CN103700872A - Total-iron complexing flow cell with high open-circuit voltage - Google Patents
Total-iron complexing flow cell with high open-circuit voltage Download PDFInfo
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Abstract
The invention discloses a total-iron complexing flow cell with high open-circuit voltage. The total-iron complexing flow cell with high open-circuit voltage is characterized in that iron complexing water solutions are adopted for the positive electrode electrolyte and the negative electrode electrolyte. Iron ions and different types of complexing agents form iron complexing electrolyte, that is, ferrous/phenanthroline complexing electrolyte is adopted for the positive electrode, and ferric iron/triethanolamine complexing electrolyte is adopted for the negative electrode, so that the electrode potentials of ferrous/ferric iron electric pairs respectively move toward the positive direction and the negative direction. The total-iron complexing flow cell consisting of the two iron complexing electrolyte has relatively high cell open-circuit voltage. The iron complex also can inhibit the hydrogen evolution reaction, prevent cross pollution of the electrolyte solution comprising different types of ions, and improve the efficiency of the flow cell.
Description
Technical field
The present invention relates to a kind of full iron complex liquid galvanic battery with high open circuit voltage, is that a kind of positive and negative the two poles of the earth electrolyte all adopts the iron complex aqueous solution, improves the full iron complex liquid galvanic battery of flow battery open circuit voltage.
Background technology
Oxidation-reducing solution galvanic battery in having the electrolyte of oxidation-reduction reaction activity, is a kind of emerging extensive energy storage technology by electrical power storage.It has the advantages such as toggle speed is fast, stored energy capacitance is large, energy efficiency is high, safe and reliable, can be widely used in energy storage and the power supply peak regulation of renewable energy system.
Electrolyte is the key technology that determines flow battery energy storage capacity, efficiency, cost and stability.The electrolyte system adopting at present is mainly divided into:
(1) positive and negative electrode element electrolysis liquid not of the same race, as iron/chromium electrolyte, sodium polysulfide/bromine electrolyte, vanadium/bromine electrolyte, zinc/bromine electrolyte etc., its common shortcoming is because variety classes ion sees through the cross pollution that the infiltration of amberplex produces, and reduces battery performance.
(2) adopt positive and negative electrode element electrolysis liquid of the same race, as full V electrolyte, full chromium electrolyte, and siderochrome, ferrovanadium mixed electrolytic solution etc., although can avoid cross pollution, because the oxidizability of pentavalent vanadium ion causes by force and easily the problems such as the electrode reaction invertibity of ion-exchange film destroy, chromium ion is poor and seriously polluted.
Above-mentioned these oxidations-right electrode potential of electricity that reduces is lower, has limited the raising of flow battery open circuit voltage and energy density.Therefore, the oxidation of exploitation high electrode current potential-reduction electricity is to becoming the study hotspot of academia.
Ferro element reserves are abundant, cheap, and oxide etch is low, it is little to pollute, but the right electrode potential of ferrous iron/ferric iron (Fe (II)/Fe (III)) electricity is lower, and standard electrode potential is only 0.77V.L.W.Hruska etc. be take Fe (II)/Fe (III) as anodal in J.Electrochemical Society128 (1981) 18-25 article, iron simple substance is negative pole, form full iron single flow battery, open circuit voltage only has 1.21V, and iron simple substance is easy and acid reaction generates hydrogen.Research shows, iron complex can make electrode potential move to plus or minus direction, thereby improves the electromotive force of battery.Below can the be down to-1.0V of anode spike potential (with respect to standard calomel electrode) of ferric iron/triethanolamine complex liquid, complexing can also suppress the generation of evolving hydrogen reaction.Y.H.Wen etc. are used as negative pole electrolyte and the anodal flow battery that forms of sodium bromide in Electrochimica Acta51 (2006) 3769-3775 article, and open circuit voltage reaches 2.0V.But this iron/bromine electrolyte does not solve cross-contamination issue, limited the raising (～69.1%) of energy efficiency.In addition, more than the anode spike potential of the complex compound that ligand forms such as ferrous iron and phenanthroline, bipyridine iron can be increased to 0.8V.M.H.Chakrabarti etc. adopt the multiple valence state of bipyridine iron complex in organic solvent to form full iron flow battery in Electrochimica Acta52 (2007) 2189-2195 article, cross pollution and liberation of hydrogen have been avoided, theoretical open circuit voltage is up to 2.4V, but in organic solvent the energy efficiency of battery lower than 30%.
Summary of the invention
The technical problem to be solved in the present invention is the full iron complex liquid galvanic battery that preparation a kind of positive and negative the two poles of the earth electrolyte all adopts the iron complex aqueous solution, has higher open circuit voltage, without cross pollution and liberation of hydrogen, thereby reaches higher battery efficiency.
The present invention is mixed with the iron complex aqueous solution by iron ion and different types of complexing agent, can make the right electrode potential of ferrous iron/ferric iron (Fe (II)/Fe (III)) electricity to plus or minus direction, move respectively.Above-mentioned iron complex, respectively as the positive and negative electrode electrolyte of flow battery, can be improved to the open circuit voltage of battery, avoid cross pollution.Iron complex can also suppress the generation of evolving hydrogen reaction, improves battery efficiency.
Technical scheme of the present invention is as follows:
A full iron complex liquid galvanic battery with high open circuit voltage, the positive and negative electrode electrolyte of flow battery all adopts the iron complex aqueous solution; Iron ion and different types of complexing agent are mixed with to the iron complex aqueous solution, different types of iron complex aqueous solution, respectively as the positive and negative electrode electrolyte of flow battery, is formed to full iron complex liquid galvanic battery.
Further feature, the anodal complex liquid (Fe (II)/Phen) that adopts Fe (II) and phenanthroline (Phen), negative pole adopts the complex liquid (Fe (III)/TEA) of Fe (III) and triethanolamine (TEA).Positive and negative electrode electrolyte is stored in respectively in electrolyte storage tank, is delivered to the positive and negative electrode participation oxidation-reduction reaction of battery during use with peristaltic pump.Adopt graphite felt as positive and negative electrode, middle for amberplex separates, graphite cake is collector plate, and polyfluortetraethylene plate is pole plate.
Described anodal Fe (II)/Phen complex liquid refers to the aqueous solution that has dissolved ferrous sulfate, phenanthroline, the concentrated sulfuric acid, and wherein the concentration of Fe (II)/Phen is 0.1～0.4mol/L, Fe (II) and Phen and H
2sO
4mol ratio be 1:3:2～1:6:10.
Described negative pole Fe (III)/TEA complex liquid refers to the aqueous solution that has dissolved ferric sulfate, triethanolamine, NaOH and sodium chloride, wherein the concentration of Fe (III)/TEA is 0.05～0.4mol/L, and Fe (III) is 1:2:5:1～1:16:20:8 with the mol ratio of TEA, NaOH and NaCl.
Described amberplex refers to cation-exchange membrane, as
film.
The invention has the beneficial effects as follows:
Than commercialization flow batteries such as existing full vanadium, siderochrome, the present invention respectively as positive and negative electrode electrolyte, prepares full iron complex liquid galvanic battery using iron complex aqueous solution Fe (II)/Phen and Fe (III)/TEA.Complexing agent Phen and TEA move respectively the right electrode potential of Fe (III)/Fe (II) electricity to positive and negative direction, thus acquisition～2.0V compared with high open circuit voltage, far above the 1.3V of all-vanadium flow battery and the 1.2V of siderochrome flow battery.The cross pollution that full iron complex liquid galvanic battery can also avoid variety classes iontophoretic injection to cause, suppresses evolving hydrogen reaction, obtains higher battery efficiency.In addition, the reserves of iron are abundant, oxide etch is weak, it is little to pollute, and therefore can reduce battery cost, improve economic and social benefit.
Accompanying drawing explanation
Below in conjunction with technical scheme and the detailed specific embodiments of the invention of accompanying drawing.
Fig. 1 is the structural representation of full iron complex liquid galvanic battery of the present invention.
In figure: 1 electrolyte storage tank; 2 electrodes; 3 amberplexes; 4 peristaltic pumps.
Fig. 2 is the cyclic voltammetry figure of positive and negative electrode iron complexing electrolyte.
In figure, abscissa is scanning voltage (volt), and ordinate is sweep current (milliampere).Fig. 2 A is that anodal Fe (II)/Phen complexing electrolyte (consists of 0.1mol/L Fe (II), 0.3mol/L Phen, 1.0mol/L H
2sO
4) cyclic voltammetry figure, Fig. 2 B is that negative pole Fe (III)/TEA complexing electrolyte (consists of 0.1mol/L Fe (III), 1mol/L TEA, 2mol/L NaOH, 0.4mol/L NaCl) cyclic voltammetry figure, graphite is work electrode, sweep speed is 20 millivolts/second.
Fig. 3 is the charge-discharge performance resolution chart of the full iron complex liquid galvanic battery prepared of the present invention.
In figure abscissa for discharge and recharge the time (hour), ordinate is charge and discharge voltage (volt).Charge and discharge electric current is 10 milliamperes, and charge and discharge cut-ff voltage is respectively 2.2 volts and 0.3 volt, latter standing 1 hour of each charge and discharge cut-off.Anode electrolyte consist of 0.3mol/L Fe (II), 0.9mol/L Phen, 1.0mol/L H
2sO
4, negative pole electrolyte consist of 0.3mol/L Fe (III), 1mol/L TEA, 2mol/L NaOH, 0.4mol/LNaCl.
Cyclic voltammetry shows, iron and phenanthroline, triethanolamine can form respectively stable complexing electrolyte, make electrode potential respectively to positive and negative direction move to 0.86V and-1.065V, and do not have evolving hydrogen reaction to occur.
Charge-discharge performance is tested and is shown, full iron complexing electrolyte flow battery of the present invention, has higher open circuit voltage.
Embodiment
Embodiment 1:
Take 2.7801g FeSO
4.7H
2o crystal is dissolved in deionized water, with mol ratio FeSO
4.7H
2o:Phen:H
2sO
4for 1:3:10 adds Phen and 98%H
2sO
4, electromagnetic agitation, to dissolving, is configured to 100mL anode electrolyte, and wherein the concentration of Fe (II)/Phen complex compound is 0.1mol/L.Take 0.9997gFe
2(SO
4)
3.xH
2o crystal is dissolved in deionized water, with mol ratio Fe
2(SO
4)
3.xH
2o:TEA:NaOH:NaCl is that 1:16:20:8 adds TEA, NaOH and NaCl, and electromagnetic agitation, to dissolving, is configured to 100mL negative pole electrolyte, and wherein the concentration of Fe (III)/TEA complex compound is 0.05mol/L.60mL positive and negative electrode electrolyte is contained in respectively in 2 fluid reservoirs, according to assembling shown in Fig. 1, helps iron complex liquid galvanic battery.Wherein, graphite felt electrode size is 2 * 2 * 0.5cm, and Nafion117 film effective area is 4cm
2.Carry out battery charging and discharging test, charge and discharge electric current is 20mA, and charge and discharge cut-ff voltage is respectively 2.2V and 0.3V.The open circuit voltage that records battery is 1.94V, is about 1.6 times of all-vanadium flow battery; Energy efficiency is 44.8%, the full iron flow battery forming higher than bipyridine iron complex/organic solvent.
Embodiment 2:
Take 5.5602g FeSO
4.7H
2o crystal is dissolved in deionized water, with mol ratio FeSO
4.7H
2o:Phen:H
2sO
4for 1:5:5 adds Phen and 98%H
2sO
4, electromagnetic agitation, to dissolving, is configured to 100mL anode electrolyte, and wherein the concentration of Fe (II)/Phen complex compound is 0.2mol/L.Take 7.9976gFe
2(SO
4)
3.xH
2o crystal is dissolved in deionized water, with mol ratio Fe
2(SO
4)
3.xH
2o:TEA:NaOH:NaCl is that 1:5:7.5:1 adds TEA, NaOH and NaCl, and electromagnetic agitation, to dissolving, is configured to 100mL negative pole electrolyte, and wherein the concentration of Fe (III)/TEA complex compound is 0.4mol/L.35mL positive and negative electrode electrolyte is contained in respectively in 2 fluid reservoirs, according to assembling shown in Fig. 1, helps iron complex liquid galvanic battery.Wherein, graphite felt electrode size is 2 * 2 * 0.5cm, and Nafion115 film effective area is 4cm
2.Carry out battery charging and discharging test, charge and discharge electric current is 40mA, and charge and discharge cut-ff voltage is respectively 2.2V and 0.3V.The open circuit voltage that records battery is 1.90V, is about 1.4 times of all-vanadium flow battery; Energy efficiency is 76.4%, higher than the full iron flow battery of Fe (III)/TEA complex compound and sodium bromide composition.
Embodiment 3:
Take 11.1204g FeSO
4.7H
2o crystal is dissolved in deionized water, with mol ratio FeSO
4.7H
2o:Phen:H
2sO
4for 1:5:2.5 adds Phen and 98%H
2sO
4, electromagnetic agitation, to dissolving, is configured to 100mL anode electrolyte, and wherein the concentration of Fe (II)/Phen complex compound is 0.4mol/L.Take 7.9976gFe
2(SO
4)
3.xH
2o crystal is dissolved in deionized water, with mol ratio Fe
2(SO
4)
3.xH
2o:TEA:NaOH:NaCl is that 1:5:7.5:1 adds TEA, NaOH and NaCl, and electromagnetic agitation, to dissolving, is configured to 100mL negative pole electrolyte, and wherein the concentration of Fe (III)/TEA complex compound is 0.4mol/L.35mL positive and negative electrode electrolyte is contained in respectively in 2 fluid reservoirs, according to assembling shown in Fig. 1, helps iron complex liquid galvanic battery.Wherein, graphite felt electrode size is 2 * 2 * 0.5cm, and Nafion115 film effective area is 4cm
2.Carry out battery charging and discharging test, charge and discharge electric current is 80mA, and charge and discharge cut-ff voltage is respectively 2.2V and 0.3V.The open circuit voltage that records battery is 1.87V, and energy efficiency is 60.5%.
Embodiment 4:
Take 8.3403g FeSO
4.7H
2o crystal is dissolved in deionized water, with mol ratio FeSO
4.7H
2o:Phen:H
2sO
4for 1:3:3.3 adds Phen and 98%H
2sO
4, electromagnetic agitation, to dissolving, is configured to 100mL anode electrolyte, and wherein the concentration of Fe (II)/Phen complex compound is 0.3mol/L.Take 5.9982g Fe
2(SO
4)
3.xH
2o crystal is dissolved in deionized water, with mol ratio Fe
2(SO
4)
3.xH
2o:TEA:NaOH:NaCl is that 1:3.3:6.7:1.3 adds TEA, NaOH and NaCl, and electromagnetic agitation, to dissolving, is configured to 100mL negative pole electrolyte, and wherein the concentration of Fe (III)/TEA complex compound is 0.3mol/L.25mL positive and negative electrode electrolyte is contained in respectively in 2 fluid reservoirs, according to assembling shown in Fig. 1, helps iron complex liquid galvanic battery.Wherein, graphite felt electrode size is 2 * 2 * 0.75cm, and Nafion115 film effective area is 4cm
2.Carry out battery charging and discharging test, charge and discharge electric current is 10mA, and charge and discharge cut-ff voltage is respectively 2.2V and 0.3V.The open circuit voltage that records battery is 1.98V, and energy efficiency is 59.2%.
In above-mentioned four embodiment, utilize the oxidation-reduction potential of variety classes iron complex to differ larger feature, at positive pole, adopt Fe (II)/Phen complexing electrolyte, negative pole to adopt Fe (III)/TEA complexing electrolyte, electrode potential is moved to positive and negative direction respectively, thereby improve the electromotive force of flow battery.Meanwhile, full iron complexing electrolyte has avoided variety classes ion to see through the cross pollution of amberplex, has suppressed the generation of evolving hydrogen reaction, thereby can improve battery efficiency.
Claims (6)
1. a full iron complex liquid galvanic battery, is characterized in that: the positive and negative electrode electrolyte of flow battery all adopts the iron complex aqueous solution; Iron ion and different types of complexing agent are mixed with to the iron complex aqueous solution, different types of iron complex aqueous solution, respectively as the positive and negative electrode electrolyte of flow battery, is formed to full iron complex liquid galvanic battery.
2. full iron complex liquid galvanic battery according to claim 1, it is characterized in that: the positive pole of full iron complex liquid galvanic battery adopts the complex liquid of Fe (II) and phenanthroline (Phen), negative pole adopts the complex liquid of Fe (III) and triethanolamine (TEA).
3. full iron complex liquid galvanic battery according to claim 2, it is characterized in that: described anodal Fe (II)/Phen complex liquid refers to the aqueous solution that has dissolved ferrous sulfate, phenanthroline, the concentrated sulfuric acid, wherein the concentration of Fe (II)/Phen is 0.1～0.4mol/L, Fe (II) and Phen and H
2sO
4mol ratio be 1:3:2～1:6:10.
4. full iron complex liquid galvanic battery according to claim 3, it is characterized in that: described negative pole Fe (III)/TEA complex liquid refers to the aqueous solution that has dissolved ferric sulfate, triethanolamine, NaOH and sodium chloride, wherein the concentration of Fe (III)/TEA is 0.05～0.4mol/L, and Fe (III) is 1:2:5:1～1:16:20:8 with the mol ratio of TEA, NaOH and NaCl.
5. according to the full iron complex liquid galvanic battery described in claim 2,3 or 4, it is characterized in that: adopt graphite felt as positive and negative electrode, middle for amberplex separates, graphite cake is collector plate, and polyfluortetraethylene plate is pole plate.
6. full iron complex liquid galvanic battery according to claim 5, is characterized in that: described amberplex refers to that cation-exchange membrane is
film.
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2017132346A1 (en) * | 2016-01-27 | 2017-08-03 | Ensync, Inc. | Zinc complex compounds for rechargeable flow battery |
| CN107431224A (en) * | 2015-04-14 | 2017-12-01 | 洛克希德马丁尖端能量存储有限公司 | For adjusting the flow battery balancing battery with Bipolar Membrane of negative electrolyte solution and catholyte solution simultaneously |
| CN107482242A (en) * | 2017-07-16 | 2017-12-15 | 常州大学 | A kind of water system single flow battery based on metal organic complex liquid stream positive pole and preparation method thereof |
| CN109346729A (en) * | 2018-09-30 | 2019-02-15 | 常州大学 | It is a kind of using carbon nanohorn/polyimides compound as the Phen of solid cathode iron complex-half flow battery of water system |
| CN109638329A (en) * | 2018-12-19 | 2019-04-16 | 中国科学技术大学 | A kind of water system flow battery |
| CN114335643A (en) * | 2021-12-16 | 2022-04-12 | 重庆大学 | Iron complex-air flow battery |
| US20220166045A1 (en) * | 2019-03-28 | 2022-05-26 | Mitsubishi Heavy Industries, Ltd. | Redox flow battery |
| WO2023158630A1 (en) * | 2022-02-15 | 2023-08-24 | Saudi Arabian Oil Company | Increasing reactant utilization in fe/v flow batteries |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN107431224A (en) * | 2015-04-14 | 2017-12-01 | 洛克希德马丁尖端能量存储有限公司 | For adjusting the flow battery balancing battery with Bipolar Membrane of negative electrolyte solution and catholyte solution simultaneously |
| CN107431224B (en) * | 2015-04-14 | 2021-01-05 | 洛克希德马丁能量有限公司 | Flow battery balancing cell with bipolar membrane for simultaneous conditioning of negative and positive electrolyte solutions |
| US10833347B2 (en) | 2015-04-14 | 2020-11-10 | Lockheed Martin Energy, Llc | Flow battery balancing cells having a bipolar membrane for simultaneous modification of a negative electrolyte solution and a positive electrolyte solution |
| WO2017132346A1 (en) * | 2016-01-27 | 2017-08-03 | Ensync, Inc. | Zinc complex compounds for rechargeable flow battery |
| CN107482242A (en) * | 2017-07-16 | 2017-12-15 | 常州大学 | A kind of water system single flow battery based on metal organic complex liquid stream positive pole and preparation method thereof |
| CN107482242B (en) * | 2017-07-16 | 2019-11-12 | 常州大学 | A kind of water system single flow battery and preparation method thereof based on metal organic complex liquid stream anode |
| CN109346729B (en) * | 2018-09-30 | 2020-10-30 | 常州大学 | Water system semi-flow battery |
| CN109346729A (en) * | 2018-09-30 | 2019-02-15 | 常州大学 | It is a kind of using carbon nanohorn/polyimides compound as the Phen of solid cathode iron complex-half flow battery of water system |
| CN109638329A (en) * | 2018-12-19 | 2019-04-16 | 中国科学技术大学 | A kind of water system flow battery |
| US20220166045A1 (en) * | 2019-03-28 | 2022-05-26 | Mitsubishi Heavy Industries, Ltd. | Redox flow battery |
| CN114335643A (en) * | 2021-12-16 | 2022-04-12 | 重庆大学 | Iron complex-air flow battery |
| CN114335643B (en) * | 2021-12-16 | 2023-10-03 | 重庆大学 | Iron complex-air flow battery |
| WO2023158630A1 (en) * | 2022-02-15 | 2023-08-24 | Saudi Arabian Oil Company | Increasing reactant utilization in fe/v flow batteries |
| US11901598B2 (en) | 2022-02-15 | 2024-02-13 | Saudi Arabian Oil Company | Increasing reactant utilization in Fe/V flow batteries |
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Application publication date: 20140402 |