CN105826520A - Water system high-voltage mixed ion secondary battery based on zinc-lithium ferric manganese phosphate - Google Patents
Water system high-voltage mixed ion secondary battery based on zinc-lithium ferric manganese phosphate Download PDFInfo
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion 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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0563—Liquid materials, e.g. for Li-SOCl2 cells
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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Abstract
The invention relates to a water system high-voltage mixed ion secondary battery. A positive pole material of the battery is a high-voltage battery positive pole material, namely zinc-lithium ferric manganese phosphate (LiFe1-xMnxPO4), the element zinc serves as the majority of a negative pole material, and electrolyte is a liquid-state or gel-state material which is formed by lithium bis(trifluoromethane sulfonimide) (LiTFSI) and soluble zinc salt as solute and water as solvent and has ionic conductivity. The battery is based on the energy storage mechanisms of a dissolution-out/deposition reaction of zinc ions (Zn2+) on a negative pole and a reversible embedding/ejection reaction of the zinc ions (Zn2+) on a positive pole, meanwhile, through the water-in-salt electrolyte formed by high-concentration LiTFSI, the electrochemical water decomposition process is inhibited, a potential window of the water system electrolyte is remarkably broadened, the zinc-lithium mixed ion secondary battery has the advantages of being high in capacity, long in cycling life, safe, environmentally friendly, low in cost and the like, and the battery can be applied to the fields such as consumer electronic equipment, electromobiles and large-scale energy storage.
Description
Technical field
The invention belongs to secondary cell field, particularly to a kind of water system high voltage hybrid ionic secondary cell based on zinc-lithium ferric manganese phosphate.
Background technology
Along with the arrival of information age, energy storage device effect in society is the most obvious.Existing electrochemistry chemical energy storage battery is mainly with lead-acid battery, nickel-cadmium cell, Ni-MH battery, flow battery and lithium ion battery etc..But, do not have a kind of energy storage system can adapt to the requirement of scale energy storage completely so far.The toxicity of plumbic acid and nickel-cadmium cell is relatively big, is unfavorable for environmental protection.Ni-mh and flow battery are expensive, and the market competitiveness is more weak.Lithium ion battery has occupied the consumption market of secondary cell 3/4, the especially application in the portable device such as notebook computer, mobile phone and video camera in after appearance more than 20 year.But, high cost limits its application in scale energy storage.Meanwhile, corresponding battery system is had higher requirement by developing rapidly of artificial intelligence's device, and this type of battery and human contact are more tight, and the requirement for safety and environmental protection is more focused on.Therefore, novel battery system high power capacity to be met and powerful requirement, simultaneously need to possess safe and eco-friendly characteristic.
Relative to traditional organic electrolyte lithium ion battery, aquo-lithium ion battery is in view of more agreeing with above-mentioned requirement.The blank of aquo-lithium ion battery is the VO that Dahn et al. proposed in 19942/LiMn2O4Battery model.But, the maximum deficiency of aquo-lithium ion battery system is the electrochemical window of aqueous electrolyte narrower (1.23 V), limits the range of choice of both positive and negative polarity, and its energy density is bigger than corresponding organic electrolysis plastidome difference.Simultaneously because liberation of hydrogen and the side reaction of analysis oxygen, the solid electrolyte interface (SEI film) in cannot being formed such as organic electrolyte system between electrolyte and electrode in aqueous electrolyte system, result in the problem that the stability of aquo-lithium ion battery is not enough.Therefore, by improving the electrochemically stable voltage window of aqueous electrolyte, the combination simultaneously optimizing positive and negative pole material is most important for high voltage, the high-energy-density water system battery system of Development of Novel.Nearest a kind of novel water system electrolyte system it would be possible to solve water system cell potential window narrows problem.Univ Maryland-Coll Park USA and AUS research laboratory disclose, at Scientific Periodicals " Science ", the aqueous electrolyte that a kind of high concentration LiTFSI is solute in November, 2015, this electrolyte presents typical salt bag water form, potential window is up to 3.0 V, and based on this electrolyte design with the LiMn being coated on stainless steel foil2O4And Mo6S8Being respectively positive pole and the aquo-lithium ion battery of negative pole, energy density is up to 84 Wh/kg, and the stability of electrolyte is further embodied in the circulating battery ability (after lower 1000 circulations of 4.5 C charge-discharge magnifications, capacitance retention rate is 68%) of excellence.
LiMnPO4Owing to higher Lithium-ion embeding current potential and theoretical capacity increasingly come into one's own.But, its relatively low electrical conductance and poor ion transmission performance are LiMnPO4The obstacle of development further.In recent years, scientific circles are coated with by nanorize, carbon and the means of doping have been achieved for necessarily being in progress.Especially by Fe2+Doping more can effectively weaken Mn3+Jahn-Teller effect, improve the cycle life of lithium manganese phosphate and multiplying power property.Aquo-lithium ion battery negative material mostly is inorganic oxide material, such as VO2、LiV3O8、TiO2、V2O3、Na2V6O16、LiTi2(PO4)4Deng.But, negative material capacitance is on the low side, and is vulnerable to the impact of oxygen and water, and in charge and discharge cycles, capacitance fall-off is too fast.Therefore, the novel negative polar body system of research high power capacity and high stability is the key that aquo-lithium ion battery develops further.Zinc-base battery be a class be the battery system of negative pole based on metallic zinc or its oxide.Research history the most nearly 200 years, its system may extend to Zn-MnO2, Zn-Ni, Zn-AgO, Zn-air battery etc..Compared to other negative materials, the advantages of zinc electrode.First, zinc rich in natural resources, cheap cost (price of zinc is far below lithium, suitable with magnesium, a little higher than aluminum), nontoxic and processing safety is high.Second, zinc electrode has relatively low reduction potential (0.76 V vs. SHE).3rd, the theoretical specific capacity of zinc electrode is high (820 mAh/g).The more important thing is, the compatibility of zinc load own water phase system and the advantage of Integration Assembly And Checkout can be carried out under air ambient.
Summary of the invention
It is contemplated that make up above-mentioned the deficiencies in the prior art, proposing a kind of novel water system high voltage zinc lithium hybrid ionic secondary cell, it has the high potential window more than 2.2 V.Inventor finds in high concentration LiTFSI(> 5 mol/L) the salt bag water electrolysis liquid system that formed adds appropriate soluble zinc salt stable hybrid ionic electrolyte can be formed.Based on this electrolyte, zinc ion (Zn2+) effective dissolution and deposition process, simultaneously positive electrode LiFe can be carried out on zinc load surface1-x Mn x PO4Effective lithium ion (Li can occur+) embed and deviate from reaction, mechanism is as follows:
Positive pole: LiFe1-x Mn x PO4⇔Li1-y Fe1-x Mn x PO4+
yLi+ +ye‒
Negative pole: Zn Zn2++
2e‒
The concrete scheme of the water system high voltage zinc lithium hybrid ionic secondary cell that the present invention proposes is as follows:
A kind of water system high voltage zinc lithium hybrid ionic secondary cell, by positive pole, negative pole, barrier film between both positive and negative polarity and containing lithium salts and zinc salt and possess the electrolyte of ionic conductivity and form, the active material of described positive pole is the lithium ferric manganese phosphate (or claiming iron manganese phosphate for lithium) being available for Lithium-ion embeding/abjection, and chemical formula is LiFe1-x Mn x PO4(1≥x≥0.01)；The active material of described negative pole is based on zinc element；Described electrolyte be the mixture with double trifluoromethanesulfonimide lithiums (LiTFSI) and soluble zinc salt as solute, water is solvent the liquid with ionic conductivity or gel state material, and pH value is 3 ~ 9.
Described positive pole includes collector and attachment cathode film on a current collector, and cathode film is made up of lithium ferric manganese phosphate, conductive agent and binding agent, and the addition of described conductive agent is the 5% ~ 50% of cathode film quality；Conductive agent can use graphite, carbon black, acetylene black, carbon fiber or CNT etc..The addition of described binding agent is the 2% ~ 30% of cathode film quality；Binding agent can use politef, water-soluble rubber, poly-inclined tetrafluoroethene or hydroxymethyl cellulose etc., and described collector is a kind of in graphite film, rustless steel, nickel, titanium, molybdenum, and collector pattern is porous, netted or thin film.
Described negative pole is simple metal zinc, kirsite or attachment negative electrode film on a current collector；Described negative electrode film is made up of the active material based on zinc element, conductive agent, porous carbon materials, corrosion inhibiter and binding agent；Described negative active core-shell material is zinc powder or the alloyed powder of zinc or zinc oxide or their mixture；The addition of described conductive agent is the 5% ~ 50% of negative electrode film quality；The preferable graphite of conductive agent, carbon black, acetylene black, carbon fiber or CNT etc..The addition of described binding agent is the 2% ~ 30% of negative electrode film quality；Binding agent is preferably politef, water-soluble rubber, poly-inclined tetrafluoroethene or hydroxymethyl cellulose etc..The addition of described porous carbon materials is the 1% ~ 30% of described negative electrode film quality；Porous carbon materials can use activated carbon, expanded graphite, carbon molecular sieve etc..The addition of described corrosion inhibiter is less than the 1% of negative electrode film quality.Corrosion inhibiter is at least one in the oxide of indium and the hydroxide of indium.Described collector is the one in graphite film, stainless steel substrates (net), nickel sheet (net), titanium sheet (net), molybdenum sheet (net).
Described electrolyte is the salt bag water form of high concentration LiTFSI, and the concentration of LiTFSI is 5 ~ 24 mol/L.
Described soluble zinc salt is one or more in zinc sulfate, zinc nitrate, zinc acetate, zinc chloride, and zinc salt concentration is 0.05 ~ 3 mol/L.
Lithium ion (Li+) can be at positive electrode active materials (LiFe1-x Mn x PO4) lattice in carry out reversible embedding and abjection, with the Mass Calculation of positive electrode active materials, described positive electrode active materials storage lithium ion (Li+) capacity not less than 100 mAh/g.
The potential window of water system high voltage zinc lithium hybrid ionic secondary cell of the present invention is not less than 2.2 V.
Water system high voltage zinc lithium hybrid ionic secondary cell of the present invention utilizes lithium ion (Li+) reversible embedding in positive electrode lattice and abjection, and zinc ion (Zn2+) dissolution in negative pole and the energy storage mechnism of deposition, this battery has the high and chargeable feature of capacity.After tested, battery of the present invention has excellent high rate performance, reversibility and circulation ability.
Accompanying drawing explanation
Fig. 1 is containing LiTFSI and ZnSO4The potential window of electrolyte.
Fig. 2 is the typical SEM figure of positive pole material phosphoric acid ferrimanganic lithium.
Fig. 3 is the XRD spectra of positive pole material phosphoric acid ferrimanganic lithium.
Fig. 4 is embodiment 1 prepared water system high voltage zinc lithium hybrid ionic secondary cell charging and discharging curve (with positive electrode active materials Mass Calculation) under 15 mA/g.
Fig. 5 is embodiment 2 prepared water system high voltage zinc lithium hybrid ionic secondary cell charging and discharging curve (with positive electrode active materials Mass Calculation) under 15 mA/g.
Fig. 6 is embodiment 3 prepared water system high voltage zinc lithium hybrid ionic secondary cell charging and discharging curve (with positive electrode active materials Mass Calculation) under 15 mA/g.
Detailed description of the invention
[embodiment
1
】
With the LiTFSI containing 21 mol/L and the ZnSO of 0.5 mol/L4Aqueous solution as electrolyte, by adding appropriate Lithium hydrate (LiOH), the pH value of electrolyte is controlled 7, the potential window of electrolyte is as shown in Figure 1.
Use commercially available iron manganese phosphate for lithium (LiFe0.2Mn0.8PO4) it is positive electrode active materials, LiFe0.2Mn0.8PO4SEM picture and XRD spectra as shown in Figures 2 and 3.By LiFe0.2Mn0.8PO4, after conductive agent acetylene black and polyfluortetraethylene of binding element mix with the mass ratio of 7:2:1, be coated on collector graphite film surface, be cut into a certain size, dry in vacuum and prepare LiFe0.2Mn0.8PO4Electrode slice.
With prepared LiFe0.2Mn0.8PO4Electrode slice is positive pole, thickness be the zinc metal sheet of 0.15 mm be negative pole, LiTFSI and ZnSO4Mixed aqueous solution be that electrolyte is assembled into battery.After tested, obtained high voltage hybrid ionic secondary cell charging and discharging curve under 15 mA/g constant currents is as shown in Figure 4.
[embodiment
2
】
Use commercially available iron manganese phosphate for lithium (LiFe0.3Mn0.7PO4) it is positive electrode active materials.By LiFe0.3Mn0.7PO4, after conductive agent acetylene black and polyfluortetraethylene of binding element mix with the mass ratio of 7:2:1, be coated on collector graphite film surface, be cut into a certain size, dry in vacuum and prepare LiFe0.3Mn0.7PO4Electrode slice.
With prepared LiFe0.3Mn0.7PO4Electrode slice is positive pole, thickness be the zinc metal sheet of 0.15 mm be negative pole, embodiment 1 preparation mixed aqueous solution be that electrolyte is assembled into battery.After tested, obtained high voltage hybrid ionic secondary cell charging and discharging curve under 15 mA/g constant currents is as shown in Figure 5.
[embodiment
3
】
After by zinc powder, porous carbon materials activated carbon, conductive agent acetylene black, polyfluortetraethylene of binding element and corrosion inhibiter Indium sesquioxide. being the ratio mixing of 50:20:20:9:1 in mass ratio, it is pressed on collector stainless (steel) wire, cut out for a certain size, in vacuum dry prepare zinc electrode.
With zinc electrode as negative pole, zinc powder quality is LiFe0.3Mn0.7PO4Ten times of quality, the LiFe prepared with embodiment 20.3Mn0.7PO4Electrode slice is positive pole, and the mixed aqueous solution of embodiment 1 preparation is that electrolyte is assembled into battery.After tested, obtained high voltage hybrid ionic secondary cell charging and discharging curve under 15 mA/g constant currents is as shown in Figure 6.
Claims (8)
1. a water system high voltage zinc lithium hybrid ionic secondary cell, by positive pole, negative pole, barrier film between both positive and negative polarity and containing lithium salts and zinc salt and possess the electrolyte of ionic conductivity and form, it is characterized in that: the active material of described positive pole is the lithium ferric manganese phosphate (or claiming iron manganese phosphate for lithium) being available for Lithium-ion embeding/abjection, and chemical formula is LiFe1-x Mn x PO4 (1≥x≥0.01)；The active material of described negative pole is based on zinc element；Described electrolyte be the mixture with double trifluoromethanesulfonimide lithiums (LiTFSI) and soluble zinc salt as solute, water is solvent the liquid with ionic conductivity or gel state material, and pH value is 3 ~ 9.
A kind of water system high voltage zinc lithium hybrid ionic secondary cell the most according to claim 1, it is characterized in that: described positive pole includes collector and attachment cathode film on a current collector, cathode film is made up of lithium ferric manganese phosphate, conductive agent and binding agent, and the addition of described conductive agent is the 5% ~ 50% of cathode film quality；The addition of described binding agent is the 2% ~ 30% of cathode film quality；Described collector is a kind of in graphite film, rustless steel, nickel, titanium, molybdenum, and collector pattern is porous, netted or thin film.
A kind of water system high voltage zinc lithium hybrid ionic secondary cell the most according to claim 1, it is characterised in that: described negative pole is simple metal zinc, kirsite or attachment negative electrode film on a current collector；Described negative electrode film is made up of the active material based on zinc element, conductive agent, porous carbon materials, corrosion inhibiter and binding agent；Described negative active core-shell material is zinc powder or the alloyed powder of zinc or zinc oxide or their mixture；The addition of described conductive agent is the 5% ~ 50% of negative electrode film quality；The addition of described binding agent is the 2% ~ 30% of negative electrode film quality；The addition of described porous carbon materials is the 1% ~ 30% of described negative electrode film quality；The addition of described corrosion inhibiter is less than the 1% of negative electrode film quality.
A kind of water system high voltage zinc lithium hybrid ionic secondary cell the most according to claim 1, it is characterised in that: described lithium salts be the concentration of LiTFSI, LiTFSI be 5 ~ 24 mol/L.
A kind of water system high voltage zinc lithium hybrid ionic secondary cell the most according to claim 1, it is characterised in that: the salt bag water form that the LiTFSI that described electrolyte is high concentration is formed.
A kind of water system high voltage zinc lithium hybrid ionic secondary cell the most according to claim 1, it is characterised in that: described soluble zinc salt is one or more in zinc sulfate, zinc nitrate, zinc acetate, zinc chloride, and zinc salt concentration is 0.05 ~ 3 mol/L.
A kind of water system high voltage zinc lithium hybrid ionic secondary cell the most according to claim 1 and 2, it is characterised in that: with the Mass Calculation of positive electrode active materials, the capacity of the active material storage lithium ion of described positive pole is not less than 100 mAh/g.
8. according to a kind of water system high voltage zinc lithium hybrid ionic secondary cell described in any claim in claim 1-6, it is characterised in that: the potential window of described hybrid ionic secondary cell is not less than 2.2 V.
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| CN107359372A (en) * | 2017-07-27 | 2017-11-17 | 中国科学院宁波材料技术与工程研究所 | A kind of aqueous electrolyte and Water based metal ion battery |
| KR20180030744A (en) * | 2016-09-16 | 2018-03-26 | 가부시끼가이샤 도시바 | Secondary battery, battery pack and vehicle |
| CN108172911A (en) * | 2018-01-11 | 2018-06-15 | 武汉大学 | A kind of full vanadium Water-soluble lithium ion battery |
| CN108365256A (en) * | 2017-01-26 | 2018-08-03 | 本田技研工业株式会社 | Lithium rechargeable battery |
| CN108565495A (en) * | 2018-04-26 | 2018-09-21 | 北京石墨烯研究院 | high-voltage lithium ion battery |
| CN108736076A (en) * | 2017-04-17 | 2018-11-02 | 常州优特科新能源科技有限公司 | A kind of aquo-lithium ion secondary cell and its preparation process |
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