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CA2525466A1 - Re-activation of de-activated nickel for nickel carbonyl production - Google Patents

Re-activation of de-activated nickel for nickel carbonyl production Download PDF

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Publication number
CA2525466A1
CA2525466A1 CA002525466A CA2525466A CA2525466A1 CA 2525466 A1 CA2525466 A1 CA 2525466A1 CA 002525466 A CA002525466 A CA 002525466A CA 2525466 A CA2525466 A CA 2525466A CA 2525466 A1 CA2525466 A1 CA 2525466A1
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Canada
Prior art keywords
nickel
carbon monoxide
carbonyl
hydrogen
gaseous mixture
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.)
Abandoned
Application number
CA002525466A
Other languages
French (fr)
Inventor
Kamran M. Khozan
Hermenegilda D. Zeta
Andres M. Torres
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.)
CVMR Corp
Original Assignee
Reprotech Ltd
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 Reprotech Ltd filed Critical Reprotech Ltd
Priority to CA002525466A priority Critical patent/CA2525466A1/en
Publication of CA2525466A1 publication Critical patent/CA2525466A1/en
Abandoned legal-status Critical Current

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    • 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
    • C22B23/06Refining
    • C22B23/065Refining carbonyl methods
    • 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

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Chemical Vapour Deposition (AREA)

Abstract

A process and apparatus for the production of a deposited metallic nickel product from an inactivated, pre-activated metallic nickel source, the process including treating the nickel source with hydrogen at a nickel activation temperature selected from 150-350°C, preferably, 150°C to effect re-activation of the nickel source;
treating the re-activated nickel with carbonylation carbon monoxide to produce a gaseous mixture containing nickel carbonyl and carbon monoxide; collecting the nickel carbonyl gaseous mixture;
and decomposing the nickel carbonyl in the gaseous mixture to produce the nickel product, and a resultant carbon monoxide gaseous mixture which is most preferably recycled back to treat the nickel source. The process provides efficacious re-activation of the de-activated nickel without the need for hydrogen sulfide or chloride anion.

Description

RE-ACTNATION OF DE-ACTIVATED NICKEL FOR
NICKEL CARBONYL PRODUCTION
FIELD OF THE INVENTION

This invention relates to a process for the re-activation of de-activated metallic nickel in the production of nickel carbonyl and subsequent deposition of metallic nickel product, therefrom; and apparatus of use in said process. The process, optionally, includes the 10 analogous process for the re-activation of de-activated iron to produce a ferronickel product.

BACKGROUND OF THE INVENTION

Nickel carbonyl, Ni(CO)4, was first produced by the reaction of metallic nickel with carbon monoxide by Mond in the early part of the 19th century. Today, one of the major industrial processes for making metallic nickel is based on the production of Ni(CO)4 and subsequent thermal decomposition thereof to Ni and CO. One known commercial process operates at about 180 C and a CO pressure of about 70 atm. It is known that the CO pressure may be reduced when the reactant nickel is catalytically activated.
Activation of the metal has been observed in the presence of mercury, sulfur in the form of H2S, hydrogen or carbon. It has been suggested that the high initial rate of formation of Ni(CO)4 and the subsequent decline to a steady state value is the result of a rapid decrease in the number of activated reaction sites which are produced upon heat treatment of the sample. A study of surface changes during carbonyl synthesis suggests that the maximum rate is associated with fundamental changes in the defect structure. All of the above methods use catalytic activation of nickel in the presence of CO.
However, it can be readily appreciated that processes that at atmospheric pressure can produce nickel, particularly, activated nickel for subsequent reaction with CO
at atmospheric pressure would provide significant capital and operating cost advantages.
Further, it can also be appreciated that processes that enable Ni(CO)4 to be manufactured at a sufficient rate as to obviate the need for storage in order to build up a sufficient supply for practical, efficient use in a subsequent nickel deposition process, would also offer significant capital and operating cost savings. To-date, in commercial operations rate limitations on the production of Ni(CO)4 require such storage facilities and operations.
There is, thus, a desire for an improved method of Ni(CO)4 production which is operable at atmospheric pressure and which is of a sufficient rate as to negate the need for storage of the Ni(CO)4 prior to use in a subsequent decomposition and/or deposition process.
Canadian Patent No. 2,461,624, published 27 September 2004 to Chemical Vapour Metal Refining Inc., describes a process for producing activated nickel for subsequent carbonylation at an efficacious rate using hydrogen in the presence of a chloride anion, preferably gaseous hydrochloric acid.
One of the disadvantages of activated nickel is that it is readily de-activated in the presence of air and moisture, and, therefore, should be utilized in the manufacture of nickel carbonyl as soon as practicable. However, de-activation of freshly prepared activated nickel inevitably occurs during transfer or storage unless stringent precautions are taken. Thus, there is a need for a means of readily re-activating de-activated nickel to a sufficient degree to facilitate the production of nickel carbonyl therefrom.
Although it is possible to use the aforesaid nickel activation processes according to the prior art, namely, gaseous HC1, H2S or H2/CI-, such entities do not also provide ready and convenient methods of re-activation.
Accordingly, there is a need for an improved process for re-activating nickel which has been allowed to become de-activated.

SUMMARY OF THE INVENTION

It is an object of the present invention to provide an improved, convenient and efficacious process for re-activating deactivated nickel.
It is a further object to, preferably, provide said process as part of a nickel carbonyl production and deposition process for the production of pure nickel product.
It is a further object to provide an aforesaid process incorporating a carbon monoxide closed-loop arrangement.
It is a further object to provide said aforesaid processes modified to provide a ferronickel material .
2 It is a further object of the invention to provide apparatus of use in the aforesaid processes.
We have surprisingly discovered that hydrogen can efficaciously re-activate de-activated nickel to enable the resultant activated nickel to react with carbon monoxide to produce nickel carbonyl at a satisfactory rate.
Accordingly, in one aspect the invention provide a process for the production of a deposited metallic nickel product from an inactivated, pre-activated metallic nickel source, said process comprising treating said nickel source with hydrogen at a nickel activation temperature selected from 150-350 C to effect re-activation of said nickel source;
treating said re-activated nickel with carbonylation carbon monoxide to produce a gaseous mixture comprising nickel carbonyl and carbon monoxide;
collecting said nickel carbonyl gaseous mixture; and decomposing said nickel carbonyl in said gaseous mixture to produce said nickel product, and a resultant carbon monoxide gaseous mixture.
Preferably, the temperature is selected from 150-200 C. Most preferably and, surprisingly, the temperature can be as low as about 150 C.
The resultant carbon monoxide gaseous mixture is, preferably, recycled to treat the nickel source to constitute in whole or in part the carbonylation carbon monoxide.
The subsequent carbonylation temperature is selected from 40-80 C, and, preferably, about 50 C.
The process as hereinabove defined may be modified to produce a deposited ferronickel alloy by incorporating an analogous process with iron carbonyl, Fe(CO)5, preferably, but not limited to Fe(CO)5 made from re-activated, de-activated iron.
Accordingly, in a further aspect, the invention provides a process as hereinabove defined further comprising treating a metallic iron source with hydrogen at an iron activation temperature selected from 150-350 C to produce activated iron;
treating said activated iron with carbonylation carbon monoxide to produce a gaseous mixture comprising iron carbonyl and carbon monoxide;
collecting said iron carbonyl gaseous mixture;
combining said nickel carbonyl gaseous mixture and said iron carbonyl gaseous mixture to produce a combiried gaseous mixture; and
3 decomposing said nickel carbonyl and said iron carbonyl in said combined mixture to produce a ferronickel product and a resultant carbon monoxide combined gaseous mixture.
Preferably, the iron activation temperature is selected from 150-200 C, and more preferably, about 50 C..
Most preferably, the invention provides a process, as hereinabove defined, wherein the metallic iron source is in admixture with the metallic nickel source when the metallic nickel source and the metallic iron source are treated with the hydrogen.
In a further aspect, the invention provides a process for the production of a deposited metallic nickel product from an inactivated, pre-activated metallic nickel source, said process 10 comprising treating said nickel source with hydrogen at a nickel activation temperature selected from 150-350 C to effect re-activation of said nickel source;
treating said re-activated nickel with carbonylation carbon monoxide to produce a gaseous mixture comprising nickel carbonyl and carbon monoxide;
collecting said nickel carbonyl gaseous mixture; and decomposing said nickel carbonyl in said gaseous mixture to produce said nickel product, and a resultant carbon monoxide gaseous mixture.
Preferably, the reaction chamber outlet conduit means comprises (i) reaction chamber outlet hydrogen conduit means;
(ii) reaction chamber outlet carbon monoxide conduit means; and (iii) hydrogen selective outlet valve means separating said outlet hydrogen conduit means from said outlet carbon monoxide conduit means.
More preferably, the reactor inlet conduit means comprises (i) reactor inlet hydrogen conduit means;
(ii) reactor inlet carbon monoxide conduit means; and (iii) selective inlet valve means separating said inlet hydrogen conduit means from said inlet carbon monoxide conduit means.
Further, preferably the means for feeding carbon monoxide to the reactor is in communication with the deposition chamber outlet means and the reactor inlet means.
BRIEF DESCRIPTION OF THE DRAWINGS
4 In order that the invention may be better understood, preferred embodiments will now be described, by way of example only, with reference to the accompanying drawing, wherein:-Fig. I is a diagrammatic flow diagram of a self-contained, closed-loop process and apparatus, according to the invention.

DETAILED DESCRIPTION OF PREFERRED EMBODIMENTS

With reference to Fig. 1, this shows generally as 10, a closed-loop apparatus comprising a reactor 12 linked to decomposition chamber 14 by conduits 16 and 18.
Reactor 12 has an inlet conduit 20 whereby hydrogen and carbon monoxide are alternatively fed, when desired, into reactor 12. Conduit 18 has connectors to hydrogen source 22 and initial carbon monoxide source 24 for passage to inlet conduit 20 through conduits 26,28 respectively when required as hereinafter described. Conduit 18 has a selector valve 30 and an initial source valve 32 for controlling the passage of carbon monoxide from chamber 14 or initial source 24 when desired, to inlet conduit 20. Control of hydrogen to inlet conduit 20, via conduit 18, for the initial activation reaction is by selection valve 34.
Reactor 12 has outlet conduit 36 through which, initially, exits spent hydrogen, to part of conduit 16, and, alternatively, spent carbon monoxide/nickel carbonyl gaseous mixture through the full length of conduit 16 to deposition chamber 14.
Conduit 18 has a selection valve 38 which directs the flow of hydrogen or carbon monoxide/nickel carbonyl, alternatively, when desired to the respective locations. The hydrogen may be collected and re-used or burnt.
Trace amounts of gaseous nickel carbonyl in apparatus 10 at the termination of the process, may be subsequently decomposed in decomposition tube 40 and carbon monoxide recycled, through conduit 42, when desired. Unwanted carbon monoxide of system 10 can be sent for incineration through conduit 44.
In operation, bubble-bed reactor 12 is filled with de-activated nickel 46 and with hydrogen from source 22, via conduits 26, 18 and 20 when valve 34 is open, and valves 30 and 32 closed. Valve 38 is open in the mode to allow hydrogen to continuously pass through and exit from system 10. The temperature of reactor 12 is maintained at about 150 C by heater 48, for about 2 hours.
5 Reactor 12 is subsequently cooled to about 50 by cooling coils 50. Gases are forced through the apparatus 10 by a blower 52, when required. A plurality of appropriate valves 54, are located and utilized where and when necessary. Gas flow is measured by flow meter 56.
In operation, de-activated nickel 46 is placed in reactor 12, which is purged with argon inert gas from cylinder 58 and heated to 150 C by heater 48. Hydrogen is passed into reactor 12 at atmospheric pressure for 2 hours from cylinder 22 through conduits 18 and 20, and passed out of outlet 36 and part of conduit 16 to exit apparatus 10 under direction of valve 38.
Reactor 12 is cooled to about 50 C, and the remaining hydrogen displaced by initial carbon monoxide stream from cylinder 24 fed through valve 32 conduits 18, 20 and its flow rate measured by meter 56.
Nickel carbonyl is formed from the hydrogen re-activated nickel in reactor 12 and carried to deposition chamber 14 with the excess carbon monoxide through conduit 36 and 16 after selection valve 38 and regular valves 54 suitably opened or closed as appropriate.
Chamber 14 contains a substrate 60 at a temperature of about 175-200 C which effects deposition of nickel by the thermal decomposition of the nickel carbonyl, as known in the art, to produce a nickel mold. The carbon monoxide produced by the thermal decomposition and that carried through conduit 18 to chamber 16 is now recycled back to reactor 12 under the direction of the plurality of valves suitably opened/closed.
The carbon monoxide recycle process to and from reactor 12 and chamber 14 is continued in this closed-loop arrangement until the desired amount of nickel carbonyl has been formed and decomposed.
Upon termination of the operation, the apparatus is purged with argon, trace amounts of nickel carbonyl is decomposed in copper tube 40 at about 200 C and unwanted carbon monoxide is incinerated. Finally, the nickel mold is removed from chamber 14.
Although this disclosure has described and illustrated certain preferred embodiments of the invention, it is to be understood that the invention is not restricted to those particular embodiments. Rather, the invention includes all embodiments which are functional or mechanical equivalence of the specific embodiments and features that have been described and illustrated.
6

Claims (14)

Claims:
1. A process for the production of a deposited metallic nickel product from an inactivated, pre-activated metallic nickel source, said process comprising treating said nickel source with hydrogen at a nickel activation temperature selected from 150-350°C to effect re-activation of said nickel source;
treating said re-activated nickel with carbonylation carbon monoxide to produce a gaseous mixture comprising nickel carbonyl and carbon monoxide;
collecting said nickel carbonyl gaseous mixture; and decomposing said nickel carbonyl in said gaseous mixture to produce said nickel product, and a resultant carbon monoxide gaseous mixture.
2. A process as defined in claim 1 wherein said nickel activation temperature is selected from 150-200°C.
3. A process as defined in claim 2 wherein said nickel activation temperature is about 50°C.
4. A process as defined in any one of claims 1-3 wherein said resultant carbon monoxide mixture is recycled to treat said nickel source to constitute in whole or in part said carbonylation carbon monoxide.
5. A process as defined in any one of claims 1 to 4 wherein said re-activated nickel is treated with said carbonylation carbon monoxide at a temperature selected from 40-80°C.
6. A process as defined in claim 5 wherein said temperature is about 50°C.
7. A process as defined in any one of claims 1 to 6 further comprising treating a metallic iron source with hydrogen at an iron activation temperature selected from 150-350°C to produce activated iron;
treating said activated iron with carbonylation carbon monoxide to produce a gaseous mixture comprising iron carbonyl and carbon monoxide;
collecting said iron carbonyl gaseous mixture;
combining said nickel carbonyl gaseous mixture and said iron carbonyl gaseous mixture to produce a combined gaseous mixture; and decomposing said nickel carbonyl and said iron carbonyl in said combined mixture to produce a ferronickel product and a resultant carbon monoxide combined gaseous mixture.
8. A process as defined in claim 7 wherein said iron activation temperature is selected from 150-200°C.
9. A process as defined in claim 8 wherein said iron activation temperature is about 50°C.
10. A process as defined in any one of claims 7 to 9 wherein said metallic iron source is in admixture with said metallic nickel source when said metallic nickel source and said metallic iron source are treated with said hydrogen.
11. A combined carbon monoxide closed-loop apparatus for producing nickel carbonyl from a metallic nickel source and carbon monoxide and decomposing said nickel carbonyl to a metal nickel product; said apparatus comprising (a) a nickel carbonyl carbonylation reactor for containing said nickel source, and having (i) a reaction chamber;
(ii) inlet conduit means for feeding an input gas selected from hydrogen and carbon monoxide to said chamber;
(iii) outlet conduit means for collecting an exit gas selected from hydrogen, carbon monoxide, nickel carbonyl and mixtures thereof from said chamber;
(iv) heating means for heating said chamber; and (v) cooling means for cooling said chamber;
(b) a nickel carbonyl deposition chamber comprising (i) deposition chamber inlet means in communication with said reactor conduit outlet means;
(ii) deposition chamber outlet means in communication with said reactor conduit inlet means;
(c) means for feeding hydrogen to said reactor inlet conduit means; and (d) means for feeding carbon monoxide to said reactor inlet conduit means.
12. Apparatus as defined in claim 11 wherein said reaction chamber outlet conduit means comprises (i) reaction chamber outlet hydrogen conduit means;
(ii) reaction chamber outlet carbon monoxide conduit means; and (iii) hydrogen selective outlet valve means separating said outlet hydrogen conduit means from said outlet carbon monoxide conduit means.
13. Apparatus as defined in claim 11 or claim 12 wherein said reactor inlet conduit means comprises (i) reactor inlet hydrogen conduit means;
(ii) reactor inlet carbon monoxide conduit means; and (iii) selective inlet valve means separating said inlet hydrogen conduit means from said inlet carbon monoxide conduit means.
14. Apparatus as defined in any one of claims 11 to 13 wherein said means for feeding carbon monoxide to said reactor is in communication with said deposition chamber outlet means and said reactor inlet means.
CA002525466A 2005-11-07 2005-11-07 Re-activation of de-activated nickel for nickel carbonyl production Abandoned CA2525466A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CA002525466A CA2525466A1 (en) 2005-11-07 2005-11-07 Re-activation of de-activated nickel for nickel carbonyl production

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CA002525466A CA2525466A1 (en) 2005-11-07 2005-11-07 Re-activation of de-activated nickel for nickel carbonyl production

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7776129B2 (en) 2007-04-24 2010-08-17 Chemical Vapour Metal Refining Inc. Apparatus and process for making high purity nickel
GB2449280B (en) * 2007-05-17 2012-12-19 Cvmr Corp Apparatus and process for making high purity nickel
CN107815556A (en) * 2017-11-17 2018-03-20 金川集团股份有限公司 A kind of activation device and method of water quenching nickel

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7776129B2 (en) 2007-04-24 2010-08-17 Chemical Vapour Metal Refining Inc. Apparatus and process for making high purity nickel
US8852315B2 (en) 2007-04-24 2014-10-07 Cvmr Corporation Apparatus and process for making high purity nickel
GB2449280B (en) * 2007-05-17 2012-12-19 Cvmr Corp Apparatus and process for making high purity nickel
CN107815556A (en) * 2017-11-17 2018-03-20 金川集团股份有限公司 A kind of activation device and method of water quenching nickel
CN107815556B (en) * 2017-11-17 2019-11-08 金川集团股份有限公司 Activation device and method for water-quenched nickel

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