Preparation of unagglomerated metal oxide particles with uniform particle size

Claim 2

A process for the production of substantially unagglomerated metal oxide particles having a mean diameter of up to about 1 micron and a substantially uniform particle size comprising: (a) providing a solution of an oxygen-containing nitrate of a first metal selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and mixtures of these; (b) adding to the solution a chelating agent selected from the group consisting of tartaric acid, citric acid, and mixtures of these; (c) adding to the solution a base selected from the group consisting of ammonium hydroxide, urea, and mixtures of these; (d) drying the solution by heating for a time and at a temperature sufficient to remove substantially all the solvent from the solution to leave a solid residue; and (e) calcining the solid residue for a time and at a temperature sufficient to form particles of said metal oxide.

Claim 3

The process of claim 1 wherein said first metal is selected from the group consisting of alkaline earth metals, lanthanide metals, metals from Group IVb of the periodic table, and mixtures of these.

Claim 4

The process of claim 1 wherein the solution has a solvent selected from the group consisting of C 1 -C 3 alcohols.

Claim 5

The process of claim 3 wherein said chelating agent is citric acid.

Claim 6

The process of claim 4 wherein said first metal is zirconium.

Claim 7

The process of claim 5 wherein said nitrate is zirconyl nitrate.

Claim 8

The process of claim 6 wherein the citric acid is added in an amount sufficient to produce a molar ratio of citric acid to zirconyl nitrate of at least about 0.5 to 1.

Claim 9

The process of claim 5 wherein said base is ammonium hydroxide.

Claim 10

The process of claim 5 further comprising the step of adding to the solution of step (a), (b) and/or (c) an oxygen containing salt of a second metal.

Claim 11

The process of claim 9 wherein said second metal salt is added in an amount sufficient to produce a second metal oxide in an amount up to about 10 mole percent of the oxide of the first metal.

Claim 12

The process of claim 10 wherein said second metal is selected from the group consisting of yttrium, magnesium and calcium.

Claim 13

A process for the production of substantially unagglomerated metal oxide particles having a mean diameter of up to about 1 micron and a substantially uniform particle size comprising: (a) providing an alkaline solution of a salt of a first metal having an ammonium cation and a carbonate anion, said first metal being selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and mixtures of these; (b) adding a chelating agent to the solution to form a chelated solution, said chelating agent being a sodium salt of an acid selected from the group consisting of EDTA, H-EDTA, NTA, DTPA, lactic acid, glycolic acid, succinic acid, and mixtures of these; (c) drying the chelated solution by heating for a time and at a temperature sufficient to remove substantially all the solvent from the solution to leave a solid residue; and (d) heating the solid residue for a time and at a temperature sufficient to convert at least a substantial portion of the residue to said metal oxide.

Claim 14

A process for the production of substantially unagglomerated metal oxide particles having a mean diameter of up to about 1 micron and a substantially uniform particle size comprising: (a) providing an alkaline solution of a salt of a first metal having an ammonium cation and a carbonate anion, said first metal being selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and mixtures of these; (b) adding a chelating agent to the solution to form a chelated solution, said chelating agent being a sodium salt of an acid selected from the group consisting of EDTA, H-EDTA, NTA, DTPA, lactic acid, glycolic acid, succinic acid, and mixtures of these; (c) drying the chelated solution by heating for a time and at a temperature sufficient to remove substantially all the solvent from the solution to leave a solid residue; and (d) heating the solid residue for a time and at a temperature sufficient to convert at least a substantial portion of the residue to said metal oxide.

Claim 15

The process of claim 12 wherein said first metal is selected from the group consisting of alkaline earth metals, lanthanide metals, metals from Group IVb of the periodic table, and mixtures of these.

Claim 16

The process of claim 13 wherein said chelating agent is a sodium salt of EDTA.

Claim 17

The process of claim 14 wherein said metal is zirconium.

Claim 18

The process of claim 14 wherein said salt is ammonium zirconium carbonate.

Claim 19

The process of claim 16 wherein the sodium salt of EDTA is added in an amount sufficient to produce a molar ratio of sodium salt to ammonium zirconium carbonate of at least about 0.5 to 1.

Claim 20

The process of claim 15 further comprising the step of adding to the solution of step (a), (b) and/or (c) an oxygen containing salt of a second metal.

Claim 21

The process of claim 18 wherein said second metal salt is added in an amount sufficient to produce a second metal oxide in an amount up to about 10 mole percent of the oxide of the first metal.

Claim 22

The process of claim 19 wherein said second metal is selected from the group consisting of yttrium, magnesium and calcium.

Claim 23

A process for the production of substantially unagglomerated metal oxide particles having a mean diameter of up to about 1 micron and a substantially uniform particle size distribution comprising: (a) providing a solution of a chelated complex of a salt of a first metal having an ammonium cation and a carbonate anion and a chelating agent, said chelating agent being a rubidium cesium, or sodium salt of an acid selected from the group consisting of EDTA, H-EDTA, NTA, DTPA, glycolic acid, succinic acid, lactic acid, and mixtures of these, said first metal being selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and mixtures of these; (b) heating the solution under alkaline conditions for a time and at a temperature sufficient to remove substantially all of the solvent from the solution to leave a solid residue; and (c) heating the solid residue for a time and at a temperature sufficient to form particles of said metal oxide.

Claim 24

A process for the production of substantially unagglomerated metal oxide particles having a mean diameter of up to about 1 micron and a substantially uniform particle size distribution comprising: (a) providing a solution of a chelated complex of a salt of a first metal having an ammonium cation and a carbonate anion and a chelating agent, said chelating agent being a rubidium cesium, or sodium salt of an acid selected from the group consisting of EDTA, H-EDTA, NTA, DTPA, glycolic acid, succinic acid, lactic acid, and mixtures of these, said first metal being selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and mixtures of these; (b) heating the solution under alkaline conditions for a time and at a temperature sufficient to remove substantially all of the solvent from the solution to leave a solid residue; and (c) heating the solid residue for a time and at a temperature sufficient to form particles of said metal oxide.

Claim 25

The process of claim 21 wherein said first metal is selected from the group consisting of alkaline earth metals, lanthanide metals, metals from Group IVb of the periodic table, and mixtures of these.

Claim 26

The process of claim 22 wherein said chelating agent is a sodium salt.

Claim 27

The process of claim 23 wherein said chelating agent is a disodium salt.

Claim 28

The process of claim 24 wherein said provided solution is an alkaline solution.

Claim 29

The process of claim 25 wherein said first metal is a metal from Group IVb of the periodic table.

Claim 30

The process of claim 26 wherein said first metal is zirconium.

Claim 31

The process of claim 21 wherein the step of heating the solution under alkaline conditions further comprises the step of adding a base to the solution to produce alkaline conditions.

Claim 32

The process of claim 28 wherein said heating is carried out for between about 4 hours and 2 days at a temperature of between about 50° C. and 100° C.

Claim 33

The process of claim 28 wherein the solvent of said solution is water.

Claim 34

The process of claim 21 wherein said first metal is zirconium.

Claim 35

The process of claim 31 wherein said provided solution contains an oxygen containing salt of a second metal.

Claim 36

The process of claim 32 wherein said second metal salt is present in an amount sufficient to produce a second metal oxide in an amount up to about 10 mole percent of the oxide of the first metal.

Claim 37

The process of claim 33 wherein said second metal is selected from the group consisting of yttrium, magnesium, and calcium.

Claim 38

A process for the production of substantially unagglomerated metal oxide particles having a substantially uniform particle size distribution and a mean diamerter of less than about 1 micron comprising; (a) providing a chelated solution selected from the group consisting of: (1) a solution of a chelated complex of an oxygen containing nitrate of a first metal selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and chelating agent selected from the group consisting of tartaric acid, citric acid, and mixtures of these; and (2) a solution of a chelated complex of an oxygen-containing salt of a first metal selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and a chelating agent selected from the group consisting of: EDTA; H-EDTA; NTA; DTPA; lactic acid; succinic acid; sodium, rubidium, or cesium salts of the foreging acids; and a mixture of these; (b) heating the chelated solution under alkaline conditions, said heating step carried out for a time and at a temperature sufficient to remove substantially all the solvent from the solution to leave a solid residue; and (c) heating the solid residue for a time and at a temperature sufficient to form particles of said metal oxide.

Claim 39

A process for the production of substantially unagglomerated metal oxide particles having a substantially uniform particle size distribution and a mean diamerter of less than about 1 micron comprising; (a) providing a chelated solution selected from the group consisting of: (1) a solution of a chelated complex of an oxygen containing nitrate of a first metal selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and chelating agent selected from the group consisting of tartaric acid, citric acid, and mixtures of these; and (2) a solution of a chelated complex of an oxygen-containing salt of a first metal selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and a chelating agent selected from the group consisting of: EDTA; H-EDTA; NTA; DTPA; lactic acid; succinic acid; sodium, rubidium, or cesium salts of the foreging acids; and a mixture of these; (b) heating the chelated solution under alkaline conditions, said heating step carried out for a time and at a temperature sufficient to remove substantially all the solvent from the solution to leave a solid residue; and (c) heating the solid residue for a time and at a temperature sufficient to form particles of said metal oxide.

Claim 40

The process of claim 35 wherein said chelated solution is a solution of a chelated complex of an oxygen-containing nitrate of a metal and a chelating agent selected from the group consisting of tartaric acid, citric acid, and mixtures of these.

Claim 41

The process of claim 36 wherein said metal is selected from the group consisting of alkaline earth metals, lanthanide metals, and metals in Group IVb of the periodic table.

Claim 42

The process of claim 37 wherein said metal is zirconium.

Claim 43

The process of claim 38 wherein the solution has a solvent selected from the group consisting of C 1 to C 3 alcohols.

Claim 44

The process of claim 35 wherein said chelated solution is a solution of a chelated complex of a salt of a metal having an ammonium cation and a carbonate anion and a chelating agent selected from the group consisting of EDTA; H-EDTA; NTA; DTPA; glycolic acid; lactic acid; succinic acid; and sodium, rubidium or cesium salts of the foregoing acids.

Claim 45

The process of claim 40 wherein said chelated solution is a solution of a chelated complex of a salt of a metal having an ammonium cation and a carbonate anion, and a chelating agent consisting of succinic acid.

Claim 46

The process of claim 41 wherein said metal is selected from the group consisting of alkaline earth metals, a lanthanide metals, and metals in group IVb.

Claim 47

The process of claim 42 wherein said metal is zirconium.

Claim 48

The process of claim 35 wherein said chelated solution is a solution of a chelated complex of an oxygen containing chloride of a metal and a chelating agent consisting of a sodium salt of glycolic acid.

Claim 49

The process of claim 44 wherein said first metal is selected from the group consisting of alkaline earth metals, lanthanide metals, and metals in Group IVb of the periodic table.

Claim 50

The process of claim 44 wherein said metal is zirconium.

Claim 51

The process of claim 35 further comprising the step of adding to the solution of step (a), (b) and/or (c) an oxygen containing salt of a second metal.

Claim 52

The process of claim 47 wherein said second metal is added in an amount sufficient to produce a second metal oxide in an amount up to about 10 mole percent of the oxide of the first metal.

Claim 53

The process of claim 48 wherein said second metal is selected from the group consisting of yttrium, magnesium and calcium.

Claim 54

A process of the production of substantially unagglomerated metal oxide particles having a substantial uniform particle size distribution and a mean diameter of less than about 1 micron comprising: (a) providing a solution of chelated complex of an oxygen containing salt of a metal selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and a chelating agent selected from the group consisting of: EDTA; H-EDTA; NTA; DTPA; glycolic acid; lactic acid; succinic acid; tartaric acid; citric acid; phthalic acid; alkali salts of the foregoing acids; and mixtures of these; (b) heating the chelated solution under alkaline conditions, said heating step carried out for a time and at a temperature sufficient to remove substantially all the solvent from the solution to leave a solid residue; and (c) heating the solid residue for a time and at a temperature sufficient to convert at least a substantial portion of the residue to said metal oxide.

Claim 55

A process of the production of substantially unagglomerated metal oxide particles having a substantial uniform particle size distribution and a mean diameter of less than about 1 micron comprising: (a) providing a solution of chelated complex of an oxygen containing salt of a metal selected from the group consisting of alkaline earth metals, lanthanide metals, transition metals exclusive of vanadium, tungsten, molybdenum, niobium and tantalum, and a chelating agent selected from the group consisting of: EDTA; H-EDTA; NTA; DTPA; glycolic acid; lactic acid; succinic acid; tartaric acid; citric acid; phthalic acid; alkali salts of the foregoing acids; and mixtures of these; (b) heating the chelated solution under alkaline conditions, said heating step carried out for a time and at a temperature sufficient to remove substantially all the solvent from the solution to leave a solid residue; and (c) heating the solid residue for a time and at a temperature sufficient to convert at least a substantial portion of the residue to said metal oxide.

Claim 56

The process of claim 50 wherein metal is selected from the group consisting of alkaline earth metals, lanthanide metals, and metals in group IVb of the periodic table.

Claim 57

The process of claim 51 wherein said metal is zirconium.

Claim 58

The process of claim 50 further comprising the step of adding to the solution an oxygen containing salt of a second metal.

Claim 59

The process of claim 53 wherein said second metal salt is added in an amount sufficient to produce a second metal oxide in an amount up to about 10 mole percent of the oxide of the first metal.

Claim 60

The process of claim 54 wherein said second metal is selected from the group consisting of yttrium, magnesium and calcium.