CN103413905A - High-voltage magnesium charge-discharge battery - Google Patents
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- CN103413905A CN103413905A CN2013102928848A CN201310292884A CN103413905A CN 103413905 A CN103413905 A CN 103413905A CN 2013102928848 A CN2013102928848 A CN 2013102928848A CN 201310292884 A CN201310292884 A CN 201310292884A CN 103413905 A CN103413905 A CN 103413905A
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Abstract
The invention belongs to the technical field of electrochemistry and particularly relates to a high-voltage magnesium charge-discharge battery. The high-voltage magnesium charge-discharge battery consists of a membrane, a cathode, an anode and an electrolyte, wherein the membrane is solid and lithium ions can pass through the membrane reversibly; the cathode is magnesium metal or magnesium alloy, the electrolyte which is in the side of the cathode is a common organic electrolyte, a polymer electrolyte, an ionic liquid electrolyte or a mixture thereof, the anode is a common anode material for a lithium ion battery, and the electrolyte which is in the side of the anode is an aqueous solution containing lithium salt or a hydrogel electrolyte. The magnesium charge-discharge battery can be used for solving the matching problem between the electrolyte and anode material of the existing magnesium charge-discharge battery and other problems, and has the advantages of high voltage and high energy density by compared with the traditional magnesium charge-discharge battery. The magnesium charge-discharge battery with high energy density can be used for storing and releasing electric power.
Description
Technical field
The invention belongs to technical field of electrochemistry, be specifically related to a kind of high-tension magnesium and discharge and recharge battery, the invention still further relates to the application that this magnesium discharges and recharges battery.
Background technology
Fossil energy day by day exhausted, environmental pollution is day by day serious, today of global warming, the energy and environment become the two large problems that the mankind pay close attention to day by day.In order to realize sustainable development, the development and utilization new forms of energy have become the grand strategy target of countries in the world.Wherein, electrochemical energy is because of its energy conversion efficiency and energy density is high, noise-less pollution, the advantage that can arbitrarily combine and move, and becomes one of most important research topic.Chemical power source has obtained exploitation at aspects such as high-tech device, green low-energy consumption transportation and regenerative resources.The energy density maximum of lithium battery, thereby be widely studied and applied (referring to: Wu Yuping, Dai Xiaobing, horse army flag, the pre-river of journey. " lithium ion battery---application and practice ". Beijing: Chemical Industry Press, 2004).Yet due to the height activity of lithium metal, the reliability of lithium battery and fail safe are difficult to be guaranteed, especially still there are many potential safety hazards in the large-sized power lithium secondary battery.And the lithium metal scarcity of resources, expensive.
Mg and Li have many similar quality, and the natural resources reserves of magnesium are abundant, and price is cheaper, environmentally safe, theoretical specific capacity more greatly 2205 mAh/g(referring to Shen Jian etc., chemical progress, 2010, the 22nd volume, the 515-521 page), magnesium metal is as negative pole, and surface does not produce dendrite, security performance is promoted greatly, so magnesium is considered to the negative material of very promising high energy density cells.Since proposition Novel magnesium secondary cell system Mg such as Israel scientist Aurbach in 2000 | 0.125M Mg (AlCl
2BuEt)
2/ THF | MgxMo
6S
8Since (referring to: Gregory T. D. etc., Nature, 2000, the 407th volume, the 724th page the-the 727th page), magnesium discharges and recharges battery and as the large capacity secondary battery system of a kind of cheapness, environmental friendliness and high safety performance, is subject to people and pays close attention to widely (referring to Feng Zhenzhen etc., Journal of The Electrochemical Society, 2006, the 153rd volume, the 689th page the-the 693rd page; NuLi Y. N. etc., Journal of the Physical Chemistry C,, the 113rd volume, the 12594th page-12597 pages in 2009).And the magnesium resource of China is very abundant, occupies first place in the world, has the advantage (referring to Shi Changxu etc., material Leader, calendar year 2001, the 15th volume, 5-6 page) that exploitation magnesium discharges and recharges the battery uniqueness.
The development that magnesium discharges and recharges battery still is subject to all many-sided restrictions: on the one hand, because magnesium is more active, in most electrolyte, all can form surface passivated membrane, cause magnesium ion to pass, thereby be difficult to carry out deposition and resolution, limited its electro-chemical activity.The simple ionization magnesium salts of tradition such as MgCl
2, Mg (ClO
4)
2, Mg (CF
3SO
3)
2Deng not realizing the reversible deposition of Mg again.RMgBr derivative series has become the main flow electrolyte of current Mg secondary cell research, but also exists electrochemical window narrower, to the problems such as corrosivity of collector (referring to John Muldoon etc., Energy & Environmental Science, 2012, the 5th volume, the 5941st page the-the 5950th page).On the other hand, the ionic radius of divalence magnesium ion is little, charge density is large, and solvation is strong, compares Li
+Embedding much more difficult, and Mg
2+In insert material, also not too easily move, the host material that can embed fast for magnesium ion is seldom (referring to E. Levi. etc., Chemistry of Material, 2010, the 22nd volume, the 860th the 868th page of Ye –), while magnesium positive electrode synthesis technique complexity, cost is higher, the magnesium positive electrode operating voltage of existing report (<2V) lower, specific energy is lower.
Summary of the invention
The object of the present invention is to provide a kind of high-tension magnesium to discharge and recharge battery, to overcome magnesium, discharge and recharge that battery operated voltage is low, energy density is low, find and the problems such as electrolyte that exploitation matches and positive electrode system difficulty, anodal production cost height.
High-tension magnesium provided by the invention discharges and recharges battery, by barrier film, negative pole (negative current collector), positive pole and electrolyte ingredient, wherein:
(1) described barrier film is that solid and lithium ion can reversiblely pass through;
(2) described negative pole is the alloy of magnesium metal or magnesium, and negative current collector is with regard to metallic copper, aluminium, silver or their alloy;
(3) electrolyte of negative side is to have the magnesium of reporting now to discharge and recharge cell electrolyte: the organic electrolyte of grignard reagent and derivative thereof, alkyl magnesium aluminum complex or organic boron-containing compound, polymer dielectric, inorganic full-solid electrolyte or ionic liquid electrolyte, or their mixture;
(4) the common positive electrode of described just very lithium ion battery;
(5) electrolyte of side of the positive electrode is the aqueous solution or the hydrogel electrolyte that contains lithium salts.
In the present invention, described barrier film comprises and contains the lithium inorganic oxide, contains lithium sulfide or contain the full solid state polymer electrolyte of lithium salts, or their mixture; The described lithium inorganic oxide that contains is LiTi
2(PO
4)
3, Li
4Ge
0.5V
0.5O
4, Li
4SiO
4, LiZr (PO
4)
2, LiB
2(PO
4)
3Or Li
2O-P
2O
5-B
2O
3Etc. ternary system, or these contain the alloy of lithium inorganic oxide; The described lithium sulfide that contains is Li
2S-GeS
2-SiS
2Or Li
3PO
4-GeS
2-SiS
2Etc. ternary system, or these contain the alloy of lithium sulfide; The described full solid state polymer electrolyte that contains lithium salts is the polyethylene glycol oxide that contains lithium salts, contain the Kynoar of lithium salts or contain the siloxanes single-ion polymer electrolyte of lithium salts, or partly or entirely fluorine replace contain lithium salts olefines single-ion polymer electrolyte.
In the present invention, the alloy of described magnesium comprises alloy or its modifier that magnesium and other metal form.
In the present invention, described organic electrolyte is for to discharge and recharge in battery electrolyte at magnesium the solution that is dissolved with lithium salts, and wherein, described lithium salts comprises LiBr, LiCl, LiPF
6, LiClO
4, LiBOB, LiDFBO or LiTFSI, or several mixture wherein, the solvent of organic electrolyte comprises the ether solvents such as oxolane or ether.
Described polymer dielectric is poly(ethylene oxide) (PEO), polyacrylonitrile (PNA), propene carbonate (PC), ethylene carbonate (EC), polyvinyl alcohol (PVA) or the Kynoar (PVDF) that contains lithium salts or magnesium salts, or is wherein several mixtures; The inorganic full-solid electrolyte is lithium ion conductor or magnesium ion conductor, as magnesium base montmorillonite solid electrolytes, phosphate base solid electrolyte series.
In the present invention, described ionic liquid electrolyte comprises and contains BF
4 -Or CF
3SO
3 -Anionoid or contain imidazoles, piperidines, pyroles, quaternary ammonium, the cationic ionic liquid of amide-type.
In the present invention, described common positive electrode comprises, comprises LiMn
2O
4, LiCoO
2, LiNiO
2, LiFePO
4, Li[Ni
1/3Co
1/3Mn
1/3] O
2, V
2O
5, MoO
3Perhaps their mixture, alloy, coating.
In the present invention, the described aqueous solution or the hydrogel electrolyte that contains lithium salts, comprise the aqueous solution or the hydrogel electrolyte that are dissolved with inorganic lithium salt or organic lithium salt; Described inorganic lithium salt comprises halide, sulfide, sulfate, nitrate or the carbonate of lithium metal; Described organic lithium salt comprises carboxylate, sulfonate or their mixture of lithium.
High-tension magnesium provided by the invention discharges and recharges battery, its structural representation such as Fig. 1.This high-tension magnesium discharges and recharges battery and adopts the matrix of metallic copper as the reversible deposition/stripping of magnesium, and reversible deposition/stripping occurs magnesium in RMgBr.
Organic electrolyte in negative pole one side is that ether solvent is dissolved with lithium salts, grignard reagent or derivatives thereof, also can be polymer dielectric or the ionic liquid electrolyte that contains lithium salts and magnesium salts; In an anodal side, common anode material for lithium-ion batteries is highly stable in water solution system (to be seen: Y.P. Wu etc., CIMTEC 2010 5th Forum on New Materials collections of thesis, 13-18 day in June, 2010, Italy, FD-1:IL12), reversible lithium ion can occur embed/deviate from reaction.The magnesium formed discharges and recharges battery and has high discharge voltage; In addition, solid membrane is all highly stable at water and organic phase, the migration of water to negative pole avoided in its use, also prevent simultaneously the migration to side of the positive electrode of the electrolyte of negative side or solvent, on the other hand, solid membrane separates the negative pole organic bath from positive pole, this design has solved the magnesium such as grignard reagent and discharged and recharged the problems such as the cell electrolyte electrochemical window is lower; Therefore, this magnesium discharge and recharge battery energy density discloseder magnesium discharge and recharge battery and have the advantage that energy density is high.
The present invention also provides this high-tension magnesium to discharge and recharge the application of battery aspect electric power storage and release.
The accompanying drawing explanation
Fig. 1 is that high-tension magnesium prepared by the present invention discharges and recharges the battery structure schematic diagram.
The performance of Fig. 2 embodiment 3 batteries.Wherein, (a) cyclic voltammetry curve under 0.05 mV/s sweep speed, (b) the first charge-discharge curve under 30 mA/g current densities.
Embodiment
Below will be described in more detail by embodiment and Comparative Examples, but protection scope of the present invention is not limited to these embodiment.
Comparative Examples 1:
The magnesium metal of take is negative electrode active material, and reversible capacity is the Mo of 128 mAh/g
3S
4For positive active material (referring to Gregory T. D. etc., Nature, 2000, the 407th volume, the 724th page the-the 727th page), the acetylene black of take is solvent as conductive agent, Kynoar as adhesive, N-methyl-pyrrolidones, after stirring into uniform slurry, be coated in equably stainless steel foil online, make anode pole piece.By after cathode pole piece and anode pole piece vacuumize, the perforated membrane of glass mat of take is barrier film, and electrolyte is THF and magnesium salts Mg (AlCl
2BuEt)
2Mixture, button battery, then vacuumize are made in sealing.Obtain take magnesium and be negative pole, Mo
3S
4For anodal magnesium discharges and recharges battery.Electric current with 0.1C is tested, and is charged as first with 0.1C and carries out constant current, is charged to 2V and changes constant voltage later into, when electric current is 0.01C, stops charging process; Discharging current is 0.1C, and final voltage is 0.2V.According to test result, the energy density that obtains average discharge volt and obtain according to the active material weight of electrode.For the purpose of more convenient, these data are summarized in table 1.
Embodiment 1:
The metal platinum of take is negative current collector, and reversible capacity is the LiCoO of 145 mAh/g
2For anodal active material, wherein the part by weight of conductive agent, adhesive, active material is 1:1:8, after stirring into uniform slurry, is coated on stainless (steel) wire, makes anode pole piece.The component of take is 19.75Li
2O-6.17Al
2O
3-37.04GeO
2-37.04P
2O
5The ceramic membrane of (for containing the lithium inorganic oxide) is barrier film, and negative side is the mixture for THF and grignard reagent EtMgBr and LiBr, and side of the positive electrode is the LiNO of 1 mol/L
3Solution.After sealing, obtain with LiCoO
2For magnesium anodal, that magnesium is negative pole discharges and recharges battery.With 0.1 mA/cm
2Electric current test, be charged as with 0.1 mA/cm
2Carry out constant current charge, be charged to 3.6V; Discharging current is 0.1 mA/cm
2, final voltage is 2.8 V.According to test result, the energy density that obtains equally average discharge volt and obtain according to the active material weight of electrode.For the purpose of more convenient, these data also are summarized in table 1.
Embodiment 2:
The argent of take is negative current collector, and reversible capacity is the LiMn of 115 mAh/g
2O
4For anodal active material, the ratio of its conductive agent, adhesive, active material is identical with embodiment 1, after stirring into uniform slurry, is coated on stainless (steel) wire, makes anode pole piece.The all solid state film (as containing the full solid state polymer electrolyte of lithium salts) that the lithium salts of 8wt.% LiTFSI+5wt.% Nafion 117 (product of the du pont company)+87wt.% PEO of take forms is that barrier film, negative side are LiPF
6, PMMA, PC, EC, Mg (SO
3CF
3)
2Polymer dielectric, side of the positive electrode are the LiNO that is dissolved with 2 mol/l of 1 wt.% Lithium polyacrylate
3The aqueous solution.After sealing, obtain with LiMn
2O
4For magnesium anodal, that magnesium is negative pole discharges and recharges battery.Test condition is with embodiment 1.According to test result, the energy density that obtains equally average discharge volt and obtain according to the active material weight of electrode.For the purpose of more convenient, these data also are summarized in table 1.
Embodiment 3:
The metallic copper of take is negative current collector, and reversible capacity is the LiFePO of 140 mAh/g
4For anodal active material, its conductive agent, adhesive, solvent are identical with embodiment 1, after stirring into uniform slurry, are coated on stainless (steel) wire, make anode pole piece.The component of take is 0.75Li
2O-0.3Al
2O
3-0.2SiO
2-0.4P
2O
5-0.1TiO
2The ceramic membrane of (for containing the lithium inorganic oxide) is barrier film, and negative side is the mixture of THF and grignard reagent and LiBr, and side of the positive electrode is the Li of 0.5 mol/L
2SO
4Aqueous electrolyte.After sealing, obtain with LiFePO
4For magnesium anodal, that magnesium is negative pole discharges and recharges battery.With 0.1 mA/cm
2Electric current test, be charged as with 0.1 mA/cm
2Carry out constant current charge, be charged to 3.5 V; Discharging current is 0.1 mA/cm
2, final voltage is 1.6V.According to test result, the energy density that obtains equally average discharge volt and obtain according to the active material weight of electrode.For the purpose of more convenient, these data also are summarized in table 1.Simultaneously, magnesium gained obtained with 0.05 mV/s sweep speed discharges and recharges battery and carries out cyclic voltammetry, and curve obtained is shown in accompanying drawing 2 (a), tests under 30 mA/g current densities, and the first charge-discharge curve of gained is shown in accompanying drawing 2 (b).
The energy density situation of the above-mentioned Comparative Examples of table 1 and embodiment (according to the Mass Calculation result out of electrode active material).
*: negative material is 1 mole of calculating by the magnesium amount.As can be seen from Table 1, the energy density of embodiment is obviously higher more than 100% than the energy density of the Comparative Examples that adopts same positive pole.
Claims (8)
1. a high-tension magnesium discharges and recharges battery, it is characterized in that: by barrier film, negative pole, positive pole and electrolyte ingredient, wherein:
(1) described barrier film is that solid and lithium ion can reversiblely pass through;
(2) described negative pole is the alloy of magnesium metal or magnesium, and negative current collector is metallic copper, aluminium or silver, or is their alloy;
(3) electrolyte of negative side is that magnesium discharges and recharges cell electrolyte: the organic electrolyte of grignard reagent and derivative thereof, alkyl magnesium aluminum complex or organic boron-containing compound, polymer dielectric, inorganic full-solid electrolyte or ionic liquid electrolyte, or their mixture;
(4) described just very lithium ion battery positive electrode commonly used;
(5) electrolyte of side of the positive electrode is the aqueous solution or the hydrogel electrolyte that contains lithium salts;
Wherein, described barrier film is to contain the lithium inorganic oxide, contain lithium sulfide or contain the full solid state polymer electrolyte of lithium salts, or is wherein several mixtures.
2. high-tension magnesium according to claim 1 discharges and recharges battery, it is characterized in that: the described lithium inorganic oxide that contains is LiTi
2(PO
4)
3, Li
4Ge
0.5V
0.5O
4, Li
4SiO
4, LiZr (PO
4)
2, LiB
2(PO
4)
3, Li
2O-P
2O
5-B
2O
3Ternary system, or these contain the alloy of lithium inorganic oxide; The described lithium sulfide that contains is Li
2S – GeS
2-SiS
2Or Li
3PO
4– GeS
2-SiS
2The ternary system formed, or these contain the alloy of lithium sulfide; The described full solid state polymer electrolyte that contains lithium salts is the polyethylene glycol oxide that contains lithium salts, contain the Kynoar of lithium salts or contain the siloxanes single-ion polymer electrolyte of lithium salts, or partly or entirely fluorine replace contain lithium salts olefines single-ion polymer electrolyte.
3. high-tension magnesium according to claim 1 and 2 discharges and recharges battery, it is characterized in that: described organic electrolyte is for to discharge and recharge in battery electrolyte at magnesium the solution that is dissolved with lithium salts, and wherein said lithium salts is LiBr, LiCl, LiPF
6, LiClO
4, LiBOB, LiDFBO or LiTFSI, or several mixture wherein, the solvent of solution is oxolane or ether ether solvent.
4. high-tension magnesium according to claim 1 and 2 discharges and recharges battery, it is characterized in that: described polymer dielectric is poly(ethylene oxide), polyacrylonitrile, propene carbonate, ethylene carbonate, polyvinyl alcohol or the Kynoar that contains lithium salts and magnesium salts, or is wherein several mixtures; The inorganic full-solid electrolyte is lithium ion conductor or magnesium ion conductor.
5. high-tension magnesium according to claim 1 and 2 discharges and recharges lithium battery, it is characterized in that: described ionic liquid electrolyte is for containing BF
4 -Or CF
3SO
3 -Anionoid or contain imidazoles, piperidines, pyroles, quaternary ammonium, the cationic ionic liquid of amide-type.
6. high-tension magnesium according to claim 1 and 2 discharges and recharges lithium battery, it is characterized in that: described positive electrode is LiMn
2O
4, LiCoO
2, LiNiO
2, LiFePO
4, Li[Ni
1/3Co
1/3Mn
1/3] O
2, V
2O
5Or MoO
3, or be wherein several mixture, alloy, coatings.
7. high-tension magnesium according to claim 1 and 2 discharges and recharges lithium battery, it is characterized in that: the described aqueous solution or the hydrogel electrolyte that contains lithium salts is the aqueous solution or the hydrogel electrolyte that is dissolved with inorganic lithium salt or organic lithium salt; Described inorganic lithium salt is halide, sulfide, sulfate, nitrate or the carbonate of lithium metal; Described organic lithium salt is carboxylate, sulfonate or their mixture of lithium.
8. according to the described high-tension magnesium of one of claim 1 ~ 7, discharge and recharge battery in the storage of electric power and the application aspect release.
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103872304A (en) * | 2014-03-18 | 2014-06-18 | 中国科学院化学研究所 | Novel magnesium secondary battery electrode material and application thereof |
| CN105655552A (en) * | 2016-01-07 | 2016-06-08 | 李震祺 | Magnesium ion battery and preparation method thereof |
| CN107665981A (en) * | 2016-07-29 | 2018-02-06 | 横店集团东磁股份有限公司 | A kind of battery and its assemble method using chloride ionic liquid as positive active material |
| CN108470940A (en) * | 2018-03-19 | 2018-08-31 | 上海交通大学 | A kind of full stress-strain Magnesium ion battery and preparation method thereof |
| CN109638257A (en) * | 2018-12-18 | 2019-04-16 | 中科廊坊过程工程研究院 | A kind of compound vanadic anhydride based material and its preparation method and application |
| CN110323412A (en) * | 2018-03-29 | 2019-10-11 | 丰田自动车株式会社 | Cathode and sulfide solid battery |
| CN110444814A (en) * | 2019-08-09 | 2019-11-12 | 南京工业大学 | Chargeable and dischargeable aqueous solution energy storage device |
| CN110760306A (en) * | 2018-07-27 | 2020-02-07 | Tcl集团股份有限公司 | Quantum dot purification method |
| CN113224387A (en) * | 2021-05-11 | 2021-08-06 | 河南大学 | Lithium-sulfur electrolyte added with Grignard reagent derivative, and preparation method and application thereof |
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Cited By (16)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103872304A (en) * | 2014-03-18 | 2014-06-18 | 中国科学院化学研究所 | Novel magnesium secondary battery electrode material and application thereof |
| CN103872304B (en) * | 2014-03-18 | 2017-02-15 | 中国科学院化学研究所 | Novel magnesium secondary battery electrode material and application thereof |
| CN105655552A (en) * | 2016-01-07 | 2016-06-08 | 李震祺 | Magnesium ion battery and preparation method thereof |
| CN105655552B (en) * | 2016-01-07 | 2018-01-12 | 李震祺 | A kind of Magnesium ion battery and preparation method thereof |
| CN107665981A (en) * | 2016-07-29 | 2018-02-06 | 横店集团东磁股份有限公司 | A kind of battery and its assemble method using chloride ionic liquid as positive active material |
| CN107665981B (en) * | 2016-07-29 | 2019-09-10 | 横店集团东磁股份有限公司 | It is a kind of using the ionic liquid containing chlorine as the battery of positive active material and its assemble method |
| CN108470940A (en) * | 2018-03-19 | 2018-08-31 | 上海交通大学 | A kind of full stress-strain Magnesium ion battery and preparation method thereof |
| CN108470940B (en) * | 2018-03-19 | 2021-01-01 | 上海交通大学 | All-organic magnesium ion battery and preparation method thereof |
| CN110323412A (en) * | 2018-03-29 | 2019-10-11 | 丰田自动车株式会社 | Cathode and sulfide solid battery |
| CN110323412B (en) * | 2018-03-29 | 2022-10-14 | 丰田自动车株式会社 | Negative electrode and sulfide solid-state battery |
| CN110760306A (en) * | 2018-07-27 | 2020-02-07 | Tcl集团股份有限公司 | Quantum dot purification method |
| CN110760306B (en) * | 2018-07-27 | 2021-11-23 | Tcl科技集团股份有限公司 | Quantum dot purification method |
| CN109638257A (en) * | 2018-12-18 | 2019-04-16 | 中科廊坊过程工程研究院 | A kind of compound vanadic anhydride based material and its preparation method and application |
| CN110444814A (en) * | 2019-08-09 | 2019-11-12 | 南京工业大学 | Chargeable and dischargeable aqueous solution energy storage device |
| CN113224387A (en) * | 2021-05-11 | 2021-08-06 | 河南大学 | Lithium-sulfur electrolyte added with Grignard reagent derivative, and preparation method and application thereof |
| CN113224387B (en) * | 2021-05-11 | 2022-05-10 | 河南大学 | Lithium-sulfur electrolyte added with Grignard reagent derivative, and preparation method and application thereof |
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