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WO2007129845A1 - Dispositif et procédé de recyclage de piles zinc-carbone et alcalines usées - Google Patents

Dispositif et procédé de recyclage de piles zinc-carbone et alcalines usées Download PDF

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Publication number
WO2007129845A1
WO2007129845A1 PCT/KR2007/002218 KR2007002218W WO2007129845A1 WO 2007129845 A1 WO2007129845 A1 WO 2007129845A1 KR 2007002218 W KR2007002218 W KR 2007002218W WO 2007129845 A1 WO2007129845 A1 WO 2007129845A1
Authority
WO
WIPO (PCT)
Prior art keywords
batteries
spent
zinc
size
separation means
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.)
Ceased
Application number
PCT/KR2007/002218
Other languages
English (en)
Inventor
Shun Myung Shin
Jeong Soo Sohn
Dong Hyo Yang
Tae Hyun Kim
Jin Gu Kang
Kyung Bae Kim
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Korea Institute of Geoscience and Mineral Resources KIGAM
Original Assignee
Korea Institute of Geoscience and Mineral Resources KIGAM
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Korea Institute of Geoscience and Mineral Resources KIGAM filed Critical Korea Institute of Geoscience and Mineral Resources KIGAM
Publication of WO2007129845A1 publication Critical patent/WO2007129845A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/52—Reclaiming serviceable parts of waste cells or batteries, e.g. recycling
    • 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
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B19/00—Obtaining zinc or zinc oxide
    • C22B19/30—Obtaining zinc or zinc oxide from metallic residues or scraps
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
    • C22B7/005—Separation by a physical processing technique only, e.g. by mechanical breaking
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
    • C22B7/006—Wet processes
    • C22B7/008—Wet processes by an alkaline or ammoniacal leaching
    • 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
    • H01M10/24—Alkaline accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/04—Cells with aqueous electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/04—Cells with aqueous electrolyte
    • H01M6/06—Dry cells, i.e. cells wherein the electrolyte is rendered non-fluid
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00—Technologies related to metal processing
    • Y02P10/20—Recycling
    • 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

Definitions

  • the present invention relates to an apparatus and method for recycling spent batteries, and more particularly to an apparatus and method, which can recover valuable metals from spent zinc-carbon batteries and alkaline batteries, using an eddy current separator and a dust collector without discharging pollutants.
  • Batteries generally include, as electrode materials, variable metals, such as nickel, manganese, lithium, cadmium, mercury, silver and cobalt, depending on the type and manufacturer thereof.
  • Battery wastes after being used for a given period of time came from primary batteries, such as zinc-carbon batteries, alkaline batteries, lithium primary batteries, silver oxide batteries and mercury batteries, and secondary batteries, such as nickel- cadmium batteries and lithium ion batteries.
  • primary batteries such as zinc-carbon batteries, alkaline batteries, lithium primary batteries, silver oxide batteries and mercury batteries
  • secondary batteries such as nickel- cadmium batteries and lithium ion batteries.
  • zinc-carbon batteries and alkaline batteries which are the majority of spent batteries, contain manganese, zinc, iron, nickel, etc., and are used annually in an amount of more than about 15,000 tons corresponding to about one billion batteries.
  • the thermal waste treatment process is a process in which spent batteries are thermally treated at a temperature of 700 0 C, and then separated into magnetic materials and non-magnetic materials through physical crushing and screening processes. Iron scrap is treated through this process in iron mills, and fine powder (32% zinc, 27% manganese and 9% iron) is treated in zinc oxide recycling firms.
  • Recymet GmbH Swiss, recycles spent batteries as well using a dry process in a manner similar to that of Chemtec GmbH.
  • Another object of the present invention is to provide an apparatus and method for recycling spent zinc-carbon batteries and alkaline batteries, which can increase the amount of valuable metals to be recovered through chemical treatment, by first removing button-type batteries by shape separation, and efficient separating, through an eddy current separator and an air classifier, metal zinc from zinc, carbon rods, membranes and cases of a large size enough to pass through a size separator.
  • Still another object of the present invention is to provide an apparatus and method for recycling spent zinc-carbon batteries and alkaline batteries, which can environmentally friendly recover valuable metals using a dust collector and a cooler without generating pollutants.
  • an apparatus for recycling spent zinc-carbon batteries and alkaline batteries comprising: a dust collection means for sucking dust generated from crushed spent batteries; a magnetic separation means for separating out magnetic materials from the crushed spent batteries; a size separation means for separating nonmagnetic materials in the crushed spent batteries according to their size; an eddy current separation means for separating zinc and carbon rods from the nonmagnetic materials larger than a given size, which have passed through the size separation means; and a recovery means for collecting valuable metals from the nonmagnetic materials smaller than a given size, which have passed through the size separation means.
  • a method for recycling spent zinc-carbon batteries and alkaline batteries comprising the steps of: sucking dust generated from crushed spent batteries; separating out magnetic materials from the crushed spent batteries; separating nonmagnetic materials in the crushed spent batteries according to their size; separating zinc and carbon rods from the nonmagnetic materials larger than a given size using an eddy current; forming powder after drying the nonmagnetic materials smaller than a given size in an electric furnace; and leaching zinc by adding the powder to an alkaline leaching solution.
  • the apparatus and method for recycling spent zinc-carbon batteries and alkaline batteries have an advantage in that dust and hazardous gas, which are generated during physical treatment processes, can be treated in an environment-friendly manner.
  • Another advantage is that the cost required for recovering valuable metals can be reduced by treating spent batteries through physical and chemical processes in one place with a batch treatment.
  • FIG. 1 is a schematic diagram of a physical treatment apparatus in the inventive apparatus for recycling spent zinc-carbon batteries and alkaline batteries.
  • FIG. 2 is a schematic diagram of a shape separation belt according to the present invention.
  • FIG. 3 is a schematic diagram of a PVC disk according to the present invention.
  • FIG. 4 is a flow diagram of a physical treatment process in the inventive method for recycling spent zinc-carbon batteries and alkaline batteries.
  • FIG. 5 is a flow diagram of a chemical treatment process in the inventive method for recycling spent zinc-carbon batteries and alkaline batteries.
  • FIG. 6 is a schematic diagram of a reactor which is a recovery means according to the present invention.
  • FIGS. 1 to 4 show an apparatus and process for physical treating spent zinc-carbon batteries and alkaline batteries according to the present invention.
  • spent batteries 101 including alkaline, zinc-carbon, alkaline/zinc-carbon and button-type batteries, are placed on a magnetic separation belt
  • the magnetic separation belt 102 separates only spent batteries from waste-containing spent batteries (S20) and transfers the separated spent batteries to a shape separation belt 104.
  • the shape separation belt 104 As shown in FIG. 2, the shape separation belt 104 according to the present invention is formed with two polygonal nets 104a and 104b with the diameter larger than that of spent button-type batteries 103 crossed each other at a distance (d) larger than the thickness of the spent button-type batteries, so that other batteries except for button-type ones do not fall into the net holes.
  • the spent batteries 101 except for the spent button-type batteries 103 are sorted by their size in the shape separation means 105 with different net sizes (S21).
  • the spent batteries sorted by their size are passed through a belt to a crushing means 106, in which they are finely crushed (S22).
  • the crushing means 106 is equipped with a dust collection means 107 made of activated carbon, so that it can collect and treat contaminants such as graphite dust generated in the process of crushing the spent batteries through a fan (not shown) in order not to be emitted to the outside (S23).
  • the crushed spent batteries are separated into magnetic materials such as iron scrap
  • the nonmagnetic materials are transferred to a size separation means 110, in which they are separated according to their size (S25).
  • the size separation means 110 consists of a vibrating 8-mesh (2.56 mm) screen, and thus separates the nonmagnetic materials into a size of 8 mesh or larger or a size smaller than 8 mesh.
  • the nonmagnetic materials of 8 mesh or larger light plastics, paper, vinyl resins, etc., which have covered the batteries, are transferred to a first reservoir 112 by the suction force of a fan (not shown) connected to the size separation means 110.
  • the first reservoir 112 comprises a pressing means (not shown), which presses plastics, paper and vinyl resins to form a fuel material 113.
  • a pressing means (not shown)
  • Heavy carbon rods and zinc plates which have fallen downward without being sucked by the fan, are passed through a transfer screw (not shown) to an eddy current separation means 114, in which they are separated into carbon rods 115 and zinc plates
  • the first reservoir 112 is connected to the dust collection means 107, which sucks dust remaining on the surface of the nonmagnetic materials (S26b).
  • the nonmagnetic fine particles smaller than 8 mesh, which have fallen on the bottom of the size separator, are collected in a second reservoir 117 by a PVC disctype transferring means 111 (S26a).
  • the PVC disc-type transferring means 111 consists of a plurality of PVC discs I l ia connected with each other by a metal wire 11 Ib and a driving gear (not shown).
  • the PVC discs I l ia collect the nonmagnetic fine particles 111c while rotating by the rotation of the driving gear (not shown). Unlike prior metal screws, the use of the PVC discs does not show a problem of screws' corrosion caused by moisture contained in fine particles to stop the operation thereof.
  • the electric furnace 118 is of cylindrical shape, able to rotate and inclined at a given angle, so that the nonmagnetic materials can be uniformly thermally treated. Meanwhile, the inclined angle of the electric furnace 118 can be adjusted to control the time required for heat treatment.
  • the heat treatment is done at a temperature of 900-1200 0 C.
  • the second reservoir 117 is connected to a conveyor- type belt so that the button- type spent batteries 103 separated in the shape separation belt 104 can be introduced into the second reservoir.
  • spent button-type batteries including spent mercury batteries can be treated.
  • the electric furnace 118 is connected to a cooling tower 119. Because cooling water flows around the cooling tower 119, mercury vapor or electrolyte vapor generated in the electric furnace 118 can be liquefied so as to prevent the emission of hazardous gas (S28a).
  • the nonmagnetic materials 120 treated in the electric furnace 118 are used as the raw material of valuable metal Mn-Zn ferrite to be recovered through chemical treatment as described below, and can be prepared into powders through a ball mill (S29a).
  • FIG. 5 is a flow chart showing a process for chemically treating spent zinc-carbon batteries and alkaline batteries according to the present invention.
  • the nonmagnetic powder prepared from the above-described physical treatment is mixed with sodium hydroxide (NaOH) as an alkaline leaching solution.
  • NaOH sodium hydroxide
  • S30 only zinc contained in the nonmagnetic powder is selectively leached (S30), and high purity zinc is recovered from the zinc-leached alkaline solution by electrowinning (S31).
  • Table 1 below shows the composition and acidity of each of the alkaline leachate and the sulfuric acid leaching solution (to be used as reaction solution), which remain after the above steps S31 and S32.
  • Table 2 shows a stoichiometric molar ratio for making Mn-Zn ferrite powder. [77] [78] Table 2
  • reaction molar ratio required for preparing Mn-Zn ferrite powder in 700 ml of the sulfuric acid leaching solution used in the reaction process is calculated.
  • each concentration of manganese, zinc and iron in 700 ml of the sulfuric acid leaching solution is calculated.
  • deficiency calculated based on manganese is 0.66 g for zinc and 4.65 g for iron.
  • concentration of zinc in the remaining alkaline leachate is 12.45 git, which corresponds to 0.66 g as converted into about 53.2 ml .
  • FIG. 6 is a schematic diagram of a reactor as a recovery means according to the present invention.
  • the reactor is equipped with a heater 46, a thermometer 43, a temperature controller 49, a stirrer 48, a motor 41 and a controller 42. Furthermore, it includes a condenser 45 for preventing the evaporation of solution caused by heat treatment, a sampling pipette 47 for injecting a sample, and a clamp 44.
  • a surfactant or ultrasonic waves can be used to prevent the aggregation of particles during the formation of ferrite.
  • the oxidation step (S36) is conducted by stirring the sulfuric acid leaching solution at a stirring speed of 400-600 rpm at a temperature of 60-90 0 C at atmospheric pressure for 60-100 minutes while supplying 02 into the solution at a flow rate of 0.5-2 I /min.
  • the material obtained from the oxidation step (S36) contains a certain amount of sodium due to sodium hydroxide used to adjust acidity.
  • a filtration step (S37) is a step of filtering the material formed through the copre- cipitation step (S35) and the oxidation step (S36). In this step, the material formed in the oxidation step (S36) is washed several times with ethanol to remove sodium. [95] According to one embodiment of the present invention, the filtrate remaining after the filtration step (S37) is used as a portion of the alkaline leachate to adjust acidity to 10-14 prior to coprecipitation. [96] According to another embodiment of the present invention, when the recovery of zinc in the electrowinning process is increased, it is possible to use an excess amount of the alkaline leachate to adjust acidity.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Environmental & Geological Engineering (AREA)
  • Geology (AREA)
  • Sustainable Development (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Processing Of Solid Wastes (AREA)

Abstract

L'invention se rapporte à un dispositif et à un procédé pour récupérer les métaux de valeur contenus dans les piles usées. Elle concerne un dispositif et un procédé de recyclage de piles zinc-carbone et de piles alcalines usées, qui permet de réduire les coûts de transport en traitant les piles usées au moyen de processus physiques et chimiques dans un même site, par lots, et de récupérer les métaux de valeur avec un haut rendement au moyen d'un séparateur à courant de Foucault, d'un collecteur de poussière et d'un refroidisseur, sans générer de polluants. Le dispositif décrit comprend des moyens de collecte de poussière qui permettent d'aspirer les poussières produites par les piles usées broyées, des moyens de séparation de matériaux magnétiques permettant de séparer les matériaux magnétiques des piles usées broyées, des moyens de séparation par taille permettant de trier des matériaux non magnétiques présents dans les piles usées écrasées selon leur taille, des moyens de séparation à courant de Foucault permettant de séparer le zinc et les bâtons de carbone des matériaux non magnétiques dépassant une taille donnée qui ont passé à travers les moyens de séparation par taille, et des moyens de récupération permettant de récupérer les métaux de valeur contenus dans les matériaux magnétique d'une taille inférieure à une taille donnée qui ont passé à travers les moyens de séparation par taille. Le procédé décrit consiste à aspirer la poussière produite dans les piles usées, à séparer les matériaux magnétiques des piles usées broyées, à trier les matériaux non magnétiques des piles usés broyées par taille, à séparer le zinc et les bâtons de carbone des matériaux non magnétiques dépassant une taille donnée à l'aide d'un courant de Foucault, à former une poudre en séchant les matériaux non magnétiques d'une taille inférieure à une taille donnée dans un four électrique, et à lixivier le zinc en ajoutant la poudre à une solution de lixiviation alcaline.
PCT/KR2007/002218 2006-05-04 2007-05-04 Dispositif et procédé de recyclage de piles zinc-carbone et alcalines usées Ceased WO2007129845A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KR10-2006-0040271 2006-05-04
KR20060040271A KR100709268B1 (ko) 2006-05-04 2006-05-04 폐망간전지 및 알카라인전지 재활용 장치 및 방법

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WO2007129845A1 true WO2007129845A1 (fr) 2007-11-15

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WO (1) WO2007129845A1 (fr)

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WO2008077905A1 (fr) * 2006-12-22 2008-07-03 Recylex S.A. Dispositif et procédé pour traiter des batteries de stockage de plomb non écrasées à un débit amélioré
JP2011105581A (ja) * 2009-11-20 2011-06-02 Korea Inst Of Geoscience & Mineral Resources マンガン及び亜鉛を含有する廃電池からの硫酸マンガン及び硫酸亜鉛の製造方法
CN108539313A (zh) * 2018-05-18 2018-09-14 刘博奕 一种废旧铅酸电池分离收集装置
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CN114583303A (zh) * 2022-01-12 2022-06-03 顺尔茨环保(北京)有限公司 一种废旧锂离子电池的破碎方法及系统
CN116116867A (zh) * 2022-09-07 2023-05-16 北京科技大学 一种废旧干电池与厨余垃圾的协同处理系统及方法
US12407035B2 (en) 2020-02-27 2025-09-02 Sk Innovation Co., Ltd. Method for recovering active metal of lithium secondary battery
US12476292B2 (en) 2020-02-10 2025-11-18 Sk Innovation Co., Ltd. Method for recovering active metal of lithium secondary battery

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KR102349189B1 (ko) * 2021-06-16 2022-01-10 구본훈 폐배터리 처리 장치
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