CN108448145A - A kind of novel organic flow battery of double ion embedded type - Google Patents
A kind of novel organic flow battery of double ion embedded type Download PDFInfo
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- CN108448145A CN108448145A CN201810193859.7A CN201810193859A CN108448145A CN 108448145 A CN108448145 A CN 108448145A CN 201810193859 A CN201810193859 A CN 201810193859A CN 108448145 A CN108448145 A CN 108448145A
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- flow 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
- H01M8/184—Regeneration by electrochemical means
- H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
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- 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
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/023—Porous and characterised by the material
- H01M8/0234—Carbonaceous material
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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 present invention discloses a kind of novel organic flow battery of double ion embedded type, the flow battery includes positive plate, negative plate, anode collection plate, negative pole currect collecting plate, positive reaction chamber, negative reaction chamber, electrolyte, anode electrolyte delivery pipe/delivery pump, electrolyte liquid delivery pipe/delivery pump and the diaphragm material between positive and negative electrode reaction chamber, it is characterised in that：The positive plate, negative plate are porous graphite membrane material.Compared to traditional aqueous electrolyte flow battery and lithium ion flow battery; technical scheme of the present invention is embedded in mechanism using double ion; operating voltage is more than 4 V; avoid the use of lithium-containing transition metal oxide positive electrode active materials, positive and negative anodes electrolyte storage tank, positive and negative anodes conductive agent, binder, collector; charge and discharge cycles number, energy density are greatly improved, cost is reduced, while solving positive and negative anodes electrolyte cross-contamination issue; preparation process is simple, is easy to large-scale production.
Description
Technical field
The invention belongs to electrochemical energy storage cell technologies, specifically design a kind of organic double ion embedded type flow battery.
Background technology
The exacerbation increasingly of energy crisis and environmental problem, accelerates the fast development of New Energy Industry.Under existing situation
Green energy resource is performed to ultimate attainment environmentally friendly electrochemical energy storage technology for giving low-carbon energy-saving emission reduction to be paid more and more attention.
Recently, country proposes to establish nearly zero carbon emission engineering based on energy internet, and wherein core content includes just regenerative resource
Power generation, distributed energy storage technology etc., to new and effective energy storage technology, more stringent requirements are proposed for this.
In recent years, tremendous development has been obtained by the extensive energy storage of representative of flow battery.The output power of flow battery
Depending on the electrode reaction area of battery and the joint number of battery unit, stored energy capacitance then depends on the volume of electrode suspension and dense
Degree, the two can be individually designed, be a kind of output power and stored energy capacitance are independent of one another, energy density is big, charge and discharge switching flexibly,
Fast response time, lower-cost novel green rechargeable battery.It has developed at present a variety of using different electrolyte solutions
Flow battery, wherein mainly water-soluble electrolytes, such as full vanadium, iron/chromium and bromine/polysulfide liquid flow energy storage battery.It is above-mentioned
Flow battery is all made of water as solvent, when the charging voltage of battery is higher than 1.23 V of electrochemical stability window of water, water meeting
Ionization is decomposed, and gas evolution is caused, simultaneously because the decomposition of water can cause active material to be precipitated, service life of battery, battery efficiency,
Safety is also affected, and is limited to output voltage, and the energy density of water system flow battery is relatively low（20~50Wh/L）；Simultaneously
Since positive and negative anodes electrolyte is different, electrolyte ion is easy to be transferred to the other side through diaphragm material, and electrolyte is caused to intersect
Osmosis pollution reduces battery efficiency.
Lithium ion flow battery is a kind of new chemical energy-storage battery, it combines the excellent of lithium ion battery and flow battery
Point, anode and cathode active materials and electrolyte, the mixture-electrode suspension of conductive agent of this new type lithium ion flow battery,
It is attached separately in two device for storing liquid, under the promotion of power circulation system, electrode suspension flows through anode by sealing pipeline
In the both sides of diaphragm redox reaction occurs for reaction chamber and negative reaction chamber.When charging, anode release Li+, through diaphragm into
Enter into electrolyte liquid, final Li+It is embedded into cathode, cardinal principle is by single Li+It is embedded between positive and negative anodes
With deintercalation, charge storage is realized.Its positive electrode is mostly lithium-containing transition metal oxide, and cathode is mostly graphite material, anti-
In multiple charge and discharge process, the cycle performance containing lithium metal oxide is poor（<1000 times）, it is easy to happen structure change, in recent years
Come by the in short supply of the resources such as lithium, cobalt, the cost of positive electrode steeply rises；In addition, positive and negative anodes electrode suspension needs two
A storage tank is stored, and battery weight is considerably increased, and reduces battery energy density（<300Wh/L）, increase cost.
Therefore, those skilled in the art is dedicated to that exploitation is a kind of to have that operating voltage higher, cycle performance be more preferable, energy
Density higher, electroless liquid cross contamination, cost is more cheap, preparation process is simple to operation, is easy to the new of large-scale production
The organic double ion embedded type flow battery of type.
Invention content
The present invention is above-mentioned in order to solve the problems, such as, provides a kind of organic double ion embedded type flow battery.
To achieve the goals above, the technical scheme is that：
A kind of novel organic flow battery of double ion embedded type, the flow battery include positive plate, negative plate, anode collection plate,
Negative pole currect collecting plate, positive reaction chamber, negative reaction chamber, electrolyte, anode electrolyte delivery pipe/delivery pump, electrolyte liquid are defeated
Send pipe/delivery pump and the diaphragm material between positive and negative electrode reaction chamber.
The positive plate, negative plate are porous graphite membrane material, after being accumulated using lamination process, are respectively placed in positive reaction
In chamber, negative reaction chamber.
The porous stone ink film is one in porous polyimide graphite film, porous expanded graphite film, porous graphene film
Kind.
The shape in the hole of the porous graphite membrane material be circular configuration, a diameter of 10 ~ 100 microns of hole, the center of circle in hole
Between distance be 50 ~ 500 microns, mass ratio shared by carbon atom is more than 99% in porous stone ink film.
In the electrolyte of the novel organic flow battery of double ion embedded type, electrolyte lithium salt is lithium hexafluoro phosphate
（LiPF6）, lithium perchlorate（LiClO4）, hexafluoroarsenate lithium（LiAsF6）, LiBF4 (LiBF4), di-oxalate lithium borate
（LiBOB）, difluorine oxalic acid boracic acid lithium（LiDFOB）, two（Trimethyl fluoride sulfonyl）Imine lithium（LiTFSI）, double fluorine sulfimide lithiums
（LiFSI）, trifluoromethanesulfonic acid lithium（LiCF3SO3）, hexafluoro-antimonic acid lithium（LiSbF6）, three（Pentafluoroethyl group）Three lithium fluophosphates
（LiFAP）In it is one or more；Solvent is that solvent is sulfolane（SL）, dimethyl carbonate（DMC）, diethyl carbonate（DEC）、
Methyl ethyl carbonate（EMC）, propene carbonate（PC）, ethylene carbonate（EC）, methyl propyl carbonate（MPC）, gamma-butyrolacton（GBL）、
Fluorinated ethylene carbonate（FEC）, ethyl acetate（EA）, tri-methyl ethyl acetate（TMEA）, methyl butyrate（MB）, methyl propionate
（MP）, ethyl propionate（EP）, propyl propionate（PP）, propyl acetate（PA）, methyl acetate（MA）, ethyl acetoacetate（EAA）, three
It is one or more in methyl acetic acid methyl esters.
The diaphragm material is single-layer polypropylene film, polyethylene film, the composite membrane of polyethylene/polypropylene/polyethylene, fiber
One kind in plain non-woven membrane, glass fibre membrane.
The electrolyte delivery pipe is stainless steel tube, silicone tube or polyfluortetraethylene pipe.
Compared with the existing technology, technical scheme of the present invention positive and negative electrode pole piece is porous graphite membrane material, itself has both
Active material, collector, electrolyte transmission channel are integrated, and anode is to carry out charge storage by anion insertion reaction,
Embedded potential is up to 4 V or more, and cathode carries out charge storage by cationic insertion reaction, and insertion potential is only<0.1
V, therefore, entire cell output voltage>4 V, substantially increase operating voltage, are promoted to be conducive to energy density；Theoretically,
Positive and negative anodes pole piece, to unconfined increase positive and negative anodes pole piece quantity, can further be improved according to reaction chamber size design
Energy density（800~1000Wh/L）；The flow battery designs, and also avoids having used standard aqueous electrolyte flow battery or have
Positive and negative anodes fluid reservoir necessary to machine lithium ion flow battery, eliminates the use of metal collector, conductive agent, binder, subtracts
Lack battery weight, and reduces battery production cost；Meanwhile positive and negative anodes electrolyte composition is identical, it is entirely avoided positive and negative anodes
Electrolyte cross-contamination issue；Carbon Materials stable structure, structure is not susceptible to change during repeated charge, cycle performance
It is greatly enhanced（>10000 times）；In addition, Carbon Materials are cheap and easy to get, it can be to avoid lithium-containing transition metal oxide positive electrode
Use, from battery cost is greatly reduced, be conducive to industrialization promotion use.
Description of the drawings
Fig. 1 is the novel organic flow battery structural schematic diagram of double ion embedded type provided in an embodiment of the present invention.
Specific implementation mode
Referring to Fig. 1, the novel organic flow battery of double ion embedded type provided by the invention, including positive plate 11, negative plate
12, anode collection plate 21, negative pole currect collecting plate 22, positive reaction chamber 31, negative reaction chamber 32, anode electrolyte delivery pipe 41, negative
Pole electrolyte delivery pipe 42, electrolyte liquid delivery pump 52, is located at positive reaction chamber and cathode is anti-at anode electrolyte delivery pump 51
Answer the diaphragm material 6 between chamber and the electrolyte of the flowing in delivery pipe, reaction chamber.
Below by embodiment, the present invention is further illustrated.
Embodiment 1：
Positive/negative plate makes：It is derived from polyimides graphite film processed, which is 20 μm.The film is placed in laser-beam drilling machine
At sample mounting table, laser ablation parameter is adjusted：Power 20W, mark speed 1500mm/s, laser focal 160mm, optical maser wavelength
1064nm, frequency 20kHz, distance starts respectively by adjusting laser beam cutting diameter and pitch-row between the diameter and hole in hole
Power supply, it is that distance is 240 μm between 50 μm, hole that Circularhole diameter is obtained after punching, and mass ratio shared by carbon atom is 99.5%.
After polyimide foraminous graphite film obtained above is cut into certain size, drying is for use.
Cell package：By the porous stone ink film of above-mentioned certain size according to positive plate/positive plate/positive plate/anode
The sequence of piece .../positive plate is placed in positive reaction chamber, the placement order of negative plate and positive plate phase in negative reaction chamber
Together, positive reaction chamber, negative reaction chamber, delivery pump, the electrolyte delivery pipe of polytetrafluoroethyltubing tubing matter, diaphragm are assembled later
To together, electrolyte is the LiPF of 1mol/L6/（Methyl ethyl carbonate+sulfolane mixed solvent）, battery is formed after encapsulation.
Battery charging and discharging is tested：Charge and discharge are carried out using 0.2 C multiplying power electric currents, voltage range is 4.0 ~ 5.2 V, through surveying
Fixed, the energy density of the flow battery is up to 950Wh/L, and after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio is
98.7%, battery efficiency 98.5%.
Embodiment 2：
Electrolytic salt in embodiment 1 is changed to LiFSI, remaining is same as Example 1.After measured, the energy of the flow battery
Density is up to 970Wh/L, and after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio 99.5%, battery efficiency is
99.3%。
Embodiment 3：
Electrolytic salt in embodiment 1 is changed to LiBF4, remaining is same as Example 1.After measured, the energy of the flow battery
Density is up to 880Wh/L, and after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio 98.2%, battery efficiency is
98.5%。
Embodiment 4：
Solvent in embodiment 1 is changed to propene carbonate, remaining is same as Example 1.After measured, the energy of the flow battery
Density is up to 890Wh/L, and after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio 98.5%, battery efficiency is
98.4%。
Embodiment 5：
Electrolytic salt in embodiment 1 is changed to LiTFSI, remaining is same as Example 1.After measured, the energy of the flow battery
Density is up to 965Wh/L, and after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio 98.7%, battery efficiency is
98.1%。
Embodiment 6：
Diaphragm in embodiment 1 is changed to the composite membrane of polyethylene/polypropylene/polyethylene, remaining is same as Example 1.Through surveying
Fixed, the energy density of the flow battery is up to 940Wh/L, and after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio is
98.7%, battery efficiency 97.9%.
Embodiment 7：
Change the polyimide foraminous graphite film in embodiment 1 into expanded graphite perforated membrane, thickness is 25 μm, adjustment punching ginseng
Number so that the pitch of holes of expanded graphite perforated membrane is 280 μm, remaining is same as Example 1.After measured, the energy of the flow battery
Metric density is up to 935Wh/L, and after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio 98.1%, battery efficiency is
98.0%。
Embodiment 8：
Changing the polyimide foraminous graphite film in embodiment 1 into porous graphene film, thickness is 20 μm, adjusts downhole parameter,
So that the pitch of holes of expanded graphite perforated membrane is 260 μm, remaining is same as Example 1.After measured, the energy of the flow battery is close
Degree is up to 825Wh/L, after lower 10000 charge and discharge of 1C multiplying power electric currents, capacity retention ratio 98.5%, and battery efficiency 98.2%.
Embodiment described above only represents the several embodiments in the present invention, the description thereof is more specific and detailed, but simultaneously
Cannot the limitation to the scope of the claims of the present invention therefore be interpreted as.It should be pointed out that for those of ordinary skill in the art
For, without departing from the inventive concept of the premise, various modifications and improvements can be made, these belong to the guarantor of the present invention
Protect range.Therefore, the protection domain of patent of the present invention should be determined by the appended claims.
Claims (6)
1. a kind of novel organic flow battery of double ion embedded type, which includes positive plate, negative plate, anode collection
Plate, negative pole currect collecting plate, positive reaction chamber, negative reaction chamber, electrolyte, anode electrolyte delivery pipe/delivery pump, electrolyte liquid
Delivery pipe/delivery pump and the diaphragm material between positive and negative electrode reaction chamber, it is characterised in that：The positive plate, negative plate
For porous graphite membrane material, after being accumulated using lamination process, it is respectively placed in positive reaction chamber, negative reaction chamber.
2. a kind of novel organic flow battery of double ion embedded type according to claim 1, it is characterised in that：It is described porous
Graphite film is one kind in porous polyimide graphite film, porous expanded graphite film, porous graphene film.
3. a kind of novel organic flow battery of double ion embedded type according to claim 1, it is characterised in that：Described is more
The shape in the hole of hole graphite film material is circular configuration, a diameter of 10 ~ 100 microns of hole, between the center of circle in hole distance be 50 ~
500 microns, mass ratio shared by carbon atom is more than 99% in porous stone ink film.
4. a kind of novel organic flow battery of double ion embedded type according to claim 1, it is characterised in that：The electrolysis
In liquid, electrolyte lithium salt is lithium hexafluoro phosphate（LiPF6）, lithium perchlorate（LiClO4）, hexafluoroarsenate lithium（LiAsF6）, tetrafluoro boron
Sour lithium (LiBF4), di-oxalate lithium borate（LiBOB）, difluorine oxalic acid boracic acid lithium（LiDFOB）, two（Trimethyl fluoride sulfonyl）Imines
Lithium（LiTFSI）, double fluorine sulfimide lithiums（LiFSI）, trifluoromethanesulfonic acid lithium（LiCF3SO3）, hexafluoro-antimonic acid lithium（LiSbF6）, three
（Pentafluoroethyl group）Three lithium fluophosphates（LiFAP）In it is one or more；Solvent is that solvent is sulfolane（SL）, dimethyl carbonate
（DMC）, diethyl carbonate（DEC）, methyl ethyl carbonate（EMC）, propene carbonate（PC）, ethylene carbonate（EC）, carbonic acid first third
Ester（MPC）, gamma-butyrolacton（GBL）, fluorinated ethylene carbonate（FEC）, ethyl acetate（EA）, tri-methyl ethyl acetate（TMEA）、
Methyl butyrate（MB）, methyl propionate（MP）, ethyl propionate（EP）, propyl propionate（PP）, propyl acetate（PA）, methyl acetate
（MA）, ethyl acetoacetate（EAA）, it is one or more in methyl trimethylacetate.
5. a kind of novel organic flow battery of double ion embedded type according to claim 1, it is characterised in that：The diaphragm
Material is single-layer polypropylene film, polyethylene film, the composite membrane of polyethylene/polypropylene/polyethylene, cellulosic nonwoven fabric film, glass
One kind in tunica fibrosa.
6. a kind of novel organic flow battery of double ion embedded type according to claim 1, it is characterised in that：The electrolysis
Liquid delivery pipe is stainless steel tube, silicone tube or polyfluortetraethylene pipe.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109244466A (en) * | 2018-11-27 | 2019-01-18 | 中国科学院青岛生物能源与过程研究所 | A kind of underwater subsurface buoy energy-storage battery |
| CN109560339A (en) * | 2018-11-27 | 2019-04-02 | 中国科学院青岛生物能源与过程研究所 | A kind of pre- embedding anion method and full battery |
| CN110137501A (en) * | 2019-03-29 | 2019-08-16 | 中国科学院青岛生物能源与过程研究所 | A kind of flexibility high-voltage lithium ion batteries and preparation method thereof |
| CN111370719A (en) * | 2020-03-19 | 2020-07-03 | 辽宁科京新材料科技有限公司 | High-conductivity bipolar plate for flow battery and continuous processing device and method thereof |
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| CN107086326A (en) * | 2016-02-14 | 2017-08-22 | 中国科学院长春应用化学研究所 | A kind of electrolyte and Dual-ion cell |
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| CN102315473A (en) * | 2011-06-28 | 2012-01-11 | 北京好风光储能技术有限公司 | Lithium ion flow redox battery |
| CN105514531A (en) * | 2014-09-23 | 2016-04-20 | 中国科学院大连化学物理研究所 | Lithium ion-halogen flow battery |
| CN107251299A (en) * | 2015-06-23 | 2017-10-13 | 松下知识产权经营株式会社 | Redox flow batteries |
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| CN109244466A (en) * | 2018-11-27 | 2019-01-18 | 中国科学院青岛生物能源与过程研究所 | A kind of underwater subsurface buoy energy-storage battery |
| CN109560339A (en) * | 2018-11-27 | 2019-04-02 | 中国科学院青岛生物能源与过程研究所 | A kind of pre- embedding anion method and full battery |
| CN110137501A (en) * | 2019-03-29 | 2019-08-16 | 中国科学院青岛生物能源与过程研究所 | A kind of flexibility high-voltage lithium ion batteries and preparation method thereof |
| CN111370719A (en) * | 2020-03-19 | 2020-07-03 | 辽宁科京新材料科技有限公司 | High-conductivity bipolar plate for flow battery and continuous processing device and method thereof |
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