CN204118182U - A kind of carbon sulphur anode composite and secondary aluminium cell - Google Patents
A kind of carbon sulphur anode composite and secondary aluminium cell Download PDFInfo
- Publication number
- CN204118182U CN204118182U CN201420511645.7U CN201420511645U CN204118182U CN 204118182 U CN204118182 U CN 204118182U CN 201420511645 U CN201420511645 U CN 201420511645U CN 204118182 U CN204118182 U CN 204118182U
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- sulphur
- carbon
- carbon nano
- pipe array
- nano pipe
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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
- Y02E60/10—Energy storage using batteries
Abstract
The utility model discloses a kind of carbon sulphur anode composite and the secondary aluminium cell comprising this positive pole, carbon sulphur anode composite comprises carbon nano pipe array, elemental sulfur and Graphene, and carbon nano pipe array vertical-growth is in conductive substrates; Elemental sulfur in carbon nano pipe array surface and nano aperture, forms carbon nano pipe array/sulphur composite material by hot melt diffusion way uniform load; Graphene uniform is coated on carbon nano pipe array/sulphur composite material surface.Carbon nano pipe array has three-dimensional network conducting matrix grain, and the load capacity of active material sulphur is improved greatly, and dispersion is more even, effectively improves the reactivity of sulphur; Its three-dimensional structure can provide effective conductive network and unobstructed ion channel simultaneously, improves the overall chemical property of positive pole; The coated loss by dissolution also can adsorbing further, stop, suppress intermediate product sulfur-based compound of Graphene, effectively improves the charge-discharge performance of battery; Carbon sulphur anode composite preparation method is simple, with low cost, environmental friendliness, and without additional conductive agent and binding agent, its specific capacity significantly improves, and energy density is also higher.
Description
Technical field
The invention belongs to battery material scientific domain, relate to a kind of carbon sulphur anode composite, be specifically related to a kind of sulphur/carbon nano pipe array anode composite of Surface coating Graphene and comprise the secondary aluminium cell of this positive pole.
Background technology
Aluminum cell can be filled as a kind of novel green chemical power source, there is high specific energy, the feature such as safe, inexpensive, pollution-free, be expected to the electrokinetic cell and the energy storage system that become high power capacity electric power storage of new generation.The theoretical volume specific capacity of aluminium is 8050mAh/cm
3, be 4 times of lithium, and chemical activity being stablized, is desirable negative material; The theoretical volume specific capacity of sulphur is 3467mAh/cm
3, be one of positive electrode that known energy density is the highest.The secondary cell formed with aluminium and sulphur is a kind of aboundresources, pollution-free, cheap, energy density is high, the energy storage system of use safety.
The electrical insulating property of sulphur causes the utilance of sulphur positive active material low, and the discharge and recharge of secondary aluminium-sulfur battery to react the Small molecular sulfur-based compound intermediate product produced soluble in electrolyte, thus cause irreversible loss and the capacity attenuation of active material, cause the self-discharge rate of battery high, cycle life is short, have impact on its large-scale application.In order to overcome the defect that elemental sulfur exists, normally elemental sulfur is loaded to and have in the carbon element class material of high-specific surface area, high porosity and excellent conductive performance, form composite positive pole, to limit the various negative effects that sulfur-based compound in cyclic process dissolves in electrolyte and causes thus.
Wherein, carbon nano-tube has the advantages such as good conductivity, draw ratio be large, can be barricaded as natural conductive network by bridge, be conducive to electrical conductivity and ion diffuse between them.But traditional carbon nano-tube is unordered reunion shape, mainly through the absorption carriage sulphur of carbon nano tube surface, the sulfur content in composite material is low, skewness.Be attached to the sulphur of carbon nano tube surface, cause the contact resistance of composite material to increase on the one hand, electrode is doubly forthright lower simultaneously, directly can dissolve in electrolyte on the other hand, cause the loss of active material in charge and discharge process, and battery energy density reduces.
Graphene is a kind of two dimensional surface nano-carbon material, has high-specific surface area, high conductivity, high mechanical properties and high-termal conductivity, is desirable energy storage material.Graphene coated sulfur materials effectively can suppress the loss of electrode active material sulphur.But because in preparation process, Graphene is very easily reunited, graphene sheet layer is easily stacking, causes the surface area of its conductive network greatly to reduce, the advantage of grapheme material itself can not be shown.
Summary of the invention
(1) goal of the invention
The object of the invention is to solve the sulphur load capacity that existing electrode exists on the low side, the problems such as specific capacity is less than normal, and energy density is low, cycle performance is not good, provide that a kind of preparation technology is simple, specific capacity is high, the anode composite of doubly forthright height, good cycle.
In order, draw ratio is high, favorable orientation, purity are high in carbon nano pipe array arrangement, avoids the inferior positions such as the sulphur load that the carbon nano-tube of applying unordered accumulation produces is uneven, contact resistance is high, can give full play to carbon nano-tube tubular material advantage.When adopting heat treatment mode carrying active substance sulphur, its huge specific area and nano-scale can provide more load byte, greatly can improve load capacity and the dispersed homogeneous degree of sulphur, effectively improve the reactivity of sulphur.Meanwhile, to being filled in nanotube and the sulphur in space between pipe, the major diameter of nanotube can produce than the more confinement effect of " long-range " and the suction-operated of common carbon-based material, can suppress the stripping of sulphur in battery charge and discharge process further, thus slow down the loss of sulphur.And be evenly coated on outer field Graphene, effectively can reduce the contact resistance caused by elemental sulfur of load on sulphur/carbon nano pipe array outer surface, can further improve the utilance of active material sulphur, improve high-rate charge-discharge capability.And the coated loss by dissolution can adsorbing further, stop, suppress intermediate product sulfur-based compound of Graphene, effectively improves the charge-discharge performance of battery.In addition, due to without additional conductive agent and binding agent, can significantly improve the specific capacity of electrode, the energy density of electrode is also higher.
The present invention also aims to provide a kind of secondary aluminium cell comprising above-mentioned anode composite.
(2) technical scheme
For achieving the above object, the invention provides following technical scheme:
A kind of carbon sulphur anode composite, comprise carbon nano pipe array, elemental sulfur and Graphene, it is characterized in that, described carbon nano pipe array vertical-growth is in conductive substrates; Described elemental sulfur in carbon nano pipe array surface and nano aperture, forms carbon nano pipe array/sulphur composite material by hot melt diffusion way uniform load; Described graphene uniform is coated on carbon nano pipe array/sulphur composite material surface.
Carbon sulphur anode composite described in scheme, is characterized in that, described carbon nano pipe array, and the caliber of carbon nano-tube is 1 ~ 50nm, pipe range 1 ~ 2000nm, tube pitch 2 ~ 100nm.
Carbon sulphur anode composite described in scheme, it is characterized in that, described conductive substrates material comprise in carbon fiber, graphite, vitrescence carbon, titanium, nickel, stainless steel, iron, copper, zinc, lead, manganese, cadmium, gold, silver, platinum, tantalum, tungsten, conductive plastics, conductive rubber or highly doped silicon any one.
Carbon sulphur anode composite described in scheme, is characterized in that, described Graphene is lamellar structure, and coated Graphene is less than 10 lamellas.
Carbon sulphur anode composite described in scheme, is characterized in that, comprise 70 ~ 80wt% sulphur, 10 ~ 20 wt % carbon nano pipe arrays, 1-20 wt % Graphene.
Scheme also provides a kind of secondary aluminium cell, comprising:
Anode composite described in (a) claim 1;
B () is containing aluminum honeycomb active material;
C () non-water is containing aluminium electrolyte.
Secondary aluminium cell described in scheme, is characterized in that, described containing aluminum honeycomb active material, comprising: metallic aluminium; Aluminium alloy, comprises the alloy containing at least one element be selected from Li, Na, K, Ca, Fe, Co, Ni, Cu, Zn, Mn, Sn, Pb, Ma, Ga, In, Cr, Ge and Al.
Secondary aluminium cell described in scheme, is characterized in that, described non-water is organic salt-aluminum halide system containing aluminium electrolyte, and wherein the mol ratio of organic salt and aluminum halide is 1:1.1 ~ 3.0.
Secondary aluminium cell described in scheme, is characterized in that, the cation of described organic salt comprises imidazol ion, pyridinium ion, pyrrolidinium ion, piperidines ion, morpholinium ion, quaternary ammonium salt ion ， quaternary alkylphosphonium salt ion and tertiary sulfosalt ion; The anion of organic salt comprises Cl
-, Br
-, I
-, PF
6 -, BF
4 -, CN
-, SCN
-, [N (CF
3sO
2)
2]
-, [N (CN)
2]
-plasma.
Organic salt described in scheme-aluminum halide system, is characterized in that, described aluminum halide is the one in aluminium chloride, aluminium bromide or silver iodide.
Described in scheme, the preparation method of secondary aluminium cell is as follows: above-mentioned anode composite is dried be cut into 40mm wide × pole piece that the long 0.33mm of 15mm is thick, the barrier film thick with 0.16mm and be wound into battery core with aluminium flake as the negative pole that negative active core-shell material is made and load nickel plating box hat, reinject electrolyte, and secondary aluminium cell is made in sealing.
(3) beneficial effect
Sulphur/carbon nano pipe array the anode composite of a kind of Surface coating Graphene provided by the invention has given full play to original advantage of both carbon nano pipe array and Graphene, has following beneficial effect:
(1) carbon nano pipe array has three-dimensional network conducting matrix grain, space between huge specific area and the pipe of nano-scale, can provide more load byte, and the load capacity of active material sulphur is improved greatly, and dispersion is more even, effectively improves the reactivity of sulphur; Its three-dimensional structure can provide effective conductive network and unobstructed ion channel simultaneously, improves the overall chemical property of positive pole.
(2) to being filled in nanotube and the sulphur in space between pipe, the major diameter of nanotube can produce the constraint than common carbon-based material more " long-range ", can suppress the stripping of sulphur in battery charge and discharge process further, thus slow down the loss of sulphur; Meanwhile, the coated loss by dissolution also can adsorbing further, stop, suppress intermediate product sulfur-based compound of Graphene, effectively improves the charge-discharge performance of battery.
(3) be evenly coated on outer field Graphene, the contact resistance that the elemental sulfur that effectively can reduce load on sulphur/carbon nano pipe array outer surface produces, can further improve the utilance of active material sulphur, improve high-rate charge-discharge capability.
(4) described anode composite preparation method is simple, with low cost, environmental friendliness, and without additional conductive agent and binding agent, its specific capacity significantly improves, and energy density is also higher.
(5) secondary aluminium cell comprising this positive pole has good high rate performance and cycle performance.
accompanying drawing explanation
Fig. 1 is combined electrode structure schematic diagram described in the utility model.
Fig. 2 is the structural representation of secondary aluminium cell described in the utility model.
Fig. 3 is the structural representation of winding-structure described in the utility model.
Wherein, 1-Graphene, 2-carbon nano pipe array, 3-sulphur, 4-upper cover, 5-insulated enclosure circle, 6-housing, 7-winding-structure, 8-positive plate, 9-barrier film, 10-negative plate.
embodiment
Be described further below with reference to the technique effect of drawings and Examples to design of the present invention, concrete structure and generation, to understand object of the present invention, characteristic sum effect fully.The following examples describe several execution mode of the present invention, and they are only illustrative, and nonrestrictive.
As shown in Figure 1, the carbon sulphur anode composite described in this embodiment, comprises Graphene 1, carbon nano pipe array 2 and sulphur 3; Wherein, carbon nano pipe array 2 is conducting matrix grain, its surface and aperture in load have sulphur 3, Graphene 1 is coated on outermost layer.
As shown in Fig. 2 ~ 3, the secondary aluminium cell described in this embodiment, it comprises battery container 6, be positioned over winding-structure 7 in battery container 6 and cell cover 4; Wherein said winding-structure comprises the repetitive structure be made up of positive plate 8, barrier film 9 and negative plate 10 successively; Insulated enclosure circle 5 is had between described winding-structure 7 and battery container.
Embodiment 1
(1) preparation of carbon nano pipe array: take stainless steel as substrate, Fe is catalyst take ethene as carbon source, and hydrogen and nitrogen are carrier gas, adopts chemical vapour deposition technique (CVD) to prepare carbon nano pipe array.
(2) composite sulfur: by the carbon nano pipe array prepared and elemental sulfur in mass ratio 1:10 put into tube furnace, be heated to 155 DEG C, passing under condition of nitrogen gas, keep 10h, form sulphur/carbon nano-tube array composite material.
(3) coated graphite alkene: configuration concentration is the graphene oxide water solution of 10mg/mL, ultrasonic disperse 10h, then adds reducing agent ammoniacal liquor to it, reacts 24h under ultrasound condition, obtain graphene dispersing solution, through vacuum filtration, washing, obtained Graphene content is the graphene dispersing solution of 8wt%, is then placed in one by the sulphur/carbon nano-tube array composite material prepared, leave standstill 24h, make the few layer graphene of its Surface coating, take out product dry 10h in 40 DEG C of baking ovens, obtained anode composite.
(4) preparation of secondary aluminium cell: above-mentioned anode composite is dried be cut into 40mm wide × pole piece that the long 0.33mm of 15mm is thick, the glass fibre thick with 0.16mm be non-to be knitted barrier film and is wound into electric stamen with aluminium flake as the negative pole of negative active core-shell material and load nickel plating box hat, add aluminium chloride-triethylamine hydrochloride ionic liquid again, AA type cylinder secondary aluminium cell is made in sealing.
During battery charging and discharging loop test, carry out charging to 2.5V with 1C, 0.1C discharges, and discharge cut-off voltage is 1.2V.Battery open circuit voltage is 1.68V, and discharge capacity is 846mAh first, and after 50 charge and discharge cycles, capability retention is 83.1%.
Embodiment 2
The preparation of carbon nano pipe array: take conductive paper of carbon fiber as substrate, Fe (NO
3)
3for catalyst, being coated in carbon paper surface in advance, take methane as carbon source, and nitrogen is protection gas, adopts chemical vapour deposition technique (CVD) to prepare carbon nano pipe array.
All the other preparation methods are with embodiment 1.Recording battery open circuit voltage is 1.65V, and discharge capacity is 839mAh first, and after 50 charge and discharge cycles, capability retention is 82.4%.
Embodiment 3
The preparation of aligned carbon nanotube is with embodiment 2.
Composite sulfur: elemental sulfur is heated to molten state, puts into wherein by the carbon nano pipe array prepared under nitrogen protection, takes out and puts into baking oven drying, form sulphur/carbon nano-tube array composite material after keeping 5 ~ 10h.
Coated graphite alkene: configuration concentration is the graphene oxide water solution of 15mg/mL, ultrasonic disperse 5h, then adds reducing agent ammoniacal liquor to it, reacts 48h under ultrasound condition, obtain graphene dispersing solution, through vacuum filtration, washing, obtained Graphene content is the graphene dispersing solution of 10wt%, is then placed in one by the sulphur/carbon nano-tube array composite material prepared, leave standstill 48h, make the few layer graphene of its Surface coating, take out product dry 10h in 40 DEG C of baking ovens, obtained anode composite.
The preparation of secondary aluminium cell and method of testing are with embodiment 1.Recording battery open circuit voltage is 1.69V, and discharge capacity is 856mAh first, and after 50 charge and discharge cycles, capability retention is 82.7%.
Although reference embodiment is to invention has been detailed description, but those skilled in the art is to be understood that, when not departing from the spirit and scope of the present invention described in appended claims and equivalent thereof, various amendment and replacement can be made to it.
Claims (5)
1. a carbon sulphur anode composite, comprises carbon nano pipe array, elemental sulfur and Graphene, it is characterized in that, described carbon nano pipe array vertical-growth is in conductive substrates; Described elemental sulfur in carbon nano pipe array surface and nano aperture, forms carbon nano pipe array/sulphur composite material by hot melt diffusion way uniform load; Described graphene uniform is coated on carbon nano pipe array/sulphur composite material surface.
2. carbon sulphur anode composite as claimed in claim 1, it is characterized in that, described carbon nano pipe array, the caliber of carbon nano-tube is 1 ~ 50nm, pipe range 1 ~ 2000nm, tube pitch 2 ~ 100nm.
3. carbon sulphur anode composite as claimed in claim 1, it is characterized in that, described conductive substrates material comprise in carbon fiber, graphite, vitrescence carbon, titanium, nickel, stainless steel, iron, copper, zinc, lead, manganese, cadmium, gold, silver, platinum, tantalum, tungsten, conductive plastics, conductive rubber or highly doped silicon any one.
4. carbon sulphur anode composite as claimed in claim 1, it is characterized in that, described Graphene is lamellar structure, and coated Graphene is less than 10 lamellas.
5. a secondary aluminium cell, comprising:
Anode composite described in (a) claim 1;
B () is containing aluminum honeycomb active material;
C () non-water is containing aluminium electrolyte.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201420511645.7U CN204118182U (en) | 2014-09-05 | 2014-09-05 | A kind of carbon sulphur anode composite and secondary aluminium cell |
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|---|---|---|---|
| CN201420511645.7U CN204118182U (en) | 2014-09-05 | 2014-09-05 | A kind of carbon sulphur anode composite and secondary aluminium cell |
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Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2017053142A1 (en) * | 2015-09-25 | 2017-03-30 | Board Of Regents, The University Of Texas System | Multi-layer carbon-sulfur cathodes |
| CN108091823A (en) * | 2016-11-22 | 2018-05-29 | 本田技研工业株式会社 | Electrode composition layer and battery |
| CN108615865A (en) * | 2018-05-02 | 2018-10-02 | 上海理工大学 | A kind of lithium sulfur battery anode material and preparation method thereof |
| CN109004192A (en) * | 2018-07-16 | 2018-12-14 | 郑州大学 | Combination electrode, the battery and preparation method thereof of graphene/graphene oxide cladding |
| CN110416491A (en) * | 2019-08-26 | 2019-11-05 | 贵州大学 | Modified ternary nickel cobalt manganese electrode of a kind of graphene coated and preparation method thereof |
| CN110518208A (en) * | 2019-08-26 | 2019-11-29 | 贵州大学 | A kind of preparation method of graphene coated cobalt acid lithium electrode |
| CN110707297A (en) * | 2018-07-10 | 2020-01-17 | 比亚迪股份有限公司 | Cathode material, preparation method thereof, lithium ion battery and vehicle |
| CN113228349A (en) * | 2019-05-14 | 2021-08-06 | 株式会社Lg化学 | Sulfur-carbon composite, and positive electrode and lithium secondary battery each containing the sulfur-carbon composite |
| CN113328061A (en) * | 2021-07-12 | 2021-08-31 | 浙江王点科技有限公司 | Preparation method of positive pole piece of lithium-sulfur battery |
| CN117239074A (en) * | 2023-09-04 | 2023-12-15 | 中能鑫储(北京)科技有限公司 | Sulfur-coated high-conductivity nano composite material, preparation method and aluminum ion battery |
| US11967702B2 (en) | 2019-05-14 | 2024-04-23 | Lg Energy Solution, Ltd. | Sulfur-carbon composite, and cathode and lithium secondary battery each comprising same |
-
2014
- 2014-09-05 CN CN201420511645.7U patent/CN204118182U/en not_active Expired - Fee Related
Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2017053142A1 (en) * | 2015-09-25 | 2017-03-30 | Board Of Regents, The University Of Texas System | Multi-layer carbon-sulfur cathodes |
| CN108091823A (en) * | 2016-11-22 | 2018-05-29 | 本田技研工业株式会社 | Electrode composition layer and battery |
| CN108615865A (en) * | 2018-05-02 | 2018-10-02 | 上海理工大学 | A kind of lithium sulfur battery anode material and preparation method thereof |
| CN110707297A (en) * | 2018-07-10 | 2020-01-17 | 比亚迪股份有限公司 | Cathode material, preparation method thereof, lithium ion battery and vehicle |
| CN110707297B (en) * | 2018-07-10 | 2021-05-14 | 比亚迪股份有限公司 | Cathode material, preparation method thereof, lithium ion battery and vehicle |
| CN109004192A (en) * | 2018-07-16 | 2018-12-14 | 郑州大学 | Combination electrode, the battery and preparation method thereof of graphene/graphene oxide cladding |
| CN109004192B (en) * | 2018-07-16 | 2021-06-04 | 郑州大学 | Graphene/graphene oxide coated composite electrode, battery and preparation method of composite electrode |
| CN113228349A (en) * | 2019-05-14 | 2021-08-06 | 株式会社Lg化学 | Sulfur-carbon composite, and positive electrode and lithium secondary battery each containing the sulfur-carbon composite |
| US11967702B2 (en) | 2019-05-14 | 2024-04-23 | Lg Energy Solution, Ltd. | Sulfur-carbon composite, and cathode and lithium secondary battery each comprising same |
| CN110518208A (en) * | 2019-08-26 | 2019-11-29 | 贵州大学 | A kind of preparation method of graphene coated cobalt acid lithium electrode |
| CN110416491A (en) * | 2019-08-26 | 2019-11-05 | 贵州大学 | Modified ternary nickel cobalt manganese electrode of a kind of graphene coated and preparation method thereof |
| CN113328061A (en) * | 2021-07-12 | 2021-08-31 | 浙江王点科技有限公司 | Preparation method of positive pole piece of lithium-sulfur battery |
| CN117239074A (en) * | 2023-09-04 | 2023-12-15 | 中能鑫储(北京)科技有限公司 | Sulfur-coated high-conductivity nano composite material, preparation method and aluminum ion battery |
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