Compositions and aggregates containing boron nitride nanotube structures, and methods for producing them.

Abstract

To provide a novel composition and aggregate that contain an independent boron nitride nanotube and have novel features.SOLUTION: A composition (or aggregate) comprises an epitaxial h-BN / BNNT structure comprising a hexagonal boron nitride structure that is epitaxial to a boron nitride nanotube structure. The composition (or aggregate) comprises an independent boron nitride nanotube wherein a total mass percentage of the independent hexagonal boron nitride and the residual boron in the composition is 35% or less. In the composition (or aggregate), 1% or less of the independent boron nitride nanotube and the boron nitride nanotube structure has dixie cup defects or bamboo defects. In the composition, at least 50% of the independent boron nitride nanotube and the boron nitride nanotube structure is a single layer. A method for producing a composition comprising an epitaxial h-BN / BNNT structure is also provided.SELECTED DRAWING: Figure 1

Description

Technical Field

[0001] Cross - Reference to Related Applications This application claims priority to U.S. Patent Application Publication No. 15 / 928,969, filed on March 22, 2018, the entire contents of which are incorporated herein by reference.

[0002] Field of the Subject Matter of the Invention The subject matter of the present invention relates to novel and unforeseen materials each comprising an atomic arrangement that includes a first region of an atomic arrangement corresponding (at least to a specified degree) to an idealized boron nitride nanotube, the atomic arrangement also including at least a second region (different from the first region), and such novel and unforeseen materials having unique combinations of properties.

[0003] In one aspect of the subject matter of the present invention, therefore, the subject matter of the present invention provides novel and unforeseen materials having unique combinations of properties. The subject matter of the present invention also provides novel compositions and aggregates comprising such novel and unforeseen materials.

[0004] The subject matter of the present invention also provides novel compositions and aggregates comprising boron nitride nanotubes and having novel features. The subject matter of the present invention also provides novel methods for manufacturing novel and unforeseen materials, compositions, and aggregates.

Background Art

[0005] Boron nitride nanotubes are nanoscale hollow tubes, with typical diameters in the range of 2 - 20 nanometers and typical lengths in the range from several tens of nanometers to several tens of micrometers. The expression "boron nitride nanotube" (or "boron nitride nanotubes") encompasses structures consisting of a single layer that is generally tube - shaped (i.e., single - wall boron nitride nanotubes), and further structures consisting of multiple layers that are each generally tube - shaped and concentric (i.e., multi - wall boron nitride nanotubes).

[0006] A hypothetical idealized boron nitride nanotube consists of one or more layers (i.e., walls), each layer consisting of a roughly tubular arrangement of boron and nitrogen atoms, where the boron and nitrogen atoms are arranged in a repeating hexagonal pattern of alternating boron and nitrogen atoms. As is well known to those skilled in the art, the idealized boron nitride nanotube can be conceptually described as a structure obtained by taking one (or more) layers of boron and nitrogen atoms, where boron and nitrogen are arranged in an alternating hexagonal repeating pattern, and curving the layers (or more) so that two sides of the layer (or each layer) touch and connect along the seam so that the alternating boron / nitrogen hexagonal repeating patterns meet, thereby providing a hollow cylindrical array of one wall (or a number of walls corresponding to the number of layers) of boron and nitrogen atoms in a continuous alternating hexagonal pattern (i.e., the seam is indistinguishable).

[0007] Boron nitride nanotubes are often compared to carbon nanotubes in terms of their corresponding chemical structure and properties. While there are similarities (e.g., excellent mechanical strength), many differences are also known, including the fact that boron nitride nanotubes are electrically insulating (whereas carbon nanotubes are electrically conductive), and that boron nitride nanotubes are stable at much higher temperatures.

[0008] Many of the outstandingly desirable properties of boron nitride nanotubes include, in particular, a strength-to-mass ratio (high strength / low density), toughness, rigidity, thermal conductivity, flame retardancy, corrosion resistance, neutron absorption / protection, friction and wear resistance, oxidation resistance, hydrophobicity, hydrogen storage capacity, and nanoparticle carrier effectiveness.

[0009] Several forms of defective boron nitride nanotubes are well known to those skilled in the art, such as dixie cup defects and bamboo defects. . [Overview of the project]

[0010] As described above, the subject matter of the present invention provides, in one embodiment, a novel and unforeseen material (defined herein as an epitaxial h-BN / BNNT structure) in which each atomic arrangement includes a first region of atomic arrangement corresponding to an idealized boron nitride nanotube (to at least a specified extent), wherein the atomic arrangement also includes at least a second region (different from the first region), and such a novel and unforeseen material has a unique combination of properties.

[0011] According to a first aspect of the subject matter of the present invention, a composition is provided comprising at least a first epitaxial h-BN / BNNT structure (as defined herein), wherein the first epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure (as defined herein) and at least a first hexagonal boron nitride structure (as defined herein), wherein the first hexagonal boron nitride structure is epitaxial with respect to the first boron nitride nanotube structure (as defined herein).

[0012] According to a second aspect of the subject matter of the present invention, an aggregate is provided comprising an integral structure comprising at least a first epitaxial h-BN / BNNT structure (as defined herein), wherein the first epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure (as defined herein) and at least a first hexagonal boron nitride structure (as defined herein), wherein the first hexagonal boron nitride structure is epitaxial with respect to the boron nitride nanotube structure (as defined herein), and the integral structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension.

[0013] The subject matter of the present invention also provides other novel compositions and aggregates comprising epitaxial h-BN / BNNT structures as defined herein. The novel and unforeseen epitaxial h-BN / BNNT structures (as defined herein) provided by the subject matter of the present invention exhibit improved properties, such as excellent adhesion to a matrix material (enhanced physical / mechanical resistance to removal from the matrix material), provide excellent nanonucleation sites for metal crystallization (e.g., when casting one or more metals such as aluminum, magnesium, or titanium having a melting point lower than the temperature at which the boron nitride nanotube structure decomposes), and can provide desirable properties even after exposure to extremely high temperatures.

[0014] The subject matter of the present invention also provides novel compositions and aggregates comprising independent boron nitride nanotubes (as defined herein) and having novel characteristics. The subject matter of the present invention also relates to high-purity compositions and aggregates comprising boron nitride nanotube structures and / or independent boron nitride nanotubes, for example, comprising boron nitride nanotube structures and / or independent boron nitride nanotubes, with residual boron and independent Compositions and aggregates in which the total amount of hexagonal boron nitride (as defined herein) is limited to less than (or less than) a certain mass percent.

[0015] According to a third aspect of the subject matter of the present invention, a composition comprising a plurality of independent boron nitride nanotubes (as defined herein) is provided, wherein the sum of [1] the total mass of all independent hexagonal boron nitride (also as defined herein) in the composition and [2] the total mass of all residual boron (also as defined herein) in the composition accounts for 35% or less of the mass of the composition.

[0016] According to a fourth aspect of the subject matter of the present invention, an aggregate is provided comprising a monolithic structure comprising a plurality of independent boron nitride nanotubes (as defined herein), wherein the monolithic structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension, and the sum of [1] the total mass of independent hexagonal boron nitride (as defined herein) in the monolithic structure and [2] the total mass of all residual boron (as defined herein) in the monolithic structure accounts for no more than 35% of the mass of the monolithic structure.

[0017] The subject matter of the present invention also relates to high-quality compositions and aggregates comprising boron nitride nanotube structures and / or independent boron nitride nanotubes, for example, compositions and aggregates comprising boron nitride nanotube structures and / or independent boron nitride nanotubes, wherein the total amount of boron nitride nanotube structures and / or independent boron nitride nanotubes having Dixie cup defects (as defined below), and boron nitride nanotube structures and / or independent boron nitride nanotubes having bamboo defects (as defined below), is limited to less than (or less than) a certain percentage.

[0018] According to a fifth aspect of the subject matter of the present invention, a composition is provided comprising at least 10 independent boron nitride nanotubes (as defined herein) having a length of at least 50 nm: [1] of the total of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] of the total of boron nitride nanotube structures (as defined herein) having a length of at least 50 nm in the composition, less than 1% of the total has at least one defect selected from Dixie cup defects (as defined herein) and bamboo defects (as defined herein).

[0019] According to a sixth aspect of the subject matter of the present invention, an aggregate is provided comprising a monolithic structure comprising a plurality of independent boron nitride nanotubes (as defined herein), wherein the monolithic structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension: [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] boron nitride nanotube structures (as defined herein) having a length of at least 50 nm in the integral structure, less than 1% of the total has at least one defect selected from Dixie cup defects (as defined herein) and bamboo defects (as defined herein).

[0020] The subject matter of the present invention also relates to compositions and aggregates comprising boron nitride nanotube structures and / or independent boron nitride nanotubes, wherein the amount of single-walled boron nitride nanotube structures and / or independent boron nitride nanotubes relative to the amount of multi-walled boron nitride nanotube structures and / or independent boron nitride nanotubes is greater than (or greater than) a certain percentage.

[0021] According to a seventh aspect of the subject matter of the present invention, a composition comprising at least 10 independent boron nitride nanotubes (as defined herein) is provided: Among the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition (also as defined herein), at least 50% of each of the total is a monolayer (also as defined herein).

[0022] According to an eighth aspect of the subject matter of the present invention, there is provided an aggregate comprising an integral structure comprising at least one independent boron nitride nanotube (as defined herein), the integral structure having a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension: Among the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in the integral structure (also as defined herein), at least 50% of each of the total is a monolayer (also as defined herein).

[0023] The subject matter of the present invention also provides novel and unforeseen materials, compositions, and novel methods for manufacturing aggregates. According to a ninth aspect of the subject matter of the present invention, there is provided a method for manufacturing a composition, the method comprising: supplying a mixture of nitrogen gas and hydrogen gas to a first region of a chamber; converting at least a portion of the mixture of nitrogen gas and hydrogen gas into a plasma; supplying a mixture of at least one boron-containing material and nitrogen gas to a second region of the chamber, thereby contacting the mixture of at least one boron-containing material and nitrogen gas with the plasma to form a reaction mixture; converting at least a portion of the mixture into an epitaxial h-BN / BNNT structure, including.

[0024] The subject matter of the present invention can be more fully understood by reference to the accompanying drawings and the following detailed description of the subject matter of the present invention.

Brief Description of the Drawings

[0025] [Figure 1] Figure 1 schematically shows a representative embodiment of an apparatus 10 that can be used for the production of an epitaxial h-BN / BNNT structure, and further a composition and / or aggregate comprising the epitaxial h-BN / BNNT structure, according to the first and second aspects of the subject matter of the present invention. [Figure 2] Figure 2 is an enlarged view of a part of Figure 1. [Figure 3] Figure 3 is a view of an epitaxial h-BN / BNNT structure. [Figure 4] Figure 4 is a TEM image of a representative part of the product of Example 1, and each of about 30% of the boron nitride nanotube structures was covered by at least 30% with epitaxial hexagonal boron nitride. [Figure 5] Figure 5 is a TEM image of a representative part of the product of Example 2, and each of about 90% of the boron nitride nanotube structures was covered by at least 30% with epitaxial hexagonal boron nitride. [Figure 6] Figure 6 is a TEM image of a part of the product of Example 2, and this image shows (inter alia) an epitaxial h-BN / BNNT structure. [Figure 7] Figure 7 is a TEM image of a part of the product of Example 2, and this image shows (inter alia) independent hexagonal boron nitride and an epitaxial h-BN / BNNT structure, one of which contains a mass of boron nitride nanotube structures. [Figure 8] Figure 8 is a TEM image of a part of the product of Example 2, and this image shows (inter alia) a mass of boron nitride nanotube structures and an epitaxial h-BN / BNNT structure. [Figure 9] Figure 9 is a TEM image of a part of the product of Example 2, and this image shows (inter alia) an epitaxial h-BN / BNNT structure. [Figure 10]Figure 10 is a TEM image of a portion of the product from Example 2, which shows (among other things) the residual boron and epitaxial h-BN / BNNT structures. [Figure 11] Figure 11 is a TEM image of a portion of the product from Example 2, which shows (among other things) the residual boron and epitaxial h-BN / BNNT structures. [Figure 12] Figure 12 is a TEM image of a portion of the product from Example 2, which shows (among other things) the epitaxial h-BN / BNNT structure. [Figure 13] Figure 13 shows a TEM image of an independent boron nitride nanotube. [Modes for carrying out the invention]

[0026] Unless otherwise specified, all terms used herein (including technical and scientific terms) have the same meaning as those generally understood by those skilled in the art in the field to which the subject matter of the present invention pertains. Terms such as those defined in commonly used dictionaries should be interpreted as having the meaning consistent with their meaning in the applicable art and the context of this disclosure, and not as ideal or overly formal unless explicitly defined herein.

[0027] Terms such as “first,” “second,” etc., are used herein to refer to various structures, epitaxial h-BN / BNNT structures, boron nitride nanotube structures, hexagonal boron nitride structures, components, percentages, percentage ranges, dimensions, areas, and connection sections, but such structures, epitaxial h-BN / BNNT structures, boron nitride nanotube structures, hexagonal boron nitride structures, components, percentages, percentage ranges, dimensions, areas, and connection sections are not limited by these numerical terms. These numerical terms are used simply to individually identify each structure, epitaxial h-BN / BNNT structure, boron nitride nanotube structure, hexagonal boron nitride structure, component, percentage, percentage range, dimension, area, or connecting section, and / or to distinguish between the structures, epitaxial h-BN / BNNT structure, boron nitride nanotube structure, hexagonal boron nitride structure, component, percentage, percentage range, dimension, area, or connecting section.

[0028] The expression “each” is used in many places herein in relation to features (or features) in multiple items (or “at least one” items, etc.), to indicate that the feature (or features) is present in each of the specified items (or individual items), in contrast to features that are provided in some way by multiple items but not necessarily by individual items, or in contrast to features that are an average of features relating to multiple items. Such use of the expression “each” takes various forms, for example: "Each material contains an arrangement of atoms..." "Multiple layers, each roughly tubular and concentric," "One or more layers (i.e., walls), each layer consisting of a roughly tubular arrangement of boron and nitrogen atoms," "At least 50% of each of the above totals is single-layered," "Each of at least one hexagonal boron nitride structure is epitaxial with respect to the boron nitride nanotube structure." "Each epitaxial h-BN / BNNT structure comprises a boron nitride nanotube structure and at least one hexagonal boron nitride structure." "Hexagonal boron nitride structures, each epitaxial with respect to a boron nitride nanotube structure," "A structure containing (or multiple structures each containing)", "For each of at least 10% of the atoms on the outermost wall of the boron nitride nanotube structure, [1] there exists an atom in the hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotube structure, and [2] there exists an atom within 10 nanometers of such an atom." Each of the boron nitride nanotube structures is in an amount that is at least 10% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition: The boron nitride nanotube structure has a length of at least 50 nm, and at least 10% of the total outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure," and "Each of the above totals, at least a portion thereof", That is the case.

[0029] As described above, according to a first aspect of the subject matter of the present invention, a composition is provided comprising at least a first epitaxial h-BN / BNNT structure, wherein the first epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure and at least a first hexagonal boron nitride structure, the first hexagonal boron nitride structure being epitaxial with respect to the first boron nitride nanotube structure.

[0030] When used herein, the expression “epitaxial h-BN / BNNT structure” means a novel and unforeseen structure provided by the subject matter of the present invention, namely a structure comprising a boron nitride nanotube structure (as defined below) and at least one hexagonal boron nitride structure (as defined below), wherein each of the at least one hexagonal boron nitride structure is epitaxial with respect to the boron nitride nanotube structure. Thus, each epitaxial h-BN / BNNT structure comprises a boron nitride nanotube structure and at least one hexagonal boron nitride structure.

[0031] As is well known to those skilled in the art, the term "epitaxial" is widely used in relation to crystal nucleation and crystal growth. A crystal is defined as atoms, molecules, or ions arranged in a regular, repeating pattern, a crystal lattice, that spans all three spatial dimensions. Crystal growth is the process by which an existing crystal grows larger as more atoms, molecules, or ions are added to their designated positions in the crystal lattice. During crystal growth, atoms, molecules, or ions need to settle into the correct lattice positions for a highly regular crystal to grow. If atoms, molecules, or ions settle into positions different from their ideal positions in the crystal lattice, defects are formed. Typically, crystal growth is often irreversible in the sense that atoms, molecules, or ions in the crystal lattice are held in place; that is, they cannot easily move from their positions, and therefore, once molecules or ions settle into their designated positions in the growing lattice, they become fixed.

[0032] Crystallization is typically understood as consisting of two processes: crystal nucleation and crystal growth. Crystal nucleation is when a new crystal is formed (i.e., when no existing crystal exists), and crystal growth is when atoms, molecules, or ions are added to an existing crystal, i.e., a nucleated (and, if desired, grown) crystal; i.e., addition to a nucleated crystal is called crystal growth, and addition to a nucleated crystal that has already grown to some extent is also called crystal growth).

[0033] Epitaxis refers to the nucleation of a crystal of a particular orientation on another crystal, the orientation being determined by the underlying crystal. The description herein that a first structure (i.e., a hexagonal boron nitride structure) is epitaxial with respect to a second structure (i.e., a boron nitride nanotube structure) means that [1] the atoms in the second structure and [2] the atoms in the first structure closest to the second structure are aligned with respect to each other in such a way that the atoms in the idealized structure corresponding to the second structure are aligned with respect to each other, i.e., they are aligned in such a way that they are a result of (or will be a result of) the nucleation of the second structure on the first structure and the growth of the second structure on the nucleated second structure.

[0034] Therefore, when used herein, the expression "hexagonal boron nitride structure that is epitaxial with respect to boron nitride nanotube structures" (and similar expressions, such as "hexagonal boron nitride structures, each of which is epitaxial with respect to boron nitride nanotube structures," "each of at least one hexagonal boron nitride structure is epitaxial with respect to boron nitride nanotube structures," "hexagonal boron nitride that is epitaxial with respect to boron nitride nanotube structures," etc.) means that each such hexagonal boron nitride structure... In this context, [1] the atoms in the hexagonal boron nitride structure and [2] the atoms in the boron nitride nanotube structure closest to the hexagonal boron nitride structure are arranged relative to each other in such a way that the atoms in the idealized hexagonal boron nitride structure (considered below) are arranged relative to each other. In other words, they are arranged in such a way that they are the result of (or will be the result of) the nucleation of the hexagonal boron nitride structure on the boron nitride nanotube structure and the growth of the hexagonal boron nitride structure on the nucleated hexagonal boron nitride structure.

[0035] Hexagonal boron nitride is characterized by a stacked two-dimensional honeycomb lattice of boron and nitrogen atoms strongly bonded by highly polar BN bonds. The layers of hexagonal boron nitride are stacked in an AA' stacking mode, meaning that a partially positively charged boron atom in one layer is located on an oppositely charged nitrogen atom in an adjacent layer.

[0036] In this specification, the expression "boron nitride nanotube structure" is used to mean a portion of an epitaxial h-BN / BNNT structure in which boron and nitrogen atoms exist in an atomic arrangement having a defect rate of 10 percent or less compared to an idealized boron nitride nanotube (considered above) of the same length, diameter, and number of walls.

[0037] Where used herein, the term "defect rate" means the percentage of atoms in a structure that are inappropriately positioned relative to the idealized structure; that is, the expression "atomic arrangement having a defect rate of 10 percent or less relative to the idealized boron nitride nanotube" means, where used herein, a structure in which the percentage of deviation from the idealized boron nitride nanotube (of the same length, diameter, and number of walls) is 10 percent or less, and such deviation is quantified by dividing the number of atoms in the actual boron nitride nanotube structure that are in positions not corresponding to each position in the idealized boron nitride nanotube by the total number of positions relative to the atoms in the idealized boron nitride nanotube (or by subtracting from 100 percent the percentage of atoms in the actual boron nitride nanotube structure that are in positions corresponding to each position in the idealized boron nitride nanotube, relative to the total number of positions in the idealized boron nitride nanotube). A single deviation is when a single atom in the idealized boron nitride nanotube is replaced by a different atom, or when a single shift occurs. For example, when comparing the atomic arrangement in an actual boron nitride nanotube structure with the atomic arrangement in an idealized boron nitride nanotube, a single set of deviations may encompass a series of atoms (one atom wide) extending around the actual boron nitride nanotube structure, and the atoms on either side of that series of atoms (excluding the series of atoms) are compared with the atomic arrangement in the idealized boron nitride nanotube.

[0038] As described above, the hypothetical idealized boron nitride nanotube consists of one or more layers (i.e., walls), each layer consisting of a roughly tubular arrangement of boron and nitrogen atoms, where the boron and nitrogen atoms are arranged in a repeating hexagonal pattern with alternating boron and nitrogen atoms.

[0039] As used herein, the expression "hexagonal boron nitride structure" refers to a portion of an epitaxial h-BN / BNNT structure in which boron and nitrogen atoms exist in an atomic arrangement having a defect rate of 10 percent or less compared to an idealized hexagonal boron nitride structure (considered below) of the same shape and number of layers.

[0040] As stated above, the term "defect rate," as used herein, means the percentage of atoms in a structure that are in an inappropriate position relative to the idealized structure. In this context, that is, in the expression "a defect rate of 10 percent or less relative to an idealized hexagonal boron nitride structure of the same shape and number of layers (considered below)," a defect rate of 10 percent or less includes structures in which the deviation from an idealized hexagonal boron nitride structure of the same shape and number of layers is 10 percent or less, and such deviations are quantified and expressed as a percentage by dividing the number of atoms in the actual atomic arrangement that are in positions that do not correspond to each position in the idealized hexagonal boron nitride structure by the total number of positions for atoms in the idealized hexagonal boron nitride structure (or by subtracting from 100 percent the percentage of atoms in the actual atomic arrangement that correspond to each position in the idealized hexagonal boron nitride structure relative to the total number of positions in the idealized hexagonal boron nitride structure). A single deviation occurs when a single atom in an idealized hexagonal boron nitride structure is replaced by a different atom, or when a single shift occurs. For example, when comparing the atomic arrangement in a real material to the atomic arrangement in an idealized hexagonal boron nitride structure, a single set of deviations encompasses a set of atoms (one atom wide) that extend across the real material, and the atoms on either side of that set of atoms (not the set of atoms) are compared to the atomic arrangement in the idealized hexagonal boron nitride structure.

[0041] As used herein, the expression "idealized hexagonal boron nitride structure" means a hypothetical ideal boron nitride structure consisting of one or more layers, each layer comprising an arrangement of boron and nitrogen atoms corresponding to a defect-free hexagonal boron nitride crystal. As is known to those skilled in the art, the boron and nitrogen atoms in a hexagonal boron nitride crystal are arranged in a repeating hexagonal pattern of alternating boron and nitrogen atoms.

[0042] As used herein, the term "hexagonal boron nitride region" refers to a region of a hexagonal boron nitride structure (e.g., a region of a single, monolithic structure). The term "hexagonal boron nitride" is used herein to mean one or more hexagonal boron nitride structures.

[0043] When used herein, the expression "boron and nitrogen atoms nucleated on a boron nitride nanotube structure" means only those boron and nitrogen atoms in contact with atoms in the boron nitride nanotube structure, from among all boron and nitrogen atoms in the hexagonal boron nitride structure, each of which is epitaxial with respect to the boron nitride nanotube structure; that is, only those boron and nitrogen atoms that are arranged in such a way that they are (or result of) nucleation of hexagonal boron nitride on the boron nitride nanotube structure. For example, when hexagonal boron nitride is nucleated and grows on a boron nitride nanotube structure, the expression "boron and nitrogen atoms nucleated on a boron nitride nanotube structure" means only those boron and nitrogen atoms nucleated on the boron nitride nanotube structure, and does not mean boron and nitrogen atoms that subsequently grow on the nucleated boron and nitrogen atoms. do not have.

[0044] Therefore, the expression "hexagonal boron nitride epitaxial with respect to boron nitride nanotube structures" (as defined above) differs from the expression "boron atoms and nitrogen atoms nucleated on boron nitride nanotube structures" in that it means all atoms present in all hexagonal boron nitride structures that are epitaxial with respect to boron nitride nanotube structures (not just boron and nitrogen atoms nucleated on boron nitride nanotubes).

[0045] The expression “independent boron nitride nanotubes” means, as used herein, a structure containing boron and nitrogen atoms in an atomic arrangement that [1] has a defect rate of 10 percent or less compared to an idealized boron nitride nanotube (considered above) of the same length, diameter, and number of walls, and [2] does not contain any hexagonal boron nitride structures that are epitaxial with respect to it (i.e., there is no hexagonal boron nitride that is epitaxial with respect to nitrogen and boron atoms in an atomic arrangement that has a defect rate of 10 percent or less compared to an idealized boron nitride nanotube).

[0046] The expression "independent hexagonal boron nitride" means, in this specification, a structure (or a plurality of structures each containing) having an atomic arrangement of boron and nitrogen atoms such that [1] it has a defect rate of 10 percent or less compared to an idealized hexagonal boron nitride structure (considered above) of the same shape and number of layers, and [2] there are no epitaxial boron nitride nanotube structures therewith (i.e., there are no boron nitride nanotubes that become epitaxial with an atomic arrangement having a defect rate of 10 percent or less compared to an idealized hexagonal boron nitride structure).

[0047] As will be discussed below, one of the features of the epitaxial h-BN / BNNT structures disclosed herein is that the hexagonal boron nitride structure (which is epitaxial with respect to the boron nitride nanotube structure) "covers" the boron nitride nanotube structure (partially or completely) is readily perceptible (e.g., by normal human vision). This specification includes definitions that allow for the quantitative determination, as a percentage, of the degree to which the boron nitride nanotube structure is covered by the hexagonal boron nitride structure for any particular boron nitride nanotube structure. For the purpose of making such quantifications definitive (i.e., extremely accurate), so that a person skilled in the art can readily determine whether any particular structure satisfies the expressions herein relating to such covering, and / or whether any particular composition or aggregate satisfies the expressions relating to at least a certain percentage of boron nitride nanotube structures, each of which is covered by at least a certain percentage, this specification includes very detailed definitions (below) for performing such calculations with sufficient accuracy.

[0048] The expression "at least 10% of the total outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure" means, as used herein, for each of at least 10% of the atoms on the outermost wall of the boron nitride nanotube structure, [1] there is an atom in a hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotube structure, and [2] there is an atom within 10 nanometers of such atom.

[0049] When the term "outermost wall" is used herein in relation to boron nitride nanotube structures, it refers to the outermost wall of a multilayer boron nitride nanotube structure (i.e., the wall furthest from the axis of the boron nitride nanotube structure and furthest from the space inside the tube), or (single-layer nitride nanotube structure). (In the case of boron nanotube structures) This means a single wall.

[0050] When used herein in relation to independent boron nitride nanotubes, the term "outermost wall" means the outermost wall of an independent multilayer boron nitride nanotube (i.e., the wall furthest from the axis of the independent boron nitride nanotube and furthest from the space within the tube), or (in the case of an independent single-wall boron nitride nanotube) a single wall.

[0051] In addition to the above definition relating to the calculation of the percentage in which boron nitride nanotube structures are covered by hexagonal boron nitride structures within an epitaxial h-BN / BNNT structure, there also exist epitaxial h-BN / BNNT structures in which multiple boron nitride nanotube structures can form a mass together, and the entire mass (containing multiple boron nitride nanotube structures) can be covered (to at least a certain percentage) by hexagonal boron nitride structures that are epitaxial with respect to the boron nitride nanotube structures within the mass (e.g., the outermost ones). For the purpose of making such quantifications sufficiently accurate so that a person skilled in the art can easily determine whether any particular structure satisfies the expressions herein relating to such coating, and / or whether any particular composition or aggregate satisfies the expressions relating to such coating, this Specification includes further definitions (starting with the definition of “mass” and certain types of masses) for making such calculations sufficiently accurate.

[0052] When used herein (e.g., in the expressions “independent boron nitride nanotube aggregate,” “boron nitride nanotube structure aggregate,” and “boron nitride nanotube structure / independent boron nitride nanotube aggregate”), the term “aggregate” means a group of at least two independent boron nitride nanotubes all in contact with each other, a group of at least two boron nitride nanotube structures all in contact with each other, or a group of at least one independent boron nitride nanotube and at least one boron nitride nanotube structure all in contact with each other. A single “clump” means a group in which each member of the group is in direct or indirect contact with all other members of the group (indirect contact between members of a group means that members are not in direct contact with each other but are in a series of directly contacting pairs of members that extend between them, i.e., the first and second members are in direct contact with each other, the third member is in direct contact with at least one of the first and second members, the fourth member is in direct contact with at least one of the first through third members, the fifth member is in direct contact with at least one of the first through fourth members, and so on). Representative examples of “clumps” being important in the context of the subject matter of this invention will be considered after the following definition of “external atoms…”.

[0053] When used herein, the expression "independent boron nitride nanotube mass" means a mass containing multiple independent boron nitride nanotubes but not containing a boron nitride nanotube structure.

[0054] When used herein, the expression "boron nitride nanotube structure mass" means a mass that contains multiple boron nitride nanotube structures but does not contain any individual boron nitride nanotubes.

[0055] The expression “boron nitride nanotube structure / independent boron nitride nanotube mass” means, as used herein, a mass containing at least one boron nitride nanotube structure and at least one independent boron nitride nanotube. Similar expressions mean similar structures, for example, any specified number (or range) of boron nitride nanotube structures and / or independent boron nitride nanotube masses means that the sum of [1] the total number of boron nitride nanotube structures and [2] the total number of independent boron nitride nanotubes is This refers to structures that are equal to (or within the specified range of) a specified number.

[0056] "[2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not a clump, The expressions "[2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, each covered by a hexagonal boron nitride structure which is epitaxial" are, As used herein, for each of [2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, it means that for each of the external atoms (as defined below), there are atoms that are [a] in a hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotubes in the mass, and [b] within 10 nanometers of such external atoms.

[0057] The expression "[2] boron nitride nanotube structure clump, [3] boron nitride nanotube structure / independent boron nitride nanotube clump, or [5] external atom of a boron nitride nanotube structure that is not a clump" is used herein to include any atom on a boron nitride nanotube structure clump, a boron nitride nanotube structure / independent boron nitride nanotube clump, or [5] a boron nitride nanotube structure that is not a clump, which has a cylindrical region of radius 0.1 angstroms that extends at least 1 mm from that atom and does not intersect with any other atom on a boron nitride nanotube structure clump, a boron nitride nanotube structure / independent boron nitride nanotube clump, or [5] a boron nitride nanotube structure that is not a clump.

[0058] A typical example of the term “clump” being important in the context of the subject matter of the present invention is when one or more boron nitride nanotube structures and / or one or more independent boron nitride nanotubes in a clump are substantially completely covered by other boron nitride nanotube structures and / or independent boron nitride nanotubes (e.g., such substantially completely covered boron nitride nanotube structures and / or one or more independent boron nitride nanotubes are in a larger clump). In such a situation, the atoms of such substantially complete boron nitride nanotube structures and / or one or more independent boron nitride nanotubes do not satisfy the above definition of “external atoms” as described herein, and therefore such atoms constitute at least 10% of the total external atoms of [2] boron nitride nanotube structure clumps, [3] boron nitride nanotube structures / independent boron nitride nanotube clumps, or [5] boron nitride nanotube structures that are not clumps. [2] A boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, each covered by a hexagonal boron nitride structure which is epitaxial to the boron nitride nanotube structure. This is not considered when determining whether the expression is satisfied.

[0059] As used herein, the expression "residual boron" means a mass consisting of (or primarily consisting of) boron and / or boron compounds. As used herein, the term "aggregate" means a single, unified structure, i.e., a structure that can be lifted by grasping any part of it (i.e., such a part can be grasped and lifted without gravity separating any part of the structure from any other part of it). (ru).

[0060] As used herein, the expression "integrated single structure" means a single structure. As used herein, the term "plural" means two or more (e.g., the phrase "plural hexagonal boron nitride structures" means two or more hexagonal boron nitride structures).

[0061] When used herein, the expression "less than or equal to" means the specified amount or less (e.g., "less than or equal to 35% of the mass of the composition" means 35% or less of the mass of the composition).

[0062] When used herein, the expression "at least" means the specified amount or more (e.g., "at least 10 boron nitride nanotube structures" means 10 or more boron nitride nanotube structures), and vice versa (e.g., "2 or more boron nitride nanotube structures" means at least 2 boron nitride nanotube structures).

[0063] The expression "[The composition or aggregate] contains at least [a specified percentage] of [a certain type of material]" (e.g., "The composition contains at least 10% by mass of hexagonal boron nitride") means that the specified type of material constitutes a specified percentage (or range of percentages) of the entire composition or aggregate, and vice versa (i.e., the expression "[The specified material] constitutes a specified percentage of [the composition or aggregate]" means that the specified percentage (or range of percentages) of the composition or aggregate is the specified material).

[0064] In expressions where "total" is characterized as the sum of the individual values ​​of two or more items, for example, the following expressions: "[1] The sum of the total mass of all independent hexagonal boron nitride in the composition and [2] the total mass of all residual boron in the composition," "[1] The sum of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the boron nitride nanotube structures having a length of at least 50 nm in the composition." "The sum of the amounts of each of the following: [1] independent boron nitride nanotube clumps having a length of at least 50 nm in the composition, [2] boron nitride nanotube structure clumps having a length of at least 50 nm in the composition, [3] boron nitride nanotube structure / independent boron nitride nanotube clumps having a length of at least 50 nm in the composition, [4] independent boron nitride nanotubes having a length of at least 50 nm, not clumps, in the composition, and [5] boron nitride nanotube structure having a length of at least 50 nm, not clumps, in the composition." Furthermore, in similar expressions in which “composition” is replaced by and / or included together with “integrated structure,” one or more of the values ​​may be zero; that is, the inclusion of an item does not necessarily mean that the value for such item is non-zero.

[0065] In this specification, the terms "plasma" and "ionized gas" are used in accordance with their well-known meanings, and refer to a substance obtained when sufficient energy is supplied to a gas, causing electrons to be released from atoms or molecules, and thus allowing ions and electrons to coexist (also referred to as the fourth state of matter, i.e., solid, liquid, gas, plasma).

[0066] As stated above, according to a first aspect of the subject matter of the present invention: At least the first epitaxial h-BN / BNNT structure, A composition containing the following is provided: The first epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure and at least a first hexagonal boron nitride structure, The first hexagonal boron nitride structure is epitaxial with respect to the first boron nitride nanotube structure.

[0067] In some embodiments according to a first aspect of the subject matter of the present invention, any other features described herein may, as appropriate, be included or excluded: [1] The sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the sum of the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition is at least 10. For each of the boron nitride nanotube structures in an amount that is at least 10% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition: The boron nitride nanotube structure has a length of at least 50 nm, and at least 10% of the total outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. Furthermore, in some of such embodiments: For each boron nitride nanotube structure in an amount that is at least a first percent (selected from 20%, 30%, 40%, 50%, 60%, 70%, 80%, and 90%) of the sum of [1] the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition, or within the range of a first percent (selected from 10% to 20%, 20% to 30%, 30% to 40%, 40% to 50%, 50% to 60%, 60% to 70%, 70% to 80%, and 80% to 90%): The boron nitride nanotube structure has a length of at least 50 nm, and at least two percent of the outermost wall of the boron nitride nanotube structure in total (selected from 10%, 20%, 30%, 40%, 50%, 60%, 70%, 80%, and 90%), or within the range of two percent in total (selected from 10%~20%, 20%~30%, 30%~40%, 40%~50%, 50%~60%, 60%~70%, 70%~80%, and 80%~90%), is covered by a hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotube structure. This includes any combination of the first percentage (or range of the first percentage) and the second percentage (or range of the second percentage).

[0068] In some embodiments according to the first aspect of the subject matter of the present invention, which may include or not include any of the other features described herein: The sum of the amounts of each of [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the composition, [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the composition, [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the composition, [4] independent boron nitride nanotubes having a length of at least 50 nm, not clusters, and [5] boron nitride nanotube structures having a length of at least 50 nm, not clusters, in the composition is at least 10. [2] A mass of boron nitride nanotube structures having a length of at least 50 nm in the composition, [3] A boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in the composition, and [5] A boron nitride nanotube structure in the composition that is not a mass but has a length of at least 50 nm, of which at least 30% of the total For each of the quantities: [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] A boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, each covered by an epitaxial hexagonal boron nitride structure. Furthermore, in some of such embodiments: The sum of the amounts of each of [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the composition, [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the composition, [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the composition, [4] independent boron nitride nanotubes having a length of at least 50 nm, not clusters, and [5] boron nitride nanotube structures having a length of at least 50 nm, not clusters, in the composition is at least 10. [2] For each of the boron nitride nanotube structure aggregates having a length of at least 50 nm in the composition, [3] boron nitride nanotube structure / independent boron nitride nanotube aggregates having a length of at least 50 nm in the composition, and [5] for each of the boron nitride nanotube structure aggregates having a length of at least 50 nm in the composition, not aggregates, that are at least a first percent (selected from 40%, 50%, 60%, 70%, 80%, and 90%) of the total, or within the range of a first percent (selected from 30%~40%, 40%~50%, 50%~60%, 60%~70%, 70%~80%, and 80%~90%): [2] Boron nitride nanotube structure aggregates, [3] Boron nitride nanotube structures / independent boron nitride nanotube aggregates, or [5] Boron nitride nanotube structures that are not aggregates, with at least two percent in total (selected from 10%, 20%, 30%, 40%, 50%, 60%, 70%, 80%, and 90%) or within the range of two percent in total (selected from 10%~20%, 20%~30%, 30%~40%, 40%~50%, 50%~60%, 60%~70%, 70%~80%, and 80%~90%) of the external atoms of the boron nitride nanotube structure aggregates, [3] Boron nitride nanotube structures / independent boron nitride nanotube aggregates, or [5] Boron nitride nanotube structures that are not aggregates, [2] A boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, each covered by an epitaxial hexagonal boron nitride structure. This includes any combination of the first percentage (or range of the first percentage) and the second percentage (or range of the second percentage).

[0069] As stated above, according to a second aspect of the subject matter of the present invention: An integrated structure including at least a first epitaxial h-BN / BNNT structure, Aggregates containing the following are provided: The first epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure and at least a first hexagonal boron nitride structure, The first hexagonal boron nitride structure is epitaxial with respect to the boron nitride nanotube structure. The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension.

[0070] In some embodiments according to a second aspect of the subject matter of the present invention, which may include or omit any of the other features described herein as appropriate: For each boron nitride nanotube structure in the integral structure, the amount is at least 10% of the sum of [1] the amount of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] the amount of boron nitride nanotube structures having a length of at least 50 nm in the integral structure: At least 10% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. Furthermore, in some of such embodiments: For each boron nitride nanotube structure in an integral structure in an amount that is at least a first percent (selected from 20%, 30%, 40%, 50%, 60%, 70%, 80%, and 90%) of the sum of [1] the amount of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] the amount of boron nitride nanotube structures having a length of at least 50 nm in the integral structure, or within the range of a first percent (selected from 10% to 20%, 20% to 30%, 30% to 40%, 40% to 50%, 50% to 60%, 60% to 70%, 70% to 80%, and 80% to 90%): At least two percent of the outermost wall of the boron nitride nanotube structure in total (selected from 20%, 30%, 40%, 50%, 60%, 70%, 80%, and 90%), or within the range of two percent in total (selected from 10%-20%, 20%-30%, 30%-40%, 40%-50%, 50%-60%, 60%-70%, 70%-80%, and 80%-90%), is covered by a hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotube structure. This includes any combination of the first percentage (or range of the first percentage) and the second percentage (or range of the second percentage).

[0071] In some embodiments according to a second aspect of the subject matter of the present invention, which may include or omit any of the other features described herein as appropriate: [2] A boron nitride nanotube structure mass having a length of at least 50 nm in a single structure, [3] A boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in a single structure, and [5] A boron nitride nanotube structure having a length of at least 50 nm, not a mass, in a single structure For each of the following amounts, the sum of the amounts of: [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the integral structure; [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [4] independent boron nitride nanotubes in the integral structure that are not clusters and have a length of at least 50 nm; and [5] boron nitride nanotube structures in the integral structure that are not clusters and have a length of at least 50 nm: [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] A boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, each covered by an epitaxial hexagonal boron nitride structure. Furthermore, in some of such embodiments: [2] A boron nitride nanotube structure mass having a length of at least 50 nm in a single structure, [3] A boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in a single structure, and [5] A boron nitride nanotube structure having a length of at least 50 nm, not a mass, in a single structure [1] Independent boron nitride nanotubes having a length of at least 50 nm in a single structure For each of the amounts of [1] boron nitride nanotube structure aggregates having a length of at least 50 nm in the integral structure, [2] boron nitride nanotube structure aggregates having a length of at least 50 nm in the integral structure / independent boron nitride nanotube aggregates, [4] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure (not aggregates), and [5] boron nitride nanotube structures having a length of at least 50 nm in the integral structure (not aggregates), that is at least a first percent (selected from 20%, 30%, 40%, 50%, 60%, 70%, 80%, and 90%) or within the range of a first percent (selected from 10%~20%, 20%~30%, 30%~40%, 40%~50%, 50%~60%, 60%~70%, 70%~80%, and 80%~90%) of the sum of the amounts of [1] boron nitride nanotube aggregates, [2] boron nitride nanotube structure aggregates having a length of at least 50 nm in the integral structure, [3] boron nitride nanotube structure / independent boron nitride nanotube aggregates having a length of at least 50 nm in the integral structure, [4] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure (not aggregates), and [5] boron nitride nanotube structure having a length of at least 50 nm in the integral structure (not aggregates), that is at least a first percent (selected from 10%~20%, 20%~30%, 30%~40%, 40%~50%, 50%~60%, 60%~70%, 70%~80%, and 80%~90%): [2] Boron nitride nanotube structure aggregates, [3] Boron nitride nanotube structures / independent boron nitride nanotube aggregates, or [5] Boron nitride nanotube structures that are not aggregates, with at least two percent in total (selected from 20%, 30%, 40%, 50%, 60%, 70%, 80%, and 90%) or within the range of two percent in total (selected from 10%-20%, 20%-30%, 30%-40%, 40%-50%, 50%-60%, 60%-70%, 70%-80%, and 80%-90%) of the external atoms of the boron nitride nanotube structure aggregates, [3] Boron nitride nanotube structures / independent boron nitride nanotube aggregates, or [5] Boron nitride nanotube structures that are not aggregates, [2] A boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, each covered by an epitaxial hexagonal boron nitride structure. This includes any combination of the first percentage (or range of the first percentage) and the second percentage (or range of the second percentage).

[0072] As stated above, according to a third aspect of the subject matter of the present invention: Multiple independent boron nitride nanotubes, A composition containing the following is provided: [1] The sum of the total mass of all independent hexagonal boron nitride in the composition and [2] the total mass of all residual boron in the composition accounts for 35% or less of the total mass of the composition.

[0073] In some embodiments of the subject matter of the present invention, which may include or omit any of the other features described herein as appropriate: [1] The sum of the total mass of all independent hexagonal boron nitride in the composition and [2] the total mass of all residual boron in the composition is less than or equal to a first percent (selected from 30%, 25%, 20%, 15%, 10%, and 5%) of the mass of the composition, or within a first percent range (selected from 30% to 350%, 25% to 30%, 20% to 25%, 15% to 20%, 10% to 15%, and 5% to 10%).

[0074] As stated above, according to a fourth aspect of the subject matter of the present invention: A single structure containing multiple independent boron nitride nanotubes, Aggregates containing the following are provided: The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. [1] The total mass of the independent hexagonal boron nitride in the integral structure and [2] the total mass of all residual boron in the integral structure together account for 35% or less of the total mass of the integral structure.

[0075] In some embodiments according to a fourth aspect of the subject matter of the present invention, which may include or omit any of the other features described herein as appropriate: [1] The total mass of all independent hexagonal boron nitrides in the integral structure and [2] in the integral structure The total mass of all residual boron, including the total mass of the boron, is less than or equal to a first percent (selected from 30%, 25%, 20%, 15%, 10%, and 5%) of the mass of the integral structure, or within a first percent range (selected from 30% to 350%, 25% to 30%, 20% to 25%, 15% to 20%, 10% to 15%, and 5% to 10%).

[0076] As stated above, according to the fifth aspect of the subject matter of the present invention: At least 10 independent boron nitride nanotubes having a length of at least 50 nm, A composition containing the following is provided: [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the composition, 1% or less of the total has at least one defect selected from Dixie cup defects and bamboo defects.

[0077] Those skilled in the art are familiar with Dixie cup defects and bamboo defects. For clarity, when the term “bamboo defect” is used herein in relation to boron nitride nanotubes, it means that the boron nitride nanotube has multiple regions in which the diameter of the boron nitride nanotube increases by at least 10% over a length of 5 nm or less (i.e., along the longitudinal direction of the boron nitride nanotube, at intervals of 5 nm or less, the diameters of each boron nitride nanotube (i.e., the diameter perpendicular to the axis of the boron nitride nanotube) differ by at least 10% (i.e., one diameter is at least 1.1 times that of the other)).

[0078] For clarity, when the term “Dixie cup defect” is used herein in reference to boron nitride nanotubes (or multiple boron nitride nanotubes), it means that each boron nitride nanotube (or each of the boron nitride nanotubes) is tapered in the sense that it has a first (broad) end and a second (narrow) end (separated from each other along the axis of the boron nitride nanotube or wall), the second (narrow) end having a diameter (perpendicular to the axis) that is 65% or less of the diameter of the first (broad) end, and the narrow end of one boron nitride nanotube is contained within the broad end of another tapered boron nitride nanotube (i.e., a plane perpendicular to the axis of the boron nitride nanotubes and in the “Dixie cup overlap” region passes through both boron nitride nanotubes).

[0079] In some embodiments according to a fifth aspect of the subject matter of the present invention, which may or may not include any of the other features described herein: [1] of the total of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] of the boron nitride nanotube structures having a length of at least 50 nm in the composition, a percentage of the total that is less than or equal to a first percentage (selected from 0.8%, 0.6%, 0.4%, 0.3%, 0.2%, and 0.1%) or within a first percentage range (selected from 0.0% to 0.1%, 0.1% to 0.2%, 0.2% to 0.3%, 0.3% to 0.4%, 0.4% to 0.6%, 0.6% to 0.8%, and 0.8% to 1.0%) has at least one defect selected from Dixie cup defects and bamboo defects.

[0080] As stated above, according to the sixth aspect of the subject matter of the present invention: A single structure containing multiple independent boron nitride nanotubes, Aggregates containing the following are provided: The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the integral structure, less than 1% of the total has at least one defect selected from Dixie cup defects and bamboo defects.

[0081] In some embodiments according to a sixth aspect of the subject matter of the present invention, which may include or omit any of the other features described herein as appropriate: [1] In the sum of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] in the sum of boron nitride nanotube structures having a length of at least 50 nm in the integral structure, a percentage of the sum that is less than or equal to a first percentage (selected from 0.8%, 0.6%, 0.4%, 0.3%, 0.2%, and 0.1%) or within a first percentage range (selected from 0.0%~0.1%, 0.1%~0.2%, 0.2%~0.3%, 0.3%~0.4%, 0.4%~0.6%, 0.6%~0.8%, and 0.8%~1.0%) has at least one defect selected from Dixie cup defects and bamboo defects.

[0082] As stated above, according to the seventh aspect of the subject matter of the present invention: At least 10 independent boron nitride nanotubes, A composition containing the following is provided: [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the composition, at least 50% of each of the total is a single layer.

[0083] In some embodiments according to a seventh aspect of the subject matter of the present invention, which may or may not include any other features described herein as appropriate, each of the monolayers, at least a portion of the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition, is present in an independent boron nitride nanotube mass, a boron nitride nanotube structure mass, or a boron nitride nanotube structure / independent boron nitride nanotube mass.

[0084] In some embodiments according to the seventh aspect of the subject matter of the present invention, which may or may not include any of the other features described herein as appropriate, [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition, each of the above 50 to 60 percent of the total is a single layer.

[0085] As stated above, according to the eighth aspect of the subject matter of the present invention: A monolithic structure containing at least one independent boron nitride nanotube, Aggregates containing the following are provided: The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the integral structure, at least 50% of each of the total is a single layer.

[0086] In some embodiments according to the eighth aspect of the subject matter of the present invention, which may or may not include any of the other features described herein, the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in an integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in an integral structure, Each of the single layers, at least a portion of it, exists as an independent boron nitride nanotube cluster, a boron nitride nanotube structure cluster, or a boron nitride nanotube structure / independent boron nitride nanotube cluster.

[0087] In some embodiments according to the eighth aspect of the subject matter of the present invention, which may or may not include any of the other features described herein as appropriate, [1] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in the integral structure, each of the above 50 to 60 percent of the total is a single layer.

[0088] In some embodiments according to any of the first, second, fifth, sixth, seventh, and eighth aspects of the subject matter of the present invention, which may or may not include any other features described herein, the combined mass of the epitaxial h-BN / BNNT structures in the composition accounts for at least 65% of the mass of the composition or integral structure (i.e., the composition according to the first, third, fifth, and seventh aspects, and the integral structure according to the second, fourth, sixth, and eighth aspects, and the same applies hereinafter in other appearances of “composition or integral structure”). In some such embodiments, the combined mass of the epitaxial h-BN / BNNT structures in the composition accounts for at least a first percentage (selected from 70%, 75%, 80%, 85%, 90%, 95%, 97%, and 99%) of the mass of the composition or the integral structure, or a percentage within the range of a first percentage (selected from 65%-70%, 70%-75%, 75%-80%, 80%-85%, 85%-90%, 90%-95%, 95%-97%, and 97%-99%).

[0089] In some embodiments according to any of the first, second, third, fourth, fifth, sixth, seventh, and eighth aspects of the subject matter of the present invention, which may or may not include any other features described herein, at least 10% by mass of the composition or integral structure comprises hexagonal boron nitride structures, each epitaxial with respect to the boron nitride nanotube structure.

[0090] In some embodiments according to any of the first, second, third, fourth, fifth, sixth, seventh, and eighth aspects of the subject matter of the present invention, which may or may not include any other features described herein, for each of at least 10% of the atoms in the composition or integral structure, the atoms are present in a hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotube structure in the composition.

[0091] In some embodiments according to either of the first and second aspects of the subject matter of the present invention, which may or may not include any other features described herein as appropriate, the combined mass of all independent hexagonal boron nitrides in the composition or integral structure, and [2] the combined mass of all amorphous borons in the composition or integral structure, account for less than 35% of the mass of the composition or integral structure. In some such embodiments, the combined mass of all independent hexagonal boron nitrides in the composition or integral structure, and [2] the combined mass of all amorphous borons in the composition or integral structure, constitutes a percentage of the mass of the composition or integral structure that is less than a first percent (selected from 30%, 25%, 20%, 15%, 10%, and 5%) or within a first percent range (selected from 10% to 20%, 20% to 30%, 30% to 40%, 40% to 50%, 50% to 60%, 60% to 70%, 70% to 80%, and 80% to 90%).

[0092] Several embodiments according to any of the first, second, third, and fourth aspects of the subject matter of the present invention, which may or may not include any of the other features described herein as appropriate. In the following case, the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition or integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition or integral structure, such that 1% or less of the total has at least one defect selected from Dixie cup defects and bamboo defects, In some such embodiments, the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition or integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition or integral structure, wherein a percentage of the total is less than or equal to a first percentage (selected from 0.8%, 0.6%, 0.4%, 0.3%, 0.2%, and 0.1%) or within a first percentage range (selected from 0.0% to 0.1%, 0.1% to 0.2%, 0.2% to 0.3%, 0.3% to 0.4%, 0.4% to 0.6%, 0.6% to 0.8%, and 0.8% to 1.0%) has at least one defect selected from Dixie cup defects and bamboo defects.

[0093] In some embodiments according to any of the first, second, third, fourth, fifth, and sixth aspects of the subject matter of the present invention, which may or may not include any of the other features described herein as appropriate, [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition or integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition or integral structure, each of which at least 50% of the total is a single layer.

[0094] In some embodiments according to any third and fourth aspects of the subject matter of the present invention, which may or may not include any other features described herein, independent hexagonal boron nitride constitutes 1 mass percent or less of the composition or aggregate. In some such embodiments, independent hexagonal boron nitride constitutes at least a first percentage (selected from 0.8%, 0.6%, 0.4%, 0.3%, 0.2%, and 0.1%) of the mass of the composition or aggregate, or a percentage within the range of the first percentage (selected from 0.0% to 0.1%, 0.1% to 0.2%, 0.2% to 0.3%, 0.3% to 0.4%, 0.4% to 0.6%, 0.6% to 0.8%, and 0.8% to 1.0%).

[0095] Figure 1 is a schematic diagram showing a typical embodiment of an apparatus 10 that can be used to produce epitaxial h-BN / BNNT structures, and further compositions and / or aggregates containing epitaxial h-BN / BNNT structures, according to first and second aspects of the subject matter of the present invention. Figure 2 is an enlarged view of a part of Figure 1 and shows a part of the apparatus 10.

[0096] The apparatus 10 comprises a plasma generator 11, a color region 12, a first reaction section 13 (defining the first reaction chamber region), and a second reaction section 14 (defining the second reaction chamber region).

[0097] The plasma generator 11 comprises a wall section 15, an electromagnetic wave generator and waveguide 16, and a sparker 17. The waveguide is an inductor, for example, in the form of a coil of several turns (usually 3 to 6) of copper tubing (1 / 4" or larger). The copper coil is a non-magnetic coil that provides high electrical conductivity. The number of turns is determined to match the inductance and electrical resistance of the inductor, which provides compatibility with high-frequency power output.

[0098] The wall portion 15 of the plasma generator 11 includes an RF-transparent region 18 that is high-frequency transparent (i.e., RF-transparent), electrically conductive, and non-magnetic. A typical example of a suitable material that can produce the RF-transparent region 18 is alumina.

[0099] The AC power supply 19 supplies high-frequency energy to an electromagnetic wave generator 16 that generates electromagnetic waves of multiple frequencies selected from a range of tens of kilohertz to thousands of gigahertz, and such electromagnetic waves pass through the RF-transparent portion 18 of the wall portion 15 of the plasma generation region 11.

[0100] Inside the plasma generator 11 is the plasma generator space 21. The sparker 17 comprises a mobile electrode 29 and a discharge projection 30. The mobile electrode 29 is configured to extend controllably within a region of the plasma generator space 21, including the region with the maximum magnetic field density and the region with the maximum electric field density. The discharge projection 30 is manufactured from an electrically conductive, non-magnetic material and is configured to create a discharge point when the mobile electrode 29 approaches, and such a discharge generates plasma. The mobile electrode 29 is configured to be withdrawn from the region with the maximum magnetic field density and the region with the maximum electric field density after such a discharge.

[0101] The plasma generator 11 has one or more ports 20 through which a material (e.g., nitrogen gas) can be introduced into the plasma generator space 21. The plasma generator 11 has a plume opening 22 through which the plume of plasma generated by the plasma generator 11 passes and enters the color space 23 inside the color region 12.

[0102] The color region 12 includes at least one reactant feed opening 24 through which a feedstock (e.g., boron powder, boron nitride, boron carbide, boron trioxide, boric acid, etc.) can be introduced (e.g., injected) into the color space 23 (and into the plasma plume) along with a carrier gas, if desired.

[0103] The first reaction vessel section 13 may be provided with one or more access ports 25 that provide access to the first reaction chamber region 26 inside the first reaction vessel section 13. One or more access ports 25 (if included) can provide access for diagnostic purposes (such as optical monitoring of the reaction), for inserting structures into the reaction chamber (e.g., quench modifiers such as wires or mesh), or for removing the product.

[0104] Similarly, the second reaction vessel section 14 may be provided with one or more access ports 27 that provide access to the second reaction chamber region 28 inside the second reaction vessel section 14. One or more access ports 27 (if included) can provide access for diagnostic purposes (such as optical monitoring of the reaction), for inserting structures into the reaction chamber (e.g., quench modifiers such as wires or mesh), or for removing the product.

[0105] The apparatus 10 further includes an external shell 31 outside the plasma generator 11 to enable cooling and / or provide a gas-liquid seal. In the embodiment shown in Figure 1, the external shell 31 is substantially concentric with respect to the plasma generator 11, with the plasma generator 11 being the internal tube and the external shell being the external tube. Holes 32 at the ends of the external shell 31 allow a coolant, such as water, to flow (in the indicated direction) to the bottom of the chamber 33 within the external shell 31 and out from the top of the chamber 33. The external shell 31 also assists in sealing the plasma generator 11, thereby helping to avoid or reduce any leakage of plasma and gas. The external shell 31 is preferably RF permeable. Typical examples of suitable materials from which the external shell 31 can be manufactured include quartz and ceramic materials.

[0106] In some embodiments, the product can be continuously or semi-continuously removed from the first reaction chamber region 26 and / or the second reaction chamber region 28 (e.g., removing the product from the first reaction chamber region 26 and / or the second reaction chamber region 28) (By conveyor) (i.e., not batch operation).

[0107] An outlet port 34 is formed in the second reaction vessel section 14, and a first exhaust line 35 is connected to the outlet port 34. A pressure regulator 36 is connected to the first exhaust line 35, and a second exhaust line 37 is connected to the pressure regulator 36, thereby enabling the exhaust of gases (e.g., nitrogen, argon, and hydrogen) and the control of the internal pressures of the first and second reaction chamber regions 26 and 28. Any suitable pressure regulator (e.g., a needle valve) may be used as the pressure regulator 36.

[0108] In the above considerations, the plasma generator is an inductively coupled plasma generator. Alternatively, the plasma generator may be a DC arc plasma generator (i.e., a plasma generator driven by a DC power supply). Those skilled in the art will be familiar with DC arc plasma generators, and any such plasma generator may be used. In some embodiments, inductively coupled plasma generators are advantageous (compared to DC arc plasma generators) in the production of compositions and / or aggregates containing boron nitride nanotubes having hexagonal boron nitride structures that are epitaxial with respect to the boron nitride nanotubes, because inductively coupled plasma generators offer a larger plasma volume, a lower plasma gas velocity, and a longer reaction time. In addition, because inductively coupled plasma generators do not have electrodes, they can be relatively maintenance-free, and (unlike DC arc plasma generators which must include electrodes) contaminants from the electrodes are not introduced into the material during production.

[0109] The power density and volume of the plasma plume can be adjusted by changing the input power to the plasma generator, by changing the pressure in the plasma generator space 21, and / or by changing the flow rate of the material supplied to the apparatus 10 (e.g., nitrogen gas, boron powder with nitrogen carrier gas, etc.).

[0110] The apparatus 10 shown in Figure 1 also, A composition (or aggregate) comprising a plurality of independent boron nitride nanotubes, according to a third aspect (or fourth aspect) of the subject matter of the present invention, wherein the sum of [1] the total mass of all independent hexagonal boron nitride in the composition (or aggregate) and [2] the total mass of all residual boron in the composition (or aggregate) accounts for 35% or less of the mass of the composition (or aggregate); A composition (or aggregate) according to the fifth aspect (or sixth aspect) of the subject matter of the present invention, comprising [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition (or aggregate) and [2] a boron nitride nanotube structure having a length of at least 50 nm in the composition (or aggregate), wherein 1% or less of the total comprises at least 10 independent boron nitride nanotubes having a length of at least 50 nm, wherein at least one defect selected from Dixie cup defects and bamboo defects; and A composition (or aggregate) according to the seventh aspect (or eighth aspect) of the subject matter of the present invention, comprising [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition (or aggregate) and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition (or aggregate), wherein at least 50% of the total each comprises at least 10 independent boron nitride nanotubes that are monolayers, It can be used to manufacture [something].

[0111] One specific representative embodiment of a method for producing an epitaxial h-BN / BNNT structure according to a first aspect of the subject matter of the present invention is: The apparatus further comprises supplying a mixture of nitrogen and hydrogen (96 parts by mass of nitrogen and 4 parts by mass of hydrogen) at a rate of 50 liters per minute to the plasma generator space 21 of the apparatus 10 shown in Figure 1 (through the port 20 of the apparatus 10 shown in Figure 1), wherein the outer diameter of the plasma generator 11 is 3.5 inches. The plasma generator 11 has an inner diameter of 2.0 inches, the length of the plasma generator 11 (in the longitudinal direction in the orientation shown in Figure 1) is 10.0 inches, the outer diameter of the color region 12 is 3.5 inches, the inner diameter of the color region 12 is 1.40 inches, the length of the color region 12 (in the longitudinal direction in the orientation shown in Figure 1) is 3.0 inches, the diameter of the plume opening 22 (connecting section between plasma generator space 21 and color space 23) is 1.38 inches, the reactant feed opening 24 is located midway along the longitudinal direction of the color region 12, the inner diameter of the first reaction vessel section 13 is 8.0 inches, and the first reaction vessel section The first reaction vessel section 13 has a length (longitudinal in the orientation shown in Figure 1) of 24 inches, the second reaction vessel section 14 has an inner diameter of 8.0 inches, the second reaction vessel section 14 has a length (longitudinal in the orientation shown in Figure 1) of 24 inches (i.e., the first reaction vessel section 13 and the second reaction vessel section 14 together form a cylindrical chamber region of uniform diameter, which is a combination of the first reaction chamber region 26 and the second reaction chamber region 28, with a diameter of 8 inches and a length of 48 inches), and the reactant feed opening 24 has a diameter of 1 / 16 inch; Ionizing nitrogen and hydrogen in the plasma generator space 21 by supplying 35-45 kW to the electromagnetic wave generator 16; and To the color space (through the reactant feed opening 24, at the highest temperature location within the apparatus 10), 20-90 mg / min of solid elemental boron powder (at room temperature before being introduced into the apparatus 10) is supplied, accompanied by nitrogen gas (e.g., 0.1-10.0 liters per minute). This includes, at the same time, maintaining the pressure in the first reaction vessel section 13 and the second reaction vessel section 14 within the range of 10 psi to 20 psi (the pressure may fluctuate within this range).

[0112] In this typical embodiment, the temperature in at least a portion of the color region 12 is about 8000K due to the heat provided by the plasma, while the temperatures in the first reaction vessel section 13 and the second reaction vessel section 14 are lower the further they are from the color region 12.

[0113] The epitaxial h-BN / BNNT structure according to the subject of this invention resembles rock candy, and (continuing this analogy) the boron nitride nanotube structure is the string, and the nucleated and grown hexagonal boron nitride is the sugar.

[0114] Boron and nitrogen ions that are not converted to boron nitride nanotube structures in the hottest zone of the apparatus become supersaturated in the apparatus and accumulate on the boron nitride nanotube structures, where they nucleate hexagonal boron nitride structures on the boron nitride nanotube structures (i.e., create structures having nucleated boron and nitrogen atoms on the boron nitride nanotube structures) and / or grow on already nucleated boron nitride structures.

[0115] The diameter of the boron nitride nanotube structures formed according to the typical embodiments described above is in the range of 3 to 30 nm overall (e.g., 90% or more). The length of the boron nitride nanotube structure formed according to the typical embodiment described above is in the range of 10 nm to 50 micrometers overall (e.g., more than 90% of it).

[0116] The boron nitride nanotube structure formed according to the representative embodiment described above is epitaxial, and the hexagonal boron nitride nodules covering it have a thickness of 1 nm to 200 nm overall (e.g., more than 90% of it) (and are easily identifiable, for example, in TEM images).

[0117] The portions of the boron nitride nanotube structure not covered by the hexagonal boron nitride structure, and the independent boron nitride nanotubes (if present), are very smooth and easily identifiable (e.g., in transmission electron microscope images (i.e., TEM images)).

[0118] The residual boron portion (in the products of the typical embodiments described above) is amorphous overall (and is readily identifiable, for example, in TEM images). Typical products include 65 parts by mass of an epitaxial h-BN / BNNT structure and 35 parts by mass of residual boron and / or independent hexagonal boron nitride (typically containing less than 1 part by mass of independent hexagonal boron nitride).

[0119] Products according to the subject matter of the present invention exhibit numerous properties that make them useful in a variety of applications. For example, epitaxial h-BN / BNNT structures have a thicker and / or rougher exterior than the corresponding independent boron nitride nanotubes, thereby allowing the epitaxial h-BN / BNNT structures to readily adhere to matrix materials, i.e., provide enhanced physical / mechanical resistance to removal from the matrix material (Figure 3 shows a diagram of an epitaxial h-BN / BNNT structure).

[0120] In addition, epitaxial h-BN / BNNT structures provide nanonucleation sites for metal crystallization (e.g., when casting metals with melting points lower than the decomposition temperature of BNNTs, such as aluminum, magnesium, or titanium).

[0121] In addition, epitaxial h-BN / BNNT structures exhibit excellent properties after being subjected to extremely high temperatures (in some cases, hexagonal boron nitride can act as a sacrificial layer for the boron nitride structure it covers).

[0122] Several embodiments of epitaxial h-BN / BNNT structures according to the subject matter of the present invention provide any combination of the advantageous properties described above. Generally, increasing the proportion of hydrogen in the mixture of nitrogen and hydrogen supplied to port 20 of apparatus 10 (i.e., more than 4 weight percent) increases the amount of epitaxial hexagonal boron nitride structures formed, while decreasing the proportion of hydrogen in the mixture of nitrogen and hydrogen supplied to port 20 of apparatus 10 (i.e., less than 4 weight percent) decreases the amount of epitaxial hexagonal boron nitride structures formed. The subject matter of the present invention is not limited to any particular theory, but it is considered that the hydrogen supplied to the mixture supplied to port 20 provides energy that assists in the nucleation of hexagonal boron nitride structures on boron nitride nanotube structures.

[0123] The solid elemental boron powder, entrained with 0.1 to 10.0 liters of nitrogen gas per minute, is supplied to the color space through the reactant feed opening 24 (having a diameter of 1 / 16 inch), which is equivalent to a nitrogen gas flow rate of approximately 53.3 cm / sec to 5330 cm / sec. While the subject matter of the present invention is not limited to any particular theory, it is believed that this high nitrogen gas flow rate allows a significant amount of boron to pass unreacted through the region where the boron nitride nanotube structure is formed, thereby providing boron that can participate in the nucleation of hexagonal boron nitride on the thus formed boron nitride nanotube structure.

[0124] If a larger apparatus is used, the flow rate of nitrogen gas accompanied by the boron feed will be increased to compensate for the larger reaction zone through which unreacted hydrogen and boron pass. Similarly, if a larger flow rate of nitrogen and hydrogen is supplied to the plasma generator space 21 (e.g., in a larger apparatus), the power supplied to the electromagnetic wave generator 16 will be increased to be sufficient to ionize the nitrogen and hydrogen.

[0125] The subject matter of this invention is not limited to any particular theory, but it is thought that the contraction due to the reduction in the diameter of the plume opening creates the flow properties that result in the formation of epitaxial h-BN / BNNT structures. The diameter of the color space 23 is the first reaction chamber region Its smaller diameter compared to the larger diameter of 26 is also thought to contribute to (or provide) the flow properties that lead to the formation of epitaxial h-BN / BNNT structures.

[0126] The above-described representative embodiments of the method are: A composition (or aggregate) comprising a plurality of independent boron nitride nanotubes, according to a third aspect (or fourth aspect) of the subject matter of the present invention, wherein the sum of [1] the total mass of all independent hexagonal boron nitride in the composition (or aggregate) and [2] the total mass of all residual boron in the composition (or aggregate) accounts for 35% or less of the mass of the composition (or aggregate); A composition (or aggregate) according to a fifth aspect (or sixth aspect) of the subject matter of the present invention, comprising [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition (or aggregate) and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition (or aggregate), wherein 1% or less of the total comprises at least 10 independent boron nitride nanotubes having a length of at least 50 nm, wherein at least one defect selected from Dixie cup defects and bamboo defects; and / or, A composition (or aggregate) according to the seventh aspect (or eighth aspect) of the subject matter of the present invention, comprising [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition (or aggregate) and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition (or aggregate), wherein at least 50% of the total each comprises at least 10 independent boron nitride nanotubes that are monolayers, It can also be used to manufacture [something].

[0127] Therefore, in addition, the subject matter of the present invention is: [1] A composition (or aggregate) having advantageously high purity, for example, in which the sum of the total mass of all independent hexagonal boron nitride in the composition (or aggregate) and [2] the total mass of all residual boron in the composition (or aggregate) accounts for 35% or less of the mass of the composition (or aggregate); [1] A composition (or aggregate) having advantageously high quality, wherein the total of independent boron nitride nanotubes having a length of at least 50 nm in the composition (or aggregate) and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition (or aggregate), such that 1% or less of the total has at least one defect selected from Dixie cup defects and bamboo defects; and / or, [1] A composition (or aggregate) having a total of independent boron nitride nanotubes having a length of at least 50 nm in the composition (or aggregate) and [2] a total of boron nitride nanotube structures having a length of at least 50 nm in the composition (or aggregate), wherein each of the at least 50% of the total is a single layer, for example, a composition (or aggregate) having a favorably high percentage of single-layer independent boron nitride nanotubes and boron nitride nanotube structures, To provide.

[0128] Such compositions or aggregates may have any combination of the above-described advantageous features, or any of the above-described advantageous features of epitaxial h-BN / BNNT structures according to the subject matter of the present invention.

[0129] As described above, according to the ninth aspect of the subject matter of the present invention, a method for producing a composition is provided, the method being: A mixture of nitrogen gas and hydrogen gas is supplied to the first region of the chamber; Converting at least a portion of a mixture of nitrogen gas and hydrogen gas into a plasma; A mixture of at least one boron-containing material and nitrogen gas is supplied to a second region of the chamber, thereby bringing the mixture of at least one boron-containing material and nitrogen gas into contact with the plasma to form a reaction mixture; Converting at least a portion of the mixture into an epitaxial h-BN / BNNT structure, Includes.

[0130] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any of the other features described herein, the chamber is: The first domain; The second domain; At least a third area; A first connecting section providing a connection between the first region and the second region; and, A second connecting section that provides a link between the second and third regions, Equipped with, The first region has at least one first region cross-sectional area that is perpendicular to the axis of the chamber extending through the first region, the second region, and the third region, The second region has at least one second region cross-sectional area that is perpendicular to the axis of the chamber, The third region has at least one third region cross-sectional area that is perpendicular to the axis of the chamber, The first connection section has at least one first connection section cross-sectional area that is perpendicular to the axis of the chamber, The second connection section has at least one second connection section cross-sectional area that is perpendicular to the axis of the chamber, Each first connecting section cross-sectional area is smaller than the first region cross-sectional area and smaller than the second region cross-sectional area. Each second connecting section cross-sectional area is smaller than the third region cross-sectional area. Furthermore, in some of such embodiments: The pressure within at least a portion of the third region is at least 10 psi; The pressure within at least a portion of the third region is in the range of 10 to 20 psi; and / or, The pressure within at least a portion of the third region is in the range of 15-20 psi.

[0131] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any of the other features described herein as appropriate, the weight percentage of hydrogen gas in the mixture of nitrogen gas and hydrogen gas is in the range of 1 mass percent to 7 mass percent (in some embodiments, at least 2 mass percent, in some embodiments, in the range of 2 mass percent to 7 mass percent, in some embodiments, 4 mass percent or about 4.0 mass percent).

[0132] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the weight percentage of hydrogen gas in the mixture of nitrogen gas and hydrogen gas is at least 3 mass percent.

[0133] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the weight percentage of hydrogen gas in the mixture of nitrogen gas and hydrogen gas is at least 4 mass percent.

[0134] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, a mixture of nitrogen gas and hydrogen gas is supplied to the first area at a rate of at least 30 liters per minute.

[0135] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, a mixture of nitrogen gas and hydrogen gas is supplied to the first area at a rate of at least 40 liters per minute.

[0136] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, a mixture of nitrogen gas and hydrogen gas is supplied to the first area at a rate of at least 50 liters per minute.

[0137] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the supply of a mixture of at least one boron-containing material and nitrogen gas to a second region of the chamber includes supplying boron at a rate of at least 20 mg / min.

[0138] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the supply of a mixture of at least one boron-containing material and nitrogen gas to a second region of the chamber includes supplying boron at a rate in the range of 20 mg / min to 90 mg / min.

[0139] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the supply of a mixture of at least one boron-containing material and nitrogen gas to a second region of the chamber includes supplying the nitrogen gas at a rate in the range of 0.1 liters per minute to 1.3 liters per minute.

[0140] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the supply of a mixture of at least one boron-containing material and nitrogen gas to a second region of the chamber includes supplying the nitrogen gas at a rate in the range of 1.3 liters per minute to 8.4 liters per minute.

[0141] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the conversion of at least a portion of a mixture of nitrogen gas and hydrogen gas into a plasma includes generating electromagnetic waves in a first region.

[0142] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the generation of electromagnetic waves includes supplying high-frequency energy to an electromagnetic wave generator at a power rate of at least 35 kW (35 to 45 kW in some embodiments).

[0143] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the generation of electromagnetic waves includes supplying high-frequency energy to an electromagnetic wave generator at an energy of at least 39 (39 to 45 kW in some embodiments).

[0144] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any of the other features described herein, the pressure in at least a portion of the chamber is at least 10 psi.

[0145] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the pressure in at least a portion of the chamber is in the range of 10 to 20 psi.

[0146] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the pressure in at least a portion of the chamber is in the range of 15 to 20 psi.

[0147] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any of the other features described herein, the method further comprises contacting at least some of the epitaxial h-BN / BNNT structures with nitric acid. In some such embodiments, the method further includes exposing at least some of the epitaxial h-BN / BNNT structures to a temperature in the range of 700 to 900°C.

[0148] In some embodiments according to the ninth aspect of the subject matter of the present invention, which may or may not include any other features described herein, the method further includes exposing at least some of the epitaxial h-BN / BNNT structures to a temperature in the range of 700 to 900°C.

[0149] Example 1 A mixture of nitrogen and hydrogen (96 parts by mass of nitrogen and 4 parts by mass of hydrogen) was supplied at a rate of 50 liters per minute to the plasma generator space of the apparatus shown in Figure 1 (through a port). The apparatus is further characterized by a plasma generator outer diameter of 3.5 inches, a plasma generator inner diameter of 2.0 inches, a plasma generator length of 10.0 inches, a color region outer diameter of 3.5 inches, a color region inner diameter of 1.40 inches, a color region length of 3.0 inches, a plume opening (connecting section between the plasma generator space and the color space) diameter of 1.38 inches, a reactant feed opening located midway along the length of the color region, a first reaction vessel section inner diameter of 8.0 inches, a first reaction vessel section length of 24 inches, a second reaction vessel section inner diameter of 8.0 inches, a second reaction vessel section length of 24 inches, and a reactant feed opening diameter of 1 / 16 inch. By supplying 39kW to the electromagnetic wave generator, nitrogen and hydrogen in the plasma generator space are ionized. Into the color space, 22 mg / min of solid elemental boron powder (at room temperature before being introduced into the apparatus) is supplied entrained with 1.3 liters / min of nitrogen gas through the reactant feed opening. The pressure in the first and second reaction vessel sections was maintained within the range of 15 psi to 20 psi (i.e., the pressure fluctuated within this range), and the temperature in at least part of the color region was approximately 8000 K.

[0150] Figure 4 is a TEM image of a representative portion of the product from Example 1, where approximately 30% of each of the boron nitride nanotube structures was covered by at least 30% epitaxial hexagonal boron nitride.

[0151] Over 50% of the total number of independent boron nitride nanotubes and boron nitride nanotube structures were monolayers, while the remainder were bilayers and multilayers. Less than 1% of the total number of independent boron nitride nanotubes and boron nitride nanotube structures had Dixie cup defects or bamboo defects.

[0152] The total mass of residual boron and independent hexagonal boron nitride was less than 35% by mass of the product. Example 2 A mixture of nitrogen and hydrogen (96 parts by mass of nitrogen and 4 parts by mass of hydrogen) is dispensed at a rate of 50 liters per minute. The plasma is supplied (through the port) to the plasma generator space of the same device used in Example 1. By supplying 39kW to the electromagnetic wave generator, nitrogen and hydrogen in the plasma generator space are ionized. Into the color space, 22 mg / min of solid elemental boron powder (at room temperature before being introduced into the apparatus) is supplied entrained with 8.4 liters / min of nitrogen gas through the reactant feed opening. The pressure in the first and second reaction vessel sections was maintained within the range of 15 psi to 20 psi (i.e., the pressure fluctuated within this range), and the temperature in at least part of the color region was approximately 8000 K.

[0153] Figure 5 is a TEM image of a representative portion of the product from Example 2, where approximately 90% of each of the boron nitride nanotube structures was covered by at least 30% epitaxial hexagonal boron nitride.

[0154] Figure 6 is a TEM image of a portion of the product from Example 2, which shows the epitaxial h-BN / BNNT structure. In the TEM image of Figure 6, the label 61 indicates an example of high-purity and high-quality boron nitride nanotubes.

[0155] In the TEM image of Figure 6, the symbol 62 indicates an example of unreacted amorphous boron. In the TEM image of Figure 6, labels 63, 64, and 65 refer to examples of epitaxial h-BN / BNNT structures.

[0156] Figure 7 is a TEM image of a portion of the product from Example 2, which shows independent hexagonal boron nitride and epitaxial h-BN / BNNT structures (one of which contains a clump of boron nitride nanotube structure).

[0157] In the TEM image of Figure 7, the label 71 refers to an example of an independent hexagonal boron nitride structure. In the TEM image of Figure 7, the label 72 refers to an example of an epitaxial h-BN / BNNT structure (containing a mass of boron nitride nanotube structures).

[0158] In the TEM image of Figure 7, the label 73 refers to an example of an epitaxial h-BN / BNNT structure (containing a single boron nitride nanotube structure). In the TEM image of Figure 7, the label 74 refers to an example of an epitaxial h-BN / BNNT structure (containing a cluster of two boron nitride nanotube structures).

[0159] Figure 8 is a TEM image of a portion of the product from Example 2, which shows clumps of boron nitride nanotube structures and epitaxial h-BN / BNNT structures. In the TEM image of Figure 8, the label 81 indicates an example of an independent clump of boron nitride nanotubes (i.e., a clump of epitaxial hexagonal boron nitride without nucleation or growth).

[0160] In the TEM image of Figure 8, the label 82 indicates an example of an epitaxial h-BN / BNNT structure (which contains boron nitride nucleation on the side of a bundle of boron nitride nanotube structures).

[0161] Figure 9 is a TEM image of a portion of the product from Example 2, which shows the epitaxial h-BN / BNNT structure. In the TEM image of Figure 9, the label 91 refers to an example of an epitaxial h-BN / BNNT structure (containing a single boron nitride nanotube structure).

[0162] In the TEM image of Figure 9, the label 92 refers to an example of an epitaxial h-BN / BNNT structure (containing a mass of boron nitride nanotube structures). Figure 10 is a TEM image of a portion of the product from Example 2, which shows the residual boron and epitaxial h-BN / BNNT structure.

[0163] In the TEM image of Figure 10, labels 101 and 102 indicate examples of residual amorphous boron. In the TEM image of Figure 10, the label 103 refers to an example of an epitaxial h-BN / BNNT structure.

[0164] In the TEM image of Figure 10, the label 104 refers to an example of an epitaxial h-BN / BNNT structure (containing a mass of boron nitride nanotube structures). Figure 11 is a TEM image of a portion of the product from Example 2, which shows the residual boron and epitaxial h-BN / BNNT structure.

[0165] In the TEM image of Figure 11, labels 111 and 112 indicate examples of residual amorphous boron. In the TEM image of Figure 11, labels 113 and 114 refer to examples of epitaxial h-BN / BNNT structures.

[0166] Figure 12 is a TEM image of a portion of the product from Example 2, which shows the epitaxial h-BN / BNNT structure. In the TEM image of Figure 12, labels 121 and 122 refer to examples of epitaxial h-BN / BNNT structures.

[0167] Over 50% of the total number of independent boron nitride nanotubes and boron nitride nanotube structures were monolayers, while the remainder were bilayers and multilayers. Less than 1% of the total number of independent boron nitride nanotubes and boron nitride nanotube structures had Dixie cup defects or bamboo defects.

[0168] The total mass of residual boron and independent hexagonal boron nitride was less than 35% by mass of the product. Figure 13 shows a TEM image of an independent boron nitride nanotube.

[0169] The following is a series of numbered sections, each defining a subject that falls within the scope of the present invention. Section 1. At least one epitaxial h-BN / BNNT structure, Includes, The first epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure and at least a first hexagonal boron nitride structure, The first hexagonal boron nitride structure is epitaxial with respect to the first boron nitride nanotube structure. composition.

[0170] Section 2.[1] The sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition is at least 10. [1] an amount of boron nitride nanotube structures that is at least 10% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] an amount of boron nitride nanotube structures having a length of at least 50 nm in the composition. hand: The boron nitride nanotube structure has a length of at least 50 nm, and at least 10% of the total outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. The composition described in Section 1.

[0171] Section 3. For each of the boron nitride nanotube structures in an amount that is at least 30% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition: The boron nitride nanotube structure has a length of at least 50 nm, and at least 30% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. The composition described in Section 2.

[0172] Section 4. For each boron nitride nanotube structure in an amount that is at least 80% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition: The boron nitride nanotube structure has a length of at least 50 nm, and at least 30% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. The composition described in Section 2.

[0173] Section 5. The sum of the amounts of each of [1] independent boron nitride nanotube clumps having a length of at least 50 nm in the composition, [2] boron nitride nanotube structure clumps having a length of at least 50 nm in the composition, [3] boron nitride nanotube structure / independent boron nitride nanotube clumps having a length of at least 50 nm in the composition, [4] independent boron nitride nanotubes having a length of at least 50 nm, not clumps, in the composition, and [5] boron nitride nanotube structures having a length of at least 50 nm, not clumps, in the composition is at least 10. [2] for each of the boron nitride nanotube structure aggregates having a length of at least 50 nm in the composition, [3] for each of the boron nitride nanotube structure / independent boron nitride nanotube aggregates having a length of at least 50 nm in the composition, and [5] for each of the boron nitride nanotube structure aggregates having a length of at least 50 nm, not aggregates, that constitute at least 30% of the total: [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, in which each boron nitride nanotube structure is covered by an epitaxial hexagonal boron nitride structure. The composition described in Section 1.

[0174] Section 6.[2] For each of the boron nitride nanotube structure aggregates having a length of at least 50 nm in the composition, [3] boron nitride nanotube structure / independent boron nitride nanotube aggregates having a length of at least 50 nm in the composition, and [5] boron nitride nanotube structure in the composition, not as aggregates, having a length of at least 50 nm, in an amount that is at least 30% of the total: [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 30% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, in which each boron nitride nanotube structure is covered by an epitaxial hexagonal boron nitride structure. The composition described in Section 5.

[0175] Section 7.[2] For each of the boron nitride nanotube structure aggregates having a length of at least 50 nm in the composition, [3] boron nitride nanotube structure / independent boron nitride nanotube aggregates having a length of at least 50 nm in the composition, and [5] boron nitride nanotube structure in the composition, not as aggregates, having a length of at least 50 nm, in an amount that is at least 80% of the total: [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 30% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, in which each boron nitride nanotube structure is covered by an epitaxial hexagonal boron nitride structure. The composition described in Section 5.

[0176] Section 8. A single integrated structure comprising at least a first epitaxial h-BN / BNNT structure, The first epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure and at least a first hexagonal boron nitride structure, The first hexagonal boron nitride structure is epitaxial with respect to the boron nitride nanotube structure. The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. Aggregates.

[0177] Section 9.[1] For each boron nitride nanotube structure in the integral structure, the amount is at least 10% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] the amount of boron nitride nanotube structures having a length of at least 50 nm in the integral structure: At least 10% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. Aggregates as described in Section 8.

[0178] Section 10.[1] For each boron nitride nanotube structure in the integral structure, the amount is at least 30% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] the amount of boron nitride nanotube structures having a length of at least 50 nm in the integral structure: At least 30% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. Aggregates as described in Section 9.

[0179] Section 11. For each boron nitride nanotube structure in the integral structure, in an amount that is at least 80% of the sum of [1] the amount of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] the amount of boron nitride nanotube structures having a length of at least 50 nm in the integral structure: At least 30% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. Aggregates as described in Section 9.

[0180] Section 12.[2] A boron nitride nanotube structure having a length of at least 50 nm in an integral structure, [3] A boron nitride nanotube structure having a length of at least 50 nm in an integral structure / an independent boron nitride nanotube structure, and [5] A boron nitride nanotube structure having a length of at least 50 nm, not as a structure, For each of the following amounts, the sum of the amounts of: [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the integral structure; [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [4] independent boron nitride nanotubes in the integral structure that are not clusters and have a length of at least 50 nm; and [5] boron nitride nanotube structures in the integral structure that are not clusters and have a length of at least 50 nm: [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, in which each boron nitride nanotube structure is covered by an epitaxial hexagonal boron nitride structure. Aggregates as described in Section 8.

[0181] Section 13.[2] A boron nitride nanotube structure mass having a length of at least 50 nm in a single structure,[3] A boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in a single structure, and[5] A boron nitride nanotube structure having a length of at least 50 nm, not a mass, For each of the following amounts, the sum of the amounts of: [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the integral structure; [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [4] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure (not clusters); and [5] boron nitride nanotube structures having a length of at least 50 nm in the integral structure (not clusters): [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 30% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, in which each boron nitride nanotube structure is covered by an epitaxial hexagonal boron nitride structure. Aggregates as described in Section 12.

[0182] Section 14.[2] A boron nitride nanotube structure having a length of at least 50 nm in a single structure, [3] A boron nitride nanotube structure having a length of at least 50 nm in a single structure / an independent boron nitride nanotube structure, and [5] A boron nitride nanotube structure having a length of at least 50 nm, not as a cluster, For each of the following amounts, the sum of the amounts of: [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the integral structure; [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [4] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure (not clusters); and [5] boron nitride nanotube structures having a length of at least 50 nm in the integral structure (not clusters): [2] Boron nitride nanotube structure clumps, [3] Boron nitride nanotube structure / independent boron nitride nanotube clumps, or [5] At least 30% of the total external atoms of a boron nitride nanotube structure that is not a clump, [2] a boron nitride nanotube structure mass, [3] a boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] a boron nitride nanotube structure that is not a mass, in which each boron nitride nanotube structure is covered by an epitaxial hexagonal boron nitride structure. Aggregates as described in Section 12.

[0183] Section 15. Compositions: Multiple independent boron nitride nanotubes, Includes, [1] The sum of the total mass of all independent hexagonal boron nitride in the composition and [2] the total mass of all residual boron in the composition is 35% or less of the total mass of the composition. composition.

[0184] Section 16.[1] The composition according to Section 15, wherein the sum of the total mass of all independent hexagonal boron nitrides in the composition and [2] the total mass of all residual boron in the composition accounts for 25% or less of the mass of the composition.

[0185] Section 17. Integrated structure containing multiple independent boron nitride nanotubes, Includes, The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. [1] The total mass of the independent hexagonal boron nitride in the integral structure and [2] the total mass of all residual boron in the integral structure together account for 35% or less of the total mass of the integral structure. Aggregates.

[0186] Section 18.[1] The aggregate described in Section 17, wherein the sum of the total mass of all independent hexagonal boron nitrides in the aggregate and [2] the total mass of all residual boron in the aggregate accounts for 25% or less of the mass of the aggregate.

[0187] Section 19. Compositions: At least 10 independent boron nitride nanotubes having a length of at least 50 nm, Includes, [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the composition, 1% or less of the total is selected from Dixie cup defects and bamboo defects. Having at least one of the selected defects, composition.

[0188] Section 20. Integrated structure containing multiple independent boron nitride nanotubes, Includes, The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. [1] Independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] In the total of boron nitride nanotube structures having a length of at least 50 nm in the integral structure, 1% or less of the total have at least one defect selected from Dixie cup defects and bamboo defects. Aggregates.

[0189] Section 21. Compositions: At least 10 independent boron nitride nanotubes, Includes, [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the composition, each of at least 50% of the total is a single layer. composition.

[0190] Section 22. The composition according to Section 21, wherein at least a portion of the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition, each of which is a single layer, is present in an independent boron nitride nanotube mass, a boron nitride nanotube structure mass, or a boron nitride nanotube structure / independent boron nitride nanotube mass.

[0191] Section 23. The composition according to Section 21, wherein of the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition, each of the 50 to 60 percent of the total is a single layer.

[0192] Section 24. A monolithic structure containing at least one independent boron nitride nanotube, Includes, The integrated structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. [1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and [2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the integral structure, each of at least 50% of the total is a single layer. Aggregates.

[0193] Section 25. The aggregate according to Section 24, wherein at least a portion of the sum of [1] independent boron nitride nanotubes having a length of at least 50 nm in an integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in an integral structure, each of which is a single layer, is present in an independent boron nitride nanotube mass, a boron nitride nanotube structure mass, or a boron nitride nanotube structure / independent boron nitride nanotube mass.

[0194] Section 26.[1] In the total of independent boron nitride nanotubes having a length of at least 50 nm in the integral structure and[2] in the total of boron nitride nanotube structures having a length of at least 50 nm in the integral structure, each of the 50-60 percent of the total is monolayer. , aggregates as described in Section 24.

[0195] Section 27. The composition according to any one of Sections 1 to 7, 19, and 21, wherein the combined mass of epitaxial h-BN / BNNT structures in the composition accounts for at least 65% of the mass of the composition.

[0196] Section 28. The composition according to Section 27, wherein the combined mass of epitaxial h-BN / BNNT structures in the composition accounts for at least 75% of the mass of the composition. Section 29. An aggregate according to any one of Sections 8-14, 20, and 24, wherein the combined mass of the epitaxial h-BN / BNNT structures in the composition accounts for at least 65% of the mass of the integral structure.

[0197] Section 30. The aggregate according to Section 29, wherein the combined mass of the epitaxial h-BN / BNNT structures in the composition accounts for at least 75% of the mass of the integral structure. Section 31. The composition according to any one of Sections 1-7, 15, 16, 19, 21-23, 27, and 28, wherein at least 10% by mass of the composition comprises hexagonal boron nitride structures, each of which is epitaxial with respect to boron nitride nanotube structures.

[0198] Aggregate according to any one of paragraphs 8 - 14, 17, 18, 20, 24 - 26, 29, and 30, comprising a hexagonal boron nitride structure in which at least 10% by mass of the monolithic structure is epitaxial with respect to the boron nitride nanotube structure respectively.

[0199] Composition according to any one of paragraphs 1 - 7, 15, 16, 19, 21 - 23, 27, 28, and 31, wherein for each of at least 10% of the atoms in the composition, the atoms are present in a hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotube structure in the composition.

[0200] Aggregate according to any one of paragraphs 8 - 14, 17, 18, 20, 24 - 26, 29, 30, and 32, wherein for each of at least 10% of the atoms in the monolithic structure, the atoms are present in a hexagonal boron nitride structure that is epitaxial with respect to the boron nitride nanotube structure in the composition.

[0201] Composition according to any one of paragraphs 1 - 7, 27, 28, 31, and 33, wherein the total of [1] the combined mass of all independent hexagonal boron nitrides in the composition and [2] the combined mass of all amorphous boron in the composition occupies less than 35% of the mass of the composition.

[0202] Aggregate according to any one of paragraphs 8 - 14, 29, 30, 32, and 34, wherein the total of [1] the combined mass of all independent hexagonal boron nitrides in the monolithic structure and [2] the combined mass of all amorphous boron in the monolithic structure occupies less than 35% of the mass of the monolithic structure.

[0203] Composition according to any one of paragraphs 1 - 7, 15, 16, 27, 28, 31, 33, and 35, wherein in the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition, 1% or less of the total has at least one defect selected from a Dixie cup defect and a bamboo defect.

[0204] Section 38. [1] Independent boron nitride nanotubes having a length of at least 50 nm in an integral structure and [2] Boron nitride nanotubes having a length of at least 50 nm in an integral structure The aggregate according to any one of sections 8-14, 17, 18, 29, 30, 32, 34, and 36, wherein, in total with respect to the tubular structure, 1% or less of the total has at least one defect selected from Dixie cup defects and bamboo defects.

[0205] Section 39.[1] A composition according to any one of Sections 1-7, 15, 16, 19, 27, 28, 31, 33, 35, and 37, wherein in the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] boron nitride nanotube structures having a length of at least 50 nm in the composition, each of the at least 50 percent of the total is a single layer.

[0206] Section 40. An aggregate according to any one of Sections 8-14, 17, 18, 20, 29, 30, 32, 34, 36, and 38, wherein in the total of [1] independent boron nitride nanotubes having a length of at least 50 nm in an integral structure and [2] boron nitride nanotube structures having a length of at least 50 nm in an integral structure, each of the at least 50 percent of the total is a single layer.

[0207] Section 41. A composition according to any one of Sections 15, 16, 27, 28, 31, 33, 35, 37, and 39, wherein independent hexagonal boron nitride accounts for 1 mass percent or less of the composition.

[0208] Section 42. An aggregate according to any one of Sections 17, 18, 29, 30, 32, 34, 36, 38, and 40, wherein independent hexagonal boron nitride accounts for 1 mass percent or less of the aggregate.

[0209] Section 43. A method for producing a composition: A mixture of nitrogen gas and hydrogen gas is supplied to the first region of the chamber; Converting at least a portion of a mixture of nitrogen gas and hydrogen gas into a plasma; A mixture of at least one boron-containing material and nitrogen gas is supplied to a second region of the chamber, thereby bringing the mixture of at least one boron-containing material and nitrogen gas into contact with the plasma to form a reaction mixture; Converting at least a portion of the mixture into an epitaxial h-BN / BNNT structure, Methods that include...

[0210] Section 44. Chamber: The first domain; The second domain; At least a third area; A first connecting section providing a connection between the first region and the second region; and, A second connecting section that provides a link between the second and third regions, Equipped with, The first region has at least one first region cross-sectional area that is perpendicular to the axis of the chamber extending through the first region, the second region, and the third region, The second region has at least one second region cross-sectional area that is perpendicular to the axis of the chamber, The third region has at least one third region cross-sectional area that is perpendicular to the axis of the chamber, The first connection section has at least one first connection section cross-sectional area that is perpendicular to the axis of the chamber, The second connection section is at least one second perpendicular to the axis of the chamber Having a connection speed cross-sectional area, Each first connecting section cross-sectional area is smaller than the first region cross-sectional area and smaller than the second region cross-sectional area. Each second connecting section cross-sectional area is smaller than the third region cross-sectional area. The method described in Section 43.

[0211] The method according to section 44, wherein the pressure in at least a portion of the third region is at least 10 psi. The method according to section 44, wherein the pressure in at least a portion of the third region is within the range of 10 to 20 psi.

[0212] The method according to section 44, wherein the pressure in at least a portion of the third region is within the range of 15 to 20 psi. The method according to any one of sections 43 to 47, wherein the weight percentage of hydrogen gas in the mixture of nitrogen gas and hydrogen gas is at least 2 mass percent.

[0213] The method according to any one of sections 43 to 47, wherein the weight percentage of hydrogen gas in the mixture of nitrogen gas and hydrogen gas is at least 3 mass percent. The method according to any one of sections 43 to 47, wherein the weight percentage of hydrogen gas in the mixture of nitrogen gas and hydrogen gas is at least 4 mass percent.

[0214] The method according to any one of sections 43 to 50, wherein the mixture of nitrogen gas and hydrogen gas is supplied to the first region in an amount of at least 30 liters per minute. The method according to any one of sections 43 to 50, wherein the mixture of nitrogen gas and hydrogen gas is supplied to the first region in an amount of at least 40 liters per minute.

[0215] The method according to any one of sections 43 to 50, wherein the mixture of nitrogen gas and hydrogen gas is supplied to the first region in an amount of at least 50 liters per minute. The method according to any one of sections 43 to 53, wherein the supply of the mixture of at least one boron-containing material and nitrogen gas to the second region of the chamber includes supplying boron at a rate of at least 20 mg / min.

[0216] Section 55. The method according to any one of Sections 43 to 53, wherein the supply of a mixture of at least one boron-containing material and nitrogen gas to a second region of a chamber is the supply of boron at a rate in the range of 20 mg / min to 90 mg / min.

[0217] Section 56. The method according to any one of Sections 43 to 55, wherein the supply of a mixture of at least one boron-containing material and nitrogen gas to a second region of a chamber comprises supplying nitrogen gas at a rate in the range of 0.1 liters per minute to 1.3 liters per minute.

[0218] Section 57. The method according to any one of Sections 43 to 55, wherein the supply of a mixture of at least one boron-containing material and nitrogen gas to a second region of a chamber comprises supplying nitrogen gas at a rate in the range of 1.3 liters per minute to 8.4 liters per minute.

[0219] Section 58. The method according to any one of Sections 43 to 57, wherein the conversion of at least a portion of a mixture of nitrogen gas and hydrogen gas into a plasma comprises generating electromagnetic waves in a first region.

[0220] Section 59. The method according to Section 58, wherein the generation of electromagnetic waves includes supplying high-frequency energy to an electromagnetic wave generator at an electrical energy of at least 35 kW. Section 60. The method according to Section 58, wherein the generation of electromagnetic waves includes supplying high-frequency energy to an electromagnetic wave generator with an electrical energy of at least 39 kW.

[0221] Section 61. The method according to any one of Sections 43 to 60, wherein the method further comprises contacting at least some of the epitaxial h-BN / BNNT structures with nitric acid. Section 62. The method according to any one of Sections 43 to 61, further comprising exposing at least some of the epitaxial h-BN / BNNT structures to a temperature in the range of 700 to 900°C.

Claims

1. A composition comprising an epitaxial h-BN / BNNT structure, The epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure and at least a first hexagonal boron nitride structure. Here, [1] The sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the sum of the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition is at least 10. For each of the boron nitride nanotube structures in an amount that is at least 10% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition, The boron nitride nanotube structure has a length of at least 50 nm, and at least 10% of the total outermost wall of the boron nitride nanotube structure is covered by a hexagonal boron nitride structure. composition.

2. For each of the boron nitride nanotube structures in an amount that is at least 30% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition, The boron nitride nanotube structure has a length of at least 50 nm, and at least 30% of the outermost wall of the boron nitride nanotube structure is covered by a hexagonal boron nitride structure. The composition according to claim 1.

3. For each of the boron nitride nanotube structures, the amount is at least 80% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition. The boron nitride nanotube structure has a length of at least 50 nm, and at least 30% of the outermost wall of the boron nitride nanotube structure is covered by a hexagonal boron nitride structure. The composition according to claim 1.

4. The total amount of each of the following is at least 10: [1] an independent boron nitride nanotube mass having a length of at least 50 nm in the composition, [2] an independent boron nitride nanotube structure mass having a length of at least 50 nm in the composition, [3] an independent boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in the composition, [4] an independent boron nitride nanotube having a length of at least 50 nm, not an aggregate, in the composition, and [5] an independent boron nitride nanotube structure having a length of at least 50 nm, not an aggregate, in the composition. [2] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition, [3] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition / independent boron nitride nanotube lumps, and [5] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition, in an amount that is at least 30% of the total, [2] A boron nitride nanotube structure mass, [3] A boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] A boron nitride nanotube structure that is not a mass, in which at least 10% of the total external atoms are covered by a hexagonal boron nitride structure. The composition according to any one of claims 1 to 3.

5. An aggregate comprising an integral structure comprising a composition comprising the epitaxial h-BN / BNNT structure described in claim 1, The aforementioned integral structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. Aggregates.

6. [2] A boron nitride nanotube structure mass having a length of at least 50 nm in an integral structure, [3] A boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in an integral structure, and [5] A boron nitride nanotube structure having a length of at least 50 nm, not a mass, For each of the following amounts, the amount is at least 10% of the sum of the amounts of: [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the integral structure; [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [4] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure, not as clusters; and [5] boron nitride nanotube structures having a length of at least 50 nm in the integral structure, not as clusters: [2] Boron nitride nanotube structure aggregate, [3] Boron nitride nanotube structure / independent boron nitride nanotube aggregate, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not an aggregate, [2] Boron nitride nanotube structure mass, [3] Boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] Boron nitride nanotube structure that is not a mass, covered by a hexagonal boron nitride structure within it. The aggregate according to claim 5.

7. Epitaxial h-BN / BNNT structure, and At least one metal, A composition comprising, The epitaxial h-BN / BNNT structure comprises at least a first boron nitride nanotube structure and at least a first hexagonal boron nitride structure. The first hexagonal boron nitride structure is epitaxial with respect to the first boron nitride nanotube structure. Here, the atoms in the first hexagonal boron nitride structure are epitaxially arranged with respect to the atoms in the first boron nitride nanotube structure that are closest to the first hexagonal boron nitride structure. The at least one of the metals is bonded to the epitaxial h-BN / BNNT structure. composition.

8. The composition according to claim 7, wherein the at least one metal comprises at least one atom selected from aluminum, magnesium, and titanium.

9. [1] The sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the sum of the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition is at least 10. For each of the boron nitride nanotube structures in an amount that is at least 10% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition, The boron nitride nanotube structure has a length of at least 50 nm, and at least 10% of the total outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. The composition according to claim 7 or 8.

10. [1] The sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the sum of the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition is at least 10. For each of the boron nitride nanotube structures in an amount that is at least 30% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition, The boron nitride nanotube structure has a length of at least 50 nm, and at least 30% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. The composition according to claim 7 or 8.

11. The total amount of each of the following is at least 10: [1] an independent boron nitride nanotube mass having a length of at least 50 nm in the composition, [2] an independent boron nitride nanotube structure mass having a length of at least 50 nm in the composition, [3] an independent boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in the composition, [4] an independent boron nitride nanotube having a length of at least 50 nm, not an aggregate, in the composition, and [5] an independent boron nitride nanotube structure having a length of at least 50 nm, not an aggregate, in the composition. [2] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition, [3] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition / independent boron nitride nanotube lumps, and [5] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition, in an amount that is at least 30% of the total, [2] Boron nitride nanotube structure aggregate, [3] Boron nitride nanotube structure / independent boron nitride nanotube aggregate, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not an aggregate, [2] The boron nitride nanotube structure mass, [3] The boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] The boron nitride nanotube structure in the boron nitride nanotube structure that is not the mass, each covered by an epitaxial hexagonal boron nitride structure. The composition according to any one of claims 7 to 10.

12. An aggregate comprising a composition comprising at least a first integral structure comprising a composition comprising an epitaxial h-BN / BNNT structure according to any one of claims 7 to 11, The aforementioned integral structure has a first dimension of at least 100 nm and a second dimension of at least 100 nm, the second dimension being perpendicular to the first dimension. Aggregates.

13. [2] A boron nitride nanotube structure mass having a length of at least 50 nm in an integral structure, [3] A boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in an integral structure, and [5] A boron nitride nanotube structure having a length of at least 50 nm, not a mass, For each of the following amounts, the amount is at least 10% of the sum of the amounts of: [1] independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [2] boron nitride nanotube structure clusters having a length of at least 50 nm in the integral structure; [3] boron nitride nanotube structure / independent boron nitride nanotube clusters having a length of at least 50 nm in the integral structure; [4] independent boron nitride nanotubes having a length of at least 50 nm in the integral structure, not as clusters; and [5] boron nitride nanotube structures having a length of at least 50 nm in the integral structure, not as clusters: [2] Boron nitride nanotube structure aggregate, [3] Boron nitride nanotube structure / independent boron nitride nanotube aggregate, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not an aggregate, [2] Boron nitride nanotube structure mass, [3] Boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] Boron nitride nanotube structure that is not a mass, covered by a hexagonal boron nitride structure within it. The aggregate according to claim 12.

14. A material comprising at least a first hexagonal boron nitride structure and at least a first boron nitride nanotube structure, The atoms in the first hexagonal boron nitride structure are epitaxially aligned with respect to the atoms in the first boron nitride nanotube structure that are closest to the first hexagonal boron nitride structure. material.

15. [1] The sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the sum of the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition is at least 10. For each of the boron nitride nanotube structures in an amount that is at least 10% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition, The boron nitride nanotube structure has a length of at least 50 nm, and at least 10% of the total outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. The composition according to claim 14.

16. [1] The sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and [2] the sum of the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition is at least 10. For each of the boron nitride nanotube structures in an amount that is at least 30% of the sum of the amount of independent boron nitride nanotubes having a length of at least 50 nm in the composition and the amount of boron nitride nanotube structures having a length of at least 50 nm in the composition, The boron nitride nanotube structure has a length of at least 50 nm, and at least 30% of the outermost wall of the boron nitride nanotube structure is covered by hexagonal boron nitride structures, each of which is epitaxial with respect to the boron nitride nanotube structure. The composition according to claim 14.

17. The total amount of each of the following is at least 10: [1] an independent boron nitride nanotube mass having a length of at least 50 nm in the composition, [2] an independent boron nitride nanotube structure mass having a length of at least 50 nm in the composition, [3] an independent boron nitride nanotube structure / independent boron nitride nanotube mass having a length of at least 50 nm in the composition, [4] an independent boron nitride nanotube having a length of at least 50 nm, not an aggregate, in the composition, and [5] an independent boron nitride nanotube structure having a length of at least 50 nm, not an aggregate, in the composition. [2] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition, [3] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition / independent boron nitride nanotube lumps, and [5] Bolts of boron nitride nanotube structures having a length of at least 50 nm in the composition, in an amount that is at least 30% of the total, [2] Boron nitride nanotube structure aggregate, [3] Boron nitride nanotube structure / independent boron nitride nanotube aggregate, or [5] At least 10% of the total external atoms of a boron nitride nanotube structure that is not an aggregate, [2] The boron nitride nanotube structure mass, [3] The boron nitride nanotube structure / independent boron nitride nanotube mass, or [5] The boron nitride nanotube structure in the boron nitride nanotube structure that is not the mass, each covered by an epitaxial hexagonal boron nitride structure. The composition according to any one of claims 14 to 16.

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