CN109830648A - A method of lithium dendrite growth is eliminated using Lorentz force - Google Patents
A method of lithium dendrite growth is eliminated using Lorentz force Download PDFInfo
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- CN109830648A CN109830648A CN201910028878.9A CN201910028878A CN109830648A CN 109830648 A CN109830648 A CN 109830648A CN 201910028878 A CN201910028878 A CN 201910028878A CN 109830648 A CN109830648 A CN 109830648A
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Abstract
The present invention discloses a kind of method for eliminating lithium dendrite growth using Lorentz force, and key step is as follows: using liquid electrolyte plastidome, the assembled battery in atmosphere of inert gases first；Secondly assembled battery is placed in inside magnetic field, inside battery electrode plane and magnetic induction line is made to keep angular range at 0-90 °；Then electrochemical property test is carried out at 0-1.5T in magnetic field strength range, collect, compare, analyze electrochemical data；Again, SEM characterization is carried out to the electrode surface after circulation, electrode Morphology is compared in observation；It finally chooses magnet and is placed in inside battery, assembled battery, chemical property is compared in analysis.Magnetic field is introduced directly into electrochemical process by the present invention, utilizes the Li of utilization+The Lorentz force being subject to eliminates Li+Aggregation depositional phenomenon at tip position, avoids the generation of dendrite.Using this method, the capacity and cyclical stability of battery are improved.
Description
Technical field
The present invention relates to lithium metal battery preparation technical fields, and in particular to one kind influences Li by Lorentz force+Movement,
And then the lithium metal battery technology of dendritic growth is eliminated, electrochemical process is influenced more particularly, to impressed field, is passed through
Regulate and control Li+Movement, promote the method for its deposition distribution more uniformization.
Background technique
In in the past few decades, based on the rechargeable battery of lithium ion in portable electronic product, electric car and intelligence
It can be flourished in power grid storage system[1].Theoretical specific volume highest (3860mAh g-1) and negative electricity chemical potential it is minimum (-
3.04V vs. standard hydrogen electrode) the characteristics of make Li become anode " Holy grail "[2].Lithium metal battery, such as Li-S and Li-O2Battery
It is considered as the candidate battery of next-generation high-energy density system.Although since the 1970s, lithium metal battery is ground
Study carefully work to have done very much, but the obstruction that its large-scale application is still out of control by dendritic growth.Leading to Li dendrite
In many reasons of problem, it is one of the main reasons that tip, which induces dendritic growth,.The internal field of protrusion tip is greater than smooth department
Internal field around point.The Li of aggregation+It can promote the growth of tip Li metal, so as to cause nonuniform deposition, form moss
Shape/dendroid Li.There has been proposed the strategies that many inhibition dendritic crystals are formed, structure design or surface including lithium anode
Processing[3], current collector construction or modification[4], modification diaphragm or insertion boundary layer[5], using high salt concentration electrolyte or add
Add agent[6], utilize solid electrolyte[7]And other methods.
Dendritic growth problem is induced for above-mentioned tip, magnetic field is introduced into electrochemical process by we, by utilizing Li+?
Generated Lorentz force is moved in magnetic field to control the distribution of lithium ion, eliminates the growth of tip dendrite.Firstly, the work pair
The mechanism that Lorentz force influences Li depositing behavior is speculated and has been analyzed.By adjusting current density and magnetic flux density, to it
Morphology and electrochemistry can be carried out monitoring, and discuss relationship between the two.Pass through founding mathematical models mould simultaneously
Intend depositing the pattern variation of Li, and further simulates the pattern variation of Li deposition with COMSOL.To verify stable magnetic field lithium
The practical application of metal anode, using permanent magnet assemble can be practical button cell.
Summary of the invention
It is a kind of raw using Lorentz force elimination Li dendrite the purpose of the invention is to overcome the deficiencies of the prior art and provide
Long method, by introducing magnetic field in electrochemical process, so that Li+Motion profile in coupled field is by Lorentz force
It acts on and deflects, avoid lithium metal from assembling in tip portion and deposit, and then the deposition distribution of uniformed metal lithium, to disappear
Except lithium dendrite growth.This method can be applied to lithium metal battery, promote the energy density and cyclical stability of battery.
To achieve the above object, the technical scheme adopted by the invention is as follows: it is a kind of using Lorentz force eliminate lithium dendrite growth
Method, comprise the following steps that
1) liquid electrolyte plastidome, the assembled battery in atmosphere of inert gases are used；
2) assembled battery is placed in inside magnetic field, inside battery electrode plane and magnetic induction line is made to keep angular range in 0-
90°；
3) electrochemical property test is carried out at 0-1.5T in magnetic field strength range, collect, compare, analyzing electrochemistry number
According to,；
4) SEM characterization is carried out to the electrode surface after circulation, electrode Morphology is compared in observation；
5) it chooses magnet and is placed in inside battery, assembled battery, chemical property is compared in analysis.
Atmosphere of inert gases is selected from argon atmosphere in the step 1), and water content is lower than 2ppm, and oxygen content is lower than 2ppm.
Electrolyte system is organic system electrolyte or solid electrolyte in the step 1).
Assembled battery is Symmetrical cells or full battery in the step 2).
Magnetic field is the magnetic field that permanent magnet generates or the magnetic field that electromagnet generates in the step 3).
Electrochemical property test includes but is not limited to cycle charge-discharge, the test of electrochemical impedance spectrogram in the step 5).
The utility model has the advantages that magnetic field is introduced directly into electrochemical process using this method, the Li of utilization is utilized+The Lorentz being subject to
Power eliminates Li+Aggregation depositional phenomenon at tip position, avoids the generation of dendrite.Using this method, the capacity of battery and
Cyclical stability is improved, specific as follows:
1, magnetic field is introduced directly into electrochemical process using this method, utilizes the Li of utilization+The Lorentz force being subject to is eliminated
Li+Aggregation depositional phenomenon at tip position, avoids the generation of dendrite.Utilize this method, the capacity and stable circulation of battery
Property is improved.
2, using this method, the roughness of lithium anode surface is reduced, alleviates electrode volume fluctuation, stabilizes solid electricity
Solve matter between phase (SEI), improve coulombic efficiency (CE), extend battery cycle life, effectively prevent dendrite pierce through battery every
Film causes short circuit, improves safety.
3, the present invention innovatively proposes that electrochemical process is regulated and controled and optimized in the way of additional physical field, nothing
Other any chemical substances need to be introduced into electrochemical system or are additionally provided energy to the system, and the physical field can be with
Evade the limitation of the conditions such as electrolyte system, electrode material type, battery types, there is great universality, can be extended to
Various electrochemical systems provide new thinking to obtain high-energy-density metal battery system.
Detailed description of the invention
Fig. 1 is the schematic diagram that 1 battery of embodiment is tested in magnetic field:
A is the schematic diagram of button cell cycle charge-discharge in magnetic field；
B is the pictorial diagram of button cell cycle charge-discharge in magnetic field.
Fig. 2 is that the influence that embodiment 1 is added with/without magnetic field to lithium metal deposition morphology compares:
A is the pattern that under no magnetic fields, lithium metal is deposited；
B is lithium metal deposition morphology after introducing magnetic field.
Fig. 3 is influence of the embodiment 1 with/without magnetic field addition to battery coulombic efficiency:
A is that current density is 0.25mh cm-2Circulation volume is 0.5mAh cm-2When, with/without the coulomb under magnetic field condition
Efficiency comparative；
B is that current density is 0.25mh cm-2Circulation volume is 1mAh cm-2When, with/without the coulomb effect under magnetic field condition
Rate comparison.
Specific embodiment
Further illustrate the present invention with reference to the accompanying drawings and examples, but the scope of protection of present invention is not limited to
In the range of embodiment statement.
Embodiment 1
1) 1,3- dioxolanes (DOL)+glycol dinitrate is dissolved in using 1M bis trifluoromethyl sulfimide lithium (LiTFSI)
Ether (DME) (1:1) is used as electrolyte, assembles Li | Li Symmetrical cells；
2) assembled Symmetrical cells are placed in inside electromagnet, keep electrode and magnetic direction angle is 90 °, such as Fig. 1
It is shown；
3) size by adjusting electromagnet input current regulates and controls magnetic field strength, adjusts magnetic field strength to B=
50mT；
4) charge-discharge test is carried out to battery using blue electric tester, sets circulating battery capacity as 3mAh cm-2, electric current
Size is 50mA cm-2, Symmetrical cells loop test is carried out, chemical property is compared in analysis；
5) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.As seen in Figure 2, under no magnetic fields, the pattern of lithium metal deposition is pellet shapes,
After introducing magnetic field, lithium metal deposition morphology is strip.It as seen in Figure 3, is 0.25mA cm in current density-2,
Capacity is respectively 0.5mAh cm-2And 1mAh cm-2Under the conditions of, the addition in magnetic field can all be obviously improved lithium metal deposition/dissolution
Coulombic efficiency.After magnetic field is added, the coulomb of battery is in 0.25mA cm-2-0.5mAh cm-2And 0.25 mA cm-2-1mAh
cm-2Coulombic efficiency under test condition, which has, to be obviously improved.
Embodiment 2
1) 1M lithium hexafluoro phosphate (LiPF is used6) in ethylene carbonate (EC)+diethyl carbonate (DEC) (1:1) conduct electricity
Liquid is solved, Li is assembled | Li Symmetrical cells；
2) assembled Symmetrical cells are placed in inside electromagnet, keep electrode and magnetic direction in 90 ° vertical；
3) size by adjusting electromagnet input current regulates and controls magnetic field strength, adjusts magnetic field strength to B=
50mT；
4) charge-discharge test is carried out to battery using blue electric tester, sets circulating battery capacity as 3mAh cm-2, electric current
Size is 50mA cm-2, Symmetrical cells loop test is carried out, chemical property is compared in analysis；
5) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
Embodiment 3
1) electrolyte is used as using 1M LiTFSI in DOL/DME (1:1), assembles Li | Li Symmetrical cells；
2) assembled Symmetrical cells are placed in inside electromagnet, keep electrode and magnetic direction in 90 °；
3) size by adjusting electromagnet input current regulates and controls magnetic field strength, adjusts magnetic field strength to B=
25mT；
4) charge-discharge test is carried out to battery using blue electric tester, sets circulating battery capacity as 3mAh cm-2, electric current
Size is 25mA cm-2, Symmetrical cells loop test is carried out, chemical property is compared in analysis；
5) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
Embodiment 4
1) 1M LiPF is used6In EC/DEC (1:1) is used as electrolyte, assembles Li | Li Symmetrical cells；
2) assembled Symmetrical cells are placed in inside electromagnet, keep electrode and magnetic direction at 0 °；
3) size by adjusting electromagnet input current regulates and controls magnetic field strength, adjusts magnetic field strength to B=
0mT；
4) charge-discharge test is carried out to battery using blue electric tester, sets circulating battery capacity as 3mAh cm-2, electric current
Size is 15mA cm-2, Symmetrical cells loop test is carried out, chemical property is compared in analysis；
5) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
Embodiment 5
1) 1M LiPF is used6In EC/DEC (1:1) is used as electrolyte, assembles Li | Li Symmetrical cells；
2) assembled Symmetrical cells are placed in inside electromagnet, keep electrode and magnetic direction at 30 °；
3) size by adjusting electromagnet input current regulates and controls magnetic field strength, adjusts magnetic field strength to B=
1.5T；
4) charge-discharge test is carried out to battery using blue electric tester, sets circulating battery capacity as 3mAh cm-2, electric current
Size is 25mA cm-2, Symmetrical cells loop test is carried out, chemical property is compared in analysis；
5) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
Embodiment 6
1) electrolyte is used as using 1M LiTFSI in DOL/DME (1:1), assembles Li | Li Symmetrical cells；
2) assembled Symmetrical cells are placed in inside electromagnet, keep electrode and magnetic direction at 60 °；
3) size by adjusting electromagnet input current regulates and controls magnetic field strength, adjusts magnetic field strength to B=
25mT；
4) charge-discharge test is carried out to battery using blue electric tester, sets circulating battery capacity as 3mAh cm-2, electric current
Size is 25mA cm-2, Symmetrical cells loop test is carried out, chemical property is compared in analysis；
5) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
Embodiment 7
1) solid electrolyte is used as using the polyethylene glycol oxide (PEO) that LiTFSI is added, assembles Li | Li Symmetrical cells；
2) assembled Symmetrical cells are placed in inside electromagnet, keep electrode and magnetic direction at 30 °；
3) size by adjusting electromagnet input current regulates and controls magnetic field strength, adjusts magnetic field strength to B=30m
T；
4) charge-discharge test is carried out to battery using blue electric tester, sets circulating battery capacity as 0.5mAh cm-2, electricity
Stream size is 0.5mA cm-2, Symmetrical cells loop test is carried out, chemical property is compared in analysis；
5) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
Embodiment 8
1) 1M LiPF is used6In EC/DEC (1:1) is used as electrolyte, replaces gasket, assembling using disc-shaped permanent magnet
Li | Li Symmetrical cells and Li | LiFePO4Full battery；
2) using blue electric tester to Li | Li Symmetrical cells carry out charge-discharge test, set circulating battery capacity as 1mAh
cm-2, size of current 0.25mAcm-2；To Li | LiFePO4Full battery carries out charge and discharge cycles test, and electrochemistry is compared in analysis
Energy；
3) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
Embodiment 9
1) 1M LiPF is used6In EC/DEC (1:1) is used as electrolyte, replaces gasket, assembling using circular permanent magnet
Li | Li Symmetrical cells and Li | LiFePO4Full battery；
2) using blue electric tester to Li | Li Symmetrical cells carry out charge-discharge test, set circulating battery capacity as 1mAh
cm-2, size of current is 0.25mA cm-2；To Li | LiFePO4Full battery carries out charge and discharge cycles test, and electrochemistry is compared in analysis
Performance；
3) battery after circulation is dismantled in glove box, after cleaning to electrode, utilizes scanning electron microscopy
Mirror observes electrode surface.
The present invention eliminates Li by introducing magnetic field, using Lorentz force+Tip assemble depositional phenomenon, to eliminate metal
The method of lithium dendrite growth.This method is easy flexibly, strong operability, the intensity and electricity in the magnetic field that can be introduced by regulation
Pond operating current size carrys out comprehensive regulation magnetic field effect.The introducing in magnetic field can effectively promote the coulombic efficiency of battery, avoid electricity
The generation of pole surface dendrite makes the cyclical stability of battery be increased dramatically.
Bibliography
[1]M.Armand,J.-M.Tarascon,Building better batteries.Nature 451,652-
657(2008).
[2]J.-M.Tarascon,M.Armand,Issues and challenges facing rechargeable
lithium batteries. Nature 414,359-367(2001).
[3]D.Lin,Y.Liu,Z.Liang,H.W.Lee,J.Sun,H.Wang,K.Yan,J.Xie,Y.Cui,Layered
reduced graphene oxide with nanoscale interlayer gaps as a stable host for
lithium metal anodes.Nat.Nanotechnol.11,626-632(2016).
[4]C.Yang,Y.Yao,S.He,H.Xie,E.Hitz,L.Hu,Ultrafine Silver Nanoparticles
for Seeded Lithium Deposition toward Stable Lithium Metal Anode.Adv.Mater.29,
1702714(2017).
[5]K.Liu,D.Zhuo,H.W.Lee,W.Liu,D.Lin,Y.Lu,Y.Cui,Extending the life of
lithium-based rechargeable batteries by reaction of lithium dendrites with a
novel silica nanoparticle sandwiched separator.Adv.Mater.29,1603987(2017).
[6]F.Ding,W.Xu,G.L.Graff,J.Zhang,M.L.Sushko,X.Chen,Y.Shao,
M.H.Engelhard, Z.Nie,J.Xiao,X.Liu,P.V.Sushko,J.Liu,J.Zhang,Dendrite-free
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mechanism.J.Am.Chem.Soc.135,4450-4456(2013).
[7]Y.Lu,Z.Tu,L.A.Archer,Stable lithium electrodeposition in liquid
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Claims (6)
1. a kind of method for eliminating lithium dendrite growth using Lorentz force, which is characterized in that comprise the following steps that
1) liquid electrolyte plastidome, the assembled battery in atmosphere of inert gases are used；
2) assembled battery is placed in inside magnetic field, inside battery electrode plane and magnetic induction line is made to keep angular range at 0-90 °；
3) electrochemical property test is carried out at 0-1.5T in magnetic field strength range, collect, compare, analyze electrochemical data；
4) SEM characterization is carried out to the electrode surface after circulation, electrode Morphology is compared in observation；
5) it chooses magnet and is placed in inside battery, assembled battery, chemical property is compared in analysis.
2. a kind of method for eliminating lithium dendrite growth using Lorentz force according to claim 1, which is characterized in that described
Atmosphere of inert gases is selected from argon atmosphere in step 1), and water content is lower than 2ppm, and oxygen content is lower than 2ppm.
3. a kind of method for eliminating lithium dendrite growth using Lorentz force according to claim 1, which is characterized in that described
Electrolyte system is organic system electrolyte or solid electrolyte in step 1).
4. a kind of method for eliminating lithium dendrite growth using Lorentz force according to claim 1, which is characterized in that described
Assembled battery is Symmetrical cells or full battery in step 2).
5. a kind of method for eliminating lithium dendrite growth using Lorentz force according to claim 1, which is characterized in that described
Magnetic field is the magnetic field that permanent magnet generates or the magnetic field that electromagnet generates in step 3).
6. a kind of method for eliminating lithium dendrite growth using Lorentz force according to claim 1, which is characterized in that described
Electrochemical property test includes but is not limited to cycle charge-discharge, the test of electrochemical impedance spectrogram in step 5).
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110783645A (en) * | 2019-09-05 | 2020-02-11 | 浙江工业大学 | Method for improving charging efficiency of secondary battery |
| CN110783646A (en) * | 2019-09-05 | 2020-02-11 | 浙江工业大学 | Regulating and controlling method for lithium battery electrode |
| CN110797589A (en) * | 2019-09-05 | 2020-02-14 | 浙江工业大学 | Method for regulating and controlling battery electrolyte environment |
| CN114284530A (en) * | 2021-06-02 | 2022-04-05 | 北京化工大学 | Battery electrolyte self-driving system |
| CN114388909A (en) * | 2022-01-17 | 2022-04-22 | 东莞东阳光科研发有限公司 | Method for in-situ removing lithium dendrites on surfaces of positive and negative electrodes of lithium ion battery |
| WO2023123730A1 (en) * | 2021-12-28 | 2023-07-06 | 上海恩捷新材料科技有限公司 | Battery containing magnetic current collectors and preparation method therefor |
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| CN207490064U (en) * | 2017-12-08 | 2018-06-12 | 中国科学院过程工程研究所 | The metal secondary batteries that a kind of quickly-chargeable is generated without dendrite |
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| US20150147604A1 (en) * | 2013-11-27 | 2015-05-28 | Robert Bosch Gmbh | Method for reducing the dendritic metal deposition on an electrode and lithium-ion rechargeable battery which uses this method |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110783645A (en) * | 2019-09-05 | 2020-02-11 | 浙江工业大学 | Method for improving charging efficiency of secondary battery |
| CN110783646A (en) * | 2019-09-05 | 2020-02-11 | 浙江工业大学 | Regulating and controlling method for lithium battery electrode |
| CN110797589A (en) * | 2019-09-05 | 2020-02-14 | 浙江工业大学 | Method for regulating and controlling battery electrolyte environment |
| CN110783645B (en) * | 2019-09-05 | 2022-01-11 | 浙江工业大学 | Method for improving charging efficiency of secondary battery |
| CN110783646B (en) * | 2019-09-05 | 2022-05-03 | 浙江工业大学 | Regulating and controlling method for lithium battery electrode |
| CN114284530A (en) * | 2021-06-02 | 2022-04-05 | 北京化工大学 | Battery electrolyte self-driving system |
| WO2023123730A1 (en) * | 2021-12-28 | 2023-07-06 | 上海恩捷新材料科技有限公司 | Battery containing magnetic current collectors and preparation method therefor |
| CN114388909A (en) * | 2022-01-17 | 2022-04-22 | 东莞东阳光科研发有限公司 | Method for in-situ removing lithium dendrites on surfaces of positive and negative electrodes of lithium ion battery |
| CN114388909B (en) * | 2022-01-17 | 2024-05-14 | 东莞东阳光科研发有限公司 | Method for removing lithium dendrites on positive and negative electrode surfaces of lithium ion battery in situ |
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