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Patent Number/Link: 
4,205,979 Process for beneficiating oxide ores

United States Patent [19]

Kindig et ale

[11]

[45]

4,205,979

Jun. 3, 1980

[54] PROCESS FOR BENEFICIATING OXIDE

ORES

[75] Inventors: James K. Kindig, Arvada; Ronald L.

Turner, Golden, both of Colo.

[73] Assignee: Hazen Research, Inc., Golden, Colo.

[21] Appl. No.: 950,176

[22] Filed: Oct. 10, 1978

[51] Int. Ct.2 C22B 1/06

[52]· U.S. Ct•......................................... 75/1 II; 75/21;

209/214; 427/252

[58] Field of Search 75/1 R, 1 T, 21, 28,

75/62,72,77,82,81, 111, 112; 423/23, 13 P, 25;

204/217,213,214;427/47,252,253,254,255

[56] References Cited

U.S. PATENT DOCUMENTS

41 Claims, No Drawings

FOREIGN PATENT DOCUMENTS

179095 7/1954 Austria 75/112

119156 8/1959 U.S.S.R 209/212

Primary Examiner-L. Dewayne Rutledge

Assistant Examiner-Michael L. Lewis

Attorney, Agent, or Firm-Sheridan, Ross, Fields &

McIntosh

In a process for beneficiating one or more mineral values

ofa metal oxide ore selected from the group consisting

of bauxite, taconite, chrysocolla, apatite, titanium

oxides and the metal oxides of Groups IIIB, IVB, VB,

VIB, VIIB, VIIIB, IB, lIB and IVA by treating the ore

with a metal containing compound, preferably iron

carbonyl, under conditions such as to selectively enhance

the magnetic susceptibility of the mineral values

to the exclusion of the gangue in order to permit a separation

between the values and gangue, the improvement

comprising pretreating the metal oxide ore by heating it

to a temperature of at least about 80· C. for a time period

of at least about 0.1 hours.

Kindig et aI 44/1 R

Glasser 75/1 T

McEwan et al. 423/417

Kindig et aI 44/1 R

ABSTRACf

211976

8/1976

1111977

7/1978

3,938,966

3,977,862

4,056,386

4,098,584

[57]

Etherington 75/1 R

Grams 75/1 T

Dean et al. 423/25

Drummond 427/252

Altmann 75/0.5

Queneau et al. 75/0.5

Queneau 427/217

Frysinger et aI 75/119

O'Neill et al. 75/0.5

IlIis et al. 75/112

Knisky et aI. .. 423/25

Sato 423/25

211913

111931

10/1938

10/1943

9/1952

7/1960

1111965

5/1966

6/1967

9/1969

111970

6/1972

1,053,486

1,789,813

2,132,404

2,332,309

2,612,440

2,944,883

3,220,875

3,252,791

3,323,903

3,466,167

3,490,899

3,669,644

4,205,979

5

1

PROCESS FOR BENEFICIATING OXIDE ORES

BACKGROUND OF THE INVENTION

1. Field of the Invention

This invention is an improvement on a means for

treating ores to separate the mineral values from gangue

material by selectively enhancing the magnetic susceptibility

of the mineral values so that they may be mag- 10

netically removed from the gangue.

2. Description of the Prior Art

As is well known, mining operations in the past for

recovering various metals (e.g., lead and copper) have

utilized high grade ore deposits where possible. Many 15

of these deposits have been exhausted and mining of

lower grade ores is increasing. The processing of these

leaner ores consumes large amounts of time, labor, reagents,

power and water with conventional processing.

In addition to the increased expense associated with 20

the extraction of these metals from low· grade ores,

proposed processes for separation of certain of the sulfide

ores are technically very difficult and involve elaborate

and expensive equipment. In many cases the expense

incurred by such separation would be greater 25

than the commercial value of the metal, such that the

mineral recovery, while theoretically possible, is economically

unfeasible.

Our copending patent application Ser. No. 921,583

filed July 3, 1978 entitled "Process For Beneficiating 30

Oxide Ores" teaches the treatment of oxide ores with a

metal containing compound under conditions such as to

selectively enhance the magnetic susceptibility of the

mineral values to the exclusion of the gangue, allowing

for a separation of these values from the gangue. How- 35

ever, it appears as though the presence of various volatile

compounds within the ore can have an adverse

effect on the recovery of mineral values in a process

which enhances the magnetic susceptibility of the min- 40

eral values. Pretreating the raw oxide ore with heat in

order to volatilize these various components, and thereafter

selectively enhancing the magnetic susceptibility

of the mineral values so that they may be physically

separated from the gangue, substantially enhances the 45

effectiveness of the separation of the mineral values

from the gangue. Additionally, pretreatment with heat,

optionally in the presence of various gaseous additives,

enhances the basic process, apparently as a result of

differing mechanisms. 50

SUMMARY OF THE INVENTION

The process of the present invention entails heat pretreatment

of a metal oxide ore selected from the group

consisting of bauxite, taconite, chrysocolla, apatite, 55

titanium oxides and the metal oxides of Groups IIIB,

IVB, VB, VIB, VIIB, VIIIB, IB, lIB, and IVA, and

thereafter treating the metal oxide ore with a metal

containing compound, preferably iron carbonyl, under

conditions such that the magnetic susceptibility of the 60

ore is. selectively enhanced to the exclusion of the

gangue. The affected or values may then be separated

from the gangue, preferably by means of a magnetic

separation.

The pretreatment is conducted at a temperature of at 65

least about 800 C. for a time period of at least about 0.1

hours. The heat pretreatment step may also be conducted

in the presence ofone or more gaseous additives,

2

for example, steam, nitrogen, hydrogen, carbon monoxide,

hydrogen sulfide, ammonia, and sulfur dioxide.

DESCRIPTION OF THE PREFERRED

EMBODIMENTS

The process of the present invention is particularly

useful for concentrating metal oxide minerals. The process

employs the heat pretreatment of the metal oxide

ore with heat or heat in conjunction with a gaseous

additive, and thereafter treating the ore with a metal

containing compound, preferably iron carbonyl, under

conditions such as to selectively enhance the magnetic

susceptibility of various mineral values contained

within the ore. The treated mixture can then be subjected

to a separation process to produce a beneficiated

product.

The heat pretreatment of the present invention is

conducted prior to initiating the reaction with the metal

containing compound. This pretreatment essentially

comprises heating the metal oxide ore in order to render

the ore more receptive to the magnetic enhancement

reaction. Thetemperature and time ofheating are interrelated,

and essentially higher temperatures require less

time. The particular time and temperature for the pretreatment

process will depend on the particular ore

being beneficiated and also the metal containing compound

with which the ore is later treated. Since metal

oxide ores as a group do not readily decompose with

heat, the pretreatment may occur over a broad range of

temperatures. The temperature must not exceed the

decomposition temperature of the mineral value, or a

temperature above which substantial vaporizaton

would occur. It is gel).erally preferred that the pretreatment

essentially comprise heating the ore to a temperature

of at least about 800 C., more preferably from about

1250 C. to about 5000 C. and most preferably to a temperature

of from about 1750 C. to about 2500 C. It is

preferred that this heat pretreatment be done for a time

period of at least about 0.1, more preferably from about

0.20 to 4 hours, and most preferably from about 0.25 to

about 1 hour.

The heat pretreatment need not be immediately followed

by the magnetic enhancement reaction. Hence,

the ore may be permitted to cool to ambient temperature,

or any other convenient temperature, prior to

conducting the magnetic susceptibility enhancement

reaction. However, if the heat pretreatment is conducted

at a temperature greater than the temperature of

the magnetic enhancement reaction, the ore must be

cooled to at least thetemperature at which the magnetic

enhancement reaction will be conducted.

It is generally preferred to maintain the heat pretreatment

temperature at least slightly above the temperature

of the magnetic enhancement reaction. This is not

an imperative requirement, however, improved results

are generally accomplished. The pretreating by heating

the ore is believed to change the ore either physically or

chemically and/or be volatilize various components

which can interfere with the magnetic enhancement

reaction. Therefore, if the magnetic enhancement reaction

is conducted at a temperature in excess of the pretreatment

temperature, it is possible that additional volatile

components could somewhat detrimentally affect

the magnetic enhancement reaction.

The heat pretreatment step may be conducted in the

presence of one or more gaseous additives, and this is

preferable under many circumstances. Examples of

suitable gaseous additives include steam, nitrogen, hy4,205,979

3

drogen, carbon monoxide, carbon dioxide, ammonia,

hydrogen sulfide, sulfur dioxide, methane, air, ethane,

propane, butane and other hyrocarbon compounds in

the gaseous state at the pretreatment temperature. Preferred

gaseous additives include steam, nitrogen, hydro- 5

gen, carbon monoxide, hydrogen sulfide, ammonia and

sulfur dioxide.

When these additives are. employed it is preferable

that they be employed in an amount of at least about 2,

more preferably at least about 12, and most preferably 10

at least about 120 cubic meters per hour per metric ton

of ore being processed.

A particular preferred additive is steam. Heat pretreatment

with steam is preferably conducted at a temperature

of at least about 1000 C., more preferably from 15

about 1500 C. to about 3500 C., and most preferably

from about 1750 C. to about 2500 C. Preferably, the

pretreatment should be conducted for at least about 0.1

hours, more preferably for at least about 0.25 hours, and

most preferably for at least 0.5 hours. The amount of 20

water preferably ranges from about 1% to about 50%,

more preferably from about 5% to about 30%, and most

preferably from about 10% to about 25%, based on the

weight of the metal oxide ore being treated.

After the ore has been subjected to this heat pretreat- 25

ment, it is then treated with a metal containing compound

in order to selectively enhance the magnetic

susceptibility of its various mineral values.

"Enhancing the magnetic susceptibility" of the ore as

used herein is intended to be defined in accordance with 30

the following discussion. Every compound of any type

has a specifically defined magnetic susceptibility, which

refers to the overall attraction of the compound to a

magnetic force. An alteration of the surface magnetic

characteristics will alter the magnetic susceptibility. 35

The metal containing compound treatment of the process

alters the surfacr characterisics of the ore particles

in order to enhance the magnetic susceptibility of the

particles. It is to be understood that the magnetic susceptibility

of the compound is not actually changed, but 40

the particle itself is changed, at least at its surface, resulting

in a particle possessing a greater magnetic susceptibility

than the original particle. For convenience of

discussion, this alternation is termed herein as "enhancing

the magnetic susceptibility" of the particle or ore 45

itself.

The metal oxide minerals which are capable of undergoing

a selective magnetic enhancement in accordance

with the process include the metal oxides of Groups

IIIB, IVB, VB, VIB, VIIB, VIIIB, IB, lIB and IVA, 50

the titanium oxides of Group IVB, aluminum hydrate,

i.e. bauxite, of Group IIIB, taconite, chrysocolla, and

apatite. It is recognized that taconite and chrysocollar

are classified as silicates and apatite is classified as a

phosphate, and it is further recognized that apatite does 55

not contain elements generally classified as metals

(other than calcium). However, for the purposes of this

inventive process they are classified as metal oxides.

The preferred oxide minerals include bauxite, apatite,

cuprite, cassiterite, carnotite, scheelite, chrysocolla and 60

hematite.

The gangue minerals from which the metal oxide ores

can be separated include those minerals which do not

undergo a sufficient magnetic susceptibility enhancement

as a result of the process. These gangue minerals 65

include, for example, silica, alumina, gypsum, muscovite,

dolomite, calcite, albite and feldspars, as well as'

various other minerals.

4

In those ores which contain naturally relatively

strongly magnetic constituents, such as magnetite, the

magnetic material may first be removed by passing the

mixture through a magnetic separator. The nonmagnetic

portion obtained by this precleaning step is then

subjected to the heat pretreatment and then treatment

with a metal containing compound. Prior to either of

the treatments, the ore must be ground to liberate the

metal oxide particles from the gangue particles, if the

respective components do not already exist in this liberated

state. The ore may be crushed finer than necessary

to achieve liberation, but this is not generally economically

possible. It is generally satisfactory to crush the

ore to minus 14 mesh, although many ores require

grinding to minus 65 mesh or finer.

Numerous metal containing compounds are capable

of enhancing the magnetic susceptibility of these metal

oxides in accordance with the invention. Many iron

containing compounds possess the capability of enhancing

the magnetic susceptibility of the mineral values of

the ore, as long as the compound is adaptable so as to

bring the iron in the compound into contact with the

mineral value under conditions such as to cause an alteration

of at least a portion of the surface of the mineral

value.

Iron containing compounds capable of exerting sufficient

vapor pressure, with iron as a component in, the

vapor, so as to bring the iron into contact with the value

at the reaction temperature are suitable, as well as other

organic and inorganic iron containing compounds

which can be dissolved and/or "dusted" and brought

into contact with the mineral value contained within the

ore. Preferred compounds within the vapor pressure

group are tl~ose which exert a vapor pressure, with iron

as a component in the vapor, of at least about 10 millimeters

of mercury, more preferably of at least about 25

millimeters of mercury and most preferably of at least

about 50 millimeters of mercury at the reaction temperature.

Examples of groupings which fall within this

vapor pressure definition include ferrocene and its derivatives

and beta-diketone compounds of iron. Specific

examples include ferrocene and iron acetylacetonate.

Other organic compounds which may be utilized to

enhance the magnetic susceptibility include those

which may be homogeneously mixed with a carrier

liquid and brought into contact with the components of

the ore. Such mixtures include, for example, solutions,

suspensions and emulsions. These compounds must be

such as to provide sufficient metal to contact the surface

of the mineral value. Suitable carrier liquids include, for

example, acetone, petroleum ether, naptha, hexane,

benzene and water; but this, of course, is dependent

upon the particular metal compound being employed.

Specific groupings include, for example, ferrocene and

its derivatives and the carboxylic acid salts of iron, such

as, iron octoate, iron naphthenate, iron stearate and

ferric acetylacetonate.

Additionally, solid organic iron containing compounds

capable of being directly mixed with the ore in

solid form possess the capability of enhancing the magnetic

susceptibility of the metal sulfides. The compound

must be in solid form at the mixing temperature and be

of sufficiently fine particle size in order to be able to be

well dispersed throughout the ore. The particle size is

preferably smaller than about 20 mesh, more preferably

smaller than about 100 mesh, and most preferably

smaller than about 400 mesh. Compounds within this

grouping include ferrocene and its derivatives, iron salts

4,205,979

5

of organic acids, and beta-diketone compounds of iron.

Specific examples include ferrous formate, 1,1'-diacetylferrocene,

and l,l'-dihydroxymethyl ferrocene.

Various inorganic compounds are also capable of

producing an enhanced magnetic susceptibility. Pre- 5

ferred inorganic compounds include ferrous chloride,

ferric chloride and the metal carbonyls, including, for

example, iron, nickel, cobalt, molybdenum, tungsten

and chromium carbonyls and derivatives of these compounds.

Iron carbonyl is a preferred carbonyl for im- 10

parting this magnetic susceptibility, particularly iron

pentacarbonyl, iron dodecacarbonyl and iron nonacarbonyi.

The more preferred metal containing compounds

capable of enhancing the magnetic susceptibility

are iron pentacarbonyl, ferrocene, ferric acetylac- 15

etonate, ferrous chloride and ferric chloride, with iron

pentacarbonyl being the most preferred.

The process is applied by contacting the iron containing

compound with the ore at a temperature wherein

the iron containing compound selectively decomposes 20

or otherwise reacts at the surface of metal oxide particles

to alter their surface characteristics, while remaining

essentially unreactive, or much less reactive, at the

surface of the gangue particles. The temperature of the

reaction is a critical parameter, and dependent primarily 25

upon the particular compound and the particular ore.

The preferred temperature can be determined by heating

a sample of the specific iron containing compound

and the specific ore together until the decomposition

reaction occurs. Suitable results generally occur over a 30

given temperature range for each system. Generally,

temperatures above the range cause non-selective decomposition

while temperatures below the range are

insufficient for the reaction to occur.

While as indicated above, techniques other than 35

vapor injection methods may be employed as applicable

depending upon the metal· containing compound being

utilized, the following discussion primarily applies to

vapor injection techniques, specifically iron pentacarbonyl,

as these are generally preferred. Similar consid- 40

erations, as can be appreciated, apply to the other described

techniques.

The preferred temperatures when iron pentacarbonyl

is employed as the treating gas are primarily dependent

upon the ore being treated. It is generally preferred to 45

select a temperature which is within a range of 125° C.,

more preferably 50° C., and most preferably 15° C.less

than the general decomposition temperature of the iron

carbonyl in the specific system. The general decomposition

temperature is intended to mean the temperature at 50

which the iron carbonyl decomposes into iron and carbon

monoxide in an indiscriminate fashion, causing a

magnetic enhancement of the gangue as well as the

metal oxide. The "specific system" is intended to include

all components and parameters, other than, of 55

course, temperature, of the precise treatment, as the

general· decomposition temperature generally varies

with different components and/or different parameters.

This decomposition temperature range can be readily

determined by analytical methods, and often a trial and

6

error approach is preferred to determine the precise

temperature range for each specific system.

The amount of the metal containing compound used

and the time of treatment can be varied to maximize the

selective enhancement treatment. With respect to iron

carbonyl the preferred amount employed is from about

0.1 to about 100 kilograms per metric ton offeed, more

preferably from about 1 to about 50 kilograms per metric

ton of feed, and most preferably from about 2 to 20

kilograms per metric ton of feed. The reaction is generally

conducted for a period of time from about 0.05 to

about 4 hours, more preferably from about 0.15 to about

2 hours, and most preferably from about 0.25 to 1 hour.

The process of this invention is not especially useful

in beneficiating oxide ores which are highly naturally

magnetic since such ores can be beneficiated by subjecting

them to a magnetic separation process or first heating

them before the magnetic process. An example of

such an ore is pyrolusite.

After the feed mixture containing the metal oxide

values has been pretreated with heat and treated with a

metal containing compound, it can then be subjected to

a physical separation process to effect the separation of

the treated metal oxides from the gangue. Any of many

commercially available magnetic separators can be used

to remove these values from the gangue. For example,

low or medium intensity separations can be made with

a permanent magnetic drum separator, electromagnetic

drum separators, induced roll separators or other configurations

known to those skilled in the art. Since most

oxides are liberated at a mesh size of 65 mesh or fmer, a

wet magnetic separation process is more effective.

Thus, high intensity, high gradient wet magnetic separators

are preferred. Also, electrostatic techniques may

be employed as the primary separation means, or in

addition to the magnetic separation means. The selective

change in surface characteristics changes the electrical

conductivity of the particle in analogous fashion

to changing the particle's magnetic characteristics. Additionally,

due to the fact that the oxide surface characteristics

have been selectively altered, the oxides are

often more amenable to processes such as flotation and

chemical leaching.

EXAMPLE I

Samples of different minerals were ground to a minus

65 mesh and mixed with minus 65 mesh silica sand to

produce 3% synthetic ores with the exception of carnotite

which was a 5% ore. Each sample was pretreated

with steam by rapidly heating the sample to 200° C.

under a nitrogen purge; thereafter the sample was

treated for 15 minutes with 200 kilograms of steam per

metric ton of sample. The reactor· was then cooled

under a nitrogen purge. Following this steam pretreatment

each sample was treated with 8 kilograms of iron

pentacarbonyl per metric ton of sample for 30 minutes

at the temperature indicated in Table l. All of the samples

were then subjected to a magnetic separation process.

The results are given in Table l.

TABLE 1

Temperature

Of Fe(CO)s Weight Grade Metal

Mineral J'reatment ('C.) Product (%) (%) Metal Distribution

Carnotite 145 Magnetic 24.0 0.059 U30g 70.0

Nonmagnetic 76.0 0.008 U30g 30.0

Calculated Feed 100.0 0.020 U30 g 100.0

Apatite 125 Magnetic 1.6 8.14 P 36.0

7

TABLE I-continued

4,205,979

8

Temperature

Of Fe(CO)s

Mineral Treatment ("C.) Product

Nonmagnetic

Calculated Feed

Scheelite 135 Magnetic

Nonmagnetic

Calculated Feed

Cuprite 125 Magnetic

Nonmagnetic

Calculated Feed

Cassiterite 128 Magnetic

Nonmagnetic

Calculated Feed

Weight Grade Metal

(%) (%) Metal Distribution

98.4 0.235 P 64.0

100.0 0.36 P 100.0

1.55 6.01 W 23.4

98.45 0.31 W 76.6

100.0 0.40 W 100.0

1.9 45.1 Cu 71.8

98.1 0.344 Cu 28.2

100.0 1.19 Cu 100.0

14.5 2.06 Sn 23.5

85.5 1.14 Sn 76.5

100.0 1.27 Sn 100.0

were then subjected to a wet magnetic separation process.

The results are presented in Table 3.

TABLE 3

Te'!'perature

of Fe(CO)s Weight Grade Metal

Mineral Treatment ("C.) Product (%) (%) Metal Distribution

Carnotite 145 Magnetic 62.5 0.047 U30s 90.7

Nonmagnetic 37.5 0.008 U30a 9.3

Calculated Feed 100.0 0.032 UJOa 100.0

Apatite 125 Magnetic 1.9 7.96 P 39.7

Nonmagnetic 98.1 0.234 P 60.3

Calculated Feed 100.0 0.38 P 100.0

Scheelite 135 Magnetic 4.4 4042 W 51.7

Nonmagnetic 95.6 0.19 W 48.3

Calculated Feed 100.0 0.38 W 100.0

Cuprite 125 Magnetic 2.9 32.6 Cu 75.3

Nonmagnetic 97.1 0.32 Cu 24.7

Calculated Feed 100.0 1.26 Cu 100.0

EXAMPLE 2

For comparison, additional samples of the same type

of ores of Example 1 were subjected to just a steam 35 EXAMPLE 4

pretreatment, and then magnetically separated. Analyses

of these comparative blanks are given in Table 2. For comparative purposes, additional samples ofthe

same type of ores of Example 3 were subjected to just

TABLE 2 the heat and nitrogen pretreatment, and then magneti-

Metal

40

cally separated. Analyses of these comparative blankS

Weight Grade Distri- are given in Table 4.

Mineral Product (%) (%) Metal bution

Carnotite Magnetic 0.71 0.321 U30S 12.6 Table 4

Nonmagnetic 99.29 0.016 U30 S 87.4 Metal

Calculated Feed 100.0 0.018 U30S 100.0 Weight Grade Distri-

Apatite Magnetic 0.48 0.518 P 0.62 45 Mineral Product (%) (%) Metal butiqil

Nonmagnetic 99.52 0.399 P 99.38 Carnotite Magnetic 1.1 0.421 U30s 20.6

Calculated Feed 100.0 0.40 P 100.00 Nonmagnetic 98.9 O.oI8 U30a 79.4

Scheelite Magnetic 1.25 1.00 W 3.1 Calculated Feed 100.0 0.022 U30S 100.0

Nonmagnetic 98.75 0.40 W 96.9 Apatite Magnetic 0.94 0.683 P 1.8

Calculated Feed 100.0 0.41 W 100.0 Nonmagnetic 99.06 0.358 P 98.2

Cuprite Magnetic 1.04 42.3 Cu 37.9

50 Calculated Feed 100.0 0.36 P 100.0

Nonmagnetic 98.96 0.728 Cu 62.1 Scheelite Magnetic I.4 0.82 W 2.&

Calculated Feed 100.0 1.16 Cu 100.0 Nonmagnetic 98.6 0.40 W 97.2

Cassiterite Magnetic 0.97 24.0 Sn 19.5 Calculated Feed 100.0 0.41 W 100.0

Nonmagnetic 99.03 0.97 Sn SO.5 Cuprite Magnetic 0.76 34.1 Cu 26.6

Calculated Feed 100.0 1.19 Sn 100.0 Nonmagnetic 99.24 0.72 Cu 73.4

5S Calculated Feed 100.0 0.97 Cu 100.0

EXAMPLE 3

Samples of different synthetic ores were prepared as

indicated in Example 1. Each of the samples in this

example was pretreated with heat and nitrogen by rapidly

heating a reactor containing the sample to 400° C. 60

during a nitrogen purge which flowed at a rate such

that one reactor volume of gas was introduced into the

system every 4.3 minutes and maintaining these conditions

for 15 minutes. Then the reactor was cooled under

a nitrogen purge. Following this pretreatment each 6S

sample was treated with 8 kilograms of iron pentacarbonyl

per metric ton of sample for 30 minutes at the

temperature indicated in Table 3. All of the samples

EXAMPLE 5

Samples of different synthetic ores were prepared as

indicated in Example 1. Each of the samples in this

example was pretreated with heat and hydrogen by

rapidly heating the reactor containing the sample to

400° C. while purging it with nitrogen. This temperature

was maintained for 15 minutes while hydrogen gas

was passed through the reactor at a flow rate of one

reactor volume of gas every 4.3 minutes. The reactor

was cooled under a purge of nitrogen gas. Each sample

was then treated with 8 kilograms of iron pentacarbonyl

4,205,979

9

per metric ton of sample for 30 minutes at the temperature

indicated in Table 5. Thereafter the samples were

subjected to a wet magnetic separation process. The

10

minutes at the temperature indicated in Table 7. The

samples were then subjected to a wet magnetic separation

process. The results are presented in Table 7.

TABLE 7

Temperature

of Fe(CO)s Weight Grade Metal

Mineral Treatment ("C.) Product (%) (%) Metal Distribution

Carnotite 145 Magnetic 54.7 0.051 U30 S 93.9

Nonmagnetic 45.3 0.004 U30S 6.1

Calculated Feed 100.0 0.030 U30S 100.0

Scheelite 135 Magnetic 5.0 4.20 W 53.8

Nonmagnetic 95.0 0.19 w 46.2

Calculated Feed 100.0 0.39 W 100.0

Cuprite 125 Magnetic 4.8 23.4 Cu 87.4

Nonmagnetic 95.2 0.17 Cu 12.6

Calculated Feed 100.0 \.29 Cu 100.0

results are given in Table 5.

TABLE5

Temperature

of Fe(CO)s Weight Grade Metal

Mineral Treatment ("C.) Product (%) (%) Metal Distribution

Carnotite 145 Magnetic 63.7 0.057 U30S 96.2

Nonmagnetic 36.3 0.004 U30S 3.8

Calculated Feed 100.0 0.038 U30S 100.0

Apatite 125 Magnetic 3.3 5.75 P 57.0

Nonmagnetic 96.7 0.148 P 43.0

Calculated Feed 100.0 0.33 P 100.0

Cuprite 125 Magnetic 3.1 3\.2 Cu 8\.4

Nonmagnetic 96.9 0.228 Cu 18.6

Calculated Feed 100.0 1.19 Cu 100.0

EXAMPLE 6

For comparative purposes, additional samples of the

same type of ores of Example 5 were subjected to just

the heat and hydrogen pretreatment, and then magneti- 40

cally separated.. Analyses ofthese comparative blanks

are given in Table 6,

EXAMPLE 8

For comparative purposes, additional samples of the

same type of ores of Example 7 were subjected to just

the heat and carbon monoxide pretreatment, and then

magnetically separated. Analyses of these comparative

blanks are given in Table 8.

TABLE8

TABLE 6

Metal

Weight Grade Distri- 45 Mineral

Mineral Product (%) (%) Metal bution Carnotite

Carnotite Magnetic 10.1 0.209 U30S 85.4

Nonmagnetic 89.9 0.004 U30S 14.6

Calculated Feed 100.0 0.025 U30S 100.0 Scheelite

Apatite Magnetic 2.2 2.91 P 16.5 Nonmagnetic 97.8 0.332 P 83.5 50

Calculated Feed 100.0 0.39 P 100.0 Cuprite

Cuprite Magnetic 0.73 44.1 Cu 34.3

Nonmagnetic 99.27 0.622 Cu 65.7

Calculated Feed 100.0 0.94 Cu 100.0

Metal

Weight Grade Distri-

Product (%) (%) Metal bution

Magnetic 8.4 0.248 U30S 85.0

Nonmagnetic 9\.6 0.004 U30S 15.0

Calculated Feed 100.0 0.024 U30S 100.0

Magnetic 2.4 0.85 W 5.0

Nonmagnetic 97.6 0.40 W 95.0

Calculated Feed 100.0 0.41 W 100.0

Magnetic 0.95 34.3 Cu 26.7

Nonmagnetic 99.05 0.904 Cu ') 73.3

Calculated Feed 100.0 \.22 Cu 100.0

55

EXAMPLE 7

Samples of different synthetic ores were prepared as

indicated in Example 1. Each of the samples in this

example was pretreated with heat and carbon monoxide 60

by rapidly heating the reactor containing the sample to

400° C. while purging it with nitrogen. This temperature

was maintained for 15 minutes while carbon monoxide

gas was passed through the reactor at a flow rate

of one reactor volume of gas every 4.3 minutes. The 65

reactor was cooled under a purge of nitrogen gas.

Thereafter each sample was treated with 8 kilograms of

iron pentacarbonyl per metric ton of sample for 30

EXAMPLE 9

For comparative purposes, samples of the same type

of ores used in the preceding examples were not given

any pretreatment but were just treated with 8 kilograms

of iron pentacarbonyl per metric ton of feed for 30

minutes at the same temperature as used in the preceding

examples. These samples were then magnetically

separated. Additionally, another series of samples of

ores were treated merely to the temperature of the iron

carbonyl treatment and given no iron carbonyl treatment;

these were also subjected to a magnetic separation

process. Analyses of these comparative results are

given below in Table 9.

4,205,979

11 12

TABLE 9

Dosage of

Fe(CO)s Weight Grade Metal

Mineral (Kg./nr; ton) Product (%) (%) Metal Distribution

Carnotite 8 Magnetic 1.4 0.731 U30S 35.3

Nonmagnetic 98.6 0.019 U30S 64.7

Calculated Feed 100.0 0.029 U30S 100.0

Carnotite 0 Magnetic 0.67 0.297 U30S 6.7

Nonmagnetic 99.33 0.028 U30S 93.3

Calculated Feed 100.0 0.030 U30S 100.0

Apatite 8 Magnetic 4.9 4.0 P 39.9

Nonmagnetic 95.1 0.31 P 60.1

Calculated Feed 100.0 0.491 P 100.0

Apatite 0 Magnetic 0.41 0.34 P 0.4

Nonmagnetic 99.59 0.36 P 99.6

Calculated Feed 100.0 0.36 P 100.0

Scheelite 8 Magnetic 27.4 2.85 W 58.6

Nonmagnetic 72.6 0.76 W 41.4

Calculated Feed 100.0 1.33 W 100.0

Scheelite 0 Magnetic 2.1 2.44 W 4.0

Nonmagnetic 97.9 1.23 W 96.0

Calculated Feed 100.0 1.25 W 100.0

Cuprite 8 Magnetic 2.1 0.165 Cu 47.3

Nonmagnetic 97.9 0.004 Cu 52.7

Calculated Feed 100.0 0.0074 Cu 100.0

Cuprite 0 Magnetic 0.54 0.417 Cu 31.5

Nonmagnetic 99.46 0.005 Cu 68.5

Calculated Feed 100.0 0.0073 Cu 100.0

Bauxite Magnetic 3.3 20.1 AI 97.9

Nonmagnetic 96.7 0.014 AI 2.1

Calculated Feed 100.0 0.677 AI 100.0

Bauxite 0 Magnetic 0.81 17.0 AI 18.7

Nonmagnetic 99.19 0.605 AI 81.3

Calculated Feed 100.0 0.738 AI 100.0

Hematite 8 Magnetic 1.14 36.2 Fe 33.9

Nonmagnetic 98.86 0.81 Fe 66.1

Calculated Feed 100.0 1.21 Fe 100.0

Hematite 0 Magnetic 0.10 22.9 Fe 3.1

Nonmagnetic 99.90 0.73 Fe 96.9

Calculated Feed 100.0 0.75 Fe 100.0

Cassiterite 8 Magnetic 3.5 4.83 Sn 14.9

Nonmagnetic 96.5 0.998 Sn 85.1

Calculated Feed 100.0 1.13 Sn 100.0

Cassiterite 0 Magnetic 0.65 23.6 Sn 10.8

Nonmagnetic 99.35 U5 Sn 89.2

Calculated Feed 100.0 1.39 Sn 100.0

EXAMPLE 10

Samples of apatite and bauxite were made into 3%

synthetic ores as indicated in Example 1. Each of these

samples was subjected to a pretreatment and thereafter

treated with 16 kilograms offerrocene per metric ton of 4S

sample. The ferrocene were mixed with the sample, and

the temperature of the reactor was slowly raised to 400·

C. over a two hour period. The system was purged with

nitrogen prior to and following the ferrocene treatment.

Finally, the samples were subjected to a wet magnetic SO

separation process. Each of the pretreatments, i.e.,

steam, heat plus nitrogen, heat plus hydrogen and heat

plus carbon monoxide, were conducted in the same

manner as the pretreatment in Examples 1,3, S, and 7,

respectively.

For comparative purposes, additional samples of the

same type of ores were subjected to just the pretreatment

followed by wet magnetic separation. Also, samples

of these ores were given no pretreatment and were

subjected to only the ferrocene treatment with subsequent

magnetic separation. Analyses of these comparative

samples are given in Table 10.

TABLE 10

Weight Grade Metal

Mineral Pretreatment Product (%) (%) Metal Distribution

Apatite Steam Magnetic 0.91 3.33 P 5.7

Nonmagnetic 99.09 0.502 P 94.3

Calculated Feed 100.0 0.53 P 100.0

Apatite Steam blank Magnetic 0.37 1.16 P 0.8

Nonmagnetic 99.63 0.53 P 99.2

Calculated Feed 100.0 0.53 P 100.0

Apatite Heat &; N2 Magnetic 0.96 3.99 P 7.2

Nonmagnetic 99.04 0.50 P 92.8

Calculated Feed 100.0 0.53 P 100.0

Apatite Heat &; N2 blank Magnetic 0.60 1.64 P 1.8

Nonmagnetic 99.40 0.53 P 98.2

Calculated Feed 100.0 0.54 P 100.0

Apatite Heat &; H2 Magnetic 1.7 4.71 P 15.0

Nonmagnetic 98.3 0.46 P 85.0

Calculated Feed 100.0 0.53 P 100.0

Apatite Heat &; H2 blank Magnetic 1.3 4.81 P 11.9

4,205,979

13 14

TABLE to-continued

Weight Grade Metal

Mineral Pretreatment Product (%) (%) Metal Distribution

Nonmagnetic 98.7 0.47 P 88.1

Calculated Feed 100.0 0.53 P 100.0

Apatite Heat&CO Magnetic 1.1 5.71 P 12.4

Nonmagnetic 98.9 0.45 P 87.6

Calculated Feed 100.0 0.51 P 100.0

Apatite Heat & CO blank Magnetic 0.77 6.40 P 9.2

Nonmagnetic 99.23 0.49 P 90.8

Calculated Feed 100.0 0.54 P 100.0

Apatite None Magnetic 5.1 2.1 P 26.1

(Ferrocene Nonmagnetic 94.9 0.32 P 73.9

treatment Calculated Feed 100.0 0.41 P 100.0

@400' c.)

Apatite None Magnetic 0.54 1.22 P 1.6

(Heat to Nonmagnetic 99.46 0.43 P 98.4

400' C. and Calculated Feed 100.0. 0.435 P 100.0

no Ferrocene)

Bauxite Steam Magnetic 2.8 23.1 Al 94.3

Nonmagnetic 97.2 0.04 Al 5.7

Calculated Feed 100.0 0.69 Al 100.0

Bauxite Steam blank Magnetic 1.33 1.71 Al 3.8

Nonmagnetic 98.67 0.59 Al 96.2

Calculated Feed 100.0 0.61 Al 100.0·

Bauxite Heat & Nz Magnetic 3.4 21.0 Al 77.9

Nonmagnetic 96.6 0.21 Al 22.1

Calculated Feed 100.0 0.92 Al 100.0

Bauxite Heat & Nz Magnetic 2.0 25.6 AI 61.3

blank Nonmagnetic 98.0 0.33 Al 38.7

Calculated Feed 100.0 0.84 Al 100.0

Bauxite Heat & Hz Magnetic 4.1 18.8 AI 86.1

Nonmagnetic 95.9 0.13 AI 13.9

Calculated Feed 100.0 0.90 Al 100.0

Bauxite Heat & Hz Magnetic 3.3 17.6 AI 77.9

blank Nonmagnetic 96.7 0.17 Al 22.1

Calculated Feed 100.0 0.75 Al 100.0

Bauxite Heat & CO Magnetic 1.8 17.3 Al 66.5

Nonmagnetic 98.2 0.16 Al 33.5

Calculated Feed 100.0 0.47 Al 100.0

Bauxite Heat & CO Magnetic 3.0 23.4 Al 75.1

blank Nonmagnetic 97.0 0.24 Al 24.9

Calculated Feed 100.0 0.93 Al 100.0

Bauxite None Magnetic 3.4 14.3 Al 86.3

(Ferrocene Nonmagnetic 96.6 0.08 AI 13.7

treatment Calculated Feed 100.0 0.563 AI 100.0

@400' c.)

None

Bauxite (Heated to Magnetic 2.4 17.7 Al 64.5

400' C. and Nonmagnetic 97.6 0.24 Al 35.5

no ferrocene) Calculated Feed 100.0 0.659 Al 100.0

EXAMPLE II 45 ments indicated in Table II were conducted in the same

manner as described in Example 1, 3, 5 or 7.

Samples of different synthetic ores were prepared as For comparative purposes, samples of the same type

indicated in Example 1. Each of these samples were of ores were subjected to just the pretreatment followed

subjected to a pretreatment and thereafter treated with by magnetic separation (these results are designated as

16 kilograms of vaporized ferric acetylacetonate per 50 blanks in Table 11). Additional samples of these ores

metric ton of sample at a temperature of 2700 C. for a were given no pretreatment and were subjected to only

period of 30 minutes. The samples were then subjected the ferric acetylacetonate treatment with subsequent

to a magnetic separation process. Each of the pretreat- magnetic separation. Analyses of these comparative

samples are given below in Table 11.

TABLE 11

Weight Grade Metal

Mineral Pretreatment Product (%) (%) Metal Distribution

Carnotite Steam Magnetic 4.1 0.089 U308 48.8

Nonmagnetic 95.9 0.004 U308 51.2

Calculated Feed 100.0 0.007 U308 100.0

Carnotite Steam Magnetic 0.52 0.092 U308 3.1

blank Nonmagnetic 99.48 O.oJ5 U308 96.9

Calculated Feed 100.0 O.oJ5 U308 100.0

Carnotite Heat & Hz Magnetic 4.1 0.122 U308 63.5

Nonmagnetic 95.9 0.003 U308 36.5

Calculated Feed 100.0 0.008 U30 8 100.0

Carnotite Heat & Hz Magnetic 6.7 0.106 U308 60.4

blank Nonmagnetic 93.3 0.005 U308 39.6

Calculated Feed 100.0 0.012 U308 100.0

Carnotite Heat & CO Magnetic 7.7 0.093 U308 79.5

15

4,205,979

16

TABLE II-continued

Weight Grade Metal

Mineral Pretreatment Product (%) (%) Metal Distribution

Nonmagnetic 92.3 0.002 U30 g 20.5

Calculated Feed 100.0 0.009 U30 g 100.0

Carnotite Heat &CO Magnetic 5.1 0.115 U30 g 46.9

blank Nonmagnetic 94.9 0.007 U30g 53.1

Calculated Feed 100.0 0.013 U30g 100.0

Carnotite None (ace- Magnetic 1.2 0.418 U30 g 25.6

tylaceto- Nonmagnetic 98.8 0.015 U30g 74.4

nate at 270· C.) Calculated Feed 100.0 0.020 U30 g 100.0

Carnotite None (heated Magnetic 0.97 0.514 U30g 21.9

to 270· C.) Nonmagnetic 99.03 0.Ql8 U30 g 78.1

Calculated Feed 100.0 0.023 U30 g 100.0

Apatite Heat & H2 Magnetic 3.2 2.15 P 13.0

Nonmagnetic 96.8 0.475 P 87.0

Calculated Feed 100.0 0.53 P 100.0

Apatite Heat & H2 Magnetic 1.3 4.81 P 11.9

blank Nonmagnetic 98.7 0.47 P 88.1

Calculated Feed 100.0 0.53 P 100.0

Apatite Heat & CO Magnetic 3.0 2.20 P 12.8

Nonmagnetic 97.0 0.464 P 87.2

Calculated Feed 100.0 0.52 P 100.0

Apatite Heat & CO Magnetic 0.77 6.40 P 9.2

blank Nonmagnetic 99.23 0.49 P 90.8

Calculated Feed 100.0 0.54 P 100.0

Apatite None (acetyl- Magnetic 2.3 0.96 P 5.8

acetonate at Nonmagnetic 97.7 0.37 P 94.2

2W c.) Calculated Feed 100.0 0.384 P 100.0

Apatite None (heated Magnetic 0.34 0.637 P 0.5

to 270· C.) Nonmagnetic 99.66 0.427 P 99.5

Calculated Feed 100.0 0.428 P 100.0

Hematite Steam Magnetic 0.62 29.8 Fe 20.1

Nonmagnetic 99.38 0.739 Fe 79.9

Calculated Feed 100.0 0.92 Fe 100.0

Hematite Steam Magnetic 0.06 17.6 Fe 1.0

blank Nonmagnetic 99.94 1.03 Fe 99.0

Calculated Feed 100.0 1.04 Fe 100.0

Hematite Heat & N2 Magnetic 0.70 26.0 Fe 19.6

Nonmagnetic 99.30 0.75 Fe 80.4

Calculated Feed 100.0 0.93 Fe 100.0

Hematite Heat & N2 Magnetic 0.05 23.4 Fe \.I

blank Nonmagnetic 99.95 1.05 Fe 98.9

Calculated Feed 100.0 1.06 Fe 100.0

Hematite Heat & H2 Magnetic 4.6 8.88 Fe 67.1

Nonmagnetic 95.4 0.21 Fe 32.9

Calculated Feed 100.0 0.61 Fe 100.0

Hematite Heat & H2 Magnetic 6.8 6.85 Fe 74.6

blank Nonmagnetic 93.2 0.17 Fe 25.4

Calculated Feed 100.0 0.62 Fe 100.0

Hematite None (acetyl- Magnetic 0.63 24.1 Fe 16.9

acetonate at Nonmagnetic 99.37 0.75 Fe 83.1

270· c.) Calculated Feed 100.0 0.90 Fe 100.0

Hematite None (heated Magnetic 0.39 5.96 Fe 2.4

to 270· C.) Nonmagnetic 99.61 0.94 Fe 97.6

Calculated Feed 100.0 0.96 Fe 100.0

Bauxite Steam Magnetic 4.3 13.3 AI 81.0

Nonmagnetic 95.7 0.14 AI 19.0

Calculated Feed 100.0 0.71 AI 100.0

Bauxite Steam Magnetic \.16 1\.1 Al 18.3

blank Nonmagnetic 98.84 0.58 AI 81.7

Calculated Feed 100.0 0.70 Al 100.0

Bauxite Heat & N2 Magnetic 2.5 20.8 Al 80.4

Nonmagnetic 97.5 0.13 AI 19.6

Calculated Feed 100.0 0.65 AI 100.0

Bauxite Heat & N2 Magnetic 1.88 17.9 AI 50.2

blank Nonmagnetic 98.12 0.34 Al 49.8

Calculated Feed 100.0 0.67 Al 100.0

Bauxite None (acetyl- Magnetic 2.4 18.9 Al 70.0

acetonate at Nonmagnetic 97.6 0.20 AI 30.0

270· c.) Calculated Feed 100.0 0.649 AI 100.0

Bauxite None (heated Magnetic 1.6 24.4 Al 48.0

to 270· C.) Nonmagnetic 98.4 0.43 AI 52.0

Calculated Feed 100.0 0.814 Al 100.0

Scheelite Steam Magnetic 4.4 1.07 W 10.1

Nonmagnetic 95.6 0.44 W 89.9

Calcul~ted Feed 100.0 0.47 W 100.0

Scheelite Steam Magnetic 1.2 \.29 W 3.1

blank Nonmagnetic 98.2 0.49 W 96.9

Calculated Feed 100.0 0.50 W 100.0

Scheelite Heat & CO Magnetic 4.5 0.936 W 8.6

Nonmagnetic 95.5 0.466 W 9\.4

Calculated Feed 100.0 0.49 W 100.0

-

17

4,20S,979

18

TABLE II-continued

Weiaht Orade Metal

Mineral Pretreatment Product (%) (%) Metal Dlatributian

Scheellte Heat ot CO Maanetie 1.9 1.55 W 5.9

blank Nanmaanetle 98.1 0.48 W 94.1

Caleulated Peed 100.0 0.50 W 100.0

ScheeUte Heat ot N2 Maanetie 3.8 1.25 W 9.8

Nanmaanetle 96.2 0.454 W 90.2

Caleulated Peed 100.0 0.48 W 100.0

ScheeUte Heat" N2 Maanetle 1.8 1.16 W 4.2

blank Nanmaanetie 98.2 0.49 W 95.8

Caleulated Peed 100.0 0.50 W 100.0

Scheellte Nane (I"etyl. Maanetie 3.1 0.96 W 7.7

I"etanate at Nanmaanetie 96.9 0.37 W 92.3

270' C.) Caleulated Peed 100.0 0.39 W 100.0

ScheeUte None (heated Maanetie 1.3 1.09 W 3.3

to 270' C.) Nanmaanetle 98.7 0.42 W 96.7

Caleulated Peed 100.0 0.43 W 100.0

EXAMPLE 12 EXAMPLE 13

Samples of carnotite and cuprite synthetic ores were 20 Samples of carnotite and cuprite synthetic ores were

prepared as indicated in Example 1.'AIIII1ple ofeach of prepared II indicated in Example 1. Asample ofeach of

these ores wu pretreated with heat and hydrolen suI- these ores WII pretreated with heat and sulfur dioxide

fide III, by rapidly heatinl the reactor containinl the IU by rapidly heatinl the reactor containinl the sample

sample to 200' C. while purlinl it with nitrolen. This 25 to 400' C. while purlinl it with nitrolen. This tempera·

temperature wu maintained for 15 minutes while hy. ture WII maintained for 15 minutes while sulfur dioxide

drogen sulfide III WII pused throulh,the reactor at a III WII passed throulh the reactor at a flow rate of one

flow rate ofone reactor volume of las beinl introduced reactor volume of III beinl introduced every 4.3 min·

into the system every 4.3 minutes. The reactor WII utes. the reactor WII cooled under a purle of nitrolen

cooled under a purle of nitrolen las. Each sample WII III. Each sample WII then treated with 8 kilolrams of

then treated with 8kilograms of iron pentacarbonyl per 30 iron pentacarbonyl per metric ton of sample for 30,

metric ton of sample for 30 minutes at a temperature of minutes at a temperature of 145' C. in the case of the

145' C. in the case of carnotite and at a temperature of carnotite ore and a temperature of 125' C. in the case of

125' C. in the case of cuprite ore. For comparative the cuprite ore. For comparative purposes, an addi·

purposes, an additional sample of each of these ores tionahample oreach ofthese ores wilsubjected only to

received merely the pretreatment in the manner indio 35 the pretreatment in the manner indicated above. All of

cated above. All of the samples were subjected to a wet the IIII1ples were subjected to a wet mqnetic separa·

magnetic separation process. Analyses of the products tion proceu and the analyses of the products thus ob·

thus obtained are presented below in Table 12. tained are given below in Table 13.

TABLE 12

Minerai

Clmotlte

Clmatlte

Cuprite

Cuprite

Pe (CO)s

Treltment

Yea

No

Yea

No

Produet

Mlanetle

Nonmlanetle

Clleullted Peed

Mlanetle

Nonmlanetie

Clleullted Peed

Mlanetle

Nonmllnetle

Clleullted Peed

Mlanetle

Nonmllnetle

Clleulltllll PHd

Weiaht Oracle

("') ("') Metll

43.8 0,024 U30.

56.2 0,00I U30.

100,0 0.011 U30.

0.86 0,187 U30.

99.14 0.008 U30.

100.0 0.010 U30.

10,3 5.08 Cu

89,7 0,89 Cu

100,0 1.32 Cu

0,77 12.1 Cu

99.23 0.40 Cu

100,0 0.49 Cu

Metll

Dlltrlbutlan

94,9

5.1

100.0

16,9

83,1

100.0

39.6

60,4

100.0

19.0

81.0

100,0

TABLE 13

Pe (CO)S Weilht Oracle Melli

Minerll Tl'Illlmenl Product ("') ("') MellI Diltrlbutlon

CArnotlle Ye~ Mllnetle 59.2 0,019 U30. 82,1

Nllnmllnetle 40,8 0.006 U30. 17.9

ClleulllllI Piled 100.0 0.014 U30i 100,0

Clrnolitll No ,Mlllnlltle Cl.99 0,161 U30. 10,3

Nonmllnelle 99.01 ' 0,014 U30. 89.7

CAleulllllI PHd 100.0 0.015 U30. 100.0

CUllrl11l YIlI Mlllnlltle 32.8 1.21 Cu 47.2

Nllnmlllnlllle 67.2 0,66 Cu 52.8

Cileullilld'PIllld 100,0 0,84 Cu 100.0

CUllrlllJ Nil Millnelie (>.33 9.35 Cu 3.9

Nllnmillnetie 99.67 0,77 Cu 96.1

Clteutlled Pelll 100,0 0.10 Cu 100,0

4,205,979

19

EXAMPLE 14

Samples of carnotite and cuprite synthetic ores were

prepared as indicated in Example 1. A sample of each of

these ores was pretreated with heat and ammonia by

rapidly heating the reactor containing the sample to

4000 C. while purging it with nitrogen. This temperature

was maintained for 15 minutes while ammonia gas

was passed through the reactor at a flow rate of one

reactor volume of gas being introduced every 4.3 min-

20

perature variations. The temperature and time of the

pretreatment are set forth in Table 15. For comparative

purposes, samples were subjected just to the pretreatment,

receiving no iron carbonyl treatment. Addition-

S ally, two samples received no pretreatment with one

beitlg subjected to the iron carbonyl treatment and the

other merely being heated to a temperature of 1450 C.

All of the samples were subjected to a wet magnetic

separation process. Analyses of the products thus ob-

10 tained are presented below in Table 15.

TABLE 15

FE (CO)s Pretreatment

Treatment Temperature Time Weight Grade UJOg

(Pretreatment) ("C.) (minutes) Product (%) (%) Distribution

Yes ISO 15 Magnetic 22.7 0.024 58.5

(Heat &. H2) Nonmagnetic 77.3 0.005 41.5

Calculated Feed 100.0 0.009 100.0

No ISO 15 Magnetic 0.92 0.033 3.0

(Heat &. H2) Nonmagnetic 99.08 0.010 97.0

Calculated Feed 100.0 0.010 100.0

Yes ISO 90 Magnetic 11.1 0.033 37.0

(Heat &. H2) Nonmagnetic 88.9 0.007 62.9

Calculated Feed 100.0 0.010 100.0

No ISO 90 Magnetic 0.73 0.061 3.1

(Heat &. H2) Nonmagnetic 99.27 0.014 96.9

Calculated Feed 100.0 0.014 100.0

Yes ISO 15 Magnetic 52.0 0.017 78.6

(Heat&. CO) Nonmagnetic 48.0 0.005 21.4

Calculated Feed 100.0 0.011 100.0

No 150 15 Magnetic 0.78 0.226 15.1

(Heat &. CO) Nonmagnetic 99.22 0.010 84.9

Calculated Feed 100.0 0.012 100.0

Yes none Magnetic \.4 0.73 34.5

Nonmagnetic 98.6 0.019 65.5

Calculated Feed 100.0 0.029 100.0

No (heated none Magnetic 0.67 0.297 6.7

to 145' C.) Nonmagnetic 99.33 0.028 93.3

Calculated Feed 100.0 0.030 100.0

utes. The reactor was cooled under a purge of nitrogen

gas. Each sample was then treated with 8 kilograms of

iron pentacarbonyl per metric ton of sample for 30

minutes at a temperature of 1450 C. in the case of the

carnotite ore and at a temperature of 1250 C. in the case 40

of the cuprite ore. All of the samples were subjected to

a wet magnetic separation process. The analyses of the

products thus obtained are presented below in Table 14.

TABLE 14

EXAMPLE 16

Chrysocolla was ground to a minus 65 mesh and

mixed with minus 65 mesh silica sand to produce a 3%

synthetic ore. A sample of this ore was pretreated with

steam in the manner described in Example 1 and another

sample was pretreated with heat and hydrogen

sulfide gas in the manner described in Example 12. Both

were then separately treated with 8 kilograms of iron

Fe (CO)s Weight Grade Metal

Mineral Treatment Product (%) (%) Metal Distribution

Carnotite Yes Magnetic 49.3 0.019 UJOg 82.2

Nonmagnetic SO.7 0.004 UJOg 17.8

Calculated Feed 100.0 0.011 UJOg 100.0

Carnotite No •Magnetic \.9 0.140 U30g 2\.3

Nonmagnetic 98.1 0.010 U30 g 78.7

Calculated Feed 100.0 0.012 U30g 100.0

Cuprite Yes Magnetic 5.6 20.6 Cu 91.S

Nonmagnetic 94,4 0.114 Cu 8.5

Calculated Feed 100.0 \.26 Cu 100.0

Cuprite No Magnetic \.6 42.9 Cu 59.7

Nonmagnetic 98.4 0.47 Cu 40.3

Calculated Feed 100.0 1.15 Cu 100.0

Samples of carnotite were made into 3% synthetic

ores as indicated in Example 1. Each of these samples

was subjected to a pretreatment and thereafter treated

with eight kilograms of iron pentacarbonyl per metric 65

ton of sample for thirty minutes at a temperature of 1350

C. The pretreatments were carried out as described in

Examples 5 and 7 with the exception of time and tem-

EXAMPLE 15 60

pentacarbonyl per metric ton of ore for 30 minutes at a

temperature of 1600 C.

For comparative purposes, additional samples of the

ore were subjected to only the steam and hydrogen

sulfide pretreatments. Also, two sets of samples of the

ore were given no pretreatment; one was subjected to

only the iron pentacarbonyl treatment and the other

sample was heated to 1600 C.

4,205,979

21

All of the samples were subjected to a wet magnetic

separation process. Anaylses of the products thus obtained

are given below in Table 16.

22

7. The process of claim 6 wherein the metal containing

compound is employed in an amount of from about

0.1 to 100 kilograms per metric ton of ore.

TABLE 16

Weight Grade Copper Separation

Pretreatment Product (%) (%) Distribution Amperage

None (Fe(DOls Magnetic 5.6 3.55 91.3 2.0

at 160' C.) Nonmagnetic 94.4 0.02 8.7

Calculated Feed 100.0 0.218 100.0

None (heated Magnetic 1.44 6.86 50.1 2.0

to 16O'C.) Nonmagnetic 98.56 0.10 49.9

Calculated Feed 100.0 0.197 100.0

Steam Magnetic 4.7 3.66 72.1 1.0

Nonmagnetic 95.3 0.07 27.9

Calculated Feed 100.0 0.239 100.0

Steam blank Magnetic 0.6 5.91 17.3 1.0

Nonmagnetic 99.4 0.17 82.7

Calculated Feed 100.0 0.204 100.0

H2S Magnetic 21.0 0.41 40.5 1.0

Nonmagnetic 79.0 0.16 59.5

Calculated Feed 100.0 0.213 100.0

H2S blank Magnetic 0.41 1.58 2.9 1.0

Nonmagnetic 99.59 0.22 97.1

Calculated Feed 100.0 0.226 100.0

None (Fe(COls Magnetic 3.5 5.11 78.8 1.0

at 160' C.) Nonmagnetic 96.5 0.05 21.2

Calculated Feed 100.0 0.227 100.0

None (heated to Magnetic 1.0 5.29 22.9 1.0

160' c.) Nonmagnetic 99.0 0.18 77.1

Calculated Feed 100.0 0.231 100.0

8. In a process for the beneficiation of a metal oxide

30 ore wherein the ore is treated with an iron carbonyl

compound under conditions which cause the iron carbonyl

compound to react substantially at the surface of

the metal oxide particles to the substantial exclusion of

the gangue particles so as to alter the surface characteristics

of the metal values thereby causing a selective

enhancement of the magnetic susceptibility of one or

more metal oxide values of the ore to the exclusion of

the gangue in order to permit a physical separation

between the values and the gangue, the improvement

comprising:

treating the ore with heat prior to its treatment with

the iron carbonyl.

9. The process of claim 8 wherein the ore is pretreated

to a temperature of at least about 800 C. for a

time period of at least about 0.1 hours.

10. The process of claim 9 wherein the ore is pretreated

to a temperature of from about 1250 C. to about

4500 C. for a time period of from about 0.20 to about 4

hours.

11. The process of claim 9 wherein the heat pretreatment

is conducted in the presence of a gas selected from

the group consisting of steam, nitrogen, hydrogen, carbon

monoxide, carbon dioxide, ammonia, hydrogen

sulfide, sulfur dioxide, methane, air, ethane, propane,

55 butane and other hydrocarbon compounds in the gaseous

state at the pretreatment temperature.

12. The process of claim 9 wherein the metal oxide

ore is selected from the group consisting of carnotite,

apatite, scheelite, cuprite, cassiterite, bauxite and hematite.

13. In a process for the beneficiation of a metal oxide

ore wherein the ore in a specific system is treated with

from about 0.1 to about 100 kilograms of a metal containing

compound per metric ton of ore at a temperature

within a range of 1250 C. less than the general

decomposition temperature of the metal containing

compound in a specific system for the ore being treated

for a period of time from about 0.05 to about 4 hours to

What is claimed is:

1. In a process for the beneficiation of a metal oxide

ore wherein the ore is treated with a metal containing

compound under conditions which cause the metal

containing compound to react substantially at the sur- 35

face of the metal oxide particles to the substantial exclusion

of the gangue particles so as to alter the surface

characteristics of the metal values thereby causing a

selective enhancement of the magnetic susceptibility of

one ore more metal oxide values of the ore to the exclu- 40

sion of the gangue in order to permit a separation between

the values and gangue, the improvement comprising:

treating the ore with heat prior to its treatment with

the metal containing compound. 45

2. The process of claim 1 wherein the heat pretreatment

is conducted at a temperature of at least about 800

C.

3. The process of claim 2 wherein the heat pretreatment

is conducted in the presence of a gas selected from 50

the group consisting of steam, nitrogen, hydrogen, carbon

monoxide, carbon dioxide, ammonia, hydrogen

sulfide, sulfur dioxide, methane, air, ethane, propane,

butane and other hydrocarbons in the gaseous state at

the pretreatment temperature.

4. The process of claim 3 wherein the gas is employed

in an amount of at least about 2 cubic meters per hour

per metric ton of metal oxide ore being processed.

5. The process of claim 3 wherein the gas is steam at

a temperature of at least about 1000 C. and employed in 60

an amount of from about I% to 50 weight percent water,

based on the weight of the metal oxide ore.

6. The process of claim 2 or claim 3 wherein the

treatment of the ore with the metal containing compound

is conducted at a temperature within a range of 65

1250 C. less than the general decomposition temperature

of the metal containing compound in a specific system

for the are being treated.

4,205,979

24

from about 2 to about 20 kilograms of an iron cOlltaining

compound per metric ton of ore at a temperature within

a range of 1250 C. less than the general decomposition

temperature of the iron containing compound in a specific

system for the ore being treated to cause the iron

containing compound to react substantially at the surface

of the metal oxide particles to the substantial exclusion

of the gangue particles so as to alter the surface

characteristics of the metal values thereby causing a

selective enhancement of the magnetic susceptibility of

one ore more metal oxide values contained in the ore to

the exclusion of the gangue in orddr to permit their

magnetic separation, the improvement comprising:

heating the ore to a temperature of from about 1250

C. to about 5000 C. for a time period of from about

0.25 to about I hour prior to its treatment with the

iron containing compound.

34. The process of claim 33 wherein the ore is selected

from the group consisting of apatite and bauxite.

35. The process of claim 34 wherein the iron containing

compound is ferrocene and the heat pretreatment is

conducted in the presence of a gas selected from the

group consisting of steam and nitrogen.

36. The process of claim 33 wherein the ore is selected

from the group consisting of carnotite, apatite

and bauxite, the iron containing compound is ferrocene

and the heat pretreatment is conducted in the presence

of a gas selected from the group consisting of hydrogen

and carbon monoxide.

37. The process of claim 33 wherein the ore is selected

from the group consisting of shceelite, hematite

and bauxite and the iron containing compound is ferric

acetylacetonate.

38. The process of claim 33 wherein the ore is selected

from the group consisting of carnotite, scheelite,

hematite and bauxite, the iron containing compound is

ferric acetylacetonate and the heat pretreatment is conducted

in the presence of steam.

39. The process of claim 33 wherein the ore is selected

from the group consisting of carnotite, apatite

and hematite, the iron containing compound is ferric

acetylacetonate and the heat pretreatment is conducted

in the presence of hydrogen.

40. The process of claim 33 wherein the ore is selected

from the group consisting of carnotite, scheelite

and apatite, the iron containing compound is ferric

acetylacetonate and the heat pretreatment is conducted

in the presence of carbon monoxide.

41. In a process for the beneficiation of a metal oxide

ore wherein the ore for the specific system is treated

with from about 0.1 to about 100 kilograms of an iron

50 containing compound selected from the group consisting

of ferrous chloride, ferric chloride, ferrocene, ferrocene

derivatives, ferric acetylacetonate and ferric acetylacetonate

derivatives per metric ton of ore at a temperature

within a range of 1250 C. less than the general

decomposition temperature of the metal containing

compound in a specific system for the ore being treated

for a period of time from about 0.05 to about 4 hours to

cause the iron containing compound to react substantially

at the surface of the metal oxide particles to the

substantial exclusion of the gangue particles so as to

alter the surface characteristics of the metal values

thereby causing a selective enhancement of the magnetic

susceptibility of one or more metal oxide values

contained in the ore to the exclusion of the gangue in

order to permit a physical separation between the values

and gangue, the improvement comprising:

heat treatment of the ore prior to treating it with the

iron containing compound.

* * * * *

23

cause the metal containing compound to react substantially

at the surface of the metal oxide particles to the

substantial exclusion of the gangue particles so as to

alter the surface characteristics of the metal values

thereby causing a selective enchancement of the mag- 5

netic susceptibility of one ore more metal oxide values

contained in the ore to the exclusion of the gangue in

order to permit a physical separation, the improvement

comprising:

heat treatment of the ore prior to treating it with the

metal containing compound. 10

14. The process of claim 1 or claim 13 wherein the

metal containing compound is an iron containing compound.

15. The process of claim 14 wherein the iron containing

compound is selected from the group consisting of 15

ferrous chloride, ferric chloride, ferrocene, ferrocene

derivatives, ferric acetylacetonate, and ferric acetylacetonate

derivatives.

16. The process of claim 1 or claim 13 wherein the

metal containing compound is a carbonyl. 20

17. The process of claim 16 wherein the carbonyl is

selected from the group consisting of iron, cobalt, and

nickel.

18. The process of claim 17 wherein the carbonyl

comprises an iron carbonyl.

19. The process of claim 13 or claim 15 wherein the 25

ore is pretreated to a temperature ofat least about 800 C.

for a time period of at least about 0.1 hours.

20. The process of claim 19 wherein the ore is pretreated

to a temperature of from about 1250 C. to about

4500 C. for a time period of from about 0.20 to about 4 30

hours.

21. The process ofclaim 19 wherein the heat pretreatment

is conducted in the presence of a gas selected from

the group consisting of steam, nitrogen, hydrogen, carbon

monoxide, carbon dioxide, ammonia, hydrogen 35

sulfide, sulfur dioxide, methane, air, ethane, propane,

butane and other hydrocarbon compounds in the gaseous

state at the pretreatment temperature.

22. The process of claim 21 wherein the gas is employed

in an amount of at least about 12 cubic meters 40

per hour per metric ton of ore being processed.

23. The process of claim 20 wherein the metal containing

compound is an iron carbonyl and the treatment

of the ore with the iron carbonyl is carried out at a

temperature within a range 150 C. less than the general

decomposition temperature of the iron carbonyl in the 45

specific system for the ore being treated.

24. The process of claim 23 wherein the heat pretreatment

is conducted in the presence of a gas selected from

the group consisting of steam, nitrogen and carbon

monoxide.

25. The process of claim 24 wherein the ore is carnotite.

26. The process of claim 24 wherein the ore is apatite.

27. The process of claim 24 wherein the ore is scheelite.

55

28. The process of claim 24 wherein the ore is cuprite.

29. The process of claim 24 wherein the ore is cassiterite.

30. The process of claim 23 wherein the heat pretreatment

is conducted in the presence of a gas selected from

the group consisting of hydrogen, hydrogen sulfide, 60

sulfur dioxide and ammonia.

31. The process of claim 30 wherein the ore is carnotite.

32. The process of claim 30 wherein the ore is cuprite.

33. In a process for the beneficiation of a metal oxide 65

ore selected from the group consisting of carnotite,

apatite, scheelite, cuprite, cassiterite, bauxite, and hematite

wherein the ore in a specific system is treated with

UNITED STATES PATENT AND TRADEMARK OFFICE

CERTIFICATE OF CORRECTION

PATENT NO.

DATED

INVENTOR(S)

4,205,979

June 3, 1980

Kindig, et al.

ISEALI -'

It is certified that error appears in the above-ldentified patent and that said letters Patent

is hereby corrected as shown below:

Column 1, line 62, delete "or" insert --ore--.

Column 2, line 32, delete "vaporizaton" insert

--vaporization--.

Column 3, line 37, delete "surfacr characterisics" insert

--surface characteristics--.

Column 3, line 53, delete " c hrysocollar" insert

--chrysocolla--.

Column 4, line 61, delete "sulfides" insert --oxides--.

Column 24, line 30, delete "shceelite,"'insert --scheelite,--

9igncd and 9calcd this

Nineteenth Day of MIIY /98/

..fttest:

RENE D. TEGTMEYER

Attestill, Officer


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