CN105514490B - A kind of electrolyte solution for lithium-sulfur cell - Google Patents
A kind of electrolyte solution for lithium-sulfur cell Download PDFInfo
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Abstract
A kind of electrolyte solution for lithium-sulfur cell, composition includes solute 1：A kind of or two kinds or more of surfactant；The surfactant concentration is 0.01-10 mol/Ls；Solute 2：A kind of or two kinds or more of lithium salts；The lithium salt is 0.1-10 mol/Ls；Solvent：One kind in straight chain ether compound or two kinds or more.The advantages such as this electrolyte solution, which has, hinders sulfur transfer, and good cycling stability, price are low.
Description
Technical field
The present invention relates to lithium-sulfur cell fields, specifically, the lithium-sulfur cell being related to includes negative metal lithium, contains element sulphur
Anode, diaphragm and electrolyte solution.
Background technology
In recent decades, the commercialization of lithium ion battery, be greatly promoted electronic equipment such as mobile phone, notebook etc.
Extensive use in life.But the energy density of lithium ion battery is universal not high, which also limits it in electric vehicle, big rule
The application of mould energy storage etc..Therefore, people are just starting to develop the battery of more height ratio capacity, as lithium is empty, lithium-sulfur cell.Wherein lithium
The closer commercialization of sulphur battery.
The theoretical specific energy density of sulphur is 2500Whkg-1, 2800WhL-1.And sulphur is cheap, resourceful, environment
Close friend, because lithium-sulfur cell promises to be next-generation commercial cells.
The study found that the main problem of lithium-sulfur cell is capacity attenuation at present.The reason of battery capacity decays has：(1) it wears
Shuttle effect.For battery in charging, the long-chain polysulfide root ion being dissolved in electrolyte can be gradually diffused into cathode, and be reduced into
Short chain polysulfide root ion, then diffusion mobility then is reduced into the more sulphur of long-chain to a part of short chain polysulfide root ion to anode again
Radical ion.Process so repeatedly is " shuttle effect "；(2) the polysulfide root ion for being diffused into cathode may further be gone back
Original is at two lithiums of lithium sulfide or vulcanization not readily dissolved.The loss of active material is not only caused in this way, and can prevent lithium ion
Conduction, battery polarization are serious；(3) the active material sulphur of battery or lithium sulfide are also battery capacity in the irreversible deposition of anode
One of the reason of decaying.
In conclusion the unordered diffusion of polysulfide is the basic reason of battery capacity decaying.To solve the above-mentioned problems,
People mainly study battery in terms of three.1), in terms of positive electrode, charcoal and sulphur are passed through into physical method or chemistry
Method carries out cladding mixing and polysulfide is prevented to be spread to cathode.2) it, in terms of electrolyte, is being electrolysed by reducing polysulfide
Dissolving diffusion in liquid.3), in terms of cathode, by additive in the electrolytic solution, it is made to form protective film in negative terminal surface
Method inhibits the shuttle effect of polysulfide.(the Pub.No. such as Yuriy V.Mikhaylik:US 2011/0059350Al) it proposes
Nitrate can inhibit the shuttle of polysulfide.Its mechanism of action is to form protective film in lithium piece negative terminal surface, is effectively improved
The coulombic efficiency of battery.And then improve the capacity stability of battery.Zhan Lin etc.
(Adv.Funct.Mater.2012.DOI:10.1002/adfm.201200696) propose five vulcanization of addition in the electrolytic solution
Phosphorus not only can form protective film in lithium piece negative terminal surface, and can dissolve the lithium sulfide of irreversible deposition, and stability test has one
It is fixed to improve, but phosphoric sulfide may also increase the dissolving of polysulfide " shuttle " effect of battery.Nearest L.F.Nazar etc.
[Energy Environ.Sci.DOI:10.1039/c4ee00372a]It is found that one kind to the almost totally insoluble liquid of polysulfide
Electrolyte.Although the discharge platform of battery is wanted than the electrolyte of common DME/DOL types, the capacity stability of battery
It is better than the latter.But article is added to a large amount of LiTFSI lithium salts in the electrolytic solution, and the price of battery will be significantly increased in this way, it is right
The commercialization of battery is unfavorable.
Invention content
The object of the present invention is to provide a kind of electrolyte solutions for lithium-sulfur cell.This electrolyte solution has resistance
Sulfur transfer, advantages, the embodiments specifically used such as good cycling stability, price be low are as follows：
Electrolyte solution forms：
(1) as the solute of electrolyte solution 1：A kind of or two kinds or more of surfactant；The surface-active
Agent concentration is 0.01-10 mol/Ls；
(2), as the solute of electrolyte solution 2：A kind of or two kinds or more of lithium salts；The lithium salt is 0.1-
10 mol/Ls；
(3), as the solvent of electrolyte solution：One kind in straight chain ether compound or two kinds or more.
The surfactant concentration is preferably 0.1-3 mol/Ls；
The lithium salt is preferably 0.2-3 mol/Ls.
One be also added in the solvent in the dioxane in ring-type ethers compound, dioxolanes, tetrahydrofuran
Kind or two kinds or more, with straight chain ether compound collectively as the solvent of electrolyte solution, ring-type ethers compound with it is straight
The volume ratio 1 of chain ether compound：20-20：1.
The surfactant can be with one kind of lower structure or two kinds or more：
Wherein M can be one kind or two kinds in H or F, m=2-20 positive integers, wherein it is preferred that m=6-14 positive integers.
Or
Wherein n=3-20 positive integers, wherein it is preferred that n=6-14 positive integers.
Or
Wherein N can be one kind or two kinds in H or F, p=2-20 positive integers, wherein it is preferred that p=6-14 positive integers.
Or
Wherein q=3-20 positive integers, wherein it is preferred that q=6-14 positive integers.
The lithium salts include it is following in one kind or two kinds or more：LiN(SO3CF3)2、LiN(SO3CF2CF3)2、
LiSO3CF3、LiBr、LiI、LiPF6,LiBOB；Wherein it is preferred that LiN (SO3CF3)2、LiSO3CF3, one kind in LiBOB or
Two kinds of person or more.
The structural formula of the straight chain ether compound is：
T=1-20 positive integers, wherein it is preferred that t=1-4 positive integers.
The surfactant that the electrolyte of the design of the present invention contains can be formed " micella " in the electrolytic solution, this " micella "
The diffusion of more lithium sulfides can be effectively controlled, the cyclical stability of battery is then improved.
Specific implementation mode
Below by embodiment, the present invention is further explained, rather than limits the present invention.
Surfactant used is for example lower shown.This is the citing of surfactant used, but not limited to this.
Embodiment 1
Electrolyte solution forms：Surfactant is surfactant (1) (as shown in Equation 1), and wherein m=8 is a concentration of
1mol/L；Lithium salts is LiN (SO3CF2CF3)2, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1), wherein t=4.
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Comparative example
Electrolyte solution forms：Lithium salts is LiN (SO3CF3)2, a concentration of 1mol/L；Solvent is solvent (5) (such as 1 institute of formula
Show), wherein t=4.
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 2
Electrolyte solution forms：Surfactant is surfactant (2) (as shown in Equation 1, wherein n=8), a concentration of
0.5mol/L；Lithium salts is LiSO3CF3, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=2) and dioxy penta
Ring, volume ratio 1:1.
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 3
Electrolyte solution forms：Surfactant is surfactant (3) (as shown in Equation 1, wherein p=6), a concentration of
0.5mol/L；Lithium salts is LiSO3CF3, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=4).
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 4
Electrolyte solution forms：Surfactant is surfactant (4) (as shown in Equation 1, wherein q=10), a concentration of
0.6mol/L；Lithium salts is LiSO3CF3, a concentration of 2mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=2) and tetrahydrochysene furan
It mutters, volume ratio 2：1.
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 5
Electrolyte solution forms：Surfactant is surfactant (1) (as shown in Equation 1, wherein m=10), a concentration of
0.6mol/L；Lithium salts is LiBOB, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=2).
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 6
Electrolyte solution forms：Surfactant is surfactant (2) (as shown in Equation 1, wherein n=12), a concentration of
1.2mol/L；Lithium salts is LiBOB, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=4).
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 7
Electrolyte solution forms：Surfactant is surfactant (3) (as shown in Equation 1, wherein p=10), a concentration of
0.5mol/L；Lithium salts is LiN (SO3CF3)2, a concentration of 2.5mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=4).
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 8
Electrolyte solution forms：Surfactant is surfactant (4) (as shown in Equation 1, wherein q=10), a concentration of
1.5mol/L；Lithium salts is LiN (SO3CF3)2, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=2) and two
Six ring of oxygen, volume ratio 1：1.
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 9
Electrolyte solution forms：Surfactant is surfactant (1) (as shown in Equation 1, wherein m=12), a concentration of
0.9mol/L；Lithium salts is LiN (SO3CF3)2, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=2) and two
Butyl oxide link, volume ratio 1：1.
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Embodiment 10
Electrolyte solution forms：Surfactant is surfactant (2) (as shown in Equation 1, wherein n=12), a concentration of
1.2mol/L；Lithium salts is LiN (SO3CF3)2, a concentration of 1mol/L；Solvent is solvent (5) (as shown in Equation 1, wherein t=6).
The cathode of lithium-sulfur cell is the lithium foil that thickness is 50 microns, and anode is prepared using following methods：30 mass fractions
The acrylonitrile-butadiene rubber latex blending of Super P charcoals, the elemental sulfur of 60 mass fractions, 10 mass fractions (solid content), is coated to aluminium foil
On.Sulfur content after drying in positive-active layer is 1.5 millis gram/cm.By above-mentioned component with anode/diaphragm/cathode
Layer structure fit together, and according to being sealed after 30 microlitres/positive area addition electrolyte every square centimeter.Static 5 is small
Shi Hou carries out battery charging and discharging with 0.1C, 1C respectively relative to the quality of positive active material sulphur.The blanking voltage of charging is
The blanking voltage of 2.8V, electric discharge are 1.5V.Carry out 100 cycles.Investigate the initial specific capacity of battery, 100 times cycle after specific capacity
And battery coulombic efficiency.Experimental result is as shown in table 1.
Table 1
The result shows that after the electrolyte of lithium-sulfur cell is added to surfactant, there is better capacity stability.Reason
The a large amount of micella for carrying negative electrical charge can be formed in the electrolytic solution for surfactant, then limit the expansion of more lithium sulfides
It dissipates, improves the cyclical stability of battery.
Claims (7)
1. a kind of application of electrolyte solution in lithium-sulfur cell, it is characterised in that：
Electrolyte solution forms：
(1) as the solute of electrolyte solution 1：A kind of or two kinds or more of surfactant；The surfactant is dense
Degree is 0.01-10 mol/Ls；
(2), as the solute of electrolyte solution 2：A kind of or two kinds or more of lithium salts；The lithium salt rubs for 0.1-10
You/liter；
(3), as the solvent of electrolyte solution：One kind in straight chain ether compound or two kinds or more；
The surfactant can be with one kind of lower structure or two kinds or more：
Wherein M is one kind or two kinds in H or F, m=
2-20 positive integers；
Or
Wherein n=3-20 positive integers；
Or
Wherein N be H or F in one kind or two kinds,
P=2-20 positive integers；
Or
Wherein q=3-20 positive integers.
2. application described in accordance with the claim 1, it is characterised in that：
The surfactant concentration is 0.1-3 mol/Ls；
The lithium salt is 0.2-3 mol/Ls.
3. according to application as claimed in claim 1 or 2, it is characterised in that：
In the solvent also be added with ring-type ethers compound in dioxane, dioxolanes, one kind in tetrahydrofuran or
Two kinds of person or more, with straight chain ether compound collectively as the solvent of electrolyte solution, ring-type ethers compound and linear
The volume ratio 1 of class compound：20-20：1.
4. application described in accordance with the claim 1, it is characterised in that：
The lithium salts include it is following in one kind or two kinds or more：LiN(SO3CF3)2、LiN(SO3CF2CF3)2、
LiSO3CF3、LiBr、LiI、LiPF6、LiBOB。
5. application described in accordance with the claim 1, it is characterised in that：
The lithium salts includes LiN (SO3CF3)2、LiSO3CF3, one kind in LiBOB or two kinds or more.
6. application described in accordance with the claim 1, it is characterised in that：
The structural formula of the straight chain ether compound is：
T=1-20 positive integers.
7. application described in accordance with the claim 1, it is characterised in that：Wherein t=1-4 positive integers.
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| KR102050837B1 (en) | 2016-02-03 | 2019-12-03 | 주식회사 엘지화학 | Electrolyte for lithium-sulfur battery and lithium-sulfur battery comprising thereof |
| KR102101396B1 (en) * | 2016-12-09 | 2020-04-16 | 주식회사 엘지화학 | Nonaqueous liquid electrolyte and lithium secondary battery including the same |
| CN110501394B (en) * | 2019-07-23 | 2021-10-12 | 江苏大学 | Preparation of electrolytic solution and application of electrolytic solution in electrochemical rapid detection of content of sanshoamides |
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| CN102055018A (en) * | 2009-11-06 | 2011-05-11 | 通用汽车环球科技运作公司 | Electrolyte for a lithium ion battery |
| CN102610790A (en) * | 2012-03-31 | 2012-07-25 | 宁德新能源科技有限公司 | Lithium ion secondary battery and anode plate of lithium ion secondary battery |
| CN103855425A (en) * | 2012-12-04 | 2014-06-11 | 中国科学院大连化学物理研究所 | Electrolyte solution of lithium-sulfur battery |
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| CN102055018A (en) * | 2009-11-06 | 2011-05-11 | 通用汽车环球科技运作公司 | Electrolyte for a lithium ion battery |
| CN102610790A (en) * | 2012-03-31 | 2012-07-25 | 宁德新能源科技有限公司 | Lithium ion secondary battery and anode plate of lithium ion secondary battery |
| CN103855425A (en) * | 2012-12-04 | 2014-06-11 | 中国科学院大连化学物理研究所 | Electrolyte solution of lithium-sulfur battery |
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