CN107180966A - A kind of new aqoue seconary battery using lithium salts and sodium salt as electrode material - Google Patents
A kind of new aqoue seconary battery using lithium salts and sodium salt as electrode material Download PDFInfo
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Abstract
The present invention relates to a kind of using lithium salts and sodium salt as the new aqoue seconary battery of electrode material.The present invention using lithium ion, sodium ion mixed aqueous solution as electrolyte, positive pole uses the inlaid scheme material containing sodium ion (or lithium ion), and negative pole uses the inlaid scheme material containing lithium ion (or sodium ion).Its charge and discharge process is related to two kinds of ion (Na+, Li+) reversible deintercalation between the electrodes.Stability of the present invention with larger power and good circulation, and with it is pollution-free, inexpensive the features such as.
Description
Technical field
It is more particularly to a kind of using lithium salts and sodium salt as electrode material the present invention relates to electrochemical technology field, lithium ion
It is that the new of electrolyte can discharge and recharge water system battery with sodium ion mixed aqueous solution.
Technical background
With continuing to develop for science and technology, the consumption to traditional energy increasingly increases, the increasingly exhaustion of fossil fuel, it is desirable to people
Research emphasis must be transferred to new energy field by class.Since the commercialization of nineteen ninety lithium ion battery, lithium-ion electric
The development in pond is advanced by leaps and bounds, the advantages of lithium ion battery of traditional organic system has specific capacity height, good cycling stability.But
It is that lithium resource is only 0.0065% in the storage of the earth's crust, therefore the price of lithium ion battery will be expensive all the more, and tradition has
There is certain potential safety hazard, and the poor-performing under larger current discharge and recharge in the lithium ion battery of body system.Therefore open
Send out novel green safety and environmental protection a kind of and cheap battery is extremely necessary.The basic functional principle of aquo-lithium ion battery is with showing
Some organic system lithium ion batteries are similar, but in aqueous phase electrolyte, the decomposition voltage of water is than larger obstacle, it is necessary to
Ensure during both positive and negative polarity deintercalate lithium ions, liberation of hydrogen, oxygen evolution reaction do not occur for the aqueous solution, therefore rarely have material can conduct
The cycle performance for the negative material being related in the both positive and negative polarity of aquo-lithium ion battery, and the patent is poor, so as to cause water system
The overall cyclical stability of lithium ion battery is poor.Other full battery of the both positive and negative polarity by electrode material of lithium salts is not solved still
The problem of lithium resource is increasingly deficient.Sodium resource relatively enriches (2.74%) in the storage of the earth's crust, cheap, and sodium and lithium are in member
Belong to same main group in plain periodic table, have similar physicochemical property, therefore a part is replaced as electrode material using sodium salt
Lithium salts has extraordinary development prospect.
The content of the invention
In order to overcome the above-mentioned deficiencies of the prior art, the invention provides one kind using lithium salts and sodium salt as electrode material, with
Lithium ion and sodium ion mixed aqueous solution are that the new of electrolyte can discharge and recharge water system battery.The technical solution adopted in the present invention
It is:It is more and there is the sodium ion of close physicochemical property as the substitute of lithium ion with lithium ion using earth content, if
Counted it is a kind of by electrode material of lithium salts and sodium salt it is new can discharge and recharge mix water system battery.
Technical scheme proposed by the present invention is:A kind of new by electrode material of lithium salts and sodium salt can discharge and recharge water system electricity
Pond, is made up of, the cathode film cathode film, negative electrode film, the barrier film fallen between and the electrolyte with ionic conductivity
With negative electrode film using current lithium ion and the electrode material of sodium-ion battery, electrolyte is using lithium ion and the mixing water of sodium ion
Solution.
In the present invention it is new can discharge and recharge mixing water system battery operation principle and existing organic series lithium ion battery,
The operation principle of water system chargeable lithium ion battery and water system chargeable sodium-ion battery is similar.During charging, Na+(Li+) from positive electrode
Na in middle abjection, electrolyte+(Li+) be embedded in negative material;During electric discharge, Na+(Li+) deviate from again from negative material, electrolyte
In Na+(Li+) be embedded in positive electrode, while discharging electric energy.
The present invention uses the natrium doping LiMn2O4 (Li being modified1-xNaxMn2O4) it is used as positive pole, the compound titanium phosphate sodium of carbon
(NaTi2(PO4)3/ C) it is used as negative pole, lithium sulfate (Li2SO4) and sodium sulphate (Na2SO4) mixed electrolytic solution of the aqueous solution constructs
It is a kind of can discharge and recharge water system battery as the new of electrode material using lithium salts and sodium salt.The system improves lithium ion water system battery
Cyclical stability, and green cleaning, safety and environmental protection, relative inexpensiveness is a kind of novel secondary battery.It is used
Extensively, can be used in large-scale energy-accumulating power station is used for the portable power source of portable set for electric automobile and mixing electric car on way
Deng field.And technological process is simple, environment relative loose is assembled, cost is also quite cheap.
Brief description of the drawings
Fig. 1 is natrium doping LiMn2O4 (Li1-xNaxMn2O4) high rate performance curve of the positive electrode in mixed electrolytic solution.
Fig. 2 is carbon compound phosphoric acid titanium sodium (NaTi2(PO4)3/ C) high rate performance song of the negative material in mixed electrolytic solution
Line.
Fig. 3 is natrium doping LiMn2O4 (Li1-xNaxMn2O4) and carbon compound phosphoric acid titanium sodium (NaTi2(PO4)3/ C) system is entirely electric
The charging and discharging curve in pond.
Embodiment
The preparation of the positive and negative pole material of the present invention and Li1-xNaxMn2O4-NaTi2(PO4)3The assembling of the full battery of/C systems
General step is as follows.
1. natrium doping manganate cathode material for lithium (Li1-xNaxMn2O4) preparation
By lithium acetate, manganese acetate, sodium acetate, citric acid, glucose is with the ratio of the amount (1-x) * 1.05: 2: x: 1: 2 of material
Example is dissolved in 100mL deionized waters, wherein control lithium excessive 5%, 15h is first stirred at room temperature by obtained mixed solution,
4h is stirred at 80 DEG C again, is subsequently placed into drying box and dark brown gel is obtained with 80 DEG C of temperature drying 12h.By the gel of gained
First 400 DEG C of pre-burning 4h in tube furnace.Then take out the sample needed for 800 DEG C of calcining 8h are produced again after grinding uniformly.
2. carbon compound phosphoric acid titanium sodium negative material (NaTi2(PO4)3/ C) preparation
By 3.4mL butyl titanates (C16H36O4Ti) it is added dropwise to containing 40mL ethylene glycol (C2H6O2) and 10mL ammoniacal liquor
(NH3·H2O (28wt.%)) mixed solution in, continuously stir after 1h, be slowly added to 10mL and contain 1725.5mg biphosphates
Ammonium (NH4H2PO4) aqueous solution, then add 10mL to contain 265mg sodium carbonate (Na again2CO3) aqueous solution.Finally by obtained canescence
After colloid stirring 3h, it is transferred in 100mL stainless steel cauldrons, and 140 DEG C of insulation 24h.Room temperature is cooled to, product is distinguished
Cleaned several times, after being dried under the conditions of 60 DEG C, product is ground, with 5 DEG C of min in Muffle furnace repeatedly with distilled water and ethanol-1
Heating rate rise to 850 DEG C, without isothermal holding, directly cool to room temperature with the furnace.The powdered NaTi of extracting waste2
(PO4)3Presoma is mixed with the tartaric acid of certain mass fraction, ultrasound 1h after stirring 30min, is allowed to well mixed, then should
Mixture in blanket of nitrogen with 3 DEG C of min-1Firing rate rises to 650 DEG C, is incubated 2h, is then cooled to room temperature, is answered with obtaining carbon
Close titanium phosphate sodium NaTi2(PO4)3/ C composite.
3. three-electrode system is tested
Respectively by both positive and negative polarity active material, acetylene black, 1%PTFE is coated on foam so that 8: 1: 1 mass ratio is well mixed
As working electrode on nickel collector, using 10*10*0.1mm platinum plate electrodes as to electrode, reference is used as using saturated calomel electrode
Electrode carries out test loop volt-ampere and charge-discharge test in the mixed aqueous solution electrolyte of lithium salts and sodium salt.
4. the assembling of the full battery of mixed system
Positive electrode uses Li1-xNaxMn2O4.Negative material uses NaTi2(PO4)3/ C, enters according to the actual capacity of material
The proportioning of row positive and negative pole material, by active material, conductive agent and binding agent are well mixed, are uniformly coated on nickel foam collection
On fluid, after drying, cathode film and negative electrode film are pressed into respectively.Barrier film uses glass fibre, and electrolyte uses lithium salts and sodium salt
Mixed aqueous solution, assembling help battery carry out charge-discharge test.
Embodiment 1
Li1-xNaxMn2O4-NaTi2(PO4)3/ C systems
Positive pole utilizes the LiMn2O4 (Li of natrium doping1-xNaxMn2O4) positive electrode, negative pole use different phosphorus content phosphoric acid
Titanium sodium and carbon composite NaTi2(PO4)3/ C, according to active material: acetylene black: binding agent=8: 1: 1 mass ratio mixing
Uniformly, it is coated in foamed nickel current collector, after drying, cathode film and negative electrode film is pressed into respectively.Using glass fibre as every
The mixed aqueous solution of film, lithium sulfate and sodium sulphate helps battery as electrolyte, assembling.As a result show, phosphorus content is 5.8% left
Right system has preferable chemical property, and its charging/discharging voltage is stable in 1.58V or so, in 600mA g-1Current density
Under, charge specific capacity is 76mAh g-1, specific discharge capacity is 61mAh g-1。
Embodiment 2
Li(NiCoMn)1/3O2-NaTi2(PO4)3/ C systems
Positive pole utilizes current commercialized anode material for lithium-ion batteries (Li (NiCoMn)1/3O2), negative pole is compound using carbon
Titanium phosphate sodium (NaTi2(PO4)3/ C) material, according to active material: acetylene black: binding agent=8: 1: 1 mass ratio mixing is equal
It is even, it is coated in foamed nickel current collector, after drying, cathode film and negative electrode film is pressed into respectively.Using glass fibre as barrier film,
The mixed aqueous solution of lithium sulfate and sodium sulphate helps battery as electrolyte, assembling.The charging/discharging voltage stabilization of the system exists
1.6V or so, in 600mA g-1Current density under, charge specific capacity be 79mAh g-1, specific discharge capacity is 59mAh g-1。
Embodiment 3
LiMn2O4-NaTi2(PO4)3/ C systems
Positive pole utilizes current commercialized lithium cell anode material lithium manganate (LiMn2O4), negative pole is combined phosphorus using carbon
Sour titanium sodium (NaTi2(PO4)3/ C) material, according to active material: acetylene black: binding agent=8: 1: 1 quality Billy is well mixed,
It is coated in foamed nickel current collector, after drying, cathode film and negative electrode film is pressed into respectively.Barrier film, sulphur are used as using glass fibre
The mixed aqueous solution of sour lithium and sodium sulphate helps battery as electrolyte, assembling.The charging/discharging voltage of the system is stable in 1.55V
Left and right, in 600mA g-1Current density under, charge specific capacity be 68mAh g-1, specific discharge capacity is 62mAh g-1。
Embodiment 4
Na3V2(PO4)3-Li4Ti5O12System
Positive pole utilizes Na3V2(PO4)3Positive electrode, negative pole uses carbon compound phosphoric acid titanium sodium (NaTi2(PO4)3/ C) material,
According to active material: acetylene black: binding agent=8: 1: 1 quality Billy is well mixed, and is coated in foamed nickel current collector, dry
Afterwards, cathode film and negative electrode film are pressed into respectively.Using glass fibre as barrier film, the mixed aqueous solution of lithium sulfate and sodium sulphate is made
For electrolyte, battery is helped in assembling.The charging/discharging voltage of the system is stable in 1.38V or so, in 600mA g-1Current density
Under, charge specific capacity is 64mAh g-1, specific discharge capacity is 59mAh g-1。
Claims (8)
1. a kind of new aqoue seconary battery using lithium salts and sodium salt as electrode material, by cathode film, negative electrode film, between both it
Between barrier film and mixed electrolytic solution composition, it is characterised in that the positive active material use lithium salts electrode material, negative pole use
Sodium salt electrode material;Or positive active material use sodium salt electrode material, negative pole use lithium salts electrode material, and with lithium salts with
The mixed aqueous solution of sodium salt as the system electrolyte.
2. it is according to claim 1 a kind of using lithium salts and sodium salt as the new aqoue seconary battery of electrode material, its feature
It is:Cathode film uses Lithium-ion embeding compound, transition metal oxide, sulfide, phosphide, chloride etc.;Negative electrode film
Using sodium ion inlaid scheme, transition metal oxide, sulfide, phosphide, chloride etc..Or cathode film using sodium from
Sub- inlaid scheme, transition metal oxide, sulfide, phosphide, chloride, negative electrode film uses Lithium-ion embeding compound,
Transition metal oxide, sulfide, phosphide, chloride etc..Electrolyte is using lithium ion and the sulfate of sodium ion, nitric acid
The mixed aqueous solution of lithium ion and sodium ion in salt, acetate, phosphate, chloride or hydroxide.
3. battery according to claim 1, it is characterised in that affiliated positive pole inlaid scheme is LiCoO2, LiMn2O4, Li
(CoNiMn)1/3O2, LiFePO4, Na3V2(PO4)3, Na0.44MnO2, Na2NiFe(CN)6, λ-MnO2Deng, in addition to above-claimed cpd
In containing other metallic elements M adulterate material.
4. battery according to claim 1, it is characterised in that affiliated negative pole inlaid scheme is NaTi2(PO4)3,
Li4Ti5O12, Na2Ti3O7, graphite, Li4Ti5O12Deng, in addition to the material that the M containing other metallic elements adulterates in above-claimed cpd
Material.
5. it is according to claim 1 a kind of using lithium salts and sodium salt as the new aqoue seconary battery of electrode material, its feature
It is that the cathode film and negative electrode film add also added with conductive agent and binding agent.
6. it is according to claim 1 a kind of using lithium salts and sodium salt as the new aqoue seconary battery of electrode material, its feature
It is that both positive and negative polarity collector uses stainless (steel) wire, nickel foam, titanium net, copper foil, the one or more such as carbon cloth.
7. it is a kind of using lithium salts and sodium salt as the new aqoue seconary battery of electrode material according to right 1, it is characterised in that
Electrolyte in electrolyte is Li2SO4, LiNO3, LiOH, LiCl and Na2SO4, NaNO3, NaOH, two or more groups in NaCl
Into lithium ion and sodium ion mixed aqueous solution, the pH value of concentration of aqueous solution solution is between 1-14, and the concentration of electrolyte is 1
The mol/L of mol/L -10.
8. a kind of using lithium salts and sodium salt as the new aqoue seconary battery of electrode material according to right 1 or 2, its feature exists
Cylinder type, square and button type etc. can be made in shape.Its shell can be organic using organic plastics, metal material or metal
Composite of material etc..
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Cited By (11)
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CN108091921A (en) * | 2017-12-27 | 2018-05-29 | 南京航空航天大学 | A kind of mixed electrolytic solution water system can fill nickel sodium/lithium battery and preparation method thereof |
CN108321442A (en) * | 2018-01-08 | 2018-07-24 | 中国科学技术大学 | Mix water system ion battery and its application |
CN108493501A (en) * | 2018-03-30 | 2018-09-04 | 华南师范大学 | The preparation method of sodium fluoride Dual-ion cell and its application in electrochemistry fluorine removal |
CN109428126A (en) * | 2017-08-30 | 2019-03-05 | 丰田自动车株式会社 | Aqueous electrolyte and aquo-lithium ion secondary cell |
CN110474111A (en) * | 2019-06-20 | 2019-11-19 | 宋君 | 3.5V aquo-lithium ion battery |
CN110854453A (en) * | 2019-11-20 | 2020-02-28 | 苏州金科发能源技术有限公司 | Manufacturing method of lithium battery capable of continuously providing high power |
CN111710859A (en) * | 2020-06-22 | 2020-09-25 | 江苏理工学院 | Water system lithium sodium ion battery and preparation method and application thereof |
CN113193166A (en) * | 2021-04-28 | 2021-07-30 | 珠海冠宇电池股份有限公司 | Positive plate, battery core and battery |
CN114725519A (en) * | 2021-01-06 | 2022-07-08 | 东莞理工学院 | Lithium ion battery electrolyte, preparation method thereof and lithium ion battery |
CN114824512A (en) * | 2022-04-13 | 2022-07-29 | 华中科技大学 | Sodium-based liquid metal battery based on replacement reaction and preparation method thereof |
CN116093255A (en) * | 2023-02-20 | 2023-05-09 | 中国科学院长春应用化学研究所 | Battery system for evaluating lithium ion and sodium ion storage compatibility of positive electrode material |
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CN114824512A (en) * | 2022-04-13 | 2022-07-29 | 华中科技大学 | Sodium-based liquid metal battery based on replacement reaction and preparation method thereof |
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