of battery is relatively low.
Electrode, as another key components of vanadium cell, is to provide active substance receiving and losing electrons generation electrochemical reaction
Place, itself is also not involved in electrochemical reaction.But the quality of its performance, directly influences the speed of active substance electron exchange
Rate, affects working current density and the energy efficiency of vanadium cell largely, thus affects the property of whole vanadium cell system
Energy.Therefore, the activity improving electrode is significant to improving vanadium cell performance.
Summary of the invention
It is an object of the invention to solve at least one in deficiencies of the prior art.
Such as, an object of the present invention is to improve working current density and the energy efficiency of vanadium cell, improves vanadium electricity
The performance in pond.
To achieve these goals, the present invention uses the electrochemistry improving vanadium battery negative electrode electrode material and electrolyte to live
Property, and the method reducing vanadium cell capacity attenuation, improve the performance of vanadium cell.
The invention provides a kind of vanadium redox battery, including anelectrode, negative electrode, barrier film, anolyte
Liquid and electrolyte liquid, described negative electrode include carbon materials matrix and be combined in carbon materials surface containing Sn eelctro-catalyst,
Described electrolyte liquid includes: the vanadium ion of 1.0mol/L～1.8mol/L, the sulphuric acid of 2.0mol/L～5.0mol/L,
The phosphate of the Sn of 0.01mol/L～0.3mol/L.
In one exemplary embodiment of the present invention, described carbon materials can be graphite felt, graphite cake, carbon paper and carbon
A kind of or the coalition of more than two kinds in cloth.
In one exemplary embodiment of the present invention, described can be Sn simple substance, Sn oxide, Sn containing Sn eelctro-catalyst
A kind of or the coalition of more than two kinds in halogenide, stannate and Sn slaine.
In one exemplary embodiment of the present invention, described Sn oxide can be SnO and/or SnO2。
In one exemplary embodiment of the present invention, described Sn halogenide can be stannous fluoride, stannous chloride, bromination
One in stannous, Tin diiodide., stannic fluoride, stannic chloride, Tin tetrabromide. and Tin tetraiodide. or more than two kinds, it is therefore preferable to protochloride
Stannum and/or stannic chloride.
In one exemplary embodiment of the present invention, described stannate can be sodium stannate and/or potassium stannate.
In one exemplary embodiment of the present invention, described Sn slaine can be stannous sulfate, STANNOUS SULPHATE CRYSTALLINE, phosphoric acid Asia
One in stannum, ditin diphosphate and phosphoric acid stannum or more than two kinds, it is therefore preferable to stannous sulfate and/or ditin diphosphate.
In one exemplary embodiment of the present invention, the phosphate of described Sn can be phosphoric acid stannous chloride, ditin diphosphate
With one or more in phosphoric acid stannum.
In one exemplary embodiment of the present invention, the phosphatic preferred content of described Sn can be 0.01mol/L
～0.2mol/L.
In one exemplary embodiment of the present invention, described in be combined in the weight containing Sn eelctro-catalyst on carbon materials surface
Amount account for the percentage ratio of described carbon materials weight (being referred to as " loading ") can be 0.1%～10%, preferably 1%～
5%.
In one exemplary embodiment of the present invention, described in be combined in carbon materials surface containing Sn eelctro-catalyst
Particle size can be 5nm～10 μm, preferably 10nm～1 μm.
Compared with prior art, the Advantageous Effects of the present invention includes:
(1) present invention by modifying the eelctro-catalyst containing Sn on carbon basal body surface so that it is has high catalysis activity, carries
High electrode material, to V (III)/V (II) electricity electro catalytic activity to reaction, reduces activation polarization, improves the voltage effect of battery
Rate and energy efficiency.
(2) present invention is by introducing the ion Han Sn in electrolyte so that the electro-chemical activity of electrolyte of vanadium redox battery, improves
Under the conditions of high current density, the utilization rate of electrolyte during discharge and recharge, improves the energy efficiency of vanadium cell simultaneously.
(3) technological process of the present invention is simple, can extend the life-span of vanadium cell, contribute to industrialized production.
Detailed description of the invention
Hereinafter, one vanadium redox battery of the present invention will be described in detail in conjunction with exemplary embodiment.
A kind of vanadium redox battery of the present invention includes anelectrode, negative electrode, barrier film, anode electrolyte and bears
Pole electrolyte.
Negative electrode can include carbon materials matrix and be combined in carbon materials surface containing Sn eelctro-catalyst, wherein, carbon
Cellulosic material can be a kind of or coalition of more than two kinds in graphite felt, graphite cake, carbon paper and carbon cloth.Containing Sn eelctro-catalyst
Can be a kind of or coalition of more than two kinds in Sn simple substance, Sn oxide, Sn halogenide, stannate and Sn slaine,
Wherein, the weight containing Sn eelctro-catalyst being combined in carbon materials surface accounts for the 0.1%～10% of described carbon materials weight, excellent
Elect 1%～5% as；The particle size containing Sn eelctro-catalyst being combined in carbon materials surface can be 5nm～10 μm, is preferably
10nm～1 μm.
Electrolyte liquid may include that the sulfur of the vanadium ion of 1.0mol/L～1.8mol/L, 2.0mol/L～5.0mol/L
Acid, the phosphate of Sn of 0.01mol/L～0.3mol/L.Wherein, the phosphate of Sn can be phosphoric acid stannous chloride, ditin diphosphate and
One or more in phosphoric acid stannum, the phosphatic preferred content of Sn can be 0.01mol/L～0.2mol/L.
In the present invention, Sn oxide can be SnO and/or SnO2；Sn halogenide can be stannous fluoride, protochloride
One in stannum, Tin dibromide., Tin diiodide., stannic fluoride, stannic chloride, Tin tetrabromide. and Tin tetraiodide. or more than two kinds, preferably
For stannous chloride and/or stannic chloride；Stannate can be sodium stannate and/or potassium stannate；Sn slaine is stannous sulfate, sulphuric acid
One in stannum, phosphoric acid stannous chloride, ditin diphosphate and phosphoric acid stannum or more than two kinds, it is therefore preferable to stannous sulfate and/or burnt phosphorus
Acid stannous.
The exemplary embodiment of the present invention is described in further detail below in conjunction with concrete example.
Embodiment 1
Be 1.6mol/L to vanadium ion concentration, sulfuric acid concentration be 3.0mol/L, V (III)/V (IV) be the 250mL of 1:1
In V electrolyte, add ditin diphosphate, make Sn in solution2+Concentration is 0.2mol/L, prepares electrolyte to be measured after stirring and dissolving.
By above-mentioned being not added with the electrolyte of additive, Nafion-117 barrier film, the graphite felt electrode of unmodified are assembled into list
Battery, wherein, the area of both positive and negative polarity graphite felt is 5*6cm2。
Embodiment 2
Be 1.6mol/L to vanadium ion concentration, sulfuric acid concentration be 3.0mol/L, V (III)/V (IV) be the 250mL of 1:1
V electrolyte adds phosphoric acid stannum, makes Sn in solution4+Concentration is 0.1mol/L, prepares electrolyte to be measured after stirring and dissolving.
By above-mentioned being not added with the electrolyte of additive, Nafion-117 barrier film, the graphite felt electrode of unmodified are assembled into list
Battery, wherein, the area of both positive and negative polarity graphite felt is 5*6cm2。
Embodiment 3
Be 1.6mol/L to vanadium ion concentration, sulfuric acid concentration be 3.0mol/L, V (III)/V (IV) be the 250mL of 1:1
V electrolyte adds ditin diphosphate and phosphoric acid stannous chloride, makes Sn in solution2+Concentration is 0.1mol/L, prepares and treat after stirring and dissolving
Survey electrolyte.
By above-mentioned being not added with the electrolyte of additive, Nafion-117 barrier film, the graphite felt electrode of unmodified are assembled into list
Battery, wherein, the area of both positive and negative polarity graphite felt is 5*6cm2。
Embodiment 4
Be 1.6mol/L to vanadium ion concentration, sulfuric acid concentration be 3.0mol/L, V (III)/V (IV) be the 250mL of 1:1
V electrolyte adds ditin diphosphate and phosphoric acid stannum, makes Sn in solution2+Concentration is 0.1mol/L, Sn4+Concentration is 0.05mol/
L, prepares electrolyte to be measured after stirring and dissolving.
By above-mentioned being not added with the electrolyte of additive, Nafion-117 barrier film, the graphite felt electrode of unmodified are assembled into list
Battery, wherein, the area of both positive and negative polarity graphite felt is 5*6cm2。
Embodiment 5
Configuration vanadium ion concentration is 1.6mol/L, sulfuric acid concentration is 3.0mol/L, V (III)/V (IV) is the 100mL of 1:1
Electrolyte of vanadium redox battery.
By above-mentioned be not added with the electrolyte of additive, Nafion-117 barrier film, the graphite felt positive pole of unmodified, Sn modify
Graphite felt negative pole is assembled into monocell, and wherein, the area of both positive and negative polarity graphite felt is 5*6cm2, the loading hundred of the Sn in graphite felt
Proportion by subtraction is 1%.
Embodiment 6
Configuration vanadium ion concentration is 1.6mol/L, sulfuric acid concentration is 3.0mol/L, V (III)/V (IV) is the 100mL of 1:1
Electrolyte of vanadium redox battery.
By above-mentioned be not added with the electrolyte of additive, Nafion-117 barrier film, the graphite felt positive pole of unmodified, Sn modify
Graphite felt negative pole is assembled into monocell, and wherein, the area of both positive and negative polarity graphite felt is 5*6cm2, the loading hundred of the Sn in graphite felt
Proportion by subtraction is 5%.
Embodiment 7
Configuration vanadium ion concentration is 1.6mol/L, sulfuric acid concentration is 3.0mol/L, V (III)/V (IV) is the 100mL of 1:1
Electrolyte of vanadium redox battery.
It is not added with the electrolyte of additive, Nafion-117 barrier film, the graphite felt positive pole of unmodified, stannous sulfate by above-mentioned
The graphite felt negative pole modified is assembled into monocell, and wherein, the area of both positive and negative polarity graphite felt is 5*6cm2, the sulphuric acid in graphite felt is sub-
The loading percentage ratio of stannum is 2%.
Comparative example
Use unmodified graphite felt and the electrolyte without any additive as blank electrolysis liquid, assemble monocell and make
For comparative example, it is 100mA/cm in electric current density2Under carry out charge-discharge test.In positive and negative electrode electrolyte, the concentration of vanadium ion is
1.6mol/L, the concentration of sulphuric acid are 3.0mol/L, and V (III)/V (IV) is 1:1.
Monocell and the monocell of comparative example assembling that embodiment 1～7 assembles are 100mA/cm in electric current density2Under survey
Test result is shown in Tables 1 and 2.
The different electrolyte liquid monocell of table 1 runs the Performance comparision of 100 circulations
| Embodiment | Average current efficiency | Average voltage efficiencies | Average energy efficiency |
| Comparative example | 95.12% | 81.20% | 77.24% |
| Embodiment 1 | 95.28% | 88.50% | 84.32% |
| Embodiment 2 | 95.53% | 88.80% | 84.83% |
| Embodiment 3 | 95.26% | 88.90% | 84.69% |
| Embodiment 4 | 95.48% | 88.80% | 84.79% |
| Embodiment 5 | 95.88% | 87.40% | 83.80% |
| Embodiment 6 | 95.80% | 87.80% | 84.10% |
| Embodiment 7 | 95.68% | 86.80% | 82.50% |
The capacity attenuation of table 2 different electrolyte liquid monocell 100 circulation compares
As can be known from Table 1, compared with the monocell of unmodified graphite felt, surface is combined with the graphite containing Sn eelctro-catalyst
Voltage efficiency and the energy efficiency of the monocell that felt assembles all are improved, and show that surface is combined with bearing containing Sn eelctro-catalyst
Pole material can improve the electro-chemical activity of negative material.Compared with the monocell of the electrolyte without any additive, contain
Voltage efficiency and the energy efficiency of the monocell that the phosphatic electrolyte of Sn assembles all are improved, and show the phosphorus containing Sn
The electrolyte of hydrochlorate can improve the electro-chemical activity of electrolyte.From Table 2, it can be seen that add the phosphatic additive of Sn
After, the discharge capacity of the 1st circulation of battery is enhanced, and battery average size attenuation rate has had bigger reduction,
The addition of additive is described, is conducive to improving the utilization rate of electrolyte and reducing battery capacity decay.Therefore, it is combined with when surface
When negative material containing Sn eelctro-catalyst and electrolyte have the phosphate containing Sn to be assembled into battery, can mutually promote, jointly
Improve the electro-chemical activity of vanadium cell, reduce the activation polarization of vanadium cell；Improve the utilization rate of electrolyte and reduce battery appearance
Amount decay.
In sum, the beneficial effect comprise that
(1) present invention by modifying the eelctro-catalyst containing Sn on carbon basal body surface so that it is has high catalysis activity, carries
High negative material, to V (III)/V (II) electricity electro catalytic activity to reaction, reduces activation polarization, improves the voltage effect of battery
Rate and energy efficiency.
(2) present invention is by introducing the phosphatic additive of Sn in electrolyte so that the electrification of electrolyte of vanadium redox battery
Learning activity, improve the utilization rate of electrolyte during discharge and recharge under the conditions of high current density, improve vanadium cell can dose-effect simultaneously
Rate；Reduce battery capacity decay, improve electrolyte service life.
(3) technological process of the present invention is simple, can extend the life-span of vanadium cell, contribute to industrialized production.
Although describing the present invention already in connection with exemplary embodiment above, but those of ordinary skill in the art should be clear
Chu, in the case of without departing from spirit and scope by the claims, can carry out various amendment to above-described embodiment.
Claims (10)
1. a vanadium redox battery, including anelectrode, negative electrode, barrier film, anode electrolyte and electrolyte liquid,
It is characterized in that, described negative electrode include carbon materials matrix and be combined in carbon materials surface containing Sn eelctro-catalyst, described
Electrolyte liquid includes: the vanadium ion of 1.0mol/L～1.8mol/L, the sulphuric acid of 2.0mol/L～5.0mol/L, 0.01mol/L
～the phosphate of the Sn of 0.3mol/L.
Vanadium redox battery the most according to claim 1, it is characterised in that described carbon materials is graphite
A kind of or the coalition of more than two kinds in felt, graphite cake, carbon paper and carbon cloth.
Vanadium redox battery the most according to claim 1, it is characterised in that described is Sn containing Sn eelctro-catalyst
One or more in simple substance, Sn oxide, Sn halogenide, stannate and Sn slaine.
Vanadium redox battery the most according to claim 3, it is characterised in that:
Described Sn oxide is SnO and/or SnO2；
Described Sn halogenide be stannous fluoride, stannous chloride, Tin dibromide., Tin diiodide., stannic fluoride, stannic chloride, Tin tetrabromide. and
One or more in Tin tetraiodide.；
Described stannate is sodium stannate and/or potassium stannate；
Described Sn slaine be in stannous sulfate, STANNOUS SULPHATE CRYSTALLINE, phosphoric acid stannous chloride, ditin diphosphate and phosphoric acid stannum one or both with
On.
Vanadium redox battery the most according to claim 1, it is characterised in that the phosphate of described Sn can be
One or more in phosphoric acid stannous chloride, ditin diphosphate and phosphoric acid stannum.
Vanadium redox battery the most according to claim 1, it is characterised in that the phosphatic consumption of described Sn
For 0.01mol/L～0.2mol/L.
Vanadium redox battery the most according to claim 1, it is characterised in that described in be combined in carbon materials table
The weight containing Sn eelctro-catalyst in face accounts for the 0.1～10% of described carbon materials weight.
Vanadium redox battery the most according to claim 7, it is characterised in that described in be combined in carbon materials table
The weight containing Sn eelctro-catalyst in face accounts for the 1～5% of described carbon materials weight.
Vanadium redox battery the most according to claim 1, it is characterised in that described in be combined in carbon materials table
The particle size containing Sn eelctro-catalyst in face is 5nm～10 μm.
Vanadium redox battery the most according to claim 9, it is characterised in that described in be combined in carbon materials
The particle size containing Sn eelctro-catalyst on surface is 10nm～1 μm.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN107221681A (en) * | 2017-06-14 | 2017-09-29 | 北京航空航天大学 | It is a kind of applied to modified electrode of all-vanadium flow battery and preparation method thereof |
| CN110071317A (en) * | 2019-05-22 | 2019-07-30 | 西南交通大学 | A kind of tin bromine flow battery |
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| CN101997129A (en) * | 2009-08-27 | 2011-03-30 | 中国科学院金属研究所 | Liquid flow battery |
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| CN110071317A (en) * | 2019-05-22 | 2019-07-30 | 西南交通大学 | A kind of tin bromine flow battery |
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