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WO2014025568A1 - Recovery of nickel using integrated continuous ion exchange and electo-winning process - Google Patents

Recovery of nickel using integrated continuous ion exchange and electo-winning process Download PDF

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Publication number
WO2014025568A1
WO2014025568A1 PCT/US2013/052608 US2013052608W WO2014025568A1 WO 2014025568 A1 WO2014025568 A1 WO 2014025568A1 US 2013052608 W US2013052608 W US 2013052608W WO 2014025568 A1 WO2014025568 A1 WO 2014025568A1
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Prior art keywords
nickel
ion exchange
solution
passing
exchange resin
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Ceased
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PCT/US2013/052608
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French (fr)
Inventor
Charles R. Marston
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Dow Global Technologies LLC
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Dow Global Technologies LLC
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Publication of WO2014025568A1 publication Critical patent/WO2014025568A1/en
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Classifications

    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B3/00Extraction of metal compounds from ores or concentrates by wet processes
    • C22B3/20Treatment or purification of solutions, e.g. obtained by leaching
    • C22B3/42Treatment or purification of solutions, e.g. obtained by leaching by ion-exchange extraction
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B23/00Obtaining nickel or cobalt
    • C22B23/04Obtaining nickel or cobalt by wet processes
    • C22B23/0453Treatment or purification of solutions, e.g. obtained by leaching
    • 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 present invention is directed toward a continuous ion exchange process for recovering nickel from a mixed metal product liquor solution.
  • CIX processes are used to recover metals from product liquor solutions (PLS), see for example WO 1996/20291 and C. Bailey et al., Removal of Nickel From Cobalt Sulphate Electrolyte Using ISEPTM Continuous Ion Exchange.
  • PLS product liquor solutions
  • CIX processes involve the use a metal recovery circuit including of a plurality of ion exchange beds, commonly arranged in carousal, which repetitively cycle through individual process zones including metal loading and elution.
  • US 7594951 describes a CIX process that includes an integrated electro- winning loop for recovering copper from the eluate.
  • interfering ions e.g. iron, sulfate
  • the described process is applicable for recovery of other metals such as nickel.
  • the present invention includes a system and method for recovering nickel from a mixed metal product liquor solution containing nickel and at least copper or iron comprising passing the product liquor solution through a plurality of ion exchange beds containing nickel selective ion exchange resin that pass through process zones as part of a repeating nickel recovery circuit.
  • the method includes the steps of: (a) passing the product liquor solution through an ion exchange bed to load nickel onto the ion exchange resin, and (b) passing a sulfuric acid solution through the loaded ion exchange bed to strip nickel from the ion exchange resin and produce an eluate having a pH less than 3.
  • the method is characterized by the additional steps of: (c) recovering the effluent and removing a portion of sulfuric acid sufficient to raise the pH of the effluent above 3, (d) electro- winning the eluate to produce electro-won nickel and a nickel-depleted raffinate, (e) combining at least a portion of the nickel-depleted raffinate with product liquor solution and repeating steps (a) through (d).
  • Figure 1 is schematic view of an embodiment the subject invention.
  • Figure 2 is a schematic view of an embodiment of a continuous exchange process applicable to the subject invention.
  • the present invention includes a system and method for recovering nickel from a mixed metal product liquor solution, sometimes also referred to as "pregnant leach solution,” hereinafter collectively abbreviated as "PLS".
  • PLS mixed metal product liquor solution
  • the source of the PLS is not particularly limited but is typically produced by heap leaching, vat leaching or pressure leaching lateritic ores.
  • the PLS includes a sulfuric acid solution including at least copper or iron, nickel and other acid soluble impurities.
  • the PLS preferably has a pH of less than 3, but more preferably less than 2.3 (e.g. from 1.3 to 2.2).
  • PLS is subject to continuous ion exchange (CIX) including the step of passing PLS through a plurality of ion exchange beds containing nickel selective ion exchange resin.
  • the beds pass through individual process zones as part of a repeating nickel recovery circuit that is described below.
  • the subject method further includes an integrated electro-winning cycle loop.
  • FIG. 1 provides a schematic overview of an embodiment of the invention including an integrated CIX and electro-winning system generally shown at 10.
  • the system includes a CIX unit (12) with multiple beds of nickel selective ion exchange resin for treating PLS (13), an acid removal unit (14) capable of removing a portion of sulfuric acid from the nickel eluate (16) exiting the CIX unit (12) in sufficient quantity to raise the pH above 3 (more preferably at least 3.2, 3.5 or even 4.0), an optional iron/copper removal unit (18) capable of removing a portion of iron or copper present in the pH adjusted eluate (20), and a nickel electro-winning unit (22) capable of electro-winning nickel from the eluate (24) resulting in a high grade nickel product (26) and a nickel depleted raffinate (28).
  • an acid removal unit (14) capable of removing a portion of sulfuric acid from the nickel eluate (16) exiting
  • the nickel depleted raffinate is recycled back to the CIX unit (12) and may be optionally supplemented with sulfuric acid (30).
  • the system (10) may optionally include an acid recovery unit (32) for recovering sulfuric acid from the acid removal unit (14) and returning the acid to the CIX (12), recycling back to the PLS (13), for storage or disposal.
  • FIG. 2 is a schematic overview of a CIX unit generally shown at 36 and adapted for use in the present method.
  • the unit includes a plurality of ion exchange beds containing nickel selective ion exchange resin (e.g. DOWEXTM M4195) that sequentially pass through individual process zones (e.g. A, B, C) as part of a nickel recovery circuit.
  • Each zone preferably includes at least one ion exchange bed or column, and in practice may include a plurality of individual beds.
  • the method includes the following sequential steps: (a) passing the PLS (13) through an ion exchange bed (zone A) to load nickel onto the ion exchange resin and produce a raffinate solution (38), and
  • the method may include additional process zones as is well known in the art, e.g. rinsing, washing, scrubbing.
  • additional process zones as is well known in the art, e.g. rinsing, washing, scrubbing.
  • optional Zone B is depicted as a rinsing step.
  • PLS, rinse solution (e.g. water), elution solution (e.g. 20% sulfuric acid) may be maintained in tanks, 13, 40, and 42 respectively. The tanks are in selective fluid communication with the ion exchange beds.
  • Fluid flow is controlled by a plurality of values and a control panel (not shown) as the beds cycle through the individual process zones (A, B and C).
  • CIX equipment for performing the subject method is available from PuriTech (e.g. IONEXTM), Ionex Separations and Calgon Carbon (e.g. ISEPTM) and is also described in US 7594951.
  • Suitable nickel selective ion exchange resins include DOWEXTM M4195 and XUS-43578 chelating resins available from The Dow Chemical Company. These resins include a styrene-divinylbenzene copolymer matrix with bis-picolylamine functional groups.
  • the acid removal unit (14) is not particularly limited and may include an acid retardation unit including a fixed bed of suitable anion exchange resin (e.g. AMBERSEPTM 4200 Sulfate or DOWEXTM 21K XLT Sulfate resins). See for example: M. J. Hatch, J. A. Dillon, Acid Retardation. Simple Physical Method for Separation of Strong Acids from Their Salts, Ind. Eng. Chem. Process Des. Dev., 1963, 2 (4), pp 253-263.
  • the acid removal unit (14) may include an engineered membrane system as described in Nystrom et al, MEMBRANE
  • the iron or copper removal unit (18) is not particularly limited and preferably includes an ion exchange resin, chelating resin or adsorbent that is selective for the metal or impurity of interest but is relatively non-selective for nickel.
  • the unit (18) may include a mixed bed of copper and iron selective resin such as AMBERLITE 747 or DIPHONIXTM resins.
  • the system operates according to a method characterized by the integration of CIX and electro-winning unit operations into a single continuous process with cost effective recycling of nickel-depleted raffinate (28) and optionally, acid (32). More specifically, the subject method includes the sequential steps of:
  • step (e) combining at least a portion of the nickel-depleted raffinate (28) with PLS (13) and repeating steps (a) through (d).
  • step (c) further includes the step of removing a portion of at least one of copper and iron (18) from the effluent (20), such as by way of ion exchange, chelation or adsorption.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Mechanical Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Geology (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Environmental & Geological Engineering (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Treatment Of Water By Ion Exchange (AREA)

Description

RECOVERY OF NICKEL USING INTEGRATED
CONTINUOUS ION EXCHANGE AND ELECTO-WINNING PROCESS FIELD
The present invention is directed toward a continuous ion exchange process for recovering nickel from a mixed metal product liquor solution.
INTRODUCTION
Continuous ion exchange (CIX) processes are used to recover metals from product liquor solutions (PLS), see for example WO 1996/20291 and C. Bailey et al., Removal of Nickel From Cobalt Sulphate Electrolyte Using ISEP™ Continuous Ion Exchange. In general, CIX processes involve the use a metal recovery circuit including of a plurality of ion exchange beds, commonly arranged in carousal, which repetitively cycle through individual process zones including metal loading and elution. US 7594951 describes a CIX process that includes an integrated electro- winning loop for recovering copper from the eluate. Unfortunately, interfering ions (e.g. iron, sulfate) quickly build up in the system and interfere with the intended electrochemistry of the electro-winning operation. This in turn requires eluate to be bled from the system or completely replaced. Given the low pH values of the eluate (e.g. less than 0.5), the described process is applicable for recovery of other metals such as nickel.
SUMMARY
The present invention includes a system and method for recovering nickel from a mixed metal product liquor solution containing nickel and at least copper or iron comprising passing the product liquor solution through a plurality of ion exchange beds containing nickel selective ion exchange resin that pass through process zones as part of a repeating nickel recovery circuit. In one embodiment, the method includes the steps of: (a) passing the product liquor solution through an ion exchange bed to load nickel onto the ion exchange resin, and (b) passing a sulfuric acid solution through the loaded ion exchange bed to strip nickel from the ion exchange resin and produce an eluate having a pH less than 3. The method is characterized by the additional steps of: (c) recovering the effluent and removing a portion of sulfuric acid sufficient to raise the pH of the effluent above 3, (d) electro- winning the eluate to produce electro-won nickel and a nickel-depleted raffinate, (e) combining at least a portion of the nickel-depleted raffinate with product liquor solution and repeating steps (a) through (d). Many additional embodiments are described. BRIEF DESCRIPTION OF THE DRAWINGS
Figure 1 is schematic view of an embodiment the subject invention.
Figure 2 is a schematic view of an embodiment of a continuous exchange process applicable to the subject invention.
DETAILED DESCRIPTION
The present invention includes a system and method for recovering nickel from a mixed metal product liquor solution, sometimes also referred to as "pregnant leach solution," hereinafter collectively abbreviated as "PLS". The source of the PLS is not particularly limited but is typically produced by heap leaching, vat leaching or pressure leaching lateritic ores. The PLS includes a sulfuric acid solution including at least copper or iron, nickel and other acid soluble impurities. The PLS preferably has a pH of less than 3, but more preferably less than 2.3 (e.g. from 1.3 to 2.2).
As part of the subject method, PLS is subject to continuous ion exchange (CIX) including the step of passing PLS through a plurality of ion exchange beds containing nickel selective ion exchange resin. The beds pass through individual process zones as part of a repeating nickel recovery circuit that is described below. In a preferred embodiment, the subject method further includes an integrated electro-winning cycle loop.
Figure 1 provides a schematic overview of an embodiment of the invention including an integrated CIX and electro-winning system generally shown at 10. The system includes a CIX unit (12) with multiple beds of nickel selective ion exchange resin for treating PLS (13), an acid removal unit (14) capable of removing a portion of sulfuric acid from the nickel eluate (16) exiting the CIX unit (12) in sufficient quantity to raise the pH above 3 (more preferably at least 3.2, 3.5 or even 4.0), an optional iron/copper removal unit (18) capable of removing a portion of iron or copper present in the pH adjusted eluate (20), and a nickel electro-winning unit (22) capable of electro-winning nickel from the eluate (24) resulting in a high grade nickel product (26) and a nickel depleted raffinate (28). The nickel depleted raffinate is recycled back to the CIX unit (12) and may be optionally supplemented with sulfuric acid (30). The system (10) may optionally include an acid recovery unit (32) for recovering sulfuric acid from the acid removal unit (14) and returning the acid to the CIX (12), recycling back to the PLS (13), for storage or disposal.
Figure 2 is a schematic overview of a CIX unit generally shown at 36 and adapted for use in the present method. The unit includes a plurality of ion exchange beds containing nickel selective ion exchange resin (e.g. DOWEX™ M4195) that sequentially pass through individual process zones (e.g. A, B, C) as part of a nickel recovery circuit. Each zone preferably includes at least one ion exchange bed or column, and in practice may include a plurality of individual beds. The method includes the following sequential steps: (a) passing the PLS (13) through an ion exchange bed (zone A) to load nickel onto the ion exchange resin and produce a raffinate solution (38), and
(b) passing a sulfuric acid solution (42) through the loaded ion exchange bed (zone C) to strip nickel from the ion exchange resin and produce an eluate (16) having a pH less than 3 (2.5, 2.3). The method may include additional process zones as is well known in the art, e.g. rinsing, washing, scrubbing. For example, optional Zone B is depicted as a rinsing step. PLS, rinse solution (e.g. water), elution solution (e.g. 20% sulfuric acid) may be maintained in tanks, 13, 40, and 42 respectively. The tanks are in selective fluid communication with the ion exchange beds. Fluid flow is controlled by a plurality of values and a control panel (not shown) as the beds cycle through the individual process zones (A, B and C). CIX equipment for performing the subject method is available from PuriTech (e.g. IONEX™), Ionex Separations and Calgon Carbon (e.g. ISEP™) and is also described in US 7594951. Suitable nickel selective ion exchange resins include DOWEX™ M4195 and XUS-43578 chelating resins available from The Dow Chemical Company. These resins include a styrene-divinylbenzene copolymer matrix with bis-picolylamine functional groups.
The acid removal unit (14) is not particularly limited and may include an acid retardation unit including a fixed bed of suitable anion exchange resin (e.g. AMBERSEP™ 4200 Sulfate or DOWEX™ 21K XLT Sulfate resins). See for example: M. J. Hatch, J. A. Dillon, Acid Retardation. Simple Physical Method for Separation of Strong Acids from Their Salts, Ind. Eng. Chem. Process Des. Dev., 1963, 2 (4), pp 253-263. By way of further example, the acid removal unit (14) may include an engineered membrane system as described in Nystrom et al, MEMBRANE
TECHNOLOGY, Volume 2000, Issue 117, January 2000, Pages 5-9.
The iron or copper removal unit (18) is not particularly limited and preferably includes an ion exchange resin, chelating resin or adsorbent that is selective for the metal or impurity of interest but is relatively non-selective for nickel. For example, the unit (18) may include a mixed bed of copper and iron selective resin such as AMBERLITE 747 or DIPHONIX™ resins.
The system operates according to a method characterized by the integration of CIX and electro-winning unit operations into a single continuous process with cost effective recycling of nickel-depleted raffinate (28) and optionally, acid (32). More specifically, the subject method includes the sequential steps of:
(a) passing the PLS (13) through an ion exchange bed (12; zone A) to load nickel onto the ion exchange resin and produce a raffinate solution (38),
(b) passing a sulfuric acid solution (42) through the loaded ion exchange bed (zone C) to strip nickel from the ion exchange resin and produce an eluate (16) having a pH less than 3, more preferably less than 2.5 and still more preferably less than 2.3, (c) recovering the effluent (16) and removing a portion of sulfuric acid (14) sufficient to raise the pH above 3, more preferably above 3.2 and still more preferably to at least 3.5,
(d) electro-winning (22) the eluate (24) to produce electro- won nickel (26) and a nickel-depleted raffinate (28), and
(e) combining at least a portion of the nickel-depleted raffinate (28) with PLS (13) and repeating steps (a) through (d). In a preferred embodiment, step (c) further includes the step of removing a portion of at least one of copper and iron (18) from the effluent (20), such as by way of ion exchange, chelation or adsorption.
Many embodiments of the invention have been described and in some instances certain embodiments, selections, ranges, constituents, or other features have been characterized as being "preferred." Characterizations of "preferred" features should in no way be interpreted as deeming such features as being required, essential or critical to the invention. Stated ranges include end points. The entire subject matter of each of the aforementioned patent documents is incorporated herein by reference.

Claims

CLAIMS:
1. A method for recovering nickel from a mixed metal product liquor solution containing nickel and at least copper or iron comprising passing the product liquor solution through a plurality of ion exchange beds containing nickel selective ion exchange resin that pass through process zones as part of a repeating nickel recovery circuit, wherein the method comprises the steps of:
(a) passing the product liquor solution through an ion exchange bed to load nickel onto the ion exchange resin (and produce a raffinate solution), and
(b) passing a sulfuric acid solution through the loaded ion exchange bed to strip nickel from the ion exchange resin and produce an eluate having a pH less than 3,
wherein the method is characterized by the steps of:
(c) recovering the effluent and removing a portion of sulfuric acid sufficient to raise the pH of the effluent above 3,
(d) electro-winning the eluate to produce electro-won nickel and a nickel-depleted raffinate,
(e) combining at least a portion of the nickel-depleted raffinate with product liquor solution and repeating steps (a) through (d).
2. The method of claim 1 wherein step (c) further comprises removing a portion of at least one of copper and iron from the effluent.
PCT/US2013/052608 2012-08-06 2013-07-30 Recovery of nickel using integrated continuous ion exchange and electo-winning process Ceased WO2014025568A1 (en)

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US201261679808P 2012-08-06 2012-08-06
US61/679,808 2012-08-06

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108658320A (en) * 2018-05-02 2018-10-16 中国科学院生态环境研究中心 A method of chemically recycling heavy metal nickel in nickel-plating waste water
CN108821485A (en) * 2018-05-02 2018-11-16 中国科学院生态环境研究中心 A kind of method of optical electro-chemistry processing chemical nickle-plating wastewater

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1996020291A1 (en) 1994-12-27 1996-07-04 Bhp Minerals International Inc. Recovery of nickel and cobalt from laterite ores
US20010001650A1 (en) * 1999-03-09 2001-05-24 William P.C. Duyvesteyn Recovery of nickel and cobalt from ore
WO2008128278A2 (en) * 2007-04-19 2008-10-30 Metallica Minerals Ltd Treatment of nickel-containing solutions
US7594951B2 (en) 2005-12-07 2009-09-29 Gordon Rossiter Process for engineered ion exchange recovery of copper and nickel

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1996020291A1 (en) 1994-12-27 1996-07-04 Bhp Minerals International Inc. Recovery of nickel and cobalt from laterite ores
US20010001650A1 (en) * 1999-03-09 2001-05-24 William P.C. Duyvesteyn Recovery of nickel and cobalt from ore
US7594951B2 (en) 2005-12-07 2009-09-29 Gordon Rossiter Process for engineered ion exchange recovery of copper and nickel
WO2008128278A2 (en) * 2007-04-19 2008-10-30 Metallica Minerals Ltd Treatment of nickel-containing solutions

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
M. J. HATCH; J. A. DILLON: "Acid Retardation. Simple Physical Method for Separation of Strong Acids from Their Salts", IND. ENG. CHEM. PROCESS DES. DEV., vol. 2, no. 4, 1963, pages 253 - 263
NYSTROM ET AL., MEMBRANE TECHNOLOGY, vol. 117, January 2000 (2000-01-01), pages 5 - 9

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108658320A (en) * 2018-05-02 2018-10-16 中国科学院生态环境研究中心 A method of chemically recycling heavy metal nickel in nickel-plating waste water
CN108821485A (en) * 2018-05-02 2018-11-16 中国科学院生态环境研究中心 A kind of method of optical electro-chemistry processing chemical nickle-plating wastewater

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