JPH07245126A - Recovery method of cobalt from used lithium secondary battery - Google Patents
Recovery method of cobalt from used lithium secondary batteryInfo
- Publication number
- JPH07245126A JPH07245126A JP3568994A JP3568994A JPH07245126A JP H07245126 A JPH07245126 A JP H07245126A JP 3568994 A JP3568994 A JP 3568994A JP 3568994 A JP3568994 A JP 3568994A JP H07245126 A JPH07245126 A JP H07245126A
- Authority
- JP
- Japan
- Prior art keywords
- sieving
- lithium secondary
- secondary battery
- cobalt
- magnetically
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 21
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 21
- 238000000034 method Methods 0.000 title claims abstract description 21
- 229910017052 cobalt Inorganic materials 0.000 title claims abstract description 19
- 239000010941 cobalt Substances 0.000 title claims abstract description 19
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 title claims abstract description 19
- 238000011084 recovery Methods 0.000 title claims 2
- 238000007873 sieving Methods 0.000 claims abstract description 17
- 239000000463 material Substances 0.000 claims description 9
- 239000002245 particle Substances 0.000 abstract description 9
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 abstract description 7
- 239000012634 fragment Substances 0.000 abstract description 4
- 229910052742 iron Inorganic materials 0.000 abstract description 4
- 229910052751 metal Inorganic materials 0.000 abstract description 4
- 239000002184 metal Substances 0.000 abstract description 4
- 230000002349 favourable effect Effects 0.000 abstract 2
- 239000012141 concentrate Substances 0.000 abstract 1
- 230000007423 decrease Effects 0.000 abstract 1
- 239000000126 substance Substances 0.000 description 5
- 229910052782 aluminium Inorganic materials 0.000 description 3
- 239000011230 binding agent Substances 0.000 description 3
- -1 cobalt Chemical class 0.000 description 3
- 239000012535 impurity Substances 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 239000000696 magnetic material Substances 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 235000008733 Citrus aurantifolia Nutrition 0.000 description 1
- 229910000863 Ferronickel Inorganic materials 0.000 description 1
- 229910003307 Ni-Cd Inorganic materials 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- 235000011941 Tilia x europaea Nutrition 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- CKFRRHLHAJZIIN-UHFFFAOYSA-N cobalt lithium Chemical compound [Li].[Co] CKFRRHLHAJZIIN-UHFFFAOYSA-N 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 239000004567 concrete Substances 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 238000007429 general method Methods 0.000 description 1
- 238000002386 leaching Methods 0.000 description 1
- 239000004571 lime Substances 0.000 description 1
- 238000007885 magnetic separation Methods 0.000 description 1
- 239000006148 magnetic separator Substances 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 239000007774 positive electrode material Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- HNJBEVLQSNELDL-UHFFFAOYSA-N pyrrolidin-2-one Chemical compound O=C1CCCN1 HNJBEVLQSNELDL-UHFFFAOYSA-N 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
- 239000002893 slag Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/54—Reclaiming serviceable parts of waste accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
-
- 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
-
- 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
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W30/00—Technologies for solid waste management
- Y02W30/50—Reuse, recycling or recovery technologies
- Y02W30/84—Recycling of batteries or fuel cells
Landscapes
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Secondary Cells (AREA)
- Processing Of Solid Wastes (AREA)
- Manufacture And Refinement Of Metals (AREA)
Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は、使用済みリチウム二次
電池から有価金属、特にコバルトを回収する方法に関す
る。FIELD OF THE INVENTION The present invention relates to a method for recovering valuable metals, particularly cobalt, from used lithium secondary batteries.
【０００２】[0002]
【従来の技術】リチウム電池は、軽量、高電気容量の電
池として知られている。この電池には、正極活物質とし
て有価金属であるコバルトを含むリチウムコバルト複合
酸化物が使用されているので、使用済みリチウム二次電
池からこのような有価物を回収することは、資源の有効
利用の観点から極めて重要である。2. Description of the Related Art Lithium batteries are known to be lightweight and have high electric capacity. Since this battery uses a lithium-cobalt composite oxide containing cobalt, which is a valuable metal, as the positive electrode active material, recovering such valuable materials from a used lithium secondary battery is an effective use of resources. Is extremely important from the perspective of.
【０００３】従来、使用済みリチウム二次電池から有価
物を回収する方法としては具体的な提案はない。ただ、
リチウム二次電池以外の一次電池や二次電池から有価物
を回収する方法はいくつか提案されているが、これらは
使用済みリチウム二次電池からコバルトを回収するのに
は適用できないものである。Conventionally, there is no concrete proposal as a method for recovering valuable materials from used lithium secondary batteries. However,
Although several methods of recovering valuable materials from primary batteries or secondary batteries other than lithium secondary batteries have been proposed, these are not applicable to recovering cobalt from used lithium secondary batteries.
【０００４】例えば、使用済みマンガン乾電池を処理す
る方法として、これを破砕後、石灰を添加して焙焼し、
焙焼残留物をふるい分けて、ふるい上を磁選するプロセ
スがあるが、使用済みリチウム二次電池をこのようなプ
ロセスで処理すると、破砕後の焙焼となるためコバルト
は酸化して非磁性となり回収できない。また、ふるい分
けにおいても、ふるい上を磁選する方法では、コバルト
はふるい下に分布してしまうので、この点でもこのプロ
セスは適用できない。For example, as a method for treating a used manganese dry battery, after crushing the manganese dry battery, lime is added and roasted,
There is a process of sieving the roasting residue and magnetically selecting it on the screen.However, if a used lithium secondary battery is treated by such a process, it will be roasted after crushing, and the cobalt will oxidize and become non-magnetic, and it will be recovered. Can not. Further, also in the sieving, cobalt is distributed under the sieving by the method of magnetic separation on the sieving, and this process cannot be applied in this respect as well.
【０００５】また、Ｎｉ−Ｃｄ電池を酸化焙焼してＣｄ
を揮発させたニッケル焼鉱を得てこれをフェロニッケル
用原料とするプロセスもあるが、使用済みリチウム二次
電池の場合は、焙焼しただけではＦｅ、Ａｌなどの不純
物が多量に残り、Ｃｏを濃縮できない。Ni-Cd batteries are oxidized and roasted to obtain Cd.
There is also a process of obtaining a nickel burned ore from which volatilized and using this as a raw material for ferronickel, but in the case of a used lithium secondary battery, only a large amount of impurities such as Fe and Al remain when burned, and Co Can not be concentrated.
【０００６】[0006]
【発明が解決しようとする課題】本発明の目的は、上記
の事情に鑑み、使用済みリチウム二次電池からコバルト
を濃縮回収する新規な方法を提供することにある。In view of the above circumstances, an object of the present invention is to provide a novel method for concentrating and recovering cobalt from a used lithium secondary battery.
【０００７】[0007]
【課題を解決するための手段】上記課題を達成するため
に、本発明は、使用済みリチウム二次電池を焙焼し、次
に粉砕した後、粉砕物をふるい分けし、ふるい下を磁力
選別することを特徴とする使用済みリチウム二次電池か
らのコバルトの回収方法にある。[Means for Solving the Problems] To achieve the above object, the present invention is to roast a used lithium secondary battery and then crush it, and then screen the crushed product and magnetically select the bottom of the screen. A method of recovering cobalt from a used lithium secondary battery, which is characterized in that
【０００８】また、前記ふるい分けは、４２０〜３３６
０μｍの目開きで行うことを特徴とする前記コバルトの
回収方法にある。また特に、前記ふるい分けは、４２０
〜３３６０μｍの目開きで行なった後、さらにそのふる
い下を１４９〜４２０μｍの目開きでふるい分けするこ
とを特徴とする前記コバルトの回収方法にある。Further, the sieving is performed in the range of 420 to 336.
The method for recovering cobalt is characterized in that it is carried out with an opening of 0 μm. In particular, the sieving is 420
The method for recovering cobalt is characterized in that after carrying out the opening of ˜3360 μm, the lower part of the sieve is further sieved with the opening of 149-420 μm.
【０００９】[0009]
【作用】本発明において、まず、使用済みリチウム二次
電池を焙焼する。この焙焼は、セパレーターに用いられ
る多孔質ポリプロピレン等、電解液成分である６フッ化
リン酸リチウム等、活物質の結着剤であるポリフッ化ビ
ニリデン等、活物質と結着剤の合剤であるＮ−メチル−
２−ピロリドン等の有機材料を分解、燃焼、または揮発
させて除去するために行う。焙焼温度は好ましくは３５
０℃以上、より好ましくは５００℃以上である。上限は
１０００℃で充分である。この焙焼においてはＣｏ等の
有価物は外装缶中に入っていて外装缶内は揮発した有機
物で還元性となるので酸化されない。In the present invention, first, the used lithium secondary battery is roasted. This roasting is a mixture of the active material and the binder, such as porous polypropylene used for the separator, lithium hexafluorophosphate as the electrolyte component, polyvinylidene fluoride as the binder for the active material, and the like. Some N-methyl-
It is performed to decompose, burn, or volatilize and remove an organic material such as 2-pyrrolidone. The roasting temperature is preferably 35
The temperature is 0 ° C or higher, more preferably 500 ° C or higher. An upper limit of 1000 ° C is sufficient. In this roasting, valuable substances such as Co are contained in the outer can, and the inside of the outer can is reduced by the volatilized organic substance, so that it is not oxidized.
【００１０】次に焙焼物を破砕、粉砕する。この粉砕は
前記焙焼により結着剤や溶剤が除去されて、非常に粉粒
になり易くなっている有価物とこの有価物より比較的破
砕され難い正極集電体として用いられるアルミニウム箔
等、負極集電体として用いられている銅ネット、銅箔等
や鉄製の円筒状外装缶とを次のふるい分けあるいは磁力
選別で分離し易くするためである。Next, the roasted product is crushed and crushed. In this pulverization, the binder and the solvent are removed by the roasting, and valuables that are very likely to be powder particles and aluminum foil used as a positive electrode current collector that is relatively less crushable than the valuables, This is because it is easy to separate the copper net, the copper foil or the like used as the negative electrode current collector and the cylindrical outer can made of iron by the following sieving or magnetic force selection.
【００１１】粉砕は、有価物がＪＩＳ−Ｚ−８８０１標
準ふるい３３６０μｍ未満の粒度となるように行うのが
好ましい。３３６０μｍより大きい粒度では次の磁力選
別の工程で得られる磁着物の有価金属品位が低下する。
破砕、粉砕には、周知の衝撃、摩擦、せん断、圧縮を単
独または組み合せて利用する破砕装置が適宜利用でき
る。The crushing is preferably carried out so that the valuable material has a particle size of less than 3360 μm according to JIS-Z-8801 standard sieve. If the particle size is larger than 3360 μm, the quality of valuable metal of the magnetic material obtained in the subsequent magnetic force selection step is deteriorated.
For crushing and crushing, well-known crushing devices that use impact, friction, shearing, and compression individually or in combination can be appropriately used.
【００１２】更に、粉砕物をふるい分けする。ふるい分
けの粒度は適宜選択するが、４２０μｍから３３６０μ
ｍの目開きが好ましい。この工程により、鉄製の円筒状
外装缶の破砕物がふるい上として取り除かれる。Further, the crushed product is screened. The particle size of sieving is appropriately selected, but 420 μm to 3360 μ
The aperture of m is preferable. By this step, the crushed material of the iron-made cylindrical outer can is removed as a sieve.
【００１３】次にふるい下を磁力選別し、有価物、特に
コバルトを磁着物として回収する。ふるい下を全量磁力
選別しても有価物を回収することができるが、磁力選別
の前に更にふるい分けを行なうと粒度の粗い有価物を早
期に回収することができ、磁力選別装置の規模を小さく
することができる。この後段のふるい分けの粒度は適宜
選択すればよいが、１４９μｍから４２０μｍが好まし
い。ふるい下は炭素などの不純物を含んでいるので磁力
選別して有価物、特にコバルトを磁着物として回収す
る。Next, the lower part of the sieve is magnetically selected to collect valuable substances, particularly cobalt as a magnetic substance. Valuable materials can be recovered even if the entire amount under the sieve is magnetically sorted, but if the sifting is further performed before the magnetic sorting, valuable materials with coarse grain size can be collected early, and the scale of the magnetic sorting apparatus is small. can do. The particle size of the latter sieving may be appropriately selected, but 149 μm to 420 μm is preferable. Since the bottom of the sieve contains impurities such as carbon, it is magnetically sorted to collect valuables, especially cobalt as a magnetic material.
【００１４】回収した有価物は、Ｃｏの他にＣｕ、Ｎ
ｉ、Ａｌなどを含んでいるが、そのまま電気炉で溶解
し、スラグを取り除いた後、酸浸出等の一般的な方法で
精錬できる。The valuable materials recovered are Cu, N, in addition to Co.
Although it contains i, Al, etc., it can be refined by a general method such as acid leaching after melting in an electric furnace as it is, removing slag.
【００１５】[0015]
【実施例】使用済みリチウム二次電池（直径１８ｍｍ、
長さ６５ｍｍ）３個を大気雰囲気のマッフル炉中にて７
００℃、２９分間の焙焼を行なった。次にこれらの焙焼
物をせん断破砕機の一種であるグッドカッター（（株）
氏家製作所製）で破砕、粉砕した。破砕、粉砕物をＪＩ
Ｓ−Ｚ−８８０１標準ふるい４２０μｍを用いてふるい
分けし、鉄製の外装缶の破片を取除いた。更にふるい下
は１４９μｍのふるいを用いてふるい分けし、ふるい下
をソレノイド式磁力選別機（（株）鷹羽科学工業製）に
て磁力選別した。磁力は９２０エルステッドに設定し
た。結果を表１に示す。[Example] Used lithium secondary battery (diameter 18 mm,
(Length 65 mm) 7 pieces in a muffle furnace in the atmosphere
Roasting was performed at 00 ° C. for 29 minutes. Next, these roasted products are Good Cutter (Co., Ltd.)
It was crushed and crushed by Ujiie Seisakusho. Crush and crush the JI
SZ-8801 standard sieve 420 μm was used for sieving to remove the fragments of the iron outer can. Further, the bottom of the sieve was sieved using a 149 μm sieve, and the bottom of the sieve was magnetically sorted by a solenoid type magnetic separator (manufactured by Takaha Kagaku Kogyo Co., Ltd.). The magnetic force was set to 920 Oersted. The results are shown in Table 1.
【００１６】[0016]
【表１】 [Table 1]
【００１７】表１から明らかなように、重量割合３０％
の磁着物に分布率６０％のＣｏが回収されている。さら
に１４９μｍ網上には、分布率３７．４％のＣｏが回収
されており、これらを合せると９７．４％のＣｏが回収
されている。As is clear from Table 1, the weight ratio is 30%.
Co having a distribution rate of 60% is recovered in the magnetic substance. Furthermore, Co having a distribution rate of 37.4% was recovered on the 149 μm net, and when these were combined, 97.4% of Co was recovered.
【００１８】[0018]
【発明の効果】本発明によれば、使用済みリチウム二次
電池から有価物であるコバルトを簡便に効率良く回収で
きる。また、コバルトは濃縮されているので、さらにこ
れを精錬する際にも不純物の影響が少ない。According to the present invention, valuable cobalt can be easily and efficiently recovered from a used lithium secondary battery. Further, since cobalt is concentrated, impurities are less affected when refining it.
Claims (3)
に粉砕した後、粉砕物をふるい分けし、ふるい下を磁力
選別することを特徴とする使用済みリチウム二次電池か
らのコバルトの回収方法。1. Recovery of cobalt from a used lithium secondary battery, characterized in that the used lithium secondary battery is roasted, then crushed, and then the crushed material is sieved and magnetically sorted under the sieve. Method.
ｍの目開きで行うことを特徴とする請求項１記載の使用
済みリチウム二次電池からのコバルトの回収方法。2. The sieving is performed in the range of 420 to 3360 μm.
The method for recovering cobalt from a used lithium secondary battery according to claim 1, wherein the method is performed with an opening of m.
ｍの目開きで行なった後、さらにそのふるい下を１４９
〜４２０μｍの目開きでふるい分けすることを特徴とす
る請求項１記載の使用済みリチウム二次電池からのコバ
ルトの回収方法。3. The sieving is performed in the range of 420 to 3360 μm.
After opening with m openings, 149 below the sieve.
The method for recovering cobalt from a used lithium secondary battery according to claim 1, wherein the method is sieving with a mesh size of ˜420 μm.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP03568994A JP3443446B2 (en) | 1994-03-07 | 1994-03-07 | Method for recovering cobalt from used lithium secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP03568994A JP3443446B2 (en) | 1994-03-07 | 1994-03-07 | Method for recovering cobalt from used lithium secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH07245126A true JPH07245126A (en) | 1995-09-19 |
| JP3443446B2 JP3443446B2 (en) | 2003-09-02 |
Family
ID=12448873
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP03568994A Expired - Lifetime JP3443446B2 (en) | 1994-03-07 | 1994-03-07 | Method for recovering cobalt from used lithium secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3443446B2 (en) |
Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH11185833A (en) * | 1997-12-25 | 1999-07-09 | Nippon Mining & Metals Co Ltd | Valuable material recovering method from used lithium battery |
| WO2004062023A1 (en) * | 2002-12-27 | 2004-07-22 | Mitsui Mining & Smelting Co., Ltd. | Method of recovering cobalt from lithium ion battery and cobalt recovering system |
| FR2868603A1 (en) * | 2004-04-06 | 2005-10-07 | Recupyl Sa Sa | METHOD FOR RECYCLING BATTERY MIXTURES AND BATTERIES BASED ON LITHIUM ANODE |
| JP2011124127A (en) * | 2009-12-11 | 2011-06-23 | Toyota Motor Corp | Method and device for recycling battery pack |
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