CN103633330A - Combined electrode for flow battery and flow energy storage battery - Google Patents
Combined electrode for flow battery and flow energy storage battery Download PDFInfo
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- CN103633330A CN103633330A CN201210312506.7A CN201210312506A CN103633330A CN 103633330 A CN103633330 A CN 103633330A CN 201210312506 A CN201210312506 A CN 201210312506A CN 103633330 A CN103633330 A CN 103633330A
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8605—Porous electrodes
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
- H01M4/8673—Electrically conductive fillers
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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
Abstract
The invention relates to a combined electrode for a flow energy storage battery and a flow energy storage battery containing the combined electrode. The combined electrode comprises a conducting layer and a catalyst layer which are superimposed mutually. The thickness of the conducting layer is 10-90% of the total thickness of the electrode. The conducting layer is made of carbon materials with good conductivity and low porosity. The catalyst layer is made of carbon materials with high electrocatalytic activity and high porosity. The self resistance of the electrode and the contact resistance between bipolar plates of the electrode are decreased, and finally the Ohm internal resistance of the flow energy storage battery is decreased. The energy efficiency and the voltage efficiency of the flow energy storage battery are raised, and therefore the working current density is raised, thus, the weight, the volume and the cost of the battery with the same output power are all decreased greatly.
Description
Technical field
The present invention relates to the liquid flow energy storage battery field in chemical energy storage technology, particularly the electrode of all-vanadium liquid flow energy storage battery.
Background technology
All-vanadium liquid flow energy storage battery has power output and capacity is separate because of it, and system is flexible; Energy efficiency is high, and the life-span is long, and operation stability and reliability are high, and self discharge is low; The addressing degree of freedom is large, pollution-free, safeguard simple, operation cost is low, the advantages such as fail safe height, aspect scale energy storage, there is vast potential for future development, the effective ways that are considered to solve the renewable energy system randomnesss such as solar energy, wind energy and intermittent unstable state feature have great demand in renewable energy power generation and intelligent grid construction.
Different from the function of general chemistry power electrode, the electrode of liquid flow energy storage battery is the place of chemical energy storage system charge and discharge reaction, itself does not participate in electrochemical reaction the electrode of this kind of battery, active material in electrolyte solution is accepted or provides electronics to complete battery chemistries reaction at electrode surface, carries out the transformation between electric energy and chemical energy and realizes storage or the release of energy.
Electrode is as one of critical component of liquid flow energy storage battery, and its performance is very big on the impact of liquid flow energy storage battery.Its conductivity directly affects the ohmic internal resistance of battery; Its surface can have influence on active material in the transmission rate of electrode interface with the affinity interaction power of electrolyte; Its electrochemical catalysis activity also will directly determine the intrinsic reaction rate of electrochemical reaction, and in a word, electrode material affects electrochemical polarization, concentration polarization and the ohmic polarization of battery, has related to whole elements of battery electrochemical impedance.These key elements affect working current density and the energy efficiency of battery largely.
At present, the lower (<100mA/cm of working current density of liquid flow energy storage battery operation
2), be only 1/10th of Proton Exchange Membrane Fuel Cells working current density, cause battery module volume large, materials demand amount is large, and cost is high.And the raising of working current density can improve the power density of battery, reduce the cost of whole system, reduce floor space and the space of energy-storage system, improve the mobility of its adaptive capacity to environment and system, the application of expansion liquid flow energy storage battery.
The working current density that improves liquid flow energy storage battery need to reduce battery polarization as much as possible, i.e. ohmic polarization, electrochemical polarization and concentration polarization reduce voltage loss.
In current published patent documentation, for the method that reduces liquid flow energy storage battery polarization, mainly contain:
(1) electrode material is metallized or oxidation modification is processed as graphite felt, carbon paper etc., metal ion or oxygen-containing functional group on carbon fiber surface is modified, improve the electro catalytic activity of electrode, reduce the electrochemical polarization of battery, as disclosed method of graphite felt being carried out to electrochemical oxidation in patent CN 101465417A and CN 101182678A.But this kind of method just reduced the electrochemical polarization of battery, to reducing the ohmic polarization of battery, there is no help.And reducing for the working current density of raising battery of ohmic polarization is more important, because electrochemical polarization is directly proportional to the logarithm of electric current, ohmic voltage drop is directly proportional with the size of electric current.Therefore, along with the raising of working current density, battery ohmic internal resistance to affect meeting increasing.
(2) research and development electrode and the integrated combination electrode of bipolar plates, integrated pole dual-pole board reduces the contact resistance between pole dual-pole board.As disclosed in CN 101009376A, bipolar plates and porous electrode are bonded together to formation integrated pole dual-pole board by conductive bonding material.Yet the ohmic internal resistance of all-vanadium liquid flow energy storage battery mainly comprises this volume resistance of electrode, bipolar plates, electrolyte and barrier film and the contact resistance between electrode and bipolar plates.The method has just reduced the contact resistance between pole dual-pole board, on accounting for electrode that internal resistance of cell proportion is larger and this volume resistance of electrolyte, there is no impact, therefore limited for the raising degree of voltage efficiency and energy efficiency.
Summary of the invention
The present invention aims to provide a kind of liquid flow energy storage battery combination electrode, and it has high electrocatalytic active and low surface resistance, can reduce the ohmic internal resistance of liquid flow energy storage battery, improves the working current density of battery, to reach the object that improves power of battery density.
For achieving the above object, the technical solution used in the present invention is:
As shown in Figure 1, a kind of liquid flow energy storage battery combination electrode, described combination electrode is by comprising that the conductive layer and the Catalytic Layer that are superimposed with each other form, conductive layer has good conductivity, the low feature of porosity, Catalytic Layer has the advantages that electro catalytic activity is high, conductive layer thickness accounts for 10 ~ 90% of electrode gross thickness, and preferably 40 ~ 75%.
Described conductive layer is carbon element class material, and porosity is 0 ~ 80%, preferably 0 ~ 50%.
Described carbon element class material is that atresia graphite cake, flexible graphite plate, volume density are 0.2 ~ 1.0gcm
-3graphite felt or carbon felt.
Described Catalytic Layer is carbon felt or graphite felt, and volume density is 0.05 ~ 0.2gcm
-3, porosity is 80 ~ 95%, preferably 88 ~ 95%.
Described combination electrode is by being prepared from conductive layer and Catalytic Layer by the mode of conducting resinl bonding.
Described conducting resinl is comprised of polymer and conductive filler, and wherein the mass ratio of polymer and conductive filler is 1/2 ~ 1/9.
Described polymer is one or two or more kinds in polypyrrole, polythiophene, polyaniline, polyethylene, polypropylene, polyvinyl chloride, epoxy resin, phenolic resins or Kynoar; Described conductive filler is one or two or more kinds in graphite, carbon black, acetylene black or carbon fiber.
Described combination electrode can also be put into successively conductive layer and Catalytic Layer in battery assembling process in electrode frame, and the mode by mechanical compaction fits together.
The liquid flow energy storage battery that adopts described combination electrode assembling, wherein liquid flow energy storage battery comprises electrode, bipolar plates and barrier film, and wherein electrodes conduct layer one side contacts with bipolar plates, and Catalytic Layer one side contacts with film.
When being assembled into battery, conductive layer contacts with bipolar plates, because conductive layer has low porosity, can make full use of the conductiving point on bipolar plates and Catalytic Layer surface, reaches the object that reduces contact resistance; Catalytic Layer contacts with film, and for electrochemical reaction provides place, due to the existence of conductive layer, Catalytic Layer thickness can be very little, to reduce this volume resistance of electrode.
Tool of the present invention has the following advantages:
(1) adopt electrode of the present invention, because the conductive layer in electrode has been used good conductivity, carbon materials that porosity is low, make to produce more contact point between bipolar plates and conductive layer, construct better conductive network, reduced the contact resistance between pole dual-pole board.
(2) adopt electrode of the present invention, due to the existence of the conductive layer of low porosity, reduced the memory space of electrolyte in battery to reduce this volume resistance of electrolyte; And reduced the thickness of the Catalytic Layer that porosity is high, reduced this volume resistance of electrode, from many aspects, reduced the ohmic internal resistance of battery, improved voltage efficiency and the energy efficiency of battery.
(3) adopt the liquid flow energy storage battery of electrode of the present invention, in energy efficiency, remain under more than 80% prerequisite, working current density can be brought up to 120mA/cm
2, battery weight, volume and the cost of identical power output are all reduced greatly.
(4) electrode structure of the present invention is simple, is easy to preparation assembling, and the material using is carbon materials cheap and easy to get, has commercialization application value.
Accompanying drawing explanation
Fig. 1 is the electrode structure schematic diagram of liquid flow energy storage battery of the present invention; Wherein: 1 conductive layer; 2 Catalytic Layer;
Fig. 2 is the charging and discharging curve figure of all-vanadium flow monocell under different current densities that adopts electrode of the present invention in the embodiment of the present invention 1;
Fig. 3 is the AC impedance spectrogram of all-vanadium flow monocell under open-circuit condition that adopts electrode of the present invention in the embodiment of the present invention 1;
Fig. 4 adopts the all-vanadium flow battery of electrode of the present invention to pile up the charging and discharging curve figure under different current densities in the embodiment of the present invention 2.
Specific embodiment
Below by specific embodiment in detail the present invention is described in detail.
The conductive layer of electrode is chosen atresia graphite cake, and 2mm is thick, and volume density is 2.0gcm
-3; Catalytic Layer is chosen carbon felt, and 3mm is thick, and volume density is 0.14gcm
-3; Electrode adopts non-integral mode, and conductive layer and Catalytic Layer are independently used.
During assembling battery, order according to end plate, gasket seal, collector plate (bipolar plates), gasket seal, electrode frame, gasket seal, conductive layer, Catalytic Layer, film, Catalytic Layer, conductive layer, gasket seal, electrode frame, gasket seal, collector plate (bipolar plates), gasket seal, end plate fits together each assembly, then under the compression of end plate, is assembled into all-vanadium flow monocell.Wherein, in electrode frame, bipolar plates one side is conductive layer, and film one side is Catalytic Layer.Compress rear electrode thickness and be about 3.8mm, electrode area is 12cm
2.Anode electrolyte is 1.5M VO
2+3M H
2sO
4solution 40ml, negative pole electrolyte is 1.5M V
3+3M H
2sO
4solution 40ml.
The charging and discharging curve of battery under different current densities as shown in Figure 2.The monocell that adopts combination electrode of the present invention, current density is 80mA/cm
2time, voltage efficiency and energy efficiency are respectively 90% and 85.4%; Current density is brought up to 140mA/cm
2time, voltage efficiency and energy efficiency still remain on 82.9% and 80%.Compare battery efficiency with comparative example and have significantly lifting.
Fig. 2 is the AC impedance spectrogram of monocell under open-circuit condition that adopts combination electrode of the present invention.Therefrom can find out, the monocell ohmic internal resistance that adopts economic benefits and social benefits electrode of the present invention is only 610m Ω cm
2, compared with comparative example significantly and reduced.
Comparative example
Electrode is chosen carbon felt, and 6mm is thick, and volume density is 0.14gcm
-3.During assembling battery, order according to end plate, gasket seal, collector plate (bipolar plates), gasket seal, electrode frame, gasket seal, electrode, film, electrode, gasket seal, electrode frame, gasket seal, collector plate (bipolar plates), gasket seal, end plate fits together each assembly, then under the compression of end plate, is assembled into all-vanadium flow monocell.Compress rear electrode thickness and be about 3.8mm, electrode area is 12cm
2.Anode electrolyte is 1.5M VO
2+3M H
2sO
4solution 40ml, negative pole electrolyte is 1.5M V
3+3M H
2sO
4solution 40ml.
Battery is 80mA/cm in current density
2time, voltage efficiency and energy efficiency are respectively 85% and 80.1%; Current density is brought up to 120mA/cm
2time, voltage efficiency and energy efficiency are respectively 77.8% and 74.5%.Monocell ohmic internal resistance is 960m Ω cm
2.
The conductive layer of electrode is chosen flexible graphite plate, and 3mm is thick, and volume density is 1.0gcm
-3, porosity is 50%; Catalytic Layer is chosen carbon felt, and 3mm is thick, and volume density is 0.14gcm
-3; Electrode adopts non-integral mode, and conductive layer and Catalytic Layer are independently used.
During assembling battery, according to end plate, gasket seal, collector plate (bipolar plates), gasket seal, electrode frame, gasket seal, conductive layer, Catalytic Layer, film, Catalytic Layer, conductive layer, gasket seal, electrode frame, gasket seal, collector plate (bipolar plates), gasket seal, electrode frame, gasket seal ... the order of collector plate (bipolar plates), gasket seal, end plate fits together each assembly, then under the compression of end plate, is assembled into all-vanadium flow battery group.Wherein, in electrode frame, bipolar plates one side is conductive layer, and film one side is Catalytic Layer.Compress rear electrode thickness and be about 5.3mm.Anode electrolyte is 1.5M VO
2+3M H
2sO
4solution 40l, negative pole electrolyte is 1.5M V
3+3M H
2sO
4solution 40l.
The charging and discharging curve of battery under different current densities and battery efficiency are as shown in Figure 4.The battery pile that adopts combination electrode of the present invention, current density is 80mA/cm
2time, voltage efficiency and energy efficiency are respectively 88.7% and 83.8%; Current density is brought up to 120mA/cm
2time, voltage efficiency and energy efficiency still remain on 83.8% and 79.8%.
Embodiment 3
The conductive layer of electrode is chosen graphite felt, and 3mm is thick, and volume density is 0.4gcm
-3; Catalytic Layer is chosen carbon felt, and 2mm is thick, and volume density is 0.14gcm
-3; Electrode adopts non-integral mode, and conductive layer and Catalytic Layer are independently used.
During assembling battery, order according to end plate, gasket seal, collector plate (bipolar plates), gasket seal, electrode frame, gasket seal, conductive layer, Catalytic Layer, film, Catalytic Layer, conductive layer, gasket seal, electrode frame, gasket seal, collector plate (bipolar plates), gasket seal, end plate fits together each assembly, then under the compression of end plate, is assembled into all-vanadium flow monocell.Wherein, in electrode frame, bipolar plates one side is conductive layer, and film one side is Catalytic Layer.Compress rear electrode thickness and be about 3.8mm, electrode area is 12cm
2.Anode electrolyte is 1.5M VO
2+3M H
2sO
4solution 40ml, negative pole electrolyte is 1.5M V
3+3M H
2sO
4solution 40ml.
The monocell that adopts combination electrode of the present invention, current density is 80mA/cm
2time, voltage efficiency and energy efficiency are respectively 88.3% and 84.9%; Current density is brought up to 120mA/cm
2time, voltage efficiency and energy efficiency still remain on 82.4% and 79.9%.
Embodiment 4
The conductive layer of electrode is chosen flexible graphite plate, and 2mm is thick, and volume density is 1.2gcm
-3; Catalytic Layer is chosen carbon felt, and 2.5mm is thick, and volume density is 0.14gcm
-3; Electrode adopts integrated mode, that is: get graphite powder 1g, carbon black 0.5g, phenolic resins 1g, add acetone 50ml, put into the ultrasonic 30min in ultrasonic pond, then by the solution blade coating mixing obtaining on flexible graphite plate surface, place in the above Catalytic Layer (carbon felt), 180 ℃ are carried out hot pressing, pressure is 0.05MPa, and the time is 30min, obtains combination electrode of the present invention.During assembling battery, order according to end plate, gasket seal, collector plate (bipolar plates), gasket seal, electrode frame, gasket seal, combination electrode, film, combination electrode, gasket seal, electrode frame, gasket seal, collector plate (bipolar plates), gasket seal, end plate fits together each assembly, then under the compression of end plate, is assembled into all-vanadium flow monocell.Compress rear electrode thickness and be about 3.8mm, electrode area is 12cm
2.Anode electrolyte is 1.5M VO
2+3M H
2sO
4solution 40ml, negative pole electrolyte is 1.5M V
3+3M H
2sO
4solution 40ml.
The monocell that adopts combination electrode of the present invention, current density is 80mA/cm
2time, voltage efficiency and energy efficiency are respectively 88.2% and 85.1%; Current density is brought up to 120mA/cm
2time, voltage efficiency and energy efficiency still remain on 82% and 79.3%.
Claims (9)
1. a flow battery combination electrode, is characterized in that: described combination electrode comprises conductive layer and the Catalytic Layer being superimposed with each other, and conductive layer thickness accounts for 10 ~ 90% of electrode gross thickness.
2. combination electrode according to claim 1, is characterized in that: described conductive is carbon element class material, and porosity is 0 ~ 80%.
3. combination electrode according to claim 2, is characterized in that: described carbon element class material is that atresia graphite cake, flexible graphite plate, volume density are 0.2 ~ 1.0gcm
-3graphite felt or volume density be 0.2 ~ 1.0gcm
-3carbon felt in one or two or more kinds be superimposed with each other and form.
4. combination electrode according to claim 1, is characterized in that: described Catalytic Layer is that one or two or more kinds in carbon felt, carbon paper, carbon cloth or graphite felt is superimposed with each other and forms, and volume density is 0.05 ~ 0.4gcm
-3, porosity is 80 ~ 95%.
5. combination electrode according to claim 1, is characterized in that: described combination electrode is by being prepared from conductive layer and Catalytic Layer by the mode of conducting resinl bonding.
6. combination electrode according to claim 5, is characterized in that: described conducting resinl is comprised of polymer and conductive filler, and wherein the mass ratio of polymer and conductive filler is 1/2 ~ 1/9.
7. combination electrode according to claim 6, is characterized in that: described polymer is one or two or more kinds in polypyrrole, polythiophene, polyaniline, polyethylene, polypropylene, polyvinyl chloride, epoxy resin, phenolic resins or Kynoar; Described conductive filler is one or two or more kinds in graphite, carbon black, acetylene black or carbon fiber.
8. combination electrode according to claim 1, is characterized in that: described combination electrode can also be put into successively conductive layer and Catalytic Layer in battery assembling process in electrode frame, and the mode by mechanical compaction fits together.
9. a liquid flow energy storage battery as claimed in claim 1, wherein liquid flow energy storage battery comprises positive pole, negative pole, bipolar plates and barrier film, it is characterized in that: described battery is to adopt described in claim 1 combination electrode as the liquid flow energy storage battery of positive pole and/or negative pole assembling, wherein combination electrode conductive layer one side contacts with bipolar plates, and Catalytic Layer one side contacts with film.
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106558704A (en) * | 2015-09-25 | 2017-04-05 | 中国科学院大连化学物理研究所 | A kind of flow battery gradient electrode and its application |
| CN112684362A (en) * | 2020-12-21 | 2021-04-20 | 深圳供电局有限公司 | Fault detection method, device and detection equipment for internal structure of storage battery |
| WO2021203932A1 (en) * | 2020-04-10 | 2021-10-14 | 国家能源投资集团有限责任公司 | Composite electrode for flow cell, flow cell, and pile |
| WO2021203935A1 (en) * | 2020-04-10 | 2021-10-14 | 国家能源投资集团有限责任公司 | Composite electrode for flow cell, flow cell, and pile |
| CN113659150A (en) * | 2021-07-09 | 2021-11-16 | 江苏大学 | Composite dual-functional electrode for eutectic solvent electrolyte flow battery |
| US11309565B2 (en) | 2017-02-28 | 2022-04-19 | Lg Chem, Ltd. | Electrode structure and redox flow battery comprising same |
| CN117423881A (en) * | 2023-12-14 | 2024-01-19 | 江苏米格新材料股份有限公司 | Method for improving effective contact surface of flow battery electrode and bipolar plate |
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106558704A (en) * | 2015-09-25 | 2017-04-05 | 中国科学院大连化学物理研究所 | A kind of flow battery gradient electrode and its application |
| CN106558704B (en) * | 2015-09-25 | 2019-11-12 | 中国科学院大连化学物理研究所 | A kind of flow battery gradient electrode and its application |
| US11309565B2 (en) | 2017-02-28 | 2022-04-19 | Lg Chem, Ltd. | Electrode structure and redox flow battery comprising same |
| WO2021203932A1 (en) * | 2020-04-10 | 2021-10-14 | 国家能源投资集团有限责任公司 | Composite electrode for flow cell, flow cell, and pile |
| WO2021203935A1 (en) * | 2020-04-10 | 2021-10-14 | 国家能源投资集团有限责任公司 | Composite electrode for flow cell, flow cell, and pile |
| CN113517451A (en) * | 2020-04-10 | 2021-10-19 | 国家能源投资集团有限责任公司 | Composite electrode for flow battery, flow battery and electric pile |
| CN112684362A (en) * | 2020-12-21 | 2021-04-20 | 深圳供电局有限公司 | Fault detection method, device and detection equipment for internal structure of storage battery |
| CN113659150A (en) * | 2021-07-09 | 2021-11-16 | 江苏大学 | Composite dual-functional electrode for eutectic solvent electrolyte flow battery |
| CN117423881A (en) * | 2023-12-14 | 2024-01-19 | 江苏米格新材料股份有限公司 | Method for improving effective contact surface of flow battery electrode and bipolar plate |
| CN117423881B (en) * | 2023-12-14 | 2024-04-02 | 江苏米格新材料股份有限公司 | Method for improving effective contact surface of flow battery electrode and bipolar plate |
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