Tda Research, Inc.

Frontier Carbon Corporation

J Michael Alford

Michael D Diener

Robert D Bolskar

James Nabity

Michael Karpuk

Bradley Dean Hitch

The invention provides improved burners, combustion apparatus, and methods for carbon nanomaterial production. The burners of the invention provide sooting flames of fuel and oxidizing gases. The condensable products of combustion produced by the burners of this invention produce carbon nanomaterials including without limitation, soot, fullerenic soot, and fullerenes. The burners of the invention do not require premixing of the fuel and oxidizing gases and are suitable for use with low vapor pressure fuels such as those containing substantial amounts of polyaromatic hydrocarbons. The burners of the invention can operate with a hot (e.g., uncooled) burner surface and require little, if any, cooling or other forms of heat sinking. The burners of the invention comprise one or more refractory elements forming the outlet of the burner at which a flame can be established. The burners of the invention provide for improved flame stability, can be employed with a wider range of fuel/oxidizer (e.g., air) ratios and a wider range of gas velocities, and are generally more efficient than burners using water-cooled metal burner plates. The burners of the invention can also be operated to reduce the formation of undesirable soot deposits on the burner and on surfaces downstream of the burner.

Burners and combustion apparatus for carbon nanomaterial production

The invention provides improved therapeutic and diagnostic fullerenes and endohedral fullerenes. The fullerenes and endohedral fullerenes of the invention are derivatized with at least two charged functional groups (and preferably more than two charged functional groups) to provide for water-solubility and improved in vivo biodistribution. Improved derivatized fullerenes and endohedral fullerenes carry a plurality of functional groups at least two of which are charged. Preferably at least about &#x2159; of the possible derivations sites on the fullerene caged carry derivatives and preferably at least about &#xbd; of the functional groups on the fullerene cage are charged groups. The invention also provides water-soluble endohedral metallofullerene with improved biodistribution which are useful as in vivo imaging agents, including MRI contrast agents.

Derivatization and solubilization of fullerenes for use in therapeutic and diagnostic applications

This invention provides improved methods for the derivatization and solubilization of fullerenes, which are particularly useful for those fullerenes that are normally insoluble and which are specifically applied, among others, to endohedral fullerenes, including endohedral metallofullerenes; empty fullerenes, including small-bandgap fullerenes and other insoluble fullerenes and to very high molecular weight fullerenic materials generated in fullerenic soot, including giant fullerenes, fullerenic polymers, carbon nanotubes and metal-carbon nanoencapsulates. More specifically the invention relates to improved methods for cyclopropanation of fullerenes. Specific reaction conditions are provided which allow for cyclopropanation reactions to be successfully performed for the first time on insoluble classes of fullerenes. Also provided is a method for purification of one or more fullerenes from a fullerenic material containing the one or more fullerenes in addition to non-fullerenic carbonaceous material, particularly amorphous carbonaceous material, by derivatizing one or more fullerenes using the methods of the invention and separating soluble derivatizes fullerenes from insoluble materials.

Derivatization and solubilization of insoluble classes of fullerenes

The invention provides a method of separating a first and a second set of fullerenes in a fullerene mixture. In the method of the invention, a stable fullerene cation is formed of one of the first or the second set of fullerenes. The fullerene cation is then separated from the other set of fullerenes. Optionally, the fullerene cation may be returned to its neutral state. The method of the invention is particularly useful for the purification and separation of endohedral fullerenes from empty fullerenes. However, the method may be applied to the purification of a broad range of endohedral and empty fullerene materials.

Purification of endohedral and other fullerenes by chemical methods

The present invention provides a combustion apparatus for the production of carbon nanomaterials including fullerenes and fullerenic soot. Most generally the combustion apparatus comprises one or more inlets for introducing an oxygen-containing gas and a hydrocarbon fuel gas in the combustion system such that a flame can be established from the mixed gases, a droplet delivery apparatus for introducing droplets of a liquid hydrocarbon feedstock into the flame, and a collector apparatus for collecting condensable products containing carbon nanomaterials that are generated in the combustion system. The combustion system optionally has a reaction zone downstream of the flame. If this reaction zone is present the hydrocarbon feedstock can be introduced into the flame, the reaction zone or both.

Combustion process for synthesis of carbon nanomaterials from liquid hydrocarbon

This invention provides improved methods for combustion synthesis of carbon nanomaterials, including fullerenes, employing multiple-ring aromatic hydrocarbon fuels selected for high carbon conversion to extractable fullerenes. The multiple-ring aromatic hydrocarbon fuels include those that contain polynuclear aromatic hydrocarbons. More specifically, multiple-ring aromatic hydrocarbon fuels contain a substantial amount of indene, methylnapthalenes or mixtures thereof. Coal tar and petroleum distillate fractions provide low cost hydrocarbon fuels containing polynuclear aromatic hydrocarbons, including without limitation, indene, methylnapthalenes or mixtures thereof.

Polynuclear aromatic hydrocarbons for fullerene synthesis in flames

The invention generally relates to purification of carbon nanomaterials, particularly fullerenes, by removal of PAHs and other hydrocarbon impurities. The inventive process involves extracting a sample containing carbon nanomaterials with a solvent in which the PAHs are substantially soluble but in which the carbon nanomaterials are not substantially soluble. The sample can be repeatedly or continuously extracted with one or more solvents to remove a greater amount of impurities. Preferred solvents include ethanol, diethyl ether, and acetone. The invention also provides a process for efficiently separating solvent extractable fullerenes from samples containing fullerenes and PAHs wherein the sample is extracted with a solvent in which both fullerenes and PAHs are substantially soluble and the sample extract then undergoes selective extraction to remove PAHs. Suitable solvents in which both fullerenes and PAHs are soluble include o-xylene, toluene, and o-dichlorobenzene. The purification process is capable of treating quantities of combustion soot in excess of one kilogram and can produce fullerenes or fullerenic soot of suitable purity for many applications.

Process for the removal of impurities from combustion fullerenes

Filter devices and methods for collection of carbon nanomaterials, including fullerenes, produced in gas phase reactors are provided. The filter devices provide for in situ cleaning of filters to release captured product for collection. Product can be released and removed from the reactor without disrupting continuous synthesis of carbon nanomaterials. The filter devices facilitate increased reactor operation and larger scale production of carbon nanomaterials. The filters are cleaned by application of a motive force and/or a gas flow to the filter. In a specific embodiment filters are cleaned by a reverse flow of gas pulses to the filter provided. The invention also provides reactor systems for gas phase synthesis of carbon nanomaterials that can be operated continuously employing the filter device of this invention. Preferred reactor systems are those which synthesize carbon nanomaterials by combustion. Methods for continuous production of carbon nanomaterials using the filtering devices and methods of this invention are also provided.

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Lakewood, CO, United States of America

J Michael Alford