CA1109645A - Process for the production of battery-grade manganese dioxide - Google Patents

Process for the production of battery-grade manganese dioxide

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Publication number
CA1109645A
CA1109645A CA339,079A CA339079A CA1109645A CA 1109645 A CA1109645 A CA 1109645A CA 339079 A CA339079 A CA 339079A CA 1109645 A CA1109645 A CA 1109645A
Authority
CA
Canada
Prior art keywords
solution
process according
mno2
precipitate
mgo
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
Application number
CA339,079A
Other languages
French (fr)
Inventor
Andre Van Der Heyden
Marc Coussement
Antoine Van Peteghem
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.)
METALLURGIE HOBOKEN-OVERPELT
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METALLURGIE HOBOKEN-OVERPELT
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Publication of CA1109645A publication Critical patent/CA1109645A/en
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Classifications

    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00Electrodes
    • H01M4/02Electrodes composed of, or comprising, active material
    • H01M4/36Selection of substances as active materials, active masses, active liquids
    • H01M4/48Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01GCOMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G45/00Compounds of manganese
    • C01G45/02Oxides
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01PINDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00Crystal-structural characteristics
    • C01P2002/60Compounds characterised by their crystallite size
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01PINDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00Particle morphology
    • C01P2004/60Particles characterised by their size
    • C01P2004/61Micrometer sized, i.e. from 1-100 micrometer
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01PINDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00Physical properties of inorganic compounds
    • C01P2006/12Surface area
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01PINDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00Physical properties of inorganic compounds
    • C01P2006/80Compositional purity

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  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

Process for the production of battery-grade manganese dioxide.

Abstract Battery-grade MnO2 is produced by (a) treating a MnCl2 solution with Cl2 and Mg(OH)2 whereby obtaining a MgCl2 solution that contains a MnO2 precipitate;
(b) allowing to digest the precipitate in the MgCl2 solution in presence of Cl2 under pressure;
(c) separating the digested precipitate from the solution; and (d) washing and drying the precipitate.
Owing to step (b), operating conditions in step (a) may be such that a concentrated MgCl2 solution is obtained, which is important for the further processing of that solu-tion by pyrohydrolysis.

Description

The present invention relates to a process for the producti-on of battery-grade manganese dioxide from a manganese chloride solution, in which said solution is treated with chlorine, while maintaining the pH of the solution between 0.5 and 3 by adding MgO and/or Mg(OH)2, so as to precipitate most of the man-ganese thereby producing a MgC12 solution poor in manganese and containing a MnO2 precipitate, the MnO2 precipitate is separated from said MgC12 solution and the MnO2 precipitate is washed and dried. This process is based upon the following reactions:

MnC12 + C12 + 2 H20 > MnO2 + 4 HC1 4 HCl + 2 MgO ~ 2 MgC12 + 2 H20 MnC12 + C12 + 2 MgO )MnO2 + 2 MgC12 Such process has been described in the United States Patent No. 3,770,868. In this known process, operating conditions are such that said separated MgC12 solution contains 48 g/l of magnesium as a chloride.
It has been found by the applicant that the above defined process is difficult to realize when it is performed under such conditions that said separated MgC12 solution contains considerably more magnesium, namely from 85 to 130 g/l of magnesium as a chloride, because it results in a manganese dioxide precipitate with high magnesium content that has to be purified by an excessive washing.
However, in such a process it is desirable to produce a concentrated MgC12 solution, since this solution normally has to be pyrohydrolized to recover MgO and HCl. Pyrohydrolyzing a dilute solution requires evaporation of excessive quantities of water.
- The object of the present invention is to provide a process as defined above, which enables one to produce both a concentrated MgC12 solution and a MnO2 precipitate that does not require an ~excessive washing.

.

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It has been found that the aforesaid-serious drawback can be avoided in a surprisingly simple way by digestion of the MnO2 precipitate in the MgCl2 solution in presence of chlorine under pressure.
The process according to the present invention is thus essentially characterized in that the MnO2 precipitate is digested in the MgCl2 solution in presence of chlorine under pressure.
Digestion is preferably performed under a chlorine pressure of at least 2 kg/cm , or else the digestion time required for obtaining a precipitate of good quality would be excessively long.
Preferably, the precipitate is allowed to digest for at least l hour, or else the chlorine pressures required would be excessively high to obtain a precipitate of good quality.
In the process of the present invention the MnO2 precip-itation itself can be carried out under atmospheric pressure, as is done in the above mentioned process of the prior art; it is however much more advantageous to perform this precipitation in an autoclave under a chlorine pressure of between 1.5 and 4.5 kg/cm , since in the latter case, MnO2 precipitates much faster.
Further details and particulars of the process of the invention will appear from the description hearafter of a pre-ferred mode of performing the process of the invention, illustrated in the attached diagram and given as a non-restrictive example.
Solutions with 110 to 130 g/l of Mn as MnCl2 and 25 to 35 g/l of ~g as MgC12 are treated. Such solutions are e.g. produced after extraction of metals such as Ni, Co, Cu and Fe from liquors resulting from the leaching of manganiferous deepsea nodules, according to the process described in the United States Patent No.
4,026,773.
MnO2 precipitation is performed, under vi`gorous stirring, ~ ~ 3 ~, , S6~
in an autoclave under chlorine pressure of between 1.5 and 4.5 kg/cm and at a temperature of between 50 and 100C, preferably between 65 and 80C.
During the precipitation reaction, the pH of the solution is kept between 1 and 2.5 by adding a suspension of magnesium hydrox-ide in a magnesium chloride solution, the solution used for preparing that suspension containing 90 to 110 g/l of Mg as a chloride and the suspension itself containing 600 to 800 g, preferably 660 to 720 g of Mg(OH)2 per litre of solution.
The aforesaid precipitation reaction is carried on until a residual manganese content of between 10 to 20 g/l is reached in the solution, said content being reached after between 30 to 120 minutes, depending on the chlorine ~ressure and the pH.
When reaching said residual manganese content, no more magnesium hydroxide is added and the precipitate is allowed to digest in the solution depleted in manganese for a 2 to 4 h period, while maintaining the chlorine pressure in the autoclave hetween 2.5 and 6 kg/cm .
- After digestion in the autoclave, the MnO2 precipitate is separated from the solution depleted in manganese by filtration, the filtration cake is washed, the washed filtration cake is re-pulped in water, it is filtered again, the filtration cake is washed with water and dried at between 100 and 110C.
In this way MnO2 is obtained, which contains 100 to 300 ppm (parts per million) of magnesium and which is battery-grade.
MgO andjor Mg(OH)2 is added to the solution depleted in manganese, that contains besides iO to 20 g/l of manganese, 85 to 100 g/l of magnesium as a chloride, so as to precipitate the residual manganese as an hydroxide and to obtain a practicaliy manganese free MgC12 solution. The so o~tained precipitate is separated from the .

.'. ' '~.

' ` ; ~ ` ' ' ' 3~ 645 demanganized MgC12 solution. rart of this solution is used to prepare the.previously mentioned magnesium hydroxide suspension and the other part is subjected to a pyrohydrolysis so as to produce MgO, that is used to prepare the previously mentioned Mg(OH)2 suspension, and HCl.

- 4a -Example 1 _________ This example relates to the production of battery-grade MnO2 according to the above described preferred mode of carrying out the process of the invention.
The starting solution contains in g/l : 114 Mn, 34 Mg, 9 Na, 5 K, 8 Ca.
The operation is performed in an autoclave with stirrer on 25 l solution, at a temperature of 75C, under a 2 kg/cm2 chlorine pressure, the stirrer rotating at a speed of 350 rpm. The pH of the solution ls maintained at 2 by addlng Mg(OH)2 as a suspension in a MgCl2 solution containing 90 g Mg/l as a chloride (720 g Mg(OH)2 per litre of solution).
After 2 hours, the Mn content of the solution has dropped to 20 g/l while the Mg content of the solution has risen to 91 g/l. No more Mg(OH)2 is added and the reaction mixture is further stirred for 2 hours, while maintaining the chlorine pressure at 4 kg/cm .
After this digestion, the MnO2 precipitate is filtered, the filtration cake is once washed with 50 l of water, the washed cake is repulped in 25 l of water at 70C (200 g of cake per liter), it is filtered again and the filtration cake is once washed with 100 l of water. The cake is dried at 105C.
In this way MnO2 is obtained with the following properties, which proves that this MnO2 is battery-grade :
- Chemical analysis :
Mn 60.5 MnO2 > 89 %
H20 2 %

- . -, , :. ,.,. ,,:, , - -- . . - : . , . :. , Cu ~ 10 ppm Ni ~ 10 ppm Co~ 10 ppm -Mg~ 200 ppm Cl~ 200 ppm x value in MnO 1.94 ~ x S 1.96 - pH : 5.2 - Physical properties :
specific surface 50 m2/g (BET) crystal structure rho-gamma average particle size 4 microns (Coulter counter) average pore diameter 15 A
- Electrochemical properties :
1) Equilibrium potential in a saturated Na4Cl solution : + 780 mv (Standard Hydrogen Electrode)
2) Test of a R12-paper line type battery made of a mixture of 85 % of MnO2 and 15 % of acetylene black :
- discharge conditions : 5 minutes/hour during 10 hours/day on a 5 ohm resistance till the potential at the battery terminals drops to 0.9 V
- discharge time : 7 hours It is to be noted that in the same conditions a commercial battery grade MnO2 has given a discharge time of 6.5 hours.

Example 2 _________ The same mode of operation as in example 1 is used, but the MnO2 precipitate i6 not digested under chlorine pressure.

'' ~ ~ -' ' '- ' '; ~

s The MnO2 precipitate is thus immediately filtered as soon as no more Mg(OH)2 is added.
The filtration cake is processed in the same way as in example l and it is stated that the thus obtained MnO2 contains-e~ percent in weight of Mg, which is not battery-grade (equilibrium potential of + 680 mv (S~E)).
In order to obtain a MnO2 quality that is comparable to the one obtained in example 1, it is necessary, as was found by the applicant, to make following additional operations (after filtration, washing, repulping in water at 70~C, filtration and washing, as performed in example l) :
repulping the cake in diluted (20 g/l) sulphuric acid (200 g of cake per litre), filtration, washing wit~ lO 1 of a lO g/l Na2CO~ solution, and washing with lO0 1 of water.

Example 3 The same mode of operation as in example l is used, but MnO2 is precipitated under atmospheric pressure, i.e. by having the chlorine bubbled in the solution.

The MnO2 quality obtained is comparable to that obtained in example l. MnO2 precipitation lasted however 15 hours while in example l this precipitation only lasted 2 hours.

.

.~: , ~.: : " . . , : - .

Claims (15)

THE EMBODIMENTS OF THE INVENTION IN WHICH AN EXCLUSIVE
PROPERTY OR PRIVILEGE IS CLAIMED ARE DEFINED AS FOLLOWS:
1. A process for the production of battery-grade manganese dioxide which comprises:
(a) contacting a manganese chloride solution with chlorine, while maintaining the pH of the solution between 0.5 and 3 by adding MgO and/or Mg(OH)2 so as to thereby produce a MgCl2 solution poor in manganese and which contains a MnO2 pre-cipitate that is contaminated by magnesium;
(b) allowing the MnO2 precipitate to digest in said MgCl2 solution in the presence of chlorine under pressure in an autoclave so as to reduce substantially the magnesium content of said MnO2 precipitate, (c) separating the digested MnO2 precipitate from the MgCl2 solution, (d) washing and drying the MnO2 precipitate.
2. A process according to claim 1 wherein the chlorine pressure is at least 2 kg/cm2 in step (b).
3. A process according to claim 2 wherein the chlorine pressure is between 2.5 and 6 kg/cm2.
4. A process according to claim 1 wherein step (b) lasts at least 1 hour.
5. A process according to claim 4 wherein step (b) lasts from 2 to 4 hours.
6. A process according to claim 1 wherein chlorine under pressure is used in step (a).
7. A process according to claim 6 wherein the chlorine pressure is between 1.5 and 4.5 kg/cm2 in step (a).
8. A process according to claim 1 wherein chlorine under atmospheric pressure is used in step (a).
9. A process according to claim 1 wherein the solution resulting from step (a) contains 10 to 20 g/l of manganese.
10. A process according to claim 1 wherein the solution resulting from step (a) contains 85 to 100 g/l of magnesium.
11. A process according to claim 1 wherein in step (a) MgO and/or Mg(OH)2 is added as a suspension in a MgCl2 solution.
12. A process according to claim 11 wherein the MgCl2 solution, in which the MgO and/or Mg(OH)2 is put into suspension, contains 90 to 110 g/l of Mg.
13. A process according to claim 11 wherein the suspension contains 360 to 480 g of Mg as MgO or Mg(OH)2 per litre.
14. A process according to claim 11 wherein MgO and/or Mg(OH)2 is added to the solution resulting from step (c) so as to pre-cipitate the manganese as an hydroxide and to produce an almost manganese free MgCl2 solution, the precipitate is separated from the demanganized MgCl2 solution, and at least part of this de-manganized MgCl2 solution is subjected to a pyrohydrolysis whereby producing MgO and HCl.
15. A process according to claim 14 wherein part of said de-manganized MgCl2 solution and part of said MgO are used to prepare said suspension of MgO and/or Mg(OH)2 in a MgCl2 solution.
CA339,079A 1978-11-06 1979-11-02 Process for the production of battery-grade manganese dioxide Expired CA1109645A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
LU80477 1978-11-06
LU80477 1978-11-06

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CA1109645A true CA1109645A (en) 1981-09-29

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CA (1) CA1109645A (en)

Families Citing this family (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5232490A (en) * 1985-11-27 1993-08-03 Leadville Silver And Gold Oxidation/reduction process for recovery of precious metals from MnO2 ores, sulfidic ores and carbonaceous materials
US6517899B1 (en) 1995-01-20 2003-02-11 Engelhard Corporation Catalyst and adsorption compositions having adhesion characteristics
US6200542B1 (en) 1995-01-20 2001-03-13 Engelhard Corporation Method and apparatus for treating the atmosphere
US6818254B1 (en) * 1995-01-20 2004-11-16 Engelhard Corporation Stable slurries of catalytically active materials
US6863984B2 (en) 1995-01-20 2005-03-08 Engelhard Corporation Catalyst and adsorption compositions having improved adhesion characteristics
US20020018742A1 (en) * 1995-01-20 2002-02-14 Engelhard Corporation Method and apparatus for treating the atmosphere
US20030166466A1 (en) * 1995-01-20 2003-09-04 Hoke Jeffrey B. Catalyst and adsorption compositions having improved adhesion characteristics
AU4701196A (en) 1995-01-20 1996-08-07 Engelhard Corporation Pollutant treating device located in vehicle compartment for cleaning ambient air
US6214303B1 (en) 1995-01-20 2001-04-10 Engelhard Corporation Method and apparatus for treating the atmosphere
US5997831A (en) * 1996-07-12 1999-12-07 Engelhard Corporation Method of catalytically treating the atmosphere and heat exchange devices produced thereby
US5836524A (en) * 1996-10-01 1998-11-17 National Science Council Liquefaction of wastes with product oil recycling
US6156283A (en) * 1998-03-23 2000-12-05 Engelhard Corporation Hydrophobic catalytic materials and method of forming the same
USH2121H1 (en) 2000-10-13 2005-08-02 The United States Of America As Represented By The Secretary Of The Navy High surface area, nanoscale, mesoporous manganese oxides with controlled solid-pore architectures and method for production thereof
US7718319B2 (en) 2006-09-25 2010-05-18 Board Of Regents, The University Of Texas System Cation-substituted spinel oxide and oxyfluoride cathodes for lithium ion batteries

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB597824A (en) * 1944-03-06 1948-02-04 Cie De Prod Chim Et Electro Me Method of manufacture of depolarizing manganese dioxides
US2473563A (en) * 1944-03-06 1949-06-21 Alais & Froges & Camarque Cie Preparation of manganese dioxide
US3414440A (en) * 1964-09-02 1968-12-03 Dow Chemical Co Gamma manganese dioxide, method of preparing and dry cell type battery employing gamma type manganese dioxide
ZA718300B (en) * 1970-12-30 1972-09-27 Broken Hill Pty Co Ltd Processing of manganese ores
US4150091A (en) * 1977-11-21 1979-04-17 Sun Ocean Ventures, Inc. Manganese ore leaching process

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Effective date: 19980929