EP2401422A2 - Procédé et dispositif de régénération de solutions de décapage contenant du peroxodisulfate - Google Patents

Procédé et dispositif de régénération de solutions de décapage contenant du peroxodisulfate

Info

Publication number
EP2401422A2
EP2401422A2 EP10722522A EP10722522A EP2401422A2 EP 2401422 A2 EP2401422 A2 EP 2401422A2 EP 10722522 A EP10722522 A EP 10722522A EP 10722522 A EP10722522 A EP 10722522A EP 2401422 A2 EP2401422 A2 EP 2401422A2
Authority
EP
European Patent Office
Prior art keywords
copper
anode
pickling
cathode
peroxodisulfate
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.)
Withdrawn
Application number
EP10722522A
Other languages
German (de)
English (en)
Inventor
Wolfgang Thiele
Hans-Jürgen FÖRSTER
Gerd Heinze
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.)
Eilenburger Elektrolyse- und Umwelttechnik GmbH
Eilenburger Elecktrolyse- und Umwelttechnik GmbH
Original Assignee
Eilenburger Elektrolyse- und Umwelttechnik GmbH
Eilenburger Elecktrolyse- und Umwelttechnik 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 Eilenburger Elektrolyse- und Umwelttechnik GmbH, Eilenburger Elecktrolyse- und Umwelttechnik GmbH filed Critical Eilenburger Elektrolyse- und Umwelttechnik GmbH
Publication of EP2401422A2 publication Critical patent/EP2401422A2/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C23COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23FNON-MECHANICAL REMOVAL OF METALLIC MATERIAL FROM SURFACE; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL; MULTI-STEP PROCESSES FOR SURFACE TREATMENT OF METALLIC MATERIAL INVOLVING AT LEAST ONE PROCESS PROVIDED FOR IN CLASS C23 AND AT LEAST ONE PROCESS COVERED BY SUBCLASS C21D OR C22F OR CLASS C25
    • C23F1/00Etching metallic material by chemical means
    • C23F1/46Regeneration of etching compositions
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25BELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00Electrolytic production of inorganic compounds or non-metals
    • C25B1/01Products
    • C25B1/28Per-compounds
    • C25B1/29Persulfates
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B15/00Obtaining copper
    • C22B15/0063Hydrometallurgy
    • C22B15/0084Treating solutions
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B7/00Working 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
    • C22B7/006Wet processes
    • 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
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00Technologies related to metal processing
    • Y02P10/20Recycling

Definitions

  • the invention relates to a method and an electrolysis cell for regenerating pickling solutions containing peroxosulphate for copper and copper materials, on the one hand, the redeemed copper recovered, on the other hand, the mordant Peroxodisul- fat and / or Peroxomonosulfat can be regenerated.
  • pickling is to be understood below all other based on similar principles chemically abrasive surface treatment methods, such as firing, etching, glazing, demetallizing, deburring u. a.
  • demetallizing z For example, the dissolution of layers consisting of copper and nickel by means of peroxosulfate demetallization solutions is in principle equivalent to the pickling of copper-nickel alloys.
  • the new regeneration process is intended to make it easy to pickle copper and copper alloys in a closed loop process, to completely or partially regenerate the etch chemicals, and to recover the redeemed copper and possibly other alloying constituents.
  • the recovered metals can be reused, the consumption of pickling chemicals drastically reduced and the accumulation of exhausted pickling solutions that can be disposed of only with great effort, be completely avoided.
  • the peroxodisulfate regeneration takes place at high anodic current densities of 40 to 70 A / dm 2 and a high total sulfate content (sulfuric acid / sulfate concentrations) of preferably> 3 mol / l and with additional use of potential-enhancing additives. Since only maximum current densities of 1, 5 to 2.5 A / dm 2 are possible to recover the copper from the spent pickling solutions in a compact, firmly adhering form, using conventional, simple plate electrolysis cells, there is a required current density ratio for the Anodic Persulfate Formation for Cathodic Copper Deposition from 20 to 30. These extremely different requirements for both electrode reactions are the main reason why it has not been possible to combine both electrode processes in a simply constructed electrolysis cell divided by cation exchange membranes.
  • a disadvantage was the relatively high expenditure on equipment for the rotating cathode and the required division of the anode compartment into a larger number of small-volume anode pockets, which in conjunction with the relatively low current capacity of a single cell with a rotating cathode to a high equipment cost for a complete technical Recycling plant led.
  • the problem to be solved by the invention therefore consists in avoiding the disadvantages of the known persulfate recycling methods and by the combination of both electrolysis processes in a comparatively simply constructed recycling electrolysis cell with planar cathodes, dispensing with the use of rotation Cathodes significantly reduce the equipment required and thereby significantly improve the efficiency of the recycling process.
  • the insensitivity of the diamond-coated anodes with respect to existing peroxomonosulfates can also be used according to the invention so that a partial stream of the spent pickling solution can be fed directly into the anode chambers, bypassing the catholyte circuit, without reducing the anodic current efficiency of the peroxodisulfate regeneration.
  • This procedure is advantageous in that, in addition, copper passes into the cathode space through the transfer of copper ions through the cation exchange membranes and can be deposited there. A corresponding amount of spent pickling solution then needs to be fed to compensate for the copper balance less in the catholyte cycle. However, even less residual peroxodisulfate is fed into the catholyte, as a result of which an even greater proportion of the remaining peroxodisulfate remains in the regenerate and can be used further for the pickling process.
  • the sulfates / peroxosulfates used are in particular those of the alkali metals and ammonium, preferably the sodium sulfate / peroxosulfate.
  • sulfates / peroxosulfates of other metals alone or in admixture with sulfates / peroxosulfates of the alkali metals.
  • the metal sulfates of alloy constituents such as nickel, zinc or even iron itself, which are enriched in pickling of alloys in the pickling bath, are capable of forming peroxodisulfates which are capable of completely or partially replacing the sodium peroxosulfate in the regenerate.
  • magnesium sulphate / peroxosulphate as the pickling medium, less as an alloy constituent but as a substitute for sodium sulphate / peroxosulphate. This has particular advantages with regard to a room temperature more than twice as high molar solubility of magnesium sulfate compared to sodium sulfate.
  • planar cathodes to be used according to the invention it is possible to use both sheets made of copper, stainless steel or titanium, and copper expanded metals, in one or more layers or in combination with cathode sheets.
  • the electrochemically active surface can be increased and also the amount of copper to be deposited per cathode surface can be increased until the cathode is changed.
  • FIG. 1 shows a cross-section illustrating the arrangement of the rod-divided anode within the anode pocket to the planar cathode (with stylized streamline profile).
  • the recycling electrolysis cell consists of the cell container 3, in which a bilaterally acting planar cathode 4 and two anode cassettes 5 are arranged.
  • the cathode-facing sides of the anode cassettes consist of vertical slotted plates in which the cation exchange membranes 6 are clamped.
  • the niobium anodes 7 of 5 to 12 mm width, which are subdivided into vertical strips or rods, are provided with a coating of doped diamond 8. They are arranged at a distance of 50 to 70 mm from the slots in the edge plates of the anode casings, as illustrated in FIG. 2 using the example of an anode which is subdivided into bars and a planar cathode which acts only on one side.
  • the exhausted pickling solution is fed from the pickling tank 1 by means of the metering pump 2 into the catholyte circuit, which is circulated by means of the catholyte circulation pump 10 out of the catholyte circulation vessel 9 via the cathode chamber.
  • One of the metered amount of pickling solution corresponding proportion of the stationary catholyte enters at 11 in the anode cassettes 5, flows through them and passes through a gas separator as reclaim back into the pickling pan 1.
  • the metering pump 14 an additional amount of a peroxodisulfate solution from the container 13, also to compensate for leaching losses to pickling solution.
  • the anulfate regeneration anodes process was investigated using a pre-decarburized pickling solution still containing peroxosulfate, using the diamond-coated anodes to be used in the invention in comparison to the smooth platinum anodes.
  • the laboratory test cell had an effective anode area of 30 cm 2 .
  • the cathode consisted of several stainless steel expanded mesh, the separation of anolyte and catholyte was a NAFION N450 cation exchange membrane.
  • the catholyte used was dil.
  • Sulfuric acid, the anolyte solution had the following basic composition: 250 g / l sodium sulfate 50 g / l sodium peroxodisulfate
  • Experiment 2 Diamond electrode as in verse 1, but after previous hydrolysis.
  • Experiment 3 Comparative experiment with smooth platinum anode, without previous hydrolysis and without potential-increasing additives.
  • Example 1 In the same divided laboratory test cell of Example 1, the following starting solutions with different cations and total sulfate contents were electrolyzed with the diamond-coated anode under the same conditions (current density 40 A / dm 2 , electrolysis time 90 min) (in contrast to Example 1 without starting persulfate contents).
  • a recycling electrolysis cell was used, which was equipped with two double-acting cathode plates made of stainless steel with an electrochemically effective total area of 200 dm 2 .
  • the three anode cassettes each contained 10 vertical, 8 mm wide diamond coated niobium anode strips.
  • the middle anode pocket was bilateral and contained two NAFION cation exchange membranes clamped in two plastic plates each fitted with vertical slots opposite the anode strips.
  • the two edge-anode cassettes were constructed analogously, but they each contained only one cation exchange membrane and were unilateral.
  • the total electrochemically active anode area was 24 dm 2 . This results in a cathode / anode area ratio of 8.33.
  • the stationary catholyte was circulated by circulation pump.
  • a metering pump 55 l of the pickling solution from the pickling tank were fed into the catholyte cycle every hour.
  • This pickling solution had the following composition:
  • the 55 l / h catholyte solution fed with 13 g / l NaPS into the anode cassettes was anodically concentrated to 65.5 g / l NaPS. This corresponds to an amount of sodium peroxodisulfate regenerate of 3,603 g / h fed into the pickling bath. Of these anodically 2.888 g / h were formed, corresponding to a real current yield of 65.0%. Including in the calculation the amount of NaPS residual contained in the catholyte fed in, which would have had to be completely reduced in previous recycling processes, results in an apparent anodic current efficiency of 81.1%.
  • the NaPS consumption without recycling was about 4,400 g / h, including the carry-over and decomposition losses, which remained approximately constant with and without recycling.
  • about 81.9% of the amount of NaPS used without recycling could be recovered by the recycling process, in addition to the recovery of 561 g / h of copper.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Mechanical Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Electrochemistry (AREA)
  • Electrolytic Production Of Metals (AREA)

Abstract

L'invention a pour objet de régénérer, par un procédé de circulation, des solutions de décapage contenant du peroxodisulfate épuisées destinées à des matériaux de cuivre, dans une cellule électrolytique de recyclage compartimentée, le cuivre dissous étant tout d'abord déposé sur la cathode, puis le peroxodisulfate de décapage étant réoxydé au niveau de l'anode. Selon l'invention, on fait appel à une solution de décapage qui est mise en circulation en passant par le bain de décapage et la cellule électrolytique de recyclage et contient, en plus de 0,2 à 1,0 mol/l de peroxodisulfate, du sulfate en excès et de l'acide sulfurique libre avec une teneur totale en sulfate de 1 à 3 mol/l. A partir de la solution de décapage épuisée, dans le cellule électrolytique de recyclage compartimentée, le cuivre dissous est récupéré au niveau de cathodes planes avec des densités de courant cathodiques de 4 à 7 A/dm2, et le catholyte contenant du peroxosulfate résiduel parcourt ensuite les espaces anodiques dans lesquels le peroxodisulfate est réoxydé avec des densités de courant de 20 à 50 A/dm2, au niveau des anodes qui se composent de métal valve revêtu de diamant et se subdivisent en bandes ou barres perpendiculaires de largeur de 5 à 10 mm. L'invention permet une mise en oeuvre efficace du procédé de régénération de solutions de décapage sans adjonction de substance augmentant le potentiel et sans que le peroxosulfate subsistant dans le bain de décapage épuisé doive être complètement supprimé avant la réoxydation anodique. De cette manière, et grâce à l'utilisation d'une cellule électrolytique de recyclage de structure relativement simple, ce procédé permet d'obtenir une bonne rentabilité pour une qualité toujours aussi élevée des surfaces traitées.
EP10722522A 2009-01-09 2010-01-07 Procédé et dispositif de régénération de solutions de décapage contenant du peroxodisulfate Withdrawn EP2401422A2 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE200910004155 DE102009004155A1 (de) 2009-01-09 2009-01-09 Verfahren und Vorrichtung zum Regenerieren von Peroxodisulfat-Beizlösungen
PCT/DE2010/000007 WO2010078866A2 (fr) 2009-01-09 2010-01-07 Procédé et dispositif de régénération de solutions de décapage contenant du peroxodisulfate

Publications (1)

Publication Number Publication Date
EP2401422A2 true EP2401422A2 (fr) 2012-01-04

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Family Applications (1)

Application Number Title Priority Date Filing Date
EP10722522A Withdrawn EP2401422A2 (fr) 2009-01-09 2010-01-07 Procédé et dispositif de régénération de solutions de décapage contenant du peroxodisulfate

Country Status (3)

Country Link
EP (1) EP2401422A2 (fr)
DE (1) DE102009004155A1 (fr)
WO (1) WO2010078866A2 (fr)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102013114881A1 (de) 2013-12-25 2015-06-25 Brose Fahrzeugteile Gmbh & Co. Kommanditgesellschaft, Hallstadt Steuersystem für eine motorische Verschlusselementanordnung eines Kraftfahrzeugs
CN108531914A (zh) * 2018-06-15 2018-09-14 哈尔滨工业大学深圳研究生院 一种h2so4/s2o82-微蚀刻废液的铜回收及同步再生微蚀刻液系统及方法
CN113088981B (zh) * 2021-04-10 2022-06-24 贵州丝域环能科技有限公司 一种不锈钢酸洗钝化液的制备、处理及再生方法

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Publication number Priority date Publication date Assignee Title
DD211129B1 (de) 1982-11-05 1986-12-17 Hermann Matschiner Kreislaufverfahren zum beizen von kupfer und kupferlegierungen
DE3469041D1 (en) * 1983-10-06 1988-03-03 Olin Corp Process for cleaning copper base materials and regenerating the cleaning solution
DE4137022C2 (de) 1991-11-11 1993-11-25 Eilenburger Chemie Werk Gmbh Verfahren und Vorrichtung zur Regenerierung schwefelsaurer, kupferhaltiger Peroxodisulfat-Beizlösungen
DE4211555C1 (de) * 1992-04-06 1993-12-02 Eilenburger Chemie Werk Gmbh Bipolare Filterpressenzelle zur Herstellung von Peroxodisulfaten
DE19506832A1 (de) 1995-02-28 1996-08-29 Eilenburger Elektrolyse & Umwelttechnik Gmbh Kreislaufverfahren zum Beizen von Kupfer und Kupferlegierungen
DE19850530A1 (de) * 1998-11-03 2000-05-25 Eilenburger Elektrolyse & Umwelttechnik Gmbh Kreislaufverfahren zum Beizen von Kupfer und Kupferlegierungen
DE19948184C2 (de) 1999-10-06 2001-08-09 Fraunhofer Ges Forschung Elektrochemische Herstellung von Peroxo-dischwefelsäure unter Einsatz von diamantbeschichteten Elektroden
DE29919231U1 (de) * 1999-11-02 2000-01-27 Eilenburger Elektrolyse Und Um Geteilte Elektrolysezelle zur kathodischen Metallrückgewinnung und/oder zur anodischen Oxidation
DE19962672A1 (de) 1999-12-23 2001-06-28 Eilenburger Elektrolyse & Umwelttechnik Gmbh Verfahren und Vorrichtung zur Herstellung oder Regenerierung von Peroxodisulfaten
DE10019683A1 (de) 2000-04-20 2001-10-25 Degussa Verfahren zur Herstellung von Alkalimetall- und Ammoniumperoxodisulfat
DE10112075C1 (de) 2001-03-12 2002-10-31 Eilenburger Elektrolyse & Umwelttechnik Gmbh Verfahren und Vorrichtung zur Rückgewinnung von Metallen, auch in Kombination mit anodischen Koppelprozessen
DE10219688A1 (de) * 2002-05-02 2003-11-20 Condias Gmbh Verfahren und Vorrichtung zur oxidativen Behandlung von Oberflächen
DE102004027623A1 (de) * 2004-06-05 2005-12-22 Degussa Initiators Gmbh & Co. Kg Verfahren zur Herstellung von Peroxodisulfaten in wässriger Lösung

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Also Published As

Publication number Publication date
WO2010078866A3 (fr) 2010-10-14
DE102009004155A1 (de) 2010-07-15
WO2010078866A2 (fr) 2010-07-15

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