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EP3339480B1 - Production électrochimique de métaux et d'alliages de terres rares comprenant une anode liquide - Google Patents

Production électrochimique de métaux et d'alliages de terres rares comprenant une anode liquide Download PDF

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Publication number
EP3339480B1
EP3339480B1 EP16205757.4A EP16205757A EP3339480B1 EP 3339480 B1 EP3339480 B1 EP 3339480B1 EP 16205757 A EP16205757 A EP 16205757A EP 3339480 B1 EP3339480 B1 EP 3339480B1
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EP
European Patent Office
Prior art keywords
liquid
anode
cathode
alloy
compartment
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EP16205757.4A
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German (de)
English (en)
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EP3339480A1 (fr
Inventor
Ana Maria Martinez CUELLAR
Arne Petter Ratvik
Karen Sende OSEN
Bjarte Arne Øye
ASBJøRN SOLHEIM
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SINTEF TTO AS
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SINTEF TTO AS
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Priority to EP16205757.4A priority Critical patent/EP3339480B1/fr
Priority to PCT/EP2017/083504 priority patent/WO2018114925A1/fr
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    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C3/00—Electrolytic production, recovery or refining of metals by electrolysis of melts
    • C25C3/34—Electrolytic production, recovery or refining of metals by electrolysis of melts of metals not provided for in groups C25C3/02 - C25C3/32
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C3/00—Electrolytic production, recovery or refining of metals by electrolysis of melts
    • C25C3/36—Alloys obtained by cathodic reduction of all their ions
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
    • C25C7/005—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells of cells for the electrolysis of melts
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
    • C25C7/02—Electrodes; Connections thereof
    • C25C7/025—Electrodes; Connections thereof used in cells for the electrolysis of melts

Definitions

  • the present invention is related to electrochemical production of rare earth alloys and metals, and especially to a one-step electrochemical production method comprising a liquid anode.
  • Rare earth alloys and metals are important ingredients in modern electronic components like semiconductors, but also in products like permanent magnets etc.
  • the Peoples Republic of China is dominating the production of rare earth (RE), and for example, in 2011 the Chinese production covered 97 % of the world market.
  • RE rare earth
  • the geological availability and distribution of RE is unevenly distributed around the world and it is therefore an international interest in developing alternative second sources of RE materials mitigating any problems related to higher prices and reliable and sustainable delivery of RE alloys and metals.
  • Prior art electrochemical refining of metals is applied both in aqueous and molten salt electrochemical processes.
  • the refining is commonly based on an impure metal containing anode being refined to a pure cathode. More noble impurities remain in the anode or anode compartment and less noble substances accumulate in the electrolyte.
  • An example of prior art is the three-layer refining of liquid aluminium dissolved in a copper containing alloy invented by Hoopes and patented in 1925.
  • the refining process takes place in a vertically arranged molten salt cell, wherein the aluminium dissolved in the copper alloy is arranged at the bottom of the cell, and the refined pure aluminium is floating at the top of the electrolyte.
  • the prior art documents CN 104 789 991 A and US2961387 A relates to electrolysis processes using the Hoopes principles.
  • a common technique in prior art when recycling used permanent magnets and scrap metals comprises a step of oxidizing the permanent magnet and scrap metal materials followed by a purifying step and electrolysis of oxidized materials dissolved in a molten salt.
  • CN 103409649B disclosing a liquid metal and molten salt reduction method and apparatus for extraction and separation of rare earth metals comprising a liquid aluminium cathode and an anode graphite rod added to a heated bath melted as an electrolyte. Lithium aluminium-lithium alloy is dissolved in the liquid aluminium.
  • Recovering RE alloys and metals from a specific electrochemical process is also subject to cost/benefit assessments in addition to environmental considerations.
  • the cost of recovered RE alloys and metals has to be on a level accepted by end users of the recovered materials. Therefore, there is a need of improved methods recovering compounds comprising rare earth, and/or rear earth alloys and/or rear earth metals.
  • An aspect of the present invention is to reduce the number of process steps, and at the same time increase output of rare earth alloys and metals from the process.
  • the present invention is based on an alloy system with high solubility of the actual rare earth metal(s) or rare earth alloy(s).
  • RE rear earth
  • a second aspect of the invention relates to an electrochemical production cell as stated in the independent claim 10
  • a parameter of interest when designing an electrolysis cell is the kinetics of the electrodes. It is believed that liquid anodes perform better in this respect than an anode consisting of solid chunks of alloys when refining rare earth elements.
  • FIG. 1 a different cell design according to the present invention with a liquid anode is schematically illustrated in Figure 1 .
  • the rare earth containing raw material is placed in the anode compartment 10 from where the RE present in the raw material (for example Nd, Dy, Pr) will be anodically dissolved in the form of ions, which will be discharged at the cathode 11 as metals and/or magnetic rare earth alloys 12.
  • the recovery of REs from the raw material can be extracted, and a valuable product (RE or alloy) can be obtained in one single electrochemical step.
  • a high temperature providing a liquid state of the used permanent magnets for example.
  • the melting point of most permanent magnets is about 1400 °C.
  • the high temperature is a challenge since the temperature may enhance corrosion of the cell materials. Therefore, according to an aspect of the present invention, a desired working temperature is below 1100 °C.
  • Providing a lower melting point when recycling permanent magnets and/or scrap metal comprising Fe can be achieved by adding low melting point materials known to achieve such an effect.
  • low melting point materials known to achieve such an effect.
  • a permanent magnet comprising Nd it is known that Cu forms low melting phases with Nd, but not with Fe.
  • Al the inventors has demonstrated that Al forms low melting areas with Nd and Fe in the Al rich regions. Calculating a ternary phase diagram of Al-Nd-Fe can be achieved with commercially available thermodynamic computer programs like FactSage as known in prior art. The same demonstration has been performed with other RE elements with similar results.
  • Si forms low melting point alloys with several elements like Cu and Al.
  • phase diagram reveals a relative large region of molten Fe-Al-Si alloys of different compositions that exist below a temperature of 1050 °C.
  • liquid content of Fe at 1050 °C varies from 20 wt% without Si present to a maximum of 50 wt% when Si is present.
  • Al-Si alloys are commercially available, which is an important aspect when considering commercial applications of a liquid anode according to the present invention comprising AlSi.
  • AlSi is added to the liquid anode.
  • Figure 2 illustrates examples of how liquidus curves of the quaternary system of AlSi-Fe-Nd can be obtained. The same type of illustrations is valid for other RE elements.
  • the cross sections of the AlSi-Fe-RE system from contact lines between the AISi corner and the Fe-RE (for example Nd) side of the triangle in figure 2 will provide liquidus curves enabling a prediction of melting points of the anode alloy when the electrolysis proceeds and the content of respectively RE and Fe decreases and increases.
  • Table 1 Alloy# Al:Si composition wt%:wt% Composition Al:Si: Magnet wt%:wt% wt% Remarks 1 70:30 54:23:23 Homogeneous 2 70:30 48:21:31 Homogeneous 3 70:30 44:19:37 Homogeneous 4 90:10 54:6:40 Homogeneous
  • a liquid anode is formed of aluminium and silicon and dissolved RE alloys with iron and boron (Al-Si-Fe-RE-B).
  • the liquid anode is forming a multinary liquid alloy system having a larger liquid domain for the RE, RE alloys or RE metals dissolved in the liquid anode. Further, the multinary liquid alloy system is provided with metal elements being more noble than the RE or the RE containing alloy(s) to be recycled.
  • a method of recycling RE alloys and/or RE metals from raw materials including permanent magnets and/or scrap metals containing RE and iron (Fe) in an electrochemical process from a molten salt comprises the steps of:
  • the added specific amounts of respectively Al and Si elements are forming a multinary liquid alloy system having a working temperature below the melting point of the rare earth containing metallic raw material, preferable in the range of 1000-1100 °C.
  • the working temperature of the liquid anode may be 1050 °C.
  • the cathode may be a Fe cathode and the reactions are as follows: anode: RE-alloy (liquid) -> RE(III) + alloy anode (liquid) + 3e - cathode: RE(III) + Fe(solid) + 3e - -> RE-Fe (liquid).
  • the step of dissolving permanent magnetic material may provide a liquid anode comprising Al-Si-Fe-RE-B.
  • the permanent magnets may be Nd based permanent magnets.
  • the cathode may be a solid cathode and the step of collecting recycled elements comprises collecting the RE(s) or RE alloy(s) in solid form.
  • the step of collecting the RE(s) or RE alloy(s) may comprise collecting liquid iron-RE(s) alloys formed through a reaction on a consumable iron cathode.
  • the RE containing permanent magnets and/or scrap metals may be delivered into the liquid anode compartment from a feeding chamber.
  • FIG. 3 illustrates an example of principles of a functional cell according to the present invention.
  • a tube or canal 20 provides transport of waste material to be recycled into the molten alloy being part of the liquid anode 21 residing in a compartment.
  • An electric lead 22 is connected to a positive electric pole 23 of the power supply.
  • the electric lead 22 is connected to a finger like electrode configuration being arranged inside the molten alloy.
  • the cathode 24 is connected to the negative pole of the power supply and at the bottom of the cell below the cathode a compartment is arranged receiving cathode products.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Electrolytic Production Of Metals (AREA)
  • Manufacture And Refinement Of Metals (AREA)

Claims (10)

  1. Procédé de recyclage d'alliages terres rares (TR) et/ou de métaux TR à partir de matières premières comportant des aimants permanents et/ou des ferrailles contenant des TR et du fer (Fe), dans un processus électrochimique à partir d'un sel fondu comprenant les étapes suivantes :
    - l'agencement d'une cellule d'électrolyse comprenant une anode liquide (21) résidant dans un compartiment d'anode en communication avec un conducteur électrique (22) de l'anode liquide, une cathode (24) et un compartiment agencé sous la cathode au fond de la cellule collectant des éléments recyclés raffinés à l'état liquide ou solide, séparés par un électrolyte liquide à base de fluorure,
    - l'alimentation des matières premières dans le compartiment d'anode liquide,
    - l'anode liquide forme un système d'alliage liquide multinaire lorsque les matières premières alimentées dans le compartiment d'anode sont dissoutes,
    - l'anode liquide comprend de l'Al et du Si ajoutés en quantités fournissant une température de point de fusion des matières ajoutées à l'intérieur du compartiment d'anode inférieure à la température de point de fusion des matières premières elles-mêmes,
    - les quantités ajoutées d'AI et de Si sont en outre sélectionnées pour fournir une région à basse température de fusion d'alliages d'Al-Si pouvant dissoudre le Fe, et une quantité en % en poids maximale ou suffisante pour maintenir les alliages Fe-Al-Si-TR fondus de différentes compositions,
    - la collecte du métal / des métaux TR ou du / des alliage(s) TR recyclé(s) raffiné(s) dans le compartiment sous la cathode au fond de la cellule d'électrolyse.
  2. Procédé selon la revendication 1, dans lequel des quantités spécifiques ajoutées d'éléments respectivement Al et Si forment un système d'alliage liquide multinaire ayant une température de travail inférieure au point de fusion du métal / des métaux TR ou du / des alliage(s) contenant des TR, de préférence dans la plage comprise entre 1 000 et 1 100 °C.
  3. Procédé selon la revendication 2, dans lequel la température de travail de l'anode liquide est de 1 050 °C.
  4. Procédé selon la revendication 1, dans lequel la cathode est une cathode en Fe et les réactions sont les suivantes : anode : alliage TR (liquide) -> TR(III) + anode en alliage (liquide) + 3e- cathode : TR(III) + Fe (solide) + 3e- -> TR-Fe (liquide).
  5. Procédé selon l'une quelconque des revendications 1 à 4, dans lequel l'étape de dissolution de la matière première fournit une anode liquide comprenant AI-Si-Fe-TR-B.
  6. Procédé selon l'une quelconque des revendications 1 à 5, dans lequel la matière première est des aimants permanents à base de Nd.
  7. Procédé selon la revendication 1, dans lequel la cathode est une cathode solide et l'étape de collecte d'éléments recyclés raffinés comprend la collecte du métal / des métaux TR ou du / des alliage(s) TR sous forme solide.
  8. Procédé selon la revendication 1, dans lequel l'étape de collecte du métal / des métaux TR ou du / des alliage(s) TR comprend la collecte du / des alliage(s) fer-TR liquide(s) formé(s) par réaction sur une cathode en fer consommable.
  9. Procédé selon la revendication 1, dans lequel les matières premières sont délivrées dans le compartiment d'anode liquide à partir d'une chambre d'alimentation.
  10. Cellule de production électrochimique agencée pour exécuter un procédé selon l'une quelconque des revendications 1 à 9, comprenant :
    - une anode liquide (21) qui comprend des quantités ajoutées d'AI et de Si telle que définie selon la revendication 1 et qui réside dans un compartiment d'anode, l'anode liquide (21) étant connectée à un pôle électrique positif (23) par l'intermédiaire d'un conducteur électrique (22), et
    - une cathode (24) connectée à un pôle négatif, la cathode étant séparée de l'anode liquide par un électrolyte liquide à base de fluorure, et
    - un compartiment de collecte du métal / des métaux TR ou du / des alliage(s) TR recyclé(s) raffiné(s) est disposé sous la cathode (24) au fond de la cellule électrochimique et dans laquelle la cellule comprend un tube ou un canal (20) pour le transport des déchets dans l'anode liquide (21).
EP16205757.4A 2016-12-21 2016-12-21 Production électrochimique de métaux et d'alliages de terres rares comprenant une anode liquide Active EP3339480B1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
EP16205757.4A EP3339480B1 (fr) 2016-12-21 2016-12-21 Production électrochimique de métaux et d'alliages de terres rares comprenant une anode liquide
PCT/EP2017/083504 WO2018114925A1 (fr) 2016-12-21 2017-12-19 Production électrochimique d'alliages et de métaux des terres rares comprenant une anode liquide immergée

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP16205757.4A EP3339480B1 (fr) 2016-12-21 2016-12-21 Production électrochimique de métaux et d'alliages de terres rares comprenant une anode liquide

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EP3339480A1 EP3339480A1 (fr) 2018-06-27
EP3339480B1 true EP3339480B1 (fr) 2021-01-13

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114590874B (zh) * 2020-12-04 2023-12-08 香港科技大学 垃圾渗滤液反渗透浓缩液的双重电化学处理方法及其装置
CN115305520A (zh) * 2021-05-08 2022-11-08 郑州大学 制备稀土金属的方法

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US2961387A (en) * 1957-09-18 1960-11-22 Timax Corp Electrolysis of rare-earth elements and yttrium
US5427657A (en) * 1994-05-19 1995-06-27 General Motors Corporation Fused fluoride electrolytes for magnesium oxide electrolysis in the production of magnesium metal
ATE229578T1 (de) * 1995-10-25 2002-12-15 Santoku Corp Verfahren zur herstellung von seltenen erdmetallen
JP6057250B2 (ja) * 2012-09-10 2017-01-11 国立大学法人名古屋大学 希土類金属の回収方法および回収装置
CN103409649B (zh) 2013-06-05 2015-02-25 哈尔滨工程大学 一种熔盐与液态金属还原萃取分离稀土的方法及其装置
CN104789991B (zh) * 2015-05-13 2017-01-25 江西理工大学 电解精炼及原位定向凝固制备高纯稀土金属的方法和装置

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