Methods and catalysts for the manufacture of carbon fibrils
AssigneeHyperion Catalysis Int'l., Inc.
InventorsDavid Moy, Asif Chishti
Life of this patent
Estimating the term…
Abstract
An improved catalyst for producing carbon fibrils is made by incorporating an effective yield-enhancing amount of a carboxylate into a fibril-forming catalyst. Alternatively, such a catalyst is made by coprecipitating a compound of a metal having fibril-forming catalytic properties and an aluminum and/or magnesium compound, optionally in the presence of carbon particles or carbon fibril aggregates. The catalyst may also be made by incorporating a compound of a fibril-forming metal onto magnesia particles in carbon particles or carbon fibril aggregates. The catalysts, methods of using them to form carbon fibrils and those carbon fibrils are also disclosed.
Claims55
A method for the manufacture of a metal-containing carbon-fibril-forming catalyst comprising incorporating an effective amount of a carboxylate into a metal-containing carbon-fibril-forming catalyst to enhance the amount of carbon fibrils produced per weight catalyst used in a gas synthesis fibril-forming process compared with the amount of fibrils which would have been produced by said gas synthesis fibril-forming process per weight of said catalyst made without said incorporation of said carboxylate, wherein said metal-containing carbon-fibril-forming catalyst comprises at least one carbon-fibril-forming catalyst metal derived from a metal-containing compound, said metal-containing compound being different from the carboxylate and also being different from a compound from which the carboxylate is derived, said carbon-fibril-forming catalyst metal being selected from the group consisting of Group VI, Group VII and the lanthanides, said carboxylate comprising an anion of a water soluble carboxylic acid.
A method for the manufacture of a metal-containing carbon-fibril-forming catalyst comprising contacting a metal-containing carbon-fibril-forming catalyst with an effective amount of a carboxylate to enhance the amount of carbon fibrils produced per weight catalyst used in a gas synthesis process compared with the amount of fibrils which would have been produced by said gas synthesis process per weight of said catalyst made without said contacting with said carboxylate, wherein said metal-containing carbon-fibril-forming catalyst comprises at least one carbon-fibril-forming catalyst metal derived from a metal-containing compound, said metal-containing compound being different from the carboxylate and also being different from a compound from which the carboxylate is derived, said carbon-fibril-forming catalyst metal being selected from the group consisting of Group VI, Group VII and the lanthanides, said carboxylate comprising an anion of a water soluble carboxylic acid.
A method for the manufacture of a metal-containing carbon-fibril-forming catalyst comprising incorporating an effective amount of a carboxylate into a metal-containing carbon-fibril-forming catalyst to enhance the amount of carbon fibrils produced per weight catalyst used in a gas synthesis fibril-forming process compared with the amount of fibrils which would have been produced by said gas synthesis fibril-forming process per weight of said catalyst made without said incorporation of said carboxylate, wherein said metal-containing carbon-fibril-forming catalyst comprises at least one carbon-fibril-forming catalyst metal derived from a metal-containing compound, said metal-containing compound being different from the carboxylate and also being different from a compound from which the carboxylate is derived, said carbon-fibril-forming catalyst metal being selected from the group consisting of Group VI, Group VII and the lanthanides, said carboxylate comprising an anion of a water soluble carboxylic acid, wherein the carbon-fibril-forming catalyst metal and a catalyst support are coprecipitated in the presence of the carboxylate to form a supported metal-containing carbon-fibril-forming catalyst.
A method for the manufacture of a metal-containing carbon-fibril-forming catalyst comprising precipitating an effective amount of a catalyst compound of a carbon-fibril-forming catalyst metal from an aqueous solution onto a slurry of support particles in the presence of an effective amount of a carboxylate to enhance the amount of carbon fibrils produced per weight catalyst used in a gas synthesis process compared with the amount of fibrils which would have been produced in said gas synthesis process per weight of said catalyst made without said precipitating in the presence of said carboxylate, wherein said metal-containing carbon-fibril-forming catalyst compound comprises at least one metal derived from a metal-containing compound, said metal-containing compound being different from the carboxylate, and also being different from a compound from which the carboxylate is derived, said carboxylate comprising an anion of a water soluble carboxylic acid.
A method for the manufacture of a metal-containing carbon-fibril-forming catalyst comprising the steps of:
- (a) forming an aqueous solution of an iron compound or iron and molybdenum compounds;
- (b) forming a slurry of catalyst support particles comprising alumina and/or magnesia particles;
- (c) mixing the solution with said slurry and precipitating the iron compound or iron and molybdenum compounds onto said alumina and/or magnesia particles in the presence of an effective amount of a carboxylate to enhance the amount of carbon fibrils produced per weight catalyst used in a gas synthesis process compared with the amount of fibrils which would have been produced by said gas synthesis process per weight of said catalyst made without said precipitating with said carboxylate, to form an impregnated support material;
- and
- (d) separating the impregnated support material from said slurry and processing the material to produce a supported metal-containing carbon-fibril-forming catalyst,
- wherein said solution, said slurry or both said solution and said slurry further comprise said carboxylate in addition to said iron compound or iron and molybdenum compounds or said alumina and/or magnesia particles.
A metal-containing carbon-fibril-forming catalyst produced by a method comprising the step of incorporating an effective amount of a carboxylate into a carbon-fibril-forming catalyst containing a metal to enhance the amount of carbon fibrils produced per weight catalyst used in a gas synthesis process compared with the amount of fibrils which would have been produced in said gas synthesis process per weight of said catalyst made without said incorporation of said carboxylate, wherein said metal is derived from a metal-containing compound which is different from said carboxylate, and which is also different from a compound from which the carboxylate is derived, said carbon-fibril-forming catalyst metal being selected from the group consisting of Group VI, Group VII and the lanthanides, said carboxylate comprising an anion of a water soluble carboxylic acid.
A method of making a carbon fibril-forming catalyst comprising the steps of:
- (a) forming an aqueous solution of a compound containing at least one metal having carbon-fibril-forming catalytic properties and an aluminum and/or magnesium compound;
- (b) coprecipitating the compound of the metal and the aluminum and/or magnesium compound in the presence of a carboxylate;
- and
- (c) processing the coprecipitate to produce a supported fibril-forming catalyst,
- wherein said metal-containing compound is different from the carboxylate and also is different from a compound from which the carboxylate is derived.
A method of making a carbon fibril-forming catalyst comprising the steps of:
- (a) forming an aqueous solution of a compound containing at least one metal having carbon-fibril-forming catalytic properties and an aluminum and/or magnesium compound;
- (b) coprecipitating the compound of the metal and the aluminum and/or magnesium compound in the presence of a carboxylate;
- and
- (c) processing the coprecipitate to produce a supported fibril-forming catalyst, wherein said metal-containing compound is different from the carboxylate and also is different from a compound from which the carboxylate is derived, wherein said compound includes iron or iron and molybdenum and said compound is precipitated to form a coprecipitate in the presence of an effective amount of a carboxylate to enhance the amount of carbon fibrils produced per weight catalyst used in a gas synthesis process compared with the amount of fibrils which would have been produced in said gas synthesis process by said catalyst made without said precipitation with said carboxylate, and wherein said coprecipitate is dried and finely ground.
A method of making a carbon fibril-forming catalyst which comprises:
- (a) forming an aqueous solution of a compound of a carbon-fibril-forming metal having carbon-fibril-forming catalytic properties and an aluminum and/or magnesium compound in the presence of a carboxylate;
- (b) coprecipitating the compound of said metal and the aluminum and/or magnesium compound to form a coprecipitate;
- and
- (c) processing the coprecipitate to produce a supported fibril-forming catalyst, wherein said metal-containing compound is different from said carboxylate and is also different from a compound from which said carboxylate is derived.
A method of making a fibril-forming catalyst comprising the steps of:
- (a) forming am aqueous mixture comprising:
- (i) an aqueous solution of a compound of a metal having a carbon-fibril-forming catalytic properties and a compound of aluminum and/or magnesium, and
- (ii) a slurry of aggregates of carbon fibrils, a preponderance of said fibrils having a length to diameter of from 3.5 to 75 nanometers and wall thickness of 0.1 to 0.4 times the said external diameter, said fibrils having graphitic layers and being substantially free of pyrolytically deposited carbon;
- (b) coprecipitating the compounding of the fibril-forming metal and the aluminum and/or magnesium compound onto the fibril aggregates in the presence of a carboxylate;
- and
- (c) processing the coprecipitated material to form a supported fibril-forming catalyst,
- wherein said metal-containing compound is different from said carboxylate and is also different from a compound from which said carboxylate is derived.
A method of making a carbon-fibril-forming catalyst which comprises:
- (a) forming an aqueous mixture comprising:
- (i) an aqueous solution of an iron compound or iron and molybdenum compounds and an aluminum and/or compound, and
- (ii) a slurry of aggregates of carbon fibrils, a preponderance of said fibrils having a length to diameter ratio of at least five, an external diameter of from 3.5 to 75 nonometers and a wall thickness of 01 to 0.4 times the said external diameter, said fibrils having graphitic layers and being substantially free of pyrolytically deposited carbon,
- (b) coprecipitating the aluminum and/or magnesium compound and the iron compound or iron and molybdenum compounds onto the fibril aggregates in the presence of a carboxylate, and
- (c) processing the coprecipitated material to form a supported fibril-forming catalyst, wherein said iron compound or iron and molybdenum compound are different from said carboxylate and are also different from a compound from which said carboxylate is derived.
A method of making a fibril-forming catalyst comprising the steps of:
- (a) forming an aqueous solution of a compound of a metal having carbon-fibril-forming catalytic properties;
- (b) forming a slurry of alumina and/or magnesia particles and aggregates of carbon fibrils, a preponderance of said fibrils having a length to diameter ratio of at least five, an external diameter of from 3.5 to 75 nanometers and a wall thickness of 0.1 to 0.4 times said external diameter, said fibrils having graphitic layers and being substantially free of pyrolytically deposited carbon;
- (c) adding the aqueous solution and the slurry together in the presence of a carboxylate, thereby causing a precipitate to form and thereby incorporating a compound of the metal onto said alumina and/or magnesia particles in said fibril aggregates;
- and
- (d) processing the precipitated material to form a supported fibril-forming catalyst,
- wherein said metal containing compound is different from said carboxylate and is also different from a compound from which said carboxylate is derived.
A method of making a carbon fibril-forming catalyst which comprises:
- (a) forming an aqueous solution of an iron compound or iron and molybdenum compounds;
- (b) forming a slurry of alumina and/or magnesia particles and aggregates of carbon fibrils, a preponderance of said fibrils having a length to diameter ratio of at least five, an external diameter of from 3.5 to 75 nanometers and a wall thickness of 0.1 to 0.4 times the said external diameter, said fibrils having graphitic layers and being substantially free of pyrolytically deposited carbon;
- (c) adding the aqueous solution and the slurry together in the presence of a carboxylate, thereby causing a precipitate to form and thereby incorporating the iron compound or iron and molybdenum compounds onto said alumina and/or magnesia particles in said fibril aggregates;
- and
- (d) processing the precipitated material to form a supported fibril-forming catalyst, wherein said iron compound or iron and molybdenum compound are different from said carboxylate and are also different from a compound from which said carboxylate is derived.
A method of making a fibril-forming catalyst comprising the steps of:
- (a) forming an aqueous mixture comprising:
- (i) an aqueous solution of a compound of a metal having carbon-fibril-forming catalytic properties and a compound of aluminum and/or magnesium and
- (ii) a slurry of structured carbon particles having an open pore structure with internal surface area;
- (b) coprecipitating the compound of the carbon-fibril-forming metal together with the aluminum and/or magnesium compound onto the carbon particles in the presence of a carboxylate;
- and
- (c) processing the coprecipitated material to form a supported fibril-forming catalyst,
- wherein said metal-containing compound is different from said carboxylate and is also different from a compound from which said carboxylate is derived.
A method of making a carbon fibril-forming catalyst which comprises:
- (a) forming an aqueous mixture comprising:
- (i) an aqueous solution of an iron compound or iron and molybdenum compounds and an aluminum and/or magnesium compound and
- (ii) a slurry of structured carbon particles having an open pore structure with internal surface area;
- (b) coprecipitating the aluminum and/or magnesium compound and the iron compound or iron and molybdenum compounds onto the carbon particles in the presence of a carboxylate;
- and
- (c) processing the coprecipitated material to form a supported fibril-forming catalyst, wherein said iron compound or iron and molybdenum compound are different from said carboxylate and are also different from a compound from which said carboxylate is derived.
A method of making a fibril-forming catalyst comprising the steps of:
- (a) forming an aqueous solution of a compound of a metal having carbon-fibril-forming catalytic properties;
- (b) forming a slurry of alumina and/or magnesia particles and structured carbon particles having an open pore structure with internal surface area;
- (c) adding the aqueous solution and the slurry together, thereby causing a precipitate to form and thereby incorporating the compound of the fibril-forming metal onto said alumina and/or magnesia particles in the carbon particles in the presence of a carboxylate;
- and
- (d) processing the precipitated material to form a supported fibril-forming catalyst,
- wherein said metal-containing compound is different from said carboxylate and is also different from a compound from which said carboxylate is derived.
A method of making a carbon fibril-forming catalyst which comprises:
- (a) forming an aqueous solution of an iron compound or iron and molybdenum compounds;
- (b) forming a slurry of alumina and/or magnesia particles and structured carbon particles having an open pore structure with internal surface area;
- (c) adding the aqueous solution and the slurry together, thereby causing a precipitate to form and thereby incorporating the iron compound or iron and molybdenum compounds onto said alumina and/or magnesia particles in the carbon particles in the presence of a carboxylate;
- and
- (d) processing the precipitated material to form a supported fibril-forming catalyst, wherein said iron compound or iron and molybdenum compound are different from said carboxylate and are also different from a compound from which said carboxylate is derived.
A catalyst for the production of carbon fibrils comprising:
- (a) a catalyst support comprising an aggregate of carbon fibrils, a preponderance of said fibrils having a length to diameter ratio of at least five, an external diameter of from 3.5 to 75 nanometers and a wall thickness of 0.1 to 0.4 times said external diameter, said fibrils having graphitic layers and being substantially free of pyrolytically deposited carbon;
- (b) a catalytically effective amount of one or more metals having carbon-fibril-forming catalytic properties supported on said aggregate;
- and
- (c) a carboxylate, wherein said metal-containing compound is different from said carboxylate and is also different from a compound from which said carboxylate is derived.
Dependencies are inferred from the claim text.