Filamentous organism-derived carbon-based materials, and methods of making and using same

Inventors

Ren, ZhiyongHUGGINS, MITCHELL TYLERBiffinger, Justin C.Love, Corey T.Lee, Se-HeeWHITELEY, JUSTIN M.

Assignees

US Department of NavyUniversity of Colorado Denver

Publication Number

US-10829420-B2

Publication Date

2020-11-10

Expiration Date

2037-07-21

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Abstract

The invention provides filamentous organism-derived carbonaceous materials doped with organic and/or inorganic compounds, and methods of making the same. In certain embodiments, these carbonaceous materials are used as electrodes in solid state batteries and/or lithium-ion batteries. In another aspect, these carbonaceous materials are used as a catalyst, catalyst support, adsorbent, filter and/or other carbon-based material or adsorbent. In yet another aspect, the invention provides battery devices incorporating the carbonaceous electrode materials.

Core Innovation

The invention provides carbonaceous materials derived from filamentous organisms comprising a graphitic, partially graphitic, or amorphous carbon matrix that includes a plurality of fibers. These fibers have diameters ranging from about 0.1 μm to about 100 μm and are in physical contact with at least one other fiber. The carbon matrix features a surface area from about 1 m2/g to about 3,000 m2/g and contains pores throughout with diameters ranging approximately from 0.1 μm to 1 cm. The carbonaceous materials can be doped with organic and/or inorganic compounds incorporated during the growth of the filamentous organisms or present on the surface of the carbon matrix.

The invention addresses the problem of developing novel carbon-based materials and manufacturing methods that are sustainable, flexible, and adaptable, particularly for electrode materials in batteries. Current sophisticated carbon architectures like carbon nanotubes, while improving battery performances, suffer from high costs and environmental impacts. There is a need for efficient manufacturing using sustainable feedstock with the ability to incorporate doping atoms to tailor properties. The invention meets this need by utilizing filamentous organisms grown in media optionally containing inorganic and/or organic compounds to produce carbonaceous materials with controlled structure and doping.

Also disclosed are methods of producing these carbonaceous materials by carbonizing filamentous organisms, such as filamentous fungi including wild type or genetically modified Neurospora crassa, under controlled heating conditions and atmospheres. These methods enable the retention of the organisms’ fibrous and porous structure after carbonization, producing graphitic materials suitable as electrodes, catalysts, adsorbents, or filters. The invention further includes battery devices incorporating the carbonaceous electrode materials, demonstrating suitability for solid state and lithium-ion batteries.

Claims Coverage

The claims include one independent claim defining the carbonaceous material and one independent claim defining a battery device comprising the carbonaceous material and a lithium-containing electrolyte. Key inventive features extracted from these claims are as follows.

Carbonaceous material structure and properties

A carbonaceous material comprising a graphitic, partially graphitic, or amorphous carbon matrix composed of a plurality of fibers, where each fiber has a diameter from about 0.1 μm to about 100 μm and is in physical contact with at least one other fiber. The carbon matrix has a surface area ranging from about 1 m2/g to about 3,000 m2/g and includes a plurality of pores throughout the matrix. Each pore independently has a diameter from about 0.1 μm to about 1 cm and is in fluid connection with at least one other pore.

Preparation from carbonized filamentous organisms

The material is prepared by carbonizing a filamentous organism optionally grown with at least one organic or inorganic compound, wherein at least a portion of these compounds is within or on the surface of the carbon matrix.

Filamentous organism selection

The filamentous organism used to prepare the carbonaceous material is selected from filamentous algae, filamentous fungi, and filamentous bacteria. In particular embodiments, the organism is wild type or genetically modified Neurospora crassa.

Carbonization conditions

Carbonization includes heating the filamentous organism to a maximum temperature between about 100° C. and about 2,500° C. at a rate of about 1° C./min to about 100° C./min, for about 1 to 100 hours, optionally in a gas flow between about 1 mL/min and about 1000 mL/min or under vacuum.

Fiber connectivity and branching

At least one fiber in the plurality is either not physically bound to others or physically bound to at least one other fiber. Fibers can be physically bound through branching points separated by about 0.1 μm to about 1000 μm along the fiber length.

Incorporation of organic and inorganic compounds

The carbon matrix contains organic and/or inorganic compounds within or on the fiber surfaces throughout the matrix. Such inorganic compounds include transition metal salts, alkali metal salts, alkaline earth metal salts, nitrate, sulfate, phosphate salts, metal or metalloid particles, and metal oxides, specifically including cobalt nitrate, sodium nitrate, magnesium sulfate, and silicon nanoparticles.

Pore size range

The pores in the carbon matrix independently have diameters ranging from about 1 μm to about 10 mm.

Material suitability for electrodes and incorporation of specific nanoparticles

The material can further comprise silicon nanoparticles, silicon oxide nanoparticles, and Co2O3 nanoparticles and is suitable for use as an electrode in solid state or lithium-ion batteries.

Battery device composition

The battery device comprises the carbonaceous material and a lithium-containing electrolyte.

The claims collectively define carbonaceous materials derived from carbonized filamentous organisms with controlled fiber and pore structures and doping with organic and inorganic compounds, particularly suitable for use as battery electrodes, and battery devices incorporating these materials.

Stated Advantages

The carbonaceous materials can be efficiently manufactured from sustainable, environmentally friendly feedstock such as filamentous organisms.

The methods allow flexible and adaptable doping of the carbon matrix with various non-carbon atoms to manipulate material properties.

The resultant carbonaceous materials maintain three-dimensional pore integrity and fibrous structure conducive to use as electrodes and catalysts.

The doped carbonaceous electrode materials demonstrate improved electrochemical performance greater than that of standard graphite, suitable for high capacity batteries.

The material can be used as binderless, free-standing electrodes reducing hazardous preparation methods and improving electrode performance.

Documented Applications

Use as electrodes in solid state batteries comprising a lithium-containing solid electrolyte.

Use as electrodes in lithium-ion batteries comprising a lithium-ion liquid electrolyte such as LiPF6 in organic solvents.

Use as catalysts or catalyst support materials doped with transition metals for catalytic oxidation or reduction reactions.

Use as adsorbents and filters leveraging the porous carbonaceous matrix.

Conversion of biomass grown in wastewater into carbonaceous materials enabling pollutant removal and resource recovery.

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