KR100716199B1 - Waste lithium primary battery processing apparatus and method - Google Patents
Waste lithium primary battery processing apparatus and method Download PDFInfo
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- KR100716199B1 KR100716199B1 KR1020060056906A KR20060056906A KR100716199B1 KR 100716199 B1 KR100716199 B1 KR 100716199B1 KR 1020060056906 A KR1020060056906 A KR 1020060056906A KR 20060056906 A KR20060056906 A KR 20060056906A KR 100716199 B1 KR100716199 B1 KR 100716199B1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B02—CRUSHING, PULVERISING, OR DISINTEGRATING; PREPARATORY TREATMENT OF GRAIN FOR MILLING
- B02C—CRUSHING, PULVERISING, OR DISINTEGRATING IN GENERAL; MILLING GRAIN
- B02C23/00—Auxiliary methods or auxiliary devices or accessories specially adapted for crushing or disintegrating not provided for in preceding groups or not specially adapted to apparatus covered by a single preceding group
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B02—CRUSHING, PULVERISING, OR DISINTEGRATING; PREPARATORY TREATMENT OF GRAIN FOR MILLING
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Abstract
본 발명의 폐 리튬 일차전지의 재처리 장치 및 그 방법은 산용액을 이용한 습식처리방식으로 리튬을 안정화시킨 후, 물리적으로 재처리함으로써, 안전하면서도 저가로 폐 리튬 일차전지를 처리할 수 있는 장치 및 그 방법을 제공하는데 목적이 있다.Apparatus and method for reprocessing waste lithium primary battery of the present invention by stabilizing lithium by a wet treatment method using an acid solution, and physically reprocessing, a device that can safely and inexpensively process waste lithium primary battery The purpose is to provide a method.
본 발명의 폐 리튬 일차전지 재처리 장치는 산용액이 담긴 방전조; 방전된 폐 리튬 일차전지를 파쇄하기 위한 파쇄기; 및 상기 파쇄된 폐 리튬 일차전지에서 발생하는 유독가스를 제거하기 위한 가스세정기를 포함한다.The waste lithium primary battery reprocessing apparatus of the present invention includes a discharge tank containing an acid solution; A crusher for crushing the discharged spent lithium primary battery; And a gas cleaner for removing toxic gas generated from the crushed waste lithium primary battery.
리튬, 일차전지, 재처리, 습식, 산용액 Lithium, Primary Battery, Reprocessing, Wet, Acid Solution
Description
도 1은 본 발명에 따른 폐 리튬 일차전지 재처리 장치의 구성도,1 is a block diagram of a waste lithium primary battery reprocessing apparatus according to the present invention,
도 2는 본 발명에 따른 폐 리튬 일차전지 재처리 흐름도,2 is a waste lithium primary battery reprocessing flowchart according to the present invention,
도 3 및 도 4는 본 발명에 따른 폐 리튬 일차전지의 방전된 이미지.3 and 4 are discharged images of the spent lithium primary battery according to the present invention.
*도면의 주요 부분에 대한 설명** Description of the main parts of the drawings *
110: 이송밸트 120: 분쇄기110: transfer belt 120: grinder
130: 출구 140: 흡기관130: outlet 140: intake pipe
150: 가스세정기 160: 자력선별기 150: gas cleaner 160: magnetic separator
본 발명은 폐 리튬 일차전지를 재활용할 수 있는 장치 및 그 방법에 관한 것으로, 보다 자세하게는 황산 수용액을 이용한 습식방법으로 재처리하는 방법에 관 한 것이다. The present invention relates to an apparatus and method for recycling waste lithium primary batteries, and more particularly, to a method of reprocessing by a wet method using an aqueous sulfuric acid solution.
리튬 일차전지는 휴대용 손전등 및 손목시계 등에 널리 사용되고 있으며, 연간 250톤의 폐기물을 발생하고 있다. 그 구조는 금속리튬을 음극활물질로 사용하고 양극으로는 이산화망간, 염화티오닐, 불화흑연, 산화구리, 이산화황 등을 사용하고 전해액으로 유기용액을 사용하고 있으며, 집전체 및 용기 등은 니켈 금속과 스테인리스 스틸을 사용하고 있다. Lithium primary batteries are widely used in portable flashlights and watches, and generate 250 tons of waste per year. Its structure uses metal lithium as anode active material, manganese dioxide, thionyl chloride, graphite fluoride, copper oxide, sulfur dioxide, etc. as an anode, and organic solution as electrolyte, and nickel metal and stainless steel for current collector and container. I use steel.
국내의 경우, 사용된 폐 리튬 일차전지를 처리하기 위한 방법으로 전량을 매립하고 있다. 그러나, 실제 수거, 운반 및 처리과정에서 전지의 방전 여부를 확인하기 어렵기 때문에 충전된 상태의 전지가 매립되는데, 전지에 사용되는 유기용매는 상온에서 불꽃이 있으면 점화되고 320℃ 정도에서는 자연 발화하는 특성이 있고, 전지 내부에는 전체 리튬금속의 10%가 방전되지 않은 상태로 남아있어 대기 중 수분과 반응을 통하여 폭발을 일으킬 수 있다. 따라서, 화재나 폭발이 일차 발생하면 주변에 있는 방전된 전지에도 영향을 미쳐 연쇄 폭발 및 화재가 발생할 수 있어 최근 매립장에서도 반입을 기피하고 있다.In Korea, the entire amount is buried as a method for treating used waste lithium primary batteries. However, since it is difficult to check whether the battery is discharged during actual collection, transportation and processing, the charged battery is buried. The organic solvent used in the battery is ignited when there is a flame at room temperature and spontaneously ignites at 320 ° C. In the battery, 10% of the total lithium metal remains undischarged and may explode through reaction with moisture in the air. Therefore, when a fire or an explosion occurs first, it may affect discharged batteries in the surroundings, and thus a chain explosion and a fire may occur.
특히, DME, THF, PC 등의 유기용매와 양극으로 사용하고 있는 물질은 인체의 중추신경의 기능을 억제를 유발하는 매우 유독한 물질로서, 이러한 유해 유기성분을 포함하고 있는 전지를 매립하는 경우 전해액의 유출로 인한 인체 및 주변 환경의 심각한 오염이 발생할 수 있는 문제점이 있다.In particular, organic solvents such as DME, THF, PC, etc., and materials used as positive electrodes are very toxic substances that cause the central nervous system function of the human body to be suppressed, and when the battery containing such harmful organic components is embedded in the electrolyte There is a problem that can cause serious pollution of the human body and the surrounding environment due to the leakage of.
국외의 경우, 미국 캘리포니아 소재 Toxco사에서는 냉각-파쇄공정을 사용하고 있다. Internationally, Toxco, California, USA, uses a cold-crushing process.
먼저, 액체 아르곤 내에서 폐 리튬전지를 -195℃까지 냉동시킨 다음, NaOH 또는 Na2CO3 수용액에 넣은 뒤 전지 케이스를 부수면 리튬금속 조각들이 용액의 표면으로 떠오른다. 이때 열과 함께 발생하는 수소가스를 배출시키면 격렬한 폭발은 일어나지 않으면서 용액에 포함되어 있는 가성소다는 산성 전해액을 중화시키고 리튬은 반응하여 리튬수산화물, 리튬황화물, 리튬탄화물 등을 생성하고 폐리튬전지는 안정화된다. 그리고, 안정화된 폐리튬전지를 원하는 크기로 반복하여 분쇄한 뒤 스크랩 금속을 분리하고 용액으로부터 탄산리튬(Lithium Carbonate)을 회수한다. First, the lithium battery is frozen in liquid argon to -195 ℃, and then placed in an aqueous NaOH or Na 2 CO 3 solution, and when the battery case is broken, lithium metal fragments rise to the surface of the solution. At this time, when the hydrogen gas generated together with heat is discharged, the caustic soda contained in the solution neutralizes the acidic electrolyte solution, and lithium reacts to produce lithium hydroxide, lithium sulfide, lithium carbide, etc. do. Then, the stabilized waste lithium battery is repeatedly pulverized to a desired size, and then scrap metal is separated and lithium carbonate (Lithium Carbonate) is recovered from the solution.
뉴질랜드의 퍼시픽리튬사에서는 폐 리튬전지로부터 고순도 리튬염을 회수하는 프로세스를 개발중에 있다. 파쇄된 폐리튬전지를 물에서 용해시키면 수용성의 리튬염과 구리, 알루미늄, 코발트 등의 불순물들이 수 ppm에서 수백 ppm까지 공존하는데, 이들을 이온교환 멤브레인을 통하여 분리시키면, 음극실에는 수산화리튬만이 농축된다. 이 정제된 리튬수산화물 수용액으로부터 고순도 탄산리튬을 침전물로 회수하는 프로세스로서 1kg의 리튬을 제조하는데 13kW/h의 에너지가 소모된다.Pacific Lithium, New Zealand, is developing a process to recover high-purity lithium salts from spent lithium batteries. When the crushed waste lithium battery is dissolved in water, water-soluble lithium salts and impurities such as copper, aluminum, and cobalt coexist from several ppm to several hundred ppm. When these are separated through an ion exchange membrane, only lithium hydroxide is concentrated in the cathode chamber. do. Energy of 13 kW / h is consumed to produce 1 kg of lithium as a process for recovering high purity lithium carbonate as a precipitate from the purified aqueous lithium hydroxide solution.
그러나, 앞서 개시한 기술의 경우, 고가의 액체 아르곤 및 높은 에너지가 필요하기 때문에, 폐 리튬전지를 재처리하는데 소요되는 비용이 높아 경제성이 낮다는 단점이 있다. However, in the case of the above-described technology, since expensive liquid argon and high energy are required, the cost of reprocessing the waste lithium battery is high, resulting in low economic efficiency.
본 발명의 폐 리튬 일차전지의 재처리 장치 및 그 방법은 산용액을 이용한 습식처리방식으로 리튬을 안정화시킨 후, 물리적으로 재처리함으로써, 안전하면서도 저가로 폐 리튬 일차전지를 처리할 수 있는 장치 및 그 방법을 제공하는데 목적이 있다. Apparatus and method for reprocessing waste lithium primary battery of the present invention by stabilizing lithium by a wet treatment method using an acid solution, and physically reprocessing, a device that can safely and inexpensively process waste lithium primary battery The purpose is to provide a method.
본 발명의 폐 리튬 일차전지 재처리 장치는 산용액이 담긴 방전조; 방전된 폐 리튬 일차전지를 파쇄하기 위한 파쇄기; 및 상기 파쇄된 폐 리튬 일차전지에서 발생하는 유독가스를 제거하기 위한 가스세정기를 포함한다.The waste lithium primary battery reprocessing apparatus of the present invention includes a discharge tank containing an acid solution; A crusher for crushing the discharged spent lithium primary battery; And a gas cleaner for removing toxic gas generated from the crushed waste lithium primary battery.
본 발명의 폐 리튬 일차전지 재처리 방법은폐 리튬 일차전지를 산용액에 넣어 방전 및 부식시키는 단계; 상기 폐 리튬 일차전지를 파쇄하는 단계; 및 상기 파쇄하는 단계에서 발생하는 유해가스를 정화하는 단계를 포함한다. The waste lithium primary battery reprocessing method of the present invention comprises the steps of discharging and corroding the waste lithium primary battery in an acid solution; Crushing the waste lithium primary battery; And purifying the noxious gas generated in the crushing step.
이하 첨부된 도면을 참조하여 본 발명의 바람직한 실시예를 상세히 설명하기로 한다. 이에 앞서, 본 명세서 및 청구범위에 사용된 용어나 단어는 통상적이거나 사전적인 의미로 한정해서 해석되어서는 아니되며, 발명자는 그 자신의 발명을 가장 최선의 방법으로 설명하기 위해 용어의 개념을 적절하게 정의할 수 있다는 원칙에 입각하여 본 발명의 기술적 사상에 부합하는 의미와 개념으로 해석되어야만 한다. Hereinafter, exemplary embodiments of the present invention will be described in detail with reference to the accompanying drawings. Prior to this, terms or words used in the specification and claims should not be construed as having a conventional or dictionary meaning, and the inventors should properly explain the concept of terms in order to best explain their own invention. Based on the principle that can be defined, it should be interpreted as meaning and concept corresponding to the technical idea of the present invention.
따라서, 본 명세서에 기재된 실시예와 도면에 도시된 구성은 본 발명의 가장 바람직한 일 실시예에 불과할 뿐이고 본 발명의 기술적 사상을 모두 대변하는 것은 아니므로, 본 출원시점에 있어서 이들을 대체할 수 있는 다양한 균등물과 변형예들 이 있을 수 있음을 이해하여야 한다.Therefore, the embodiments described in the specification and the drawings shown in the drawings are only the most preferred embodiment of the present invention and do not represent all of the technical idea of the present invention, various modifications that can be replaced at the time of the present application It should be understood that there may be equivalents and variations.
도 1 및 도 2는 본 발명에 따른 폐 리튬 일차전지 재처리 장치의 구성도와 재처리 공정의 흐름도를 도시한 것이다.1 and 2 illustrate a configuration diagram and a flowchart of a reprocessing process of a waste lithium primary battery reprocessing apparatus according to the present invention.
먼저, 폐 리튬 일차전지의 해체공정은 전지를 포장하고 있는 케이스(ABS 수지), 리튬 전지에 붙어 있는 비닐 및 전선을 제거(S100)한 후, 산용액이 들어있는 방전조(도시안됨)에 투입시킨다(S200). First, the dismantling process of the spent lithium primary battery removes the case (ABS resin) that packs the battery, the vinyl and the electric wire attached to the lithium battery (S100), and then puts it in the discharge tank (not shown) containing the acid solution. (S200).
본 발명의 일실시예에 따른 산용액은 0.4 ~ 0.6몰의 황산 수용액을 사용하고, 폐전지를 포장하고 있는 금속 소재의 케이스는 도 3 및 도 4에서 도시된 바와 같이 방전조에 들어있는 산용액에 의하여 부식이 되는데, 그 반응식은 아래와 같다.Acid solution according to an embodiment of the present invention uses a sulfuric acid solution of 0.4 ~ 0.6 mol, the case of the metal material for packaging the waste battery by the acid solution contained in the discharge tank as shown in Figure 3 and 4 Corrosion, the reaction is as follows.
그리고, 음극으로 사용되는 염화티오닐의 경우 물과 반응하여 산성으로 변하기 때문에 케이스의 부식에 소모되는 황산을 보충해 줄 필요없이, 물만 보충하면 지속적인 재처리를 할 수 있다.In addition, in case of thionyl chloride used as a negative electrode, it reacts with water to change acid so that it is not necessary to replenish sulfuric acid consumed for corrosion of the case.
본 발명의 일실시예에 따르면, 황산의 농도를 달리하여 전지 케이스를 부식시키는 속도를 조절할 수 있다.According to one embodiment of the invention, by varying the concentration of sulfuric acid it is possible to control the rate of corrosion of the battery case.
부식이 지속적으로 진행되면, 산용액은 부식되어 약해진 케이스 틈에 유입되어 폐전지 내부에 있는 리튬과 반응하게 된다. 이때의 반응식은 아래와 같고, 반응시 기포발생과 함께 산용액의 색이 짙은 초록색으로 변하면서, 리튬은 점차 안정화 된다.As corrosion continues, acid solutions enter the weakened case openings and react with lithium inside the spent battery. At this time, the reaction formula is as follows, and the color of the acid solution is changed to dark green with bubble generation during the reaction, lithium is gradually stabilized.
본 발명에 따른 산용액은 0.4~0.6몰의 황산 수용액을 사용하여 리튬전지의 방전 및 스테인레스 케이스를 국부적으로 부식시켜 안정화하는데 사용한다.The acid solution according to the present invention is used to stabilize the discharge of the lithium battery and the local corrosion of the stainless case using 0.4 ~ 0.6 mol sulfuric acid aqueous solution.
방전조에서 산용액에 의하여 수일간 방전과 함께 부식되어 안정화된 전지를 건조시킨 다음 이송밸트(110)에 실어 파쇄기(120)로 이송하여 파쇄한다(S300). Drying the battery stabilized by corrosion with the discharge for several days by the acid solution in the discharge tank and then carried in the
파쇄과정에서 발생하는 황 가스 및 분진을 제거하기 위하여 파쇄기(120)와 파쇄된 폐전지가 배출되는 출구(130)에 집진기를 포함한 가스세정기(150)의 흡기관(140)을 연결하여 처리한다(S400).In order to remove sulfur gas and dust generated during the shredding process, the
파쇄물은 콘베어 벨트에 의하여 자력 선별기(160)를 거쳐 자성체와 비자성체로 분리됨으로써, 유가금속이 회수된다. The crushed matter is separated into a magnetic substance and a nonmagnetic substance through the magnetic separator by the
본 발명은 이상에서 살펴본 바와 같이 바람직한 실시예를 들어 도시하고 설명하였으나, 상기한 실시예에 한정되지 아니하며 본 발명의 정신을 벗어나지 않는 범위 내에서 당해 발명이 속하는 기술분야에서 통상의 지식을 가진 자에 의해 다양한 변경과 수정이 가능할 것이다.Although the present invention has been shown and described with reference to the preferred embodiments as described above, it is not limited to the above embodiments and those skilled in the art without departing from the spirit of the present invention. Various changes and modifications will be possible.
본 발명의 폐 리튬 일차전지 재처리 장치 및 그 방법은 황산용액을 사용하여 전지 케이스를 부식시킴으로써, 리튬금속과 H2O의 접촉에 따른 과열 및 폭발등을 예 방하여 리튬금속의 안정적인 반응을 유도할 수 있고, 음극으로 사용되는 염화티오닐의 경우 물과 반응하여 산성으로 변하기 때문에 케이스의 부식에 소모되는 황산을 계속 보충해 줄 필요없이, 물만 보충해주면 된다는 점에서 안전하면서도 저렴한 비용으로 폐 리튬 일차전지를 처리할 수 있는 현저하고도 유리한 효과가 있다. Waste lithium primary battery reprocessing apparatus and method of the present invention by using a sulfuric acid solution to corrode the battery case, preventing overheating and explosion due to the contact of lithium metal and H 2 O to induce a stable reaction of lithium metal In case of thionyl chloride, which is used as a negative electrode, it reacts with water and becomes acidic, so it is not necessary to continuously replenish sulfuric acid which is consumed in case corrosion. There is a remarkable and advantageous effect of treating a battery.
Claims (4)
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Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR100860972B1 (en) | 2008-01-30 | 2008-09-30 | 한국지질자원연구원 | Stable Disassembly of Waste Lithium-ion Secondary Battery |
| KR101077280B1 (en) | 2009-10-29 | 2011-10-27 | 허욱환 | Recycling apparatus and method of the waste lithium battery |
| KR101352638B1 (en) | 2012-02-08 | 2014-01-20 | 한국지질자원연구원 | Method for recovering metals from mixed waste batteries |
| KR20180084235A (en) | 2017-01-16 | 2018-07-25 | 라상원 | Apparatus for processing waste lithium battery |
| CN109904549A (en) * | 2019-03-28 | 2019-06-18 | 费晓平 | A safety dismantling device for waste lithium battery |
| KR102024688B1 (en) * | 2019-04-04 | 2019-09-24 | 주식회사 티엠프라자 | Wasted battery perforation device |
| CN112246835A (en) * | 2020-10-04 | 2021-01-22 | 湖南金源新材料股份有限公司 | A kind of dismantling and separating method of waste lithium ion battery |
| KR20220015564A (en) | 2020-07-31 | 2022-02-08 | 주식회사 셀젠 | Discharge apparatus for waste lithium batteries with ignition and explosion protection |
| KR20220028723A (en) | 2020-08-31 | 2022-03-08 | 주식회사 셀젠 | Automatic discharge apparatus for waste lithium batteries with ignition and explosion protection |
| CN114618864A (en) * | 2022-02-25 | 2022-06-14 | 江西环锂新能源科技有限公司 | Process for extracting lithium salt from waste lithium battery |
| CN115608493A (en) * | 2022-06-16 | 2023-01-17 | 江西铭鑫环保设备有限公司 | Complete equipment for charged crushing and sorting of waste lithium batteries |
| KR20230110876A (en) | 2022-01-17 | 2023-07-25 | 재단법인 포항금속소재산업진흥원 | Discharge apparatus for waste battery capable of automatically adjusting concentration and temperature of salt water |
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| JPS61488A (en) | 1984-06-11 | 1986-01-06 | Kazuo Hamaoka | Apparatus for treating waste dry battery |
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| JPS61488A (en) | 1984-06-11 | 1986-01-06 | Kazuo Hamaoka | Apparatus for treating waste dry battery |
Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR100860972B1 (en) | 2008-01-30 | 2008-09-30 | 한국지질자원연구원 | Stable Disassembly of Waste Lithium-ion Secondary Battery |
| KR101077280B1 (en) | 2009-10-29 | 2011-10-27 | 허욱환 | Recycling apparatus and method of the waste lithium battery |
| KR101352638B1 (en) | 2012-02-08 | 2014-01-20 | 한국지질자원연구원 | Method for recovering metals from mixed waste batteries |
| KR20180084235A (en) | 2017-01-16 | 2018-07-25 | 라상원 | Apparatus for processing waste lithium battery |
| CN109904549A (en) * | 2019-03-28 | 2019-06-18 | 费晓平 | A safety dismantling device for waste lithium battery |
| KR102024688B1 (en) * | 2019-04-04 | 2019-09-24 | 주식회사 티엠프라자 | Wasted battery perforation device |
| KR20220015564A (en) | 2020-07-31 | 2022-02-08 | 주식회사 셀젠 | Discharge apparatus for waste lithium batteries with ignition and explosion protection |
| KR20220028723A (en) | 2020-08-31 | 2022-03-08 | 주식회사 셀젠 | Automatic discharge apparatus for waste lithium batteries with ignition and explosion protection |
| CN112246835A (en) * | 2020-10-04 | 2021-01-22 | 湖南金源新材料股份有限公司 | A kind of dismantling and separating method of waste lithium ion battery |
| KR20230110876A (en) | 2022-01-17 | 2023-07-25 | 재단법인 포항금속소재산업진흥원 | Discharge apparatus for waste battery capable of automatically adjusting concentration and temperature of salt water |
| CN114618864A (en) * | 2022-02-25 | 2022-06-14 | 江西环锂新能源科技有限公司 | Process for extracting lithium salt from waste lithium battery |
| CN114618864B (en) * | 2022-02-25 | 2023-03-10 | 江西环锂新能源科技有限公司 | Process for extracting lithium salt from waste lithium battery |
| CN115608493A (en) * | 2022-06-16 | 2023-01-17 | 江西铭鑫环保设备有限公司 | Complete equipment for charged crushing and sorting of waste lithium batteries |
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