CA2032768C - Process for the removal of sodium polysulphide from run-down sodium/sulphur batteries - Google Patents

Process for the removal of sodium polysulphide from run-down sodium/sulphur batteries

Info

Publication number
CA2032768C
CA2032768C CA 2032768 CA2032768A CA2032768C CA 2032768 C CA2032768 C CA 2032768C CA 2032768 CA2032768 CA 2032768 CA 2032768 A CA2032768 A CA 2032768A CA 2032768 C CA2032768 C CA 2032768C
Authority
CA
Canada
Prior art keywords
sodium
sulphur
solution
scrap
batteries
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.)
Expired - Fee Related
Application number
CA 2032768
Other languages
French (fr)
Other versions
CA2032768A1 (en
Inventor
Edgar Bilger
Urban Gubisch
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.)
Evonik Operations GmbH
Original Assignee
Degussa GmbH
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 Degussa GmbH filed Critical Degussa GmbH
Publication of CA2032768A1 publication Critical patent/CA2032768A1/en
Application granted granted Critical
Publication of CA2032768C publication Critical patent/CA2032768C/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

Links

Classifications

    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/54Reclaiming serviceable parts of waste accumulators
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02WCLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00Technologies for solid waste management
    • Y02W30/50Reuse, recycling or recovery technologies
    • Y02W30/84Recycling 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)
  • Manufacture And Refinement Of Metals (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)
  • Catalysts (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)

Abstract

In a process for the removal of sodium polysulphide from run-down sodium/sulphur batteries, the cells are crushed while taking safety measures. The scrap metal is treated in a sodium cyanide solution and on separating the insoluble components the solution obtained is treated with air in the presence of manganese dioxide. The solution then contains sodium thiocyanate and sodium hydroxide. The latter can be reacted with CO2Na2CO3, precipitated and separated out.

Description

The present invention relates to a process for the removal of sodium polysulphide from run-down sodium/sulphur batteries while permitting the recovery of an alkaline sodium thiocyanate solution. Sodium thiocyanate is used, for example, in the chemical and pharmaceutical industries for the production of organic thio-cyanates, isothiocyanates, mustard oils, pesticides, biocides, in the photo industry for toning, sensitizing and stabilizing and for the production of gloss-forming agents in galvanotechnics.

No process for the removal of sodium polysulphide from Na/S batteries while simultaneously recovering sodium thiocyanates is known from the literature.

It is an object of the present invention to remove sodium polysulphide from run-down sodium/sulphur batteries while recovering assets, namely, sodium thiocyanate in the form of an alkaline or soda-alkaline solution.

According to a first aspect of the invention there is provided a process for the removal of sodium polysulphide from run-down sodium/sulphur batteries while permitting the recovery of an alkaline sodium thiocyanate solution comprising mechanically crushing batteries or cell sets removed from battery boxes and containing sodium polysulphide and possibly sodium residues to a finely divided scrap having a grain diameter of up to 30 mm, treating the scrap with an aqueous sodium cyanide solution whose cyanide content is in a molar ratio the total sulphur consisting of S0 or S 2, such as 1:1, while stirring, separating the insoluble components of the scrap from the solution, mixing the solution with 0.1 to 20% by weight of manganese dioxide relative to the total sulphur as catalyst, and selectively oxidizing the sulphidic sulphur by passing air through at temperatures ranging from room temperature to 110C for the intermediate formation of elementary sulphur, and concluding the reaction of said 20327~8 sulphur with the residual sodium cyanide to sodium thiocyanate.

Important steps of this method thus are as follows:
shredding the run-down batteries to finely divided scrap, feeding the scrap into an aqueous sodium cyanide solution and reacting while utilizing the heat of reaction, separating the non-reacting components, selectively oxidizing the sulphidic sulphur to elementary sulphur, followed by an in-situ reaction with free sodium cyanide to sodium thiocyanate. The selective oxidation of the sulphidic sulphur in the presence of manganese dioxide and the use of air as oxidizing agent are particularly important.

According to a further aspect of the invention there is provided a process for the removal of sodium polysulphide from run-down sodium/sulphur batteries while permitting the recovery of an alkaline sodium thiocyanate solution, comprising mechanically crushing the batteries or cell setsremoved from battery boxes and containing sodium polysulphide and possibly sodium residues to a finely divided scrap having a grain diameter of up to 30 mm, mixing while stirring an aqueous sodium cyanide solution whose cyanide content is in a molar ratio to the total sulphur present, consisting of S0 or S 2, such as 1:1, with 0.1 to 20% by weight of manganese dioxide relative to the total sulphur, selectively oxidizing the sulphidic sulphur by passing air through at temperatures ranging from room temperature to 110C for the intermediate formation of elementary sulphu, concluding the reaction of said sulphur with residual sodium cyanide to sodium thiocyanate, and separating the insoluble components from the aqueous solution of the sodium thiocyanate product.

In this slightly modified process sodium cyanide solution is mixed with the scrap and the catalyst while stirring and is allowed to react, whereupon the oxidation with air is carried out. Finally the insoluble substances are removed from the solution of the sodium thiocyanate formed.

In the process according to the two alternatives aqueous sodium cyanide solutions having a content of 15 to 35% by weight are applied. The concentration preferably is 20 to 30~ by weight.

In the two alternatives the reaction of the polysulphide with the cyanide is exothermic. It has been found that it is favourable to reheat to the boiling temperature. In order to carry out the reaction of the formally nonvalent sulphur with the sodium cyanide quantitatively, it is advantageous to maintain a postreaction time of 1 to 40, preferably 5 to 30 minutes at reflux temperature. On completion of the reaction of this sulphur portion, the sulphidic sulphur is selectively oxidized to sulphur by passing air through the reaction mixture in the presence of the catalyst, whereupon it is reacted in situ with free sodium cyanide to sodium thiocyanate.

For the two methods a number of favourable variants are equally applicable; they will be described hereafter:

It has been found that it is favourable when the mechanical comminution of the batteries or of the cell sets is carried out under an atmosphere of water vapour or inert gas.

The batteries or the cell sets are preferably crushed to scrap having a grain diameter < 10 mm.

In order to intensify the action of the sodium cyanide solution on the scrap, the scrap can be treated with said 20~2768 solution, or when proceeding according to the second alternative, the scrap can be treated with said solution in the presence of a catalyst while reheating to the boiling temperature.

Within the total range of the applicable catalyst concentration the application of 2 to 7% by weight of catalyst, relative to the total sulphur, has proved to be particularly suitable.

For the selective oxidation of the sulphidic sulphur the lo turbulent motion caused by the injection of air into the reactor filling usually is sufficient. However, it is even better when the reaction mixture is stirred while the air is passing through.

The selective oxidation of the sulphidic sulphur can be carried out most easily at temperatures of 50 to 80C.

The product solution which contains the sodium thiocyanate and can be obtained by means of the two methods according to the present invention is alkaline because of its content of sodium hydroxides. According to a favourable embodiment of the present invention the alkaline reaction can be reduced in that the sodium hydroxide contained in the solution of the sodium thiocyanate product is converted into sodium carbonate by passing carbon dioxide through or injecting it and that the carbonate precipitated in the form of solids or by cooling is removed from the product solution which then is alkaline with soda. This can be done by means of filtration.

When operating according to the present invention yields of up to 98.7% relative to the total sulphur are obtained.

The present invention will be described in more detail by means of the following examples:

Example 1 2.50 g (7 moles) of a 98% sodium cyanide are dissolved in 1150 g of water in a three-necked flask provided with agitator, reflux condenser, thermometer and lockable inlet pipe. 353 g (7 moles) of scrap shredded beforehand from cell sets in an atmosphere of water vapour and having a total sulphur content of 63.6 % by weight are rapidly added while stirring. Because of the exothermic reaction the temperature increases from 25C to 95C. The reaction mixture is further heated to the boiling temperature (110C) and stirred for 20 minutes. The reaction mixtures is exactly filtered with suction by means of a tin strip filter and transferred into a glass tube having a frit fused at the bottom, mixed with 45 g of manganese dioxide (MnO2) and heated to 65C, whereupon 424 standard litres of air (3.98 moles of 2) are passed through from below. Upon cooling to room temperature 44.8 standard litres (2 moles) of carbon dioxide are passed through the reaction solution from below while the pH value decreases from pH 13.9 to pH 8Ø The precipitated deposit is filtered with suction. The filtrate contains 6.91 moles of sodium thiocyanate, i.e., a yield of 98,7%.

Example 2 150 g (3 moles) of a 98% sodium cyanide are dissolved in 550 g of water in a three-necked flask provided with agitator, reflux condenser, thermometer and lockable inlet pipe. 250 g (3 moles) of shredded cell material having a total sulphur content of 38.4% by weight are rapidly added, while stirring. Because of the exothermic reaction the temperature increases from room temperature to 93C. Heating is contained up to the boiling temperature (110C), followed by stirring at this temperature for 7 minutes, whereupon 0.096 g of manganese dioxide (MnO2) are added. A glass tube having a frit fused at the bottom is inserted in the reaction mixture. At 110C 200 standard litres of air (1.88 moles of 2) are passed through this tube into the reaction mixture.
S The hot reaction mixtures is exactly filtered with suction, cooled to room temperature and filled into a glass tube having a frit that is fused at the bottom. 22.4 standard litres (1 moles) of carbon dioxide are then passed through the solution from below. At the same time the pH value decreases from pH 13.0 to pH 8Ø The precipitated deposit is filtered with suction. The solution contains 2.79 moles of sodium thiocyanate, i.e., a yield of 93.1%.

Claims (9)

1. A process for the removal of sodium polysulphide from run-down sodium/sulphur batteries while permitting the recovery of an alkaline sodium thiocyanate solution, comprising mechanically crushing the batteries or cell sets taken from battery boxes and containing sodium polysulphide and optionally sodium residues to a finely divided scrap having a grain size of up to 30 mm, treating the scrap with an aqueous sodium cyanide solution whose cyanide content is in a molar ratio to the total sulphur present, consisting of S0 or S-2, of about 1:1, while stirring, separating the insoluble components of the scrap from the solution, mixing the solution with 0.1 to 20% by weight of manganese dioxide relative to the total sulphur as catalyst, and selectively oxidizing the sulphidic sulphur by passing air through at temperatures ranging from room temperature to 110°C for the intermediate formation of elementary sulphur and concluding the latter's reaction with the residual sodium cyanide present to sodium thiocyanate.
2. A process for the removal of sodium polysulphide from run-down sodium/sulphur batteries while permitting recovery of an alkaline sodium thiocyanate solution, comprising mechanically crushing batteries or cell sets removed from battery boxes and containing sodium polysulphide and optionally sodium residues to a finely divided scrap having a grain diameters of up to 30 mm, mixing an aqueous sodium cyanide solution whose cyanide content is in a molar ratio to the total sulphur present, consisting of S° or S-2, of about 1:1, with the scrap while stirring, with 0.1 to 20% by weight of manganese dioxide relative to the total sulphur as catalyst, selectively oxidizing the sulphidic sulphur by passing air through at temperatures ranging from room temperature to 110°C for the intermediate formation of elementary sulphur, concluding the latter's reaction with the residual sodium cyanide to sodium thiocyanate, and separating the unsoluble compounds from the aqueous solution of the sodium thiocyanate product.
3. A process as claimed in claim 1 or 2, wherein the batteries or cell sets are mechanically comminuted under an atmosphere of water vapour or inert gas.
4. A process as claimed in claim 1 or 2, wherein the batteries or cell sets are crushed to scrap having a grain diameter < 10 mm.
5. A process as claimed in claim 1 or 2, wherein the scrap is treated with the sodium cyanide solution or, when following the procedure defined in claim 2, the scrap is treated with said solution in the presence of the catalyst while reheating to the boiling temperature.
6. A process as claimed in claim 1 or 2, wherein 2 to
7% by weight of catalyst, relative to the total sulphur, are used.

7. A process as claimed in claim 1 or 2, wherein the reaction mixture is stirred while air is passed through.
8. A process as claimed in claim 1 or 2, wherein the selective oxidation of the sulphidic sulphur is carried out at 50 to 80°C.
9. A process as claimed in claim 1 or 2, wherein the sodium hydroxide contained in the solution of the sodium thiocyanate product is converted into sodium carbonate by passing carbon dioxide through or by injecting it, whereupon the carbonate deposited in the form of solids or precipitated by cooling is removed from the solution, which then is made alkaline with soda.
CA 2032768 1989-12-22 1990-12-20 Process for the removal of sodium polysulphide from run-down sodium/sulphur batteries Expired - Fee Related CA2032768C (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DEP3942516.9-45 1989-12-22
DE19893942516 DE3942516C1 (en) 1989-12-22 1989-12-22

Publications (2)

Publication Number Publication Date
CA2032768A1 CA2032768A1 (en) 1991-06-23
CA2032768C true CA2032768C (en) 1997-07-01

Family

ID=6396165

Family Applications (1)

Application Number Title Priority Date Filing Date
CA 2032768 Expired - Fee Related CA2032768C (en) 1989-12-22 1990-12-20 Process for the removal of sodium polysulphide from run-down sodium/sulphur batteries

Country Status (5)

Country Link
US (1) US5055283A (en)
EP (1) EP0433654B1 (en)
JP (1) JPH03203173A (en)
CA (1) CA2032768C (en)
DE (2) DE3942516C1 (en)

Families Citing this family (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE4224884A1 (en) * 1992-07-28 1994-02-03 Batenus Gmbh & Co Kg Process for the recovery of raw materials from pre-sorted, used goods, in particular from used electrochemical batteries and accumulators
DE4227511C1 (en) * 1992-08-20 1993-07-22 Silent Power Gmbh, 4300 Essen, De
JP2741834B2 (en) * 1993-03-24 1998-04-22 日本碍子株式会社 Method and apparatus for treating sodium-sulfur battery
DE19856071A1 (en) * 1998-12-04 2000-06-15 Degussa Process for avoiding water contamination with non-resident organisms
CN103373734B (en) * 2013-07-18 2015-07-15 江苏燎原环保科技股份有限公司 Method for preparing high-quality potassium rhodanide by using coke oven gas waste liquor with sulfur and cyanogen removed
JP6476598B2 (en) * 2014-06-03 2019-03-06 三菱マテリアル株式会社 Method for recovering sodium from sodium-sulfur battery, apparatus for recovering sodium from sodium-sulfur battery
KR102576614B1 (en) * 2021-05-17 2023-09-07 목포대학교산학협력단 Method for recovering valuable metals from waste lithium ion batteries

Family Cites Families (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3459498A (en) * 1965-05-07 1969-08-05 Jefferson Chem Co Inc Conversion of cyanates to thiocyanates
US4024229A (en) * 1970-11-06 1977-05-17 The Mead Corporation Production of polysulfide with PTFE coated catalyst
US4290192A (en) * 1979-12-20 1981-09-22 Ford Motor Company Method of making a sodium sulfur battery
DE3000563A1 (en) * 1980-01-09 1981-07-16 Basf Ag, 6700 Ludwigshafen METHOD FOR DETOXIFYING CYANIDE-CONTAINING REACTION SOLUTIONS AND SEWAGE
FI65807C (en) * 1980-04-16 1984-07-10 Outokumpu Oy REFERENCE TO A SULFID CONCENTRATION
DE3101369C2 (en) * 1981-01-17 1987-01-08 Klöckner-Humboldt-Deutz AG, 5000 Köln Process for smelting fine-grained sulphidic copper ore concentrate
US4508683A (en) * 1982-03-15 1985-04-02 Doll Brian E Control of cyanides in FCC reactor by injection of ammonium polysulfide
NL8303659A (en) * 1982-11-11 1984-06-01 Kloeckner Humboldt Deutz Ag METHOD FOR WINNING ZINC.
FI68661C (en) * 1983-10-27 1985-10-10 Rm Metal Consulting Ky FOERFARANDE FOER RAFFINERING AV SULFIDKONCENTRAT INNEHAOLLANDEARSENIK ANTIMON OCH VISMUT
CA1307652C (en) * 1986-05-13 1992-09-22 Iron Otto Simek Mte sulphur recovery process
US4719019A (en) * 1986-12-10 1988-01-12 Srini Vasan Treatment of thiocyanate containing waste liquor
US4977044A (en) * 1989-10-03 1990-12-11 Hughes Aircraft Company Sodium-sulfur thermal battery

Also Published As

Publication number Publication date
CA2032768A1 (en) 1991-06-23
US5055283A (en) 1991-10-08
EP0433654A2 (en) 1991-06-26
DE59001792D1 (en) 1993-07-22
JPH03203173A (en) 1991-09-04
EP0433654B1 (en) 1993-06-16
EP0433654A3 (en) 1991-12-18
DE3942516C1 (en) 1991-08-01

Similar Documents

Publication Publication Date Title
US5405430A (en) Recovery of precious metals from evaporite sediments
US5482534A (en) Extraction or recovery of non-ferrous metal values from arsenic-containing materials
US3911078A (en) Method for removing arsenic and antimony from copper ore concentrates
CA2027973A1 (en) Method of reprocessing jarosite-containing residues
EP0119685A1 (en) Hydrometallurgical arsenopyrite process
CA2032768C (en) Process for the removal of sodium polysulphide from run-down sodium/sulphur batteries
US4078917A (en) Extraction of antimony trioxide from antimony sulfide ore
CA2247098A1 (en) Process for stabilization of arsenic
JP2025508244A (en) Purification of MnSO4 solution
EA005711B1 (en) Method for obtaining cobalt and nickel from ores and ore concentrates
US3909211A (en) Coal desulfurization process
US5279743A (en) Process of using chloric acid to separate zinc oxide and manganese oxide
US3684489A (en) Method of recovering metals from sulfide-containing mixtures
US2923600A (en) Method of producing lithium sulphate from beta spodumene
FI69111B (en) FOERFARANDE FOER ATT TILLVARATAGA KOBOLT FRAON EXTRAKTIONSLOESNINGAR AV NICKEL
US3322532A (en) Process for recovering the metal content of middlings, slags, low-grade ores, and concentrates
US5324500A (en) Method for processing residues of barium sulfide or strontium sulfide leaching
FI70200B (en) FRAMSTAELLNING AV ARSENSYRA
US4482377A (en) Separation of zinc from a zinc-copper alloy
US2972517A (en) Method of producing lithium sulphate from alpha and beta spodumene
US4169131A (en) Process for recovering caustic alkali from spent alkali liquor
US2430632A (en) Preparation of a tungsten sulfide containing catalyst
JP4486215B2 (en) How to recover the pesticide
CN106834713B (en) A method of from arsenic-containing smoke dust comprehensively recovering valuable metal and the solid arsenic mineral of regulation and control growth method synthesis
WO1982002540A1 (en) Wet oxidation of organic matter

Legal Events

Date Code Title Description
EEER Examination request
MKLA Lapsed