CN103985851A - Sodium ion battery anode material and sodium iron battery comprising anode material - Google Patents

Sodium ion battery anode material and sodium iron battery comprising anode material Download PDF

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Publication number
CN103985851A
CN103985851A CN201410230166.2A CN201410230166A CN103985851A CN 103985851 A CN103985851 A CN 103985851A CN 201410230166 A CN201410230166 A CN 201410230166A CN 103985851 A CN103985851 A CN 103985851A
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sodium
ion battery
positive electrode
anode material
battery positive
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曹余良
杨汉西
苑丁丁
艾新平
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Wuhan University WHU
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Wuhan University WHU
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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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/364—Composites as mixtures
    • 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
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • 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
    • Y02E60/10—Energy storage using batteries

Abstract

The invention discloses a sodium ion battery anode material and a sodium iron battery comprising the anode material, and belongs to the technical field of energy source materials. The sodium ion battery anode material comprises a conductive additive and Na3-xM2LO6, wherein x is greater than or equal to 0 and smaller than 2; M is one or more of Fe, Co, Ni, Cu, Zn, Mg, V and Cr; L is one or more of Sb, Te, Nb, Bi and P. The preparation method comprises the steps of mixing sodium carbonate, M oxide and L oxide according to a stoichiometric proportion, ball-milling, calcining and ball-milling so as to obtain the sodium ion battery anode material. The sodium ion battery anode material has the advantages of high sodium storage capacity, good stability and excellent rate capability, and has extremely high energy density and power density; the assembled sodium iron battery has extremely good cycling stability, is green and clean, safe and environmentally friendly and low in cost, and is an extremely excellent electrochemical energy storage system; moreover, the preparation method of the anode material is extremely simple, and raw materials are low in price and easily available.

Description

One Na-like ions cell positive material and comprise the sodium-ion battery of this positive electrode
Technical field
The invention discloses a Na-like ions cell positive material and comprise the sodium-ion battery of this positive electrode, belong to energy and material technical field.
Background technology
Traditional fossil energy is (as coal, oil, natural gas etc.) reserves are limited, and due to uncontrolled exploitation and the use of nearly two a century, make the existing fossil energy reserves difficulty that sharply less, exploitation becomes, therefore cannot meet the needs of the growing production of the mankind and existence.More seriously, fossil fuel has caused environmental pollution, harm people's health.Therefore find environmental protection new forms of energy, promoting Renewable Energy Development has become trend of the times.The regenerative resource such as solar energy, wind energy has the feature such as aboundresources, cleanliness without any pollution, is the fundamental way that solves energy problem.But solar energy and wind energy etc. are because being subject to the restriction of natural conditions to have intermittence, the feature such as unstable, and can not control with demand, be difficult to generate electricity by way of merging two or more grid systems, must utilize extensive energy-storage system to ensure the continuity of grid stability and supply of electric power.
There is multiple technologies route in existing extensive energy storage technology, as lead-acid battery, flow battery, sodium-sulphur battery and advanced lithium ion battery etc., they were all once considered as possible electrical network energy storage device.But the inherent shortcomings such as that these battery systems exist is with high costs, resource-constrained, long-term cycle life are poor, poor stability cannot meet growing actual needs.Recently, sodium-ion battery, because the reserves of sodium are abundant and with low cost, can cause widely and pay close attention to for extensive energy storage field.
Transition metal oxide (NaMO 2, M=Ni, Co, Fe, Mn, V etc.) and be one of study hotspot of sodium-ion battery positive electrode, it has and is similar to now industrialized LiCoO 2the working condition of material, may realize the commercialization of sodium-ion battery at first.But, NaMO at present 2material is faced with the shortcomings such as storage sodium capacity is low, and poor stability and high rate performance are poor, and these factors have stoped NaMO 2the further large-scale application of material.
Summary of the invention
The shortcomings such as problem to be solved by this invention is low for above-mentioned existing transition metal oxide positive electrode storage sodium capacity, and poor stability and high rate performance are poor, provide a Na-like ions cell positive material and comprise the sodium-ion battery of this positive electrode.
Object of the present invention is achieved through the following technical solutions:
A kind of sodium-ion battery positive electrode, comprises conductive additive and Na 3-xm 2lO 6, wherein 0≤x < 2; M is one or more in Fe, Co, Ni, Cu, Zn, Mg, V, Cr; L is one or more in Sb, Te, Nb, Bi, P.
The content of described conductive additive is below 50 wt%, described Na 3-xm 2lO 6content be 50wt%-95wt%.
Described conductive additive is conductive carbon.
Described conductive carbon is one or more in graphite, acetylene black, Super P, middle phase microballoon, Ketjen black.
Described Na 3-xm 2lO 6for Na 3ni 2sbO 6, Na 3co 2sbO 6, Na 3cu 2sbO 6, Na 3coNiSbO 6, Na 3ni 2sb 0.9nb 0.1o 6, Na 3ni 2sb 0.5nb 0.5o 6, Na 2.5ni 2sb 0.5te 0.5o 6, Na 3ni 1.5zn 0.5sbO or Na 3ni 1.9mg 0.1sbO 6.
A method of preparing above-mentioned sodium-ion battery positive electrode, comprises the steps:
(1) sodium carbonate, M oxide and L oxide are mixed according to stoichiometric proportion, ball milling, obtains mixed-powder;
(2) the mixed-powder calcining of being prepared by step (1), obtains Na 3-xm 2lO 6.
(3) Na being prepared by step (2) 3-xm 2lO 6with conductive carbon ball milling, obtain sodium-ion battery positive electrode.
Ball-milling Time in described step (1) is 4-10h.
Roasting condition in described step (2) is: 800 DEG C-1200 DEG C of temperature, time 6-24h.
Ball milling in described step (3) is high-energy ball milling or planetary ball mill, and the time is 0.5h-6h.
The application of above-mentioned sodium-ion battery positive electrode in sodium-ion battery.
In the sodium-ion battery positive electrode that the present invention proposes, Na 3-xm 2lO 6for layer structure, Na +be positioned at M 2lO 6interlayer, has highly stable crystal structure, can realize stable sodium ion and embeds and deviate from.
Sodium-ion battery positive electrode provided by the invention, storage sodium capacity is high, and good stability and high rate performance are good, have very high energy density and power density; The sodium-ion battery of assembling has very excellent cyclical stability, and green clean, and safety and environmental protection is with low cost, is a kind of very excellent electrochemical energy storage system.
The preparation method of sodium-ion battery positive electrode provided by the invention is very simple, and raw material is cheap and easy to get.
Brief description of the drawings
Fig. 1 is Na prepared by the embodiment of the present invention 1 3ni 2sbO 6the charging and discharging curve of material
Fig. 2 is Na prepared by the embodiment of the present invention 2 3co 2sbO 6the charging and discharging curve of material.
Fig. 3 is Na prepared by the embodiment of the present invention 3 3niCoSbO 6the charging and discharging curve of material.
Fig. 4 is Na prepared by the embodiment of the present invention 4 3ni 1.5zn 0.5sbO 6the cycle performance figure of material.
Embodiment
Below in conjunction with drawings and Examples, technical scheme of the present invention is described in further detail.
Embodiment 1.
By 0.15 mol Na 2cO 3, 0.2 mol NiO and 0.05 mol Sb 2o 3mix, be placed in high-energy ball milling tank, high-energy ball milling 4h, then mixture is calcined 12h at 800 DEG C, can prepare Na 3ni 2sbO 6.Again by made Na 3ni 2sbO 6with acetylene black (10 wt%) high-energy ball milling mixing 30min, obtain Na 3ni 2sbO 6/ C positive electrode.This positive electrode is mixed by the weight ratio of 7:2:1 with vinylidene (PVDF), acetylene black, be coated to and on aluminium foil, make electrode film.Taking this electrode film as work electrode, sodium metal sheet is to electrode, 1mol L -1naPF 6(solvent is the mixture of EC and DEC, and the volume ratio of EC and DEC is 1:1) carries out electro-chemical test for electrolyte is assembled into 2016 type button cells.Fig. 1 is its constant current charge-discharge curve (0.1 C(20mA g -1) discharge and recharge within the scope of current density, 2-4.0 V), as seen from the figure, the reversible capacity of positive electrode is 117 mAh g -1, discharge potential platform is 3.3V.
Embodiment 2.
By 0.15 mol Na 2cO 3, 0.1 mol Co 2o 3with 0.05 mol Sb 2o 5, being placed in high-energy ball milling tank, high-energy ball milling 4h then calcines 24h at 900 DEG C, can prepare Na 3co 2sbO 6.Again by made Na 3co 2sbO 6with Super P(20 wt%) planetary ball mill mixing 6h, obtain Na 3co 2sbO 6/ C positive electrode.
Prepare electrode film and it is carried out to constant current charge-discharge test by the method in embodiment 1, Fig. 2 is its constant current charge-discharge curve (0.1 C(20mA g -1) under current density and within the scope of 2-4.0 V, discharge and recharge), as seen from the figure, the head week discharge capacity of material is 88 mAh g -1.
Embodiment 3
By 0.15 mol Na 2cO 3, 0.05 mol Co 2o 3, 0.1 mol NiO and 0.05 mol Sb 2o 3, being placed in high-energy ball milling tank, high-energy ball milling 6h then calcines 6h at 1200 DEG C, can prepare Na 3coNiSbO 6.Again by made Na 3coNiSbO 6with Ketjen black (5 wt%) planetary ball mill mixing 6h, obtain Na 3coNiSbO 6/ C positive electrode.
Prepare electrode film and to row constant current charge-discharge test by method in embodiment 1, Fig. 3 for this reason material at 0.1 C(20mA/g) charging and discharging curve under current density, in figure, show that the first all specific discharge capacities of this material are 90 mAh g -1, there is higher storage sodium capacity.
Embodiment 4
By 0.15 mol Na 2cO 3, 0.075 mol NiO, 0.025 mol MgO and 0.05 mol Sb 2o 3, being placed in high-energy ball milling tank, high-energy ball milling 10h then calcines 8h at 900 DEG C, can prepare Na 3ni 1.5zn 0.5sbO 6.Again by made Na 3ni 1.5zn 0.5sbO 6with graphite (5 wt%) planetary ball mill mixing 6h, obtain Na 3ni 1.5zn 0.5sbO 6/ C positive electrode.
Prepare electrode film and it carried out to constant current charge-discharge test by method in embodiment 1, Fig. 4 for this reason material at 0.1 C(20mA/g) 50 weeks cyclic curve figure under current density, in figure, result shows that this material not only has 120 mAh g -1reversible capacity, and 50 weeks capability retentions are 87 %, have good cycle performance.
Embodiment 5
By 0.15 mol Na 2cO 3, 0.075 mol NiO, 0.01 mol MgO and 0.05 mol Sb 2o 3, being placed in high-energy ball milling tank, high-energy ball milling 10h then calcines 8h at 900 DEG C, can prepare Na 3ni 1.9mg 0.1sbO 6.Again by made Na 3ni 1.9mg 0.1sbO 6with middle phase microballoon (15 wt%) planetary ball mill mixing 6h, obtain Na 3ni 1.9mg 0.1sbO 6/ C positive electrode.
Prepare electrode film and it is carried out to constant current charge-discharge test by method in embodiment 1, at 0.1 C(20mA g -1) under current density and within the scope of 2-4.0 V, discharge and recharge, this material is first has 130 mAh g week -1reversible capacity, the capacity after 100 weeks that circulates still maintains 85% of initial capacity, has extraordinary cycle performance.
Embodiment 6
By 0.125 mol Na 2cO 3, 0.1mol NiO, 0.025 mol TeO 2with 0.025 mol Sb 2o 3, being placed in high-energy ball milling tank, high-energy ball milling 10h then calcines 8h at 900 DEG C, can prepare Na 2.5ni 2sb 0.5te 0.5o 6.Again by made Na 2.5ni 2sb 0.5te 0.5o 6with acetylene black (30 wt%) planetary ball mill mixing 6h, obtain Na 2.5ni 2sb 0.5te 0.5o 6/ C positive electrode.
Prepare electrode film and it is carried out to constant current charge-discharge test by method in embodiment 1, at 0.1 C(20mA g -1) under current density and within the scope of 2-4.0 V, discharge and recharge, this material has 70 mAh g -1reversible capacity.
Embodiment 7
By 0.15 mol Na of stoichiometric proportion 2cO 3, 0.1 mol NiO, 0.01 mol Nb 2o 5with 0.0225 mol Sb 2o 3, being placed in high-energy ball milling tank, high-energy ball milling 10h then calcines 8h at 900 DEG C, can prepare Na 3ni 2sb 0.9nb 0.1o 6.Again by made Na 3ni 2sb 0.9nb 0.1o 6with Ketjen black/graphite (the mass ratio 1:1 of Ketjen black and graphite, the addition of Ketjen black/graphite is 35 wt%) planetary ball mill mixing 6h, obtain Na 3ni 2sb 0.9nb 0.1o 6/ C positive electrode.
Prepare electrode film and it is carried out to constant current charge-discharge test by method in embodiment 1, at 0.1 C(20mA g -1) under current density and within the scope of 2-4.0 V, discharge and recharge, this material has 105 mAh g -1reversible capacity.
Embodiment 8
By 0.15 mol Na of stoichiometric proportion 2cO 3, 0.1 mol NiO, 0.025 mol Nb 2o 5with 0.025 mol Sb 2o 3, being placed in high-energy ball milling tank, high-energy ball milling 8h then calcines 12h at 900 DEG C, can prepare Na 3ni 2sb 0.5nb 0.5o 6.Again by made Na 3ni 2sb 0.5nb 0.5o 6with Ketjen black (addition of Ketjen black is 50 wt%) planetary ball mill mixing 3h, obtain Na 3ni 2sb 0.5nb 0.5o 6/ C positive electrode.
Prepare electrode film and it is carried out to constant current charge-discharge test by method in embodiment 1, at 0.1 C(20mA g -1) under current density and within the scope of 2-4.0 V, discharge and recharge, this material has 100 mAh g -1reversible capacity.

Claims (10)

1. a sodium-ion battery positive electrode, is characterized in that: comprise conductive additive and Na 3-xm 2lO 6, wherein 0≤x < 2; M is one or more in Fe, Co, Ni, Cu, Zn, Mg, V, Cr; L is one or more in Sb, Te, Nb, Bi, P.
2. a kind of sodium-ion battery positive electrode according to claim 1, is characterized in that: the content of described conductive additive is below 50 wt%, described Na 3-xm 2lO 6content be 50wt%-95wt%.
3. according to a kind of sodium-ion battery positive electrode described in claim 1 or 2, it is characterized in that: described conductive additive is conductive carbon.
4. a kind of sodium-ion battery positive electrode according to claim 3, is characterized in that: described conductive carbon is one or more in graphite, acetylene black, Super P, middle phase microballoon, Ketjen black.
5. according to a kind of sodium-ion battery positive electrode described in claim 1 or 2, it is characterized in that: described Na 3-xm 2lO 6for Na 3ni 2sbO 6, Na 3co 2sbO 6, Na 3cu 2sbO 6, Na 3coNiSbO 6, Na 3ni 2sb 0.9nb 0.1o 6, Na 3ni 2sb 0.5nb 0.5o 6, Na 2.5ni 2sb 0.5te 0.5o 6, Na 3ni 1.5zn 0.5sbO or Na 3ni 1.9mg 0.1sbO 6.
6. a method of preparing sodium-ion battery positive electrode described in claim 1-4 any one, is characterized in that comprising the steps:
(1) sodium carbonate, M oxide and L oxide are mixed according to stoichiometric proportion, ball milling, obtains mixed-powder;
(2) the mixed-powder calcining of being prepared by step (1), obtains Na 3-xm 2lO 6;
(3) Na being prepared by step (2) 3-xm 2lO 6with conductive carbon ball milling, obtain sodium-ion battery positive electrode.
7. a kind of preparation method of sodium-ion battery positive electrode according to claim 6, is characterized in that: the Ball-milling Time in described step (1) is 4-10h.
8. a kind of preparation method of sodium-ion battery positive electrode according to claim 6, is characterized in that: the roasting condition in described step (2) is: 800 DEG C-1200 DEG C of temperature, time 6-24h.
9. a kind of preparation method of sodium-ion battery positive electrode according to claim 6, is characterized in that: the ball milling in described step (3) is high-energy ball milling or planetary ball mill, the time is 0.5h-6h.
10. according to the application of a kind of sodium-ion battery positive electrode in sodium-ion battery described in claim 1-4 any one.
CN201410230166.2A 2014-05-28 2014-05-28 Sodium ion battery anode material and sodium iron battery comprising anode material Pending CN103985851A (en)

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104495941A (en) * 2014-12-19 2015-04-08 桂林电子科技大学 Preparation method of sodium-ion battery positive electrode material
CN104722309A (en) * 2015-03-06 2015-06-24 三峡大学 Visible-light-responded photocatalyst K2Ni2Sb8O23 and preparation method thereof
CN107078350A (en) * 2014-08-22 2017-08-18 法拉典有限公司 The storage and/or transport of sodium-ion battery
CN108155371A (en) * 2017-12-25 2018-06-12 哈尔滨师范大学 The method that nanoscale antimony base transition metal oxide sodium ion battery electrode material is prepared using discarded animal organic matter as template
CN114005987A (en) * 2021-10-26 2022-02-01 山东玉皇新能源科技有限公司 Sodium ion battery positive electrode material additive and sodium ion battery positive electrode material
CN115995533A (en) * 2022-11-28 2023-04-21 深圳市山木新能源科技股份有限公司 Layered composite oxide of sodium ion battery

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Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107078350A (en) * 2014-08-22 2017-08-18 法拉典有限公司 The storage and/or transport of sodium-ion battery
CN104495941A (en) * 2014-12-19 2015-04-08 桂林电子科技大学 Preparation method of sodium-ion battery positive electrode material
CN104722309A (en) * 2015-03-06 2015-06-24 三峡大学 Visible-light-responded photocatalyst K2Ni2Sb8O23 and preparation method thereof
CN108155371A (en) * 2017-12-25 2018-06-12 哈尔滨师范大学 The method that nanoscale antimony base transition metal oxide sodium ion battery electrode material is prepared using discarded animal organic matter as template
CN114005987A (en) * 2021-10-26 2022-02-01 山东玉皇新能源科技有限公司 Sodium ion battery positive electrode material additive and sodium ion battery positive electrode material
CN114005987B (en) * 2021-10-26 2024-03-22 山东玉皇新能源科技有限公司 Additive for positive electrode material of sodium ion battery and positive electrode material of sodium ion battery
CN115995533A (en) * 2022-11-28 2023-04-21 深圳市山木新能源科技股份有限公司 Layered composite oxide of sodium ion battery
CN115995533B (en) * 2022-11-28 2023-11-17 深圳市山木新能源科技股份有限公司 Layered composite oxide of sodium ion battery

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