Method for producing carbonaceous material and carbonaceous material

Abstract

To provide a method for simply producing a material containing carbon substance whose structure is precisely controlled under mild conditions, and a material containing carbon substance in which a carbon substance and an inorganic substance are covalently bonded.SOLUTION: A method for producing a material containing a carbon substance includes a heating step (I) of heating a composition containing a compound (A) and an inorganic substance in which a condensation reaction between the same molecules and / or different molecules is induced by heating. A heating temperature in the heating step (I) is (T-150)°C or more where the condensation reaction temperature of the compound (A) is T°C. The material containing carbon substance is a carbon substance containing material containing a carbon substance and an inorganic substance. At least a part of the carbon substance is covalently bonded to at least a part of the inorganic substance.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] The present invention relates to a method for producing a carbonaceous material and the carbonaceous material. [Background technology]

[0002] In light of recent trends toward resource and energy conservation, lightweight carbon materials have been developed and are being used in various fields. Carbon-containing materials such as carbon-coated inorganic particles and hollow carbon microparticles have been reported as compounds containing such lightweight carbon materials that are useful in various fields (e.g., Patent Documents 1 to 4, Non-Patent Documents 1 to 4). Activated carbon and carbon black are also known as industrially produced carbon-containing materials.

[0003] However, conventional carbon-containing materials such as carbon-coated inorganic particles and hollow carbon microparticles must be produced by forming a carbon material film on the surface of inorganic particles to be carbon-coated or microparticles that form the base of the hollow structure through a gas-phase reaction, a high-temperature deposition reaction, or the like, making them difficult to apply to industrial production that involves mass production at low cost.

[0004] Furthermore, the above-mentioned carbon-containing materials, including industrially produced activated carbon and carbon black, have various functional groups. Therefore, it is difficult to precisely control the structure of the carbon-containing material, which results in a problem of variations in physical properties. In recent years, there has been a demand for carbon-containing materials that can reliably exhibit targeted physical properties, and therefore, there is a demand for the development of carbon-containing materials with precisely controlled structures. [Prior art documents] [Patent documents]

[0005] [Patent Document 1] Japanese Patent Application Publication No. 7-187849 [Patent Document 2] Japanese Patent Application Publication No. 7-267618 [Patent Document 3] Japanese Patent Application Laid-Open No. 2005-281065 [Patent Document 4] Japanese Patent Application Laid-Open No. 2010-168251 [Non-patent literature]

[0006] [Non-Patent Document 1] Dawei Pan et.al., Langmuir, 22, 5872-5876(2006) [Non-patent document 2] V.Ruiz et.al., Electrochemistry Communications, 24, 35-38(2012) [Non-patent document 3] H.Nishihara et.al., Adv.Funct.Mater., 26, 6418-6427(2016) [Non-patent document 4] Riichiro Saito, "Graphene's Cutting-Edge Technology and Expanding Applications", Chapter 2. Fundamental Properties of Graphene, 3. Optoelectronic Properties of Graphene Summary of the Invention [Problem to be solved by the invention]

[0007] An object of the present invention is to provide a method for easily producing a carbonaceous material that is soluble in a solvent or a carbonaceous material that has a precisely controlled structure under mild conditions, and to provide a carbonaceous material in which a carbonaceous material and an inorganic substance are bonded by a covalent bond. [Means for solving the problem]

[0008] The method for producing a carbon material-containing material of the present invention includes the steps of: A method for producing a carbonaceous material, comprising: The method includes a heating step (I) of heating a composition containing a compound (A) that undergoes a condensation reaction between identical molecules and / or different molecules by heating, and an inorganic substance; The heating temperature in the heating step (I) is (T-150)°C or higher when the condensation reaction temperature of the compound (A) is T°C. However, the condensation reaction temperature T in this specification means the condensation reaction temperature in the absence of a catalyst (support).

[0009] In one embodiment, the method includes, after the heating step (I), a carbon material removing step of removing at least a part of the carbon material generated by heating the compound (A).

[0010] In one embodiment, the method further comprises a heating step (II) of heating after the carbon material removing step.

[0011] In one embodiment, the method includes, after the heating step (I), an inorganic substance removal step of removing the inorganic substance.

[0012] In one embodiment, the method further comprises a heating step (II) of heating after the inorganic substance removing step.

[0013] In one embodiment, the molecular weight of the compound (A) is 500 or less.

[0014] In one embodiment, the condensation reaction temperature of the compound (A) is 450° C. or lower.

[0015] In one embodiment, the condensation reaction temperature of the compound (A) is 400° C. or lower.

[0016] In one embodiment, when the compound (A) is subjected to TG-DTA analysis under a nitrogen gas atmosphere at a temperature rising rate of 10°C / min from 40°C, the weight ratio (M500 / M50) of the weight M500 at a temperature of 50°C to the initial weight M50 at a temperature of 50°C is 0.2 or more.

[0017] In one embodiment, the condensation reaction is promoted by an acid catalyst.

[0018] In one embodiment, the condensation reaction is (a) Condensation reaction by forming and eliminating HO from -H and -OH groups; (b) a condensation reaction between an -H group and an -OR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate ROH; (c) a condensation reaction in which an HX group is formed from an -H group and an -X group (X is a halogen or CN) and then eliminated; (d) Condensation reaction by forming and eliminating NH3 from the -H group and the -NH2 group. (e) a condensation reaction between an -H group and an -NHR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RNH2; (f) -H group and -NR 1 R 2 Group (R 1 , R 2 is any suitable substituted or unsubstituted alkyl group) and R 1 R 2 condensation reaction by the formation and elimination of NH (g) Condensation reaction of -H and -SH groups to form and eliminate H2S, (h) a condensation reaction between an -H group and an -SR group (wherein R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RSH; (i) a condensation reaction between an -H group and an -OOCR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RCOOH; (j) Condensation reaction of -H group with -OSO(OH) group to form and eliminate H2SO3, (k) a condensation reaction between an -H group and an -OSO2R group (wherein R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RSO2(OH); (l) a condensation reaction between a -H group and a -OSO2(OR) group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate ROSO3H; and (m) Condensation reaction of -H group and -OSO2(OH) group to form and eliminate H2SO4, At least one selected from the group consisting of:

[0019] In one embodiment, the inorganic substance is at least one selected from the group consisting of inorganic oxides, inorganic nitrides, inorganic sulfides, inorganic carbides, and insoluble salts.

[0020] In one embodiment, the inorganic oxide is an inorganic oxide particle having a functional group on the surface.

[0021] In one embodiment, the inorganic oxide particles are at least one selected from the group consisting of silica particles, alumina particles, titania particles, magnesium oxide particles, polyacid particles, metal particles at least a portion of whose surface is oxidized, composite oxide particles, and solid solution oxide particles.

[0022] In one embodiment, the metal constituting the polyacid particles is at least one selected from the group consisting of molybdenum, vanadium, tungsten, niobium, titanium, and tantalum.

[0023] In one embodiment, the decomposition temperature of the inorganic oxide is 800° C. or higher.

[0024] The carbon material-containing material of the present invention is A carbon material-containing material containing a carbon material and an inorganic substance, At least a portion of the carbon material and at least a portion of the inorganic material are bonded by a covalent bond.

[0025] In one embodiment, the carbon material-containing material of the present invention comprises: 13 C-NMR analysis shows a peak between 125 ppm and 135 ppm.

[0026] In one embodiment, the carbon material-containing material of the present invention comprises: 13 C-NMR analysis shows a peak between 140 ppm and 160 ppm. [Effects of the Invention]

[0027] According to the present invention, it is possible to provide a method for simply producing a carbonaceous material that is soluble in a solvent or a carbonaceous material that has a precisely controlled structure under mild conditions. Furthermore, it is possible to provide a carbonaceous material in which a carbonaceous material and an inorganic substance are bonded by a covalent bond. [Brief explanation of the drawings]

[0028] [Figure 1] 1 is a schematic cross-sectional view showing an organic-inorganic composite, which is one embodiment of a carbon material-containing material obtained by the production method of the present invention. [Figure 2] 1 is a schematic cross-sectional view showing a core-shell particle, which is an example of a carbon material-containing particle, which is one embodiment of a carbon material-containing material obtained by the production method of the present invention. [Figure 3] FIG. 2 is a diagram showing XPS spectra (C1s) of organic-inorganic composites (1) to (4) obtained in Examples 1 to 4. [Figure 4] FIG. 2 is a measurement diagram showing the results of DTA analysis in TG-DTA analysis of organic-inorganic composites (1) to (4) obtained in Examples 1 to 4. [Figure 5] FIG. 2 is an IR spectrum diagram of organic-inorganic composites (1) to (4) obtained in Examples 1 to 4. [Figure 6] FIG. 2 is a Raman spectrum diagram of organic-inorganic composites (1) to (4) obtained in Examples 1 to 4. [Figure 7] FIG. 1 is a diagram showing XPS spectra (C1s) of organic-inorganic composites (5) to (8) obtained in Examples 5 to 8. [Figure 8] FIG. 2 is an IR spectrum diagram of organic-inorganic composites (5) to (8) obtained in Examples 5 to 8. [Figure 9] FIG. 1 is a Raman spectrum diagram of organic-inorganic composite (9) obtained in Example 9. [Figure 10] FIG. 1 is an SEM photograph of highly carbonized core-shell particles (9) obtained in Example 9. [Figure 11] FIG. 1 is a Raman spectrum of the surface of highly carbonized core-shell particles (9) obtained in Example 9. [Figure 12] FIG. 13C-NMR diagrams of highly carbonized core-shell particles (9) obtained in Example 9 and particles obtained in Comparative Example 3. [Figure 13] FIG. 29Si-NMR diagrams of the highly carbonized core-shell particles (9) obtained in Example 9, the particles obtained in Comparative Example 3, and silica particles. [Figure 14] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (10) obtained in Example 10. [Figure 15] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (11) obtained in Example 11. [Figure 16] FIG. 1 is a graph comparing the Vickers hardness of a sintered body obtained by SPS sintering of highly carbonized core-shell particles (11) and a sintered body obtained by SPS sintering of aluminum. [Figure 17] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (12) obtained in Example 12. [Figure 18] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (13) obtained in Example 13. [Figure 19] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (14) obtained in Example 14. [Figure 20] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (15) obtained in Example 15. [Figure 21] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (16) obtained in Example 16. [Figure 22] FIG. 1 is a Raman spectrum of the surface of the highly carbonized core-shell particle (17) obtained in Example 17. [Figure 23] FIG. 1 is a Raman spectrum of the surface of highly carbonized core-shell particles (18) obtained in Example 18. [Figure 24] FIG. 1 is a Raman spectrum of the surface of highly carbonized core-shell particles (19) obtained in Example 19. [Figure 25] FIG. 2 is a Raman spectrum of the surface of the highly carbonized core-shell particle (20) obtained in Example 20. [Figure 26] FIG. 2 is a Raman spectrum of the surface of the organic-inorganic composite (21) obtained in Example 21. [Figure 27] FIG. 2 is a Raman spectrum of the surface of the highly carbonized core-shell particle (21) obtained in Example 21. [Figure 28] FIG. 2 is a Raman spectrum of the surface of the organic-inorganic composite (22) obtained in Example 22. [Figure 29] FIG. 2 is a Raman spectrum of the surface of the highly carbonized core-shell particle (22) obtained in Example 22. [Figure 30] FIG. 2 is a Raman spectrum of the surface of the organic-inorganic composite (23) obtained in Example 23. [Figure 31] FIG. 2 is a Raman spectrum of the surface of the highly carbonized core-shell particle (23) obtained in Example 23. [Figure 32] FIG. 2 is a Raman spectrum of the surface of the organic-inorganic composite (24) obtained in Example 24. [Figure 33] FIG. 2 is a Raman spectrum of the surface of the highly carbonized core-shell particle (24) obtained in Example 24. DETAILED DESCRIPTION OF THE INVENTION

[0029] <<1. Method for producing carbon-containing material>> The method for producing a carbon-containing material of the present invention includes a heating step (I) of heating a composition containing a compound (A) that undergoes a condensation reaction between identical molecules and / or different molecules by heating, and an inorganic substance, and the heating temperature in the heating step (I) is (T-150)°C or higher when the condensation reaction temperature of the compound (A) is T°C.

[0030] In the heating step (I), a composition containing compound (A) and an inorganic substance is heated, which undergoes condensation reactions between identical molecules and / or different molecules. The blending ratio of compound (A) to inorganic substance is preferably 0.01% by mass to 1,000,000% by mass, more preferably 0.1% by mass to 100,000% by mass, and particularly preferably 1% by mass to 1,000% by mass, relative to 100% by mass of the inorganic substance. When the blending ratio of compound (A) to inorganic substance is within the above range, a carbonaceous material-containing material with a more precisely controlled structure can be produced more easily under milder conditions. The blending ratio of these inorganic substances to compound (A) can be adjusted as desired depending on the physical properties of the target composite. For example, by adjusting the blending ratio of inorganic substance to compound (A), the physical properties and morphology of the resulting carbonaceous material-containing material (e.g., solubility in solvents, shape (particulate or non-particulate) of the carbonaceous or inorganic component, size, etc.) can be controlled.

[0031] The composition containing the compound (A) that undergoes a condensation reaction between the same molecules and / or different molecules upon heating and an inorganic substance may contain any other appropriate components, such as a solvent, a catalyst, a base material, a carrier, etc., as long as the effects of the present invention are not impaired.

[0032] The composition to be heated in the heating step (I) may be prepared by any suitable method as long as the effects of the present invention are not impaired. Examples of such methods include a method in which the compound (A) and the inorganic substance are mixed in a solid state by any suitable method (e.g., crushing, pulverization, etc.). Another example includes a method in which the compound (A), the inorganic substance, the solvent, and, if necessary, other components other than the solvent are mixed by any suitable method (e.g., ultrasonic treatment, etc.), and the solvent is removed by any suitable method (e.g., vacuum drying). Crushing may also be performed as necessary.

[0033] The heating temperature in the heating step (I) is (T-150)°C or higher, preferably (T-150 to T+50)°C, more preferably (T-130 to T+45)°C, even more preferably (T-100 to T+40)°C, particularly preferably (T-80 to T+35)°C, and most preferably (T-50 to T+30)°C, when the condensation reaction temperature of compound (A) is T°C. In the method for producing a carbonaceous material of the present invention, the catalytic ability of the inorganic substance and the reactivity of the functional groups on the inorganic substance with the carbonaceous material are high, so that the reaction can proceed and carbonization can proceed at a temperature relatively low compared to the condensation reaction temperature of compound (A), as described above. By adjusting the heating temperature within the above range, a carbonaceous material that is soluble in a solvent or a carbonaceous material that has a more precisely controlled structure can be produced more easily under milder conditions.

[0034] The condensation reaction temperature of compound (A) can be determined by TG-DTA analysis, specifically as follows. (1) When one type of compound is used as compound (A), the compound (A) is analyzed by TG-DTA in a nitrogen gas atmosphere by increasing the temperature from 40°C at a rate of 10°C / min, and the lowest peak-top temperature in the DTA is determined as the condensation reaction temperature (T°C) of compound (A). (2) When a mixture of two or more compounds is used as compound (A), the mixture is subjected to TG-DTA analysis in a nitrogen gas atmosphere by increasing the temperature from 40°C at a rate of 10°C / min, and the peak-top temperature on the lowest temperature side of the DTA is determined as the condensation reaction temperature (T°C) of compound (A) (a mixture of two or more compounds). (3) However, when compound (A) as a single compound or a mixture of two or more compounds contains impurities such as solvents, water, or hydration water, a DTA peak (sometimes referred to as an impurity peak) associated with the elimination of the impurity may be observed at a temperature lower than the condensation reaction temperature. In such cases, the above-mentioned impurity peak is ignored to determine the condensation reaction temperature of compound (A). Usually, the above-mentioned impurity peak is ignored, and the lowest DTA peak top temperature is determined to be the condensation reaction temperature of compound (A).

[0035] The heating temperature in the heating step (I) is preferably 200°C to 500°C, more preferably 220°C to 400°C, even more preferably 230°C to 350°C, and most preferably 250°C to 300°C. By adjusting the heating temperature within the above range, carbonaceous material-containing materials that are soluble in solvents and carbonaceous material-containing materials with more precisely controlled structures can be produced more easily under milder conditions. In particular, because the heating temperature in the heating step (I) is so low, carbonaceous material-containing materials can be produced industrially under milder conditions.

[0036] The heating time in the heating step (I) is preferably 0.1 to 120 hours, more preferably 0.5 to 100 hours, even more preferably 1 to 50 hours, and most preferably 2 to 24 hours. By adjusting the heating time within the above range, a carbonaceous material containing a solvent soluble material or a carbonaceous material containing a more precisely controlled structure can be produced more easily under milder conditions.

[0037] ≪1-1. Compound (A)≫ When compound (A) is heated, a condensation reaction occurs between identical molecules and / or different molecules. Therefore, compound (A) can typically become a carbon material through the heating step (I) in which a composition containing compound (A) and an inorganic substance is heated.

[0038] Compound (A) is preferably solid at 23°C and has a melting point. Having a melting point allows it to melt during the firing process, allowing intermolecular reactions to proceed smoothly. If it does not have a melting point, it will not melt during the firing process, and the positions of the molecules will be fixed, making it difficult for intermolecular reactions to be promoted and difficult for it to become a carbon material. By using such a compound (A), condensation reactions can be promoted, decomposition reactions can be suppressed, and the solubility of the carbon material contained in the resulting carbon material-containing material in solvents can be improved (for example, more of the carbon material components can be dissolved in the solvent, or the number of solvents in which the carbon material can be dissolved can be increased).

[0039] The skeleton of compound (A) that does not contribute to condensation preferably has an aromatic structure. The aromatic skeleton can make the carbon component of the resulting carbon material more stable. Examples of such aromatic structures include aromatic structures consisting of carbon atoms, such as benzene and naphthalene; and heteroaromatic structures consisting of carbon atoms and heteroatoms (such as nitrogen and oxygen), such as pyridine, pyrimidine, furan, and thiophene. Among these, aromatic structures and heteroaromatic structures having a six-membered ring structure, such as benzene and pyridine, are more preferred.

[0040] The molecular weight of compound (A) may be any appropriate molecular weight within a range that does not impair the effects of the present invention. In order to further exhibit the effects of the present invention, the molecular weight is preferably 500 or less, more preferably 75 to 450, even more preferably 80 to 400, and most preferably 100 to 350.

[0041] The condensation reaction temperature of compound (A) may be any appropriate temperature within a range that does not impair the effects of the present invention. In order to further exhibit the effects of the present invention, the condensation reaction temperature is preferably 450°C or lower, more preferably 400°C or lower, even more preferably 200°C to 370°C, and particularly preferably 250°C to 350°C.

[0042] When compound (A) is subjected to TG-DTA analysis in a nitrogen gas atmosphere under conditions of a temperature increase from 40°C at a rate of 10°C / minute, the weight ratio (M500 / M50) of the weight M500 at a temperature of 500°C to the initial weight M50 at a temperature of 50°C is preferably 0.2 or more, more preferably 0.2 to 0.9, and most preferably 0.3 to 0.8, in order to further exhibit the effects of the present invention. By using compound (A) whose weight ratio (M500 / M50) falls within the above range, a sufficient amount of carbon material can remain in the carbon material-containing material after heating.

[0043] [Representative embodiment of compound (A) (embodiment 1)] A representative embodiment (embodiment 1) of compound (A) is an aromatic compound that decomposes upon heating to generate radicals on the aromatic ring. The aromatic compound with radicals generated on the aromatic ring can undergo a condensation reaction between identical molecules and / or different molecules to produce a carbon material.

[0044] The aromatic compound that decomposes upon heating to generate radicals on the aromatic ring is preferably an aromatic compound that generates a gas upon heating (a gas that is in a gaseous state at room temperature and normal pressure).

[0045] Any suitable aromatic compound that generates a gas upon heating can be used as the aromatic compound that generates a gas upon heating. Such a gas that is in a gaseous state at room temperature and normal pressure is preferably at least one selected from CO, CO2, N2, O2, H2, and NO2.

[0046] In addition, when the gas that is in a gaseous state at room temperature and normal pressure as described above is at least one selected from CO, CO2, and O2, the obtained carbon material-containing material preferably has at least one aspect selected from the group consisting of the following (1) to (6).

[0047] (1) The ratio of all carbon-oxygen bonds, i.e., the total amount of C-O bonds and C=O bonds, to the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), as determined by C1s XPS analysis, is preferably 10% or more, more preferably 20% or more, and even more preferably 25% or more, with the upper limit of this ratio being preferably 35% or less. In a carbonaceous material, if the ratio of the total amount of C-O bonds and C=O bonds to the total amount of C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds as determined by C1s XPS analysis is within the above range, the carbonaceous material can be a novel carbonaceous material with various physical properties, such as solubility, that differ from conventionally known simple carbon materials.

[0048] (2) The ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.) determined by C1s XPS analysis is preferably 50% or more, more preferably 60% or more, even more preferably 65% ​​or more, particularly preferably 70% or more, and most preferably 75% or more. The upper limit of this ratio is preferably 90% or less. In a carbon-containing material, if the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of C-O bonds and C=O bonds determined by C1s XPS analysis is within the above range, the carbon-containing material can have an increased structural control rate of the carbon material portion and a more precisely controlled structure. The structural control rate indicates the proportion of bonds derived from the desired reaction relative to the total number of bonds. In the present invention, the total number of bonds corresponds to the total number of C-O bonds and C=O bonds, and the bonds derived from the desired reaction correspond to the total number of C-O bonds derived from ethers and C-O bonds derived from alcohols. A high structural control rate, in other words, means that there are many bonds derived from the desired reaction and few bonds derived from undesired reactions. In the present invention, the bonds derived from undesired reactions are C=O bonds derived from decomposition reactions, and the lower the structural control rate, the more the decomposition reaction is suppressed. Such a carbonaceous material can be said to be a carbonaceous material with a more precisely controlled structure.

[0049] (3) The ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all bonds, i.e., C-C bonds, C-H bonds, C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), and C-O bonds (including carbonyl-derived C-O bonds, carboxyl-derived C-O bonds, ester-derived C-O bonds, lactone-derived C-O bonds, etc.), as determined by C1s XPS analysis, is preferably 15% or more, more preferably 17% or more, and even more preferably 20% or more. The upper limit of this ratio is preferably 30% or less. In a carbonaceous material, if the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all bonds as determined by C1s XPS analysis is within the above range, the carbonaceous material can be said to have a more precisely controlled structure.

[0050] (4) This is an embodiment in which the ratio of all carbon-oxygen bonds, i.e., the total amount of C-C bonds and C-H bonds, to the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), as determined by C1s XPS analysis, is within the range described in (1) above, and the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all carbon-oxygen bonds, i.e., C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), as determined by C1s XPS analysis, is within the range described in (2) above. In such an embodiment, the carbon material-containing material can further increase the solubility of the carbon material portion and can further increase the structural control rate of the carbon material portion. Furthermore, in such an embodiment, the structure of the carbon material-containing material can be controlled more precisely.

[0051] (5) In IR analysis, preferably, 1660 cm -1 ~1800cm -1 In the IR analysis of carbon-containing materials, no peak due to C=O stretching vibration is observed between 1660 cm -1 ~1800cm -1 If no peak due to C=O stretching vibration is observed between 1660 cm and 1660 cm, the structure of the carbonaceous material can be more precisely controlled. -1 ~1800cm -1 The reason why the structure of the carbonaceous material can be controlled more precisely when no peak due to C=O stretching vibration is observed between these is as described above.

[0052] (6) The carbon material in the carbon-containing material is soluble in the solvent.

[0053] Examples of aromatic compounds that generate CO and / or CO upon heating include aromatic compounds having a "-C(=O)-" and / or "-OC(=O)-" structure (e.g., aromatic ketone derivatives, aromatic ester derivatives, acid anhydrides, etc.).

[0054] Examples of aromatic compounds that generate CO and / or CO2 upon heating include the following compounds:

[0055] [ka]

[0056] Examples of aromatic compounds that generate N2 upon heating include aromatic compounds having a "-NH-NH-" structure, a "-N=N-" structure, or a "-N3" structure (e.g., aromatic azo compounds, aromatic azide compounds, triazole-substituted aromatic compounds, tetrazole-substituted aromatic compounds, triazine or a derivative thereof, tetrazine or a derivative thereof, aromatic hydrazine derivatives, etc.).

[0057] Examples of aromatic compounds that generate N2 upon heating include the following compounds: In the following compounds, R represents a hydrogen atom, or an alkyl group, aryl group, or heteroaryl group that may have a substituent.

[0058] [ka]

[0059] Examples of aromatic compounds that generate O2 upon heating include aromatic compounds having an "-OO-" structure (such as aromatic carbon oxides and aromatic peroxides).

[0060] Examples of aromatic compounds that generate O2 upon heating include the following compounds: In the following compounds, R represents a hydrogen atom, or an alkyl group, aryl group, or heteroaryl group that may have a substituent.

[0061] [ka]

[0062] Examples of aromatic compounds that generate H2 upon heating include condensed polycyclic aromatic compounds having a "-CH2-" structure (such as phenalene compounds).

[0063] Examples of aromatic compounds that generate H2 when heated include the following compounds:

[0064] [ka]

[0065] Examples of aromatic compounds that generate NO2 upon heating include aromatic compounds having a "-NO2" structure (such as aromatic nitro compounds).

[0066] Examples of aromatic compounds that generate NO2 when heated include the following compounds:

[0067] [ka]

[0068] Aromatic compounds that decompose upon heating to generate radicals on the aromatic ring are compounds that exhibit thermal decomposition, in which at least a portion of the skeleton undergoes dissociation and decomposition to generate gas molecules (preferably at least one selected from CO, CO2, N2, O2, H2, and NO2), and radicals are generated on the remaining aromatic ring. By using such aromatic compounds, the reaction occurs solely through their own decomposition without the need for a reaction catalyst. This prevents the presence of chemical reaction by-products or reaction catalysts in the carbon material, which can become fatal impurities, resulting in the production of higher-quality carbon materials. Furthermore, by using such aromatic compounds, carbon materials can be produced in a relatively mild temperature environment without the use of flammable gases. Furthermore, such aromatic compounds can exhibit high reactivity without the need for a catalyst.

[0069] [Representative embodiment of compound (A) (embodiment 2)] A representative embodiment (embodiment 2) of compound (A) is a compound in which a condensation reaction results in the formation and elimination of one neutral molecule from two or more groups. In embodiment 2, one compound may have two or more groups, or two or more compounds may combine groups to form two or more groups. Such compound (A) can undergo a condensation reaction between identical molecules and / or different molecules to form a carbon material.

[0070] As the condensation reaction, any appropriate condensation reaction can be adopted as long as it is a condensation reaction in which one neutral molecule is formed from two or more groups and then eliminated, as long as it does not impair the effects of the present invention. By adopting such a condensation reaction, it may be possible to carry out the reaction at a relatively low temperature. Examples of such condensation reactions include: (a) Condensation reaction by forming and eliminating HO from -H and -OH groups; (b) a condensation reaction between an -H group and an -OR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate ROH; (c) a condensation reaction in which an HX group is formed from an -H group and an -X group (X is a halogen or CN) and then eliminated; (d) Condensation reaction by forming and eliminating NH3 from the -H group and the -NH2 group. (e) a condensation reaction between an -H group and an -NHR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RNH2; (f) -H group and -NR 1 R 2 Group (R 1 , R 2 is any suitable substituted or unsubstituted alkyl group) and R 1 R 2 condensation reaction by the formation and elimination of NH (g) Condensation reaction of -H and -SH groups to form and eliminate H2S, (h) a condensation reaction between an -H group and an -SR group (wherein R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RSH; (i) a condensation reaction between an -H group and an -OOCR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RCOOH; (j) Condensation reaction of -H group with -OSO(OH) group to form and eliminate H2SO3, (k) a condensation reaction between an -H group and an -OSO2R group (wherein R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RSO2(OH); (l) a condensation reaction between a -H group and a -OSO2(OR) group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate ROSO3H; (m) Condensation reaction of -H group and -OSO2(OH) group to form and eliminate H2SO4, In particular, if the desorbed neutral components are gaseous components at the desorption temperature (calcination temperature), they are not incorporated into the carbon material and remain in the gas phase, making them less likely to become impurities.

[0071] Among the above condensation reactions, in particular, (a) Condensation reaction by forming and eliminating HO from -H and -OH groups; (b) a condensation reaction between an -H group and an -OR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate ROH; (i) a condensation reaction between an -H group and an -OOCR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RCOOH; In this case, the carbon material-containing material obtained preferably has at least one aspect selected from the group consisting of the following (1) to (6).

[0072] (1) The ratio of all carbon-oxygen bonds, i.e., the total amount of C-O bonds and C=O bonds, to the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), as determined by C1s XPS analysis, is preferably 10% or more, more preferably 20% or more, and even more preferably 25% or more, with the upper limit of this ratio being preferably 35% or less. In a carbonaceous material, if the ratio of the total amount of C-O bonds and C=O bonds to the total amount of C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds as determined by C1s XPS analysis is within the above range, the carbonaceous material can be a novel carbonaceous material with various physical properties, such as solubility, that differ from conventionally known simple carbon materials.

[0073] (2) The ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.) determined by C1s XPS analysis is preferably 50% or more, more preferably 60% or more, even more preferably 65% ​​or more, particularly preferably 70% or more, and most preferably 75% or more. The upper limit of this ratio is preferably 90% or less. In a carbon-containing material, if the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of C-O bonds and C=O bonds determined by C1s XPS analysis is within the above range, the carbon-containing material can have an increased structural control rate of the carbon material portion and a more precisely controlled structure. In other words, the lower the ratio of C=O bonds resulting from the decomposition reaction, the more the decomposition reaction is suppressed, and such a carbonaceous material can be said to be a carbonaceous material with a more precisely controlled structure.

[0074] (3) The ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all bonds, i.e., C-C bonds, C-H bonds, C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), and C-O bonds (including carbonyl-derived C-O bonds, carboxyl-derived C-O bonds, ester-derived C-O bonds, lactone-derived C-O bonds, etc.), as determined by C1s XPS analysis, is preferably 15% or more, more preferably 17% or more, and even more preferably 20% or more. The upper limit of this ratio is preferably 30% or less. In a carbonaceous material, if the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all bonds as determined by C1s XPS analysis is within the above range, the carbonaceous material can be said to have a more precisely controlled structure.

[0075] (4) This is an embodiment in which the ratio of all carbon-oxygen bonds, i.e., the total amount of C-C bonds and C-H bonds, to the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), as determined by C1s XPS analysis, is within the range described in (1) above, and the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all carbon-oxygen bonds, i.e., C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), as determined by C1s XPS analysis, is within the range described in (2) above. In such an embodiment, the carbon material-containing material can further increase the solubility of the carbon material portion and can further increase the structural control rate of the carbon material portion. Furthermore, in such an embodiment, the structure of the carbon material-containing material can be controlled more precisely.

[0076] (5) In IR analysis, preferably, 1660 cm -1 ~1800cm -1 In the IR analysis of carbon-containing materials, no peak due to C=O stretching vibration is observed between 1660 cm -1 ~1800cm -1 If no peak due to C=O stretching vibration is observed between 1660 cm and 1660 cm, the structure of the carbonaceous material can be more precisely controlled. -1 ~1800cm -1 The reason why the structure of the carbonaceous material can be controlled more precisely when no peak due to C=O stretching vibration is observed between these is as described above.

[0077] (6) The carbon material in the carbon-containing material is soluble in the solvent.

[0078] As a representative example of a condensation reaction, the condensation reaction (a) above) in which H2O is formed from a -H group and a -OH group and then eliminated will be described.

[0079] One embodiment of compound (A) in embodiment 2 (sometimes referred to as embodiment (X)) is compound (a1) having a skeleton consisting of one six-membered carbon ring structure or compound (a2) having a skeleton in which two or more six-membered carbon ring structures are bonded and / or fused, in which half of the substituents not contributing to the formation of the skeleton structure are -OH groups and the other half are -H groups.

[0080] In embodiment (X), (i) When the compound (A) is a compound (a1) having a skeleton consisting of one 6-membered carbon ring structure, (ii) When the compound (A) is a compound (a2) having a skeleton in which two or more 6-membered carbon ring structures are bonded and / or fused, Either of the following two cases can be adopted.

[0081] In embodiment (X), "substituents not contributing to the formation of the skeleton" refers to substituents not contributing to the formation of the skeleton of the "skeleton consisting of one six-membered carbon ring structure" in the case of (i) above or the "skeleton in which two or more six-membered carbon ring structures are bonded and / or fused" in the case of (ii) above. For example, in the case of (i) above, when compound (a1) having a skeleton consisting of one six-membered carbon ring structure is represented by chemical formula (a1-1) shown below, the substituents not contributing to the formation of the skeleton consisting of one six-membered carbon ring structure are six -OH groups and six -H groups, and when compound (a1) having a skeleton consisting of one six-membered carbon ring structure is represented by chemical formula (a1-2) shown below, the substituents not contributing to the formation of the skeleton consisting of one six-membered carbon ring structure are three -OH groups and three -H groups. Furthermore, for example, in the case of (ii) above, when compound (a2) having a skeleton in which two or more six-membered carbon ring structures are bonded and / or fused is represented by chemical formula (a2-1) shown later, the substituents that do not contribute to the structural formation of the skeleton in which two or more six-membered carbon ring structures are bonded and / or fused are six -OH groups and six -H groups.

[0082] In embodiment (X), half of the substituents not contributing to the formation of the structure of compound (a1) having a skeleton consisting of one six-membered carbon ring structure are -OH groups and the other half are -H groups, and half of the substituents not contributing to the formation of the structure of compound (a2) having a skeleton in which two or more six-membered carbon ring structures are bonded and / or fused are -OH groups and the other half are -H groups. By having such a substituent configuration, compound (A) can effectively undergo a dehydration reaction between identical molecules and / or different molecules upon heating.

[0083] The compound (A) that can be used in embodiment (X) is a compound (a1) having a skeleton consisting of one six-membered carbon ring structure or a compound (a2) having a skeleton in which two or more six-membered carbon ring structures are bonded and / or fused, and any appropriate compound can be used as long as it does not impair the effects of the present invention, as long as half of the substituents that do not contribute to the formation of the skeleton are -OH groups and the other half are -H groups. Examples of such compounds (A) include the following compounds.

[0084] [ka]

[0085] Among the compounds (A) that can be employed in embodiment (X), phloroglucinol (compound (a1-2)) and hexahydroxytriphenylene (HHTP) (compound (a2-1)) are preferred because they are presumed to easily undergo a condensation reaction in which HO is formed from a -H group and a -OH group and then eliminated, and the reaction is presumed to proceed easily at low temperatures.

[0086] Another embodiment of compound (A) in embodiment 2 (sometimes referred to as embodiment (Y)) is two or more compounds selected from compound (a1) having a skeleton consisting of one six-membered carbon ring structure and / or compound (a2) having a skeleton in which two or more six-membered carbon ring structures are bonded and / or fused, in which half of the total number of substituents that do not contribute to the formation of the skeleton structure of compound (a1) and the total number of substituents that do not contribute to the formation of the skeleton structure of compound (a2) are -OH groups, and the other half are -H groups.

[0087] In embodiment (Y), (i) When the compound (A) is composed of two or more compounds selected from the compound (a1) having a skeleton consisting of one 6-membered carbon ring structure, (ii) When the compound (A) is composed of two or more compounds (a2) having a skeleton in which two or more 6-membered carbon ring structures are bonded and / or fused, (iii) When compound (A) is composed of one or more compounds (a1) having a skeleton consisting of one 6-membered carbon ring structure and one or more compounds (a2) having a skeleton in which two or more 6-membered carbon ring structures are bonded and / or fused, One of the following three cases can be adopted.

[0088] In embodiment (Y), "the total number of substituents not contributing to the formation of the skeleton of compound (a1) and the total number of substituents not contributing to the formation of the skeleton of compound (a2)" has the following meaning. That is, in the case of (i) above, it means the total number of substituents not contributing to the formation of the skeleton of "a skeleton consisting of one six-membered carbon ring structure" in each of two or more compounds (a1). In the case of (ii) above, it means the total number of substituents not contributing to the formation of the skeleton of "a skeleton consisting of two or more bonded and / or fused six-membered carbon ring structures" in each of two or more compounds (a2). In the case of (iii) above, it means the total number of substituents not contributing to the formation of the skeleton of "a skeleton consisting of one six-membered carbon ring structure" in each of one or more compounds (a1) and the total number of substituents not contributing to the formation of the skeleton of "a skeleton consisting of two or more bonded and / or fused six-membered carbon ring structures" in each of one or more compounds (a2).

[0089] In embodiment (Y), for example, in the case of (i) above, when two or more types of compounds (a1) are represented by the following chemical formulas (a1-5) and (a1-6), the substituents that do not contribute to the formation of the skeleton structure consisting of one 6-membered carbon ring structure of the compound represented by chemical formula (a1-5) are two -OH groups and four -H groups, and the substituents that do not contribute to the formation of the skeleton structure consisting of one 6-membered carbon ring structure of the compound represented by chemical formula (a1-6) are four -OH groups and two -H groups, for a total of six -OH groups and six -H groups. Furthermore, for example, in the case of (iii) above, when one or more compounds (a1) are represented by the following chemical formulas (a1-5) and (a1-7), and one or more compounds (a2) are represented by the following chemical formula (a2-3), the substituents that do not contribute to the formation of a skeleton structure consisting of one six-membered carbon ring structure in the compound represented by chemical formula (a1-5) are two -OH groups and four -H groups, the substituents that do not contribute to the formation of a skeleton structure consisting of one six-membered carbon ring structure in the compound represented by chemical formula (a1-7) are six -OH groups, and the substituents that do not contribute to the formation of a skeleton structure in which two or more six-membered carbon ring structures are bonded and / or fused in the compound represented by chemical formula (a2-3) are two -OH groups and six -H groups.

[0090] [ka]

[0091] [ka]

[0092] By using such a compound (A), the reaction occurs through its own dehydration reaction without the need for a reaction catalyst, which prevents by-products of the chemical reaction or reaction catalysts from being present in the carbon material and becoming fatal impurities, thereby enabling the production of a higher quality carbon material. Furthermore, by using such a compound (A), a carbon material can be produced in a relatively mild temperature environment without using flammable gases. Furthermore, such a compound (A) can have high reactivity without the need for a catalyst.

[0093] A preferred embodiment of the compound (A) in embodiment 2 is a compound having three or more phenolic hydroxyl groups in the molecule.

[0094] As the compound having three or more phenolic hydroxyl groups in the molecule, any appropriate compound having three or more phenolic hydroxyl groups in the molecule can be used as long as it does not impair the effects of the present invention.

[0095] In a compound having three or more phenolic hydroxyl groups in a molecule, the aromatic ring to which the phenolic hydroxyl groups are bonded is preferably a hydrocarbon aromatic ring. Although the effects of the present invention can be achieved even if the aromatic ring to which the phenolic hydroxyl groups are bonded is a heteroaromatic ring, the carbon material obtained can be more stable if the aromatic ring has a more stable ring structure. Note that the heteroaromatic ring refers to an aromatic ring whose ring structure is formed by carbon and an element other than carbon, unlike a hydrocarbon aromatic ring whose ring structure is formed by carbon.

[0096] A compound having three or more phenolic hydroxyl groups in the molecule may have a substituent other than the phenolic hydroxyl group. Any appropriate substituent may be used as such a substituent as long as it does not impair the effects of the present invention. In order to further enhance the effects of the present invention, it is preferable that such a substituent be only a hydroxyl group. Although the effects of the present invention can be achieved even when a substituent other than a hydroxyl group is present, the absence of a substituent other than a hydroxyl group makes it easier to prevent side reactions and facilitates the formation of a carbon material. Note that the "hydroxyl group" as a substituent other than a phenolic hydroxyl group herein refers to a hydroxyl group that is not phenolic. Naturally, a substituent is a group that replaces a hydrogen group (-H).

[0097] As the elements constituting the compound having three or more phenolic hydroxyl groups in the molecule, any appropriate elements can be used as long as they do not impair the effects of the present invention. In terms of enhancing the effects of the present invention, it is preferable that such elements are only carbon, oxygen, and hydrogen. Although the effects of the present invention can be achieved even when elements other than carbon, oxygen, and hydrogen are present, the absence of elements other than carbon, oxygen, and hydrogen makes it easier to prevent side reactions and more easily produce a carbon material.

[0098] For a compound having three or more phenolic hydroxyl groups in the molecule, the condensation reaction temperature of the compound is preferably in the range of 200° C. to 450° C., more preferably in the range of 200° C. to 400° C., in order to more effectively exhibit the effects of the present invention. This allows for effective conversion into a carbon material.

[0099] The compound having three or more phenolic hydroxyl groups in the molecule may be one type or two or more types. Even in the case of two or more types, the intermolecular condensation reaction temperature is preferably within the above-mentioned range.

[0100] Examples of compounds having three or more phenolic hydroxyl groups in the molecule include compounds represented by general formulas (1) to (11).

[0101] [ka]

[0102] In each of the general formulas (1) to (11), X represents a hydrogen atom or a hydroxyl group, and three or more of the Xs are hydroxyl groups (phenolic hydroxyl groups).

[0103] Here, the phenolic hydroxyl group means a hydroxyl group bonded to an aromatic ring. That is, in general formula (1), three or more of the six Xs bonded to the aromatic ring are phenolic hydroxyl groups, in general formula (2), three or more of the six Xs bonded to the aromatic ring are phenolic hydroxyl groups, in general formula (3), three or more of the ten Xs bonded to the aromatic ring are phenolic hydroxyl groups, in general formula (4), three or more of the eleven Xs bonded to the aromatic ring are phenolic hydroxyl groups, in general formula (5), three or more of the nine Xs bonded to the aromatic ring are phenolic hydroxyl groups, and in general formula (6), nine Xs bonded to the aromatic ring are phenolic hydroxyl groups. Three or more of the X's are phenolic hydroxyl groups; in general formula (7), three or more of the ten X's bonded to the aromatic ring are phenolic hydroxyl groups; in general formula (8), three or more of the eleven X's bonded to the aromatic ring are phenolic hydroxyl groups; in general formula (9), three or more of the nine X's bonded to the aromatic ring are phenolic hydroxyl groups; in general formula (10), three or more of the nine X's bonded to the aromatic ring are phenolic hydroxyl groups; and in general formula (11), three or more of the twelve X's bonded to the aromatic ring are phenolic hydroxyl groups.

[0104] Among compounds having three or more phenolic hydroxyl groups in the molecule, phloroglucinol and hexahydroxytriphenylene are preferred, and phloroglucinol is more preferred, because it is believed that a condensation reaction is likely to occur in which HO is formed from the -H group and the -OH group and then eliminated, and the reaction is likely to proceed easily.

[0105] [Representative embodiment of compound (A) (embodiment 3)] A representative embodiment (Embodiment 3) of Compound (A) simultaneously employs both Embodiment 1 and Embodiment 2. That is, Embodiment 3 is an aromatic compound that decomposes upon heating to generate radicals on the aromatic ring, and is a compound that undergoes a condensation reaction to form and eliminate one neutral molecule from two or more groups. Such Compound (A) can undergo a condensation reaction between identical molecules and / or different molecules to produce a carbon material.

[0106] A specific example of the structure of embodiment 3 is compound (a3-1). When compound (a3-1) is heated, carbon dioxide molecules are eliminated, generating radicals (reaction active sites) on the aromatic ring, and the hydroxyl group and hydrogen group undergo intermolecular dehydration, causing a condensation reaction.

[0107] [ka]

[0108] By using such a compound (A), the reaction occurs through its own dehydration reaction without the need for a reaction catalyst, which prevents by-products of the chemical reaction or reaction catalysts from being present in the carbon material and becoming fatal impurities, thereby enabling the production of a higher quality carbon material. Furthermore, by using such a compound (A), a carbon material can be produced in a relatively mild temperature environment without using flammable gases. Furthermore, such a compound (A) can have high reactivity without the need for a catalyst.

[0109] ≪1-2. Inorganic substances≫ Any suitable inorganic substance can be used as long as it does not impair the effects of the present invention. As such an inorganic substance, for example, a particulate inorganic substance (inorganic particles), a non-particulate inorganic substance (for example, a fibrous inorganic substance, a thin film inorganic substance, etc.) can be used. As the inorganic substance, a particulate inorganic substance (inorganic particles) is preferred.

[0110] The inorganic substance may be of only one kind or of two or more kinds.

[0111] The inorganic substance is preferably at least one selected from the group consisting of inorganic oxides, inorganic nitrides, inorganic sulfides, inorganic carbides, and insoluble salts.

[0112] Examples of the "inorganic oxide" referred to in the present invention include a metal whose surface is oxidized, preferably a metal whose surface is at least partially oxidized, because, as will be described later, a metal generally has a portion thereof, preferably at least a portion thereof, oxidized. Such metals are preferably metals that are easily oxidized, such as magnesium (Mg), calcium (Ca), strontium (Sr), barium (Ba), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), indium (In), gallium (Ga), iron (Fe), cobalt (Co), nickel (Ni), copper (Cu), zinc (Zn), cadmium (Cd), aluminum (Al), tin (Sn), lanthanum (La), yttrium (Y), cerium (Ce), and silicon (Si). More preferably, copper (Cu), aluminum (Al), and silicon (Si) are used. That is, such metals are easily oxidized, and a portion thereof, preferably at least a portion of the surface thereof, is oxidized, and is included in the "inorganic oxide" referred to in the present invention.

[0113] Specific examples of the "inorganic oxide" referred to in the present invention include silica, alumina, titania, polyacid, partially oxidized metals (preferably metals with at least a portion of their surface oxidized), composite oxides, and solid solution oxides. That is, the "inorganic oxide" referred to in the present invention may be an oxide consisting of a single metal element, a composite oxide consisting of two or more metal elements, or a so-called solid solution oxide in which a different element is further dissolved in an oxide consisting of a single metal element (also called a single metal oxide) or a composite oxide. The different element in the solid solution oxide may be a metal element or a non-metal element other than oxygen, such as nitrogen or fluorine.

[0114] The inorganic oxide may be one kind or two or more kinds. Examples of using two or more kinds of inorganic oxides include a case where two or more kinds of inorganic oxides are simply used in combination (mixed, etc.) and a case where two or more kinds of inorganic oxides are bound together.

[0115] Examples of the "oxides consisting of one type of constituent metal element" include magnesium oxide, calcium oxide, strontium oxide, barium oxide, titanium oxide, zirconium oxide, hafnium oxide, vanadium oxide, niobium oxide, tantalum oxide, chromium oxide, molybdenum oxide, tungsten oxide, manganese oxide, indium oxide, gallium oxide, iron oxide, cobalt oxide, nickel oxide, copper oxide, zinc oxide, cadmium oxide, aluminum oxide, tin oxide, lanthanum oxide, yttrium oxide, cerium oxide, and silicon oxide, and preferred are magnesium oxide, titanium oxide (titania), aluminum oxide (alumina), and silicon oxide (silica).

[0116] As the "composite oxide having two or more constituent metal elements," any appropriate composite oxide can be used as long as the effects of the present invention are not impaired. Typical examples of such composite oxides include oxides containing two or more metals, such as composite oxides with a perovskite structure and composite oxides with a spinel structure.

[0117] Typical examples of double oxides with a perovskite structure are oxides represented by the formula ABO3 (A and B represent different elements), such as perovskite (perovskite, CaTiO3), barium titanate (BaTiO3), strontium titanate (SrTiO3), lead zirconate titanate (Pb(Zr,Ti)O3), barium zirconate (BaZrO3), and lithium niobate (LiNbO3).

[0118] Examples of double oxides with a spinel structure include spinel (MgAl2O4), lithium titanate (LiTi2O4), and chrysoberyl (BeAl2O4).

[0119] As the "solid solution oxide," any appropriate solid solution oxide can be used as long as it does not impair the effects of the present invention. Typical examples of such solid solution oxides include single metal oxides or composite oxides in which different metal elements and / or nonmetal elements other than oxygen, such as nitrogen and fluorine, are dissolved.

[0120] The "inorganic oxide" referred to in the present invention may be in any form (i.e., for example, inorganic oxide particles or non-particulate inorganic oxide), and may be entirely or partially composed of an inorganic oxide. The embodiment in which a portion of an inorganic oxide is present is preferably an embodiment having an inorganic oxide on the surface.

[0121] An embodiment in which a portion is an inorganic oxide (preferably, an embodiment having an inorganic oxide on the surface) includes, for example, a metal whose surface is oxidized (preferably, a metal whose surface is at least partially oxidized), regardless of its shape. A metal can be partially oxidized (preferably, at least a portion of its surface) in the presence of oxygen. Therefore, "an embodiment having an inorganic oxide on the surface," which is one form of inorganic oxide in the present invention, includes a metal whose surface is at least partially oxidized, regardless of its shape.

[0122] When inorganic oxide particles are used as the inorganic oxide, a carbonaceous material containing a large number of inorganic oxide particles can typically be obtained by heating a composition containing compound (A) and an inorganic oxide in the heating step (I) (in this case, a particulate carbonaceous material can be obtained by crushing, etc.). However, by adjusting the blending ratio of compound (A) and the inorganic oxide, a particulate carbonaceous material can also be obtained by heating a composition containing compound (A) and an inorganic oxide in the heating step (I).

[0123] When a fibrous inorganic oxide is used as the inorganic oxide, for example, a fibrous core-shell fiber can be obtained instead of the core-shell particles described later, and when a fibrous inorganic oxide is used, for example, a tubular hollow carbon material can be obtained instead of the hollow carbon microparticles described later.

[0124] When a thin film inorganic oxide is used as the inorganic oxide, a layered carbonaceous material can be obtained by heating a composition containing compound (A) and an inorganic oxide in a heating step (I). Furthermore, by further subjecting such a layered carbonaceous material to a heating step (II), a carbonaceous material removing step, or an inorganic oxide removing step, which will be described later, various thin film carbonaceous materials can be obtained.

[0125] The decomposition temperature of the inorganic oxide is preferably 800°C or higher, more preferably 850°C or higher, even more preferably 900°C or higher, and particularly preferably 950°C or higher, in order to further exert the effects of the present invention.

[0126] In the present invention, inorganic oxide particles are preferred as the inorganic oxide in that the effects of the present invention can be more effectively exhibited.

[0127] The "inorganic oxide particles" referred to in this specification are preferably particles whose entire particle is an inorganic oxide, or particles whose part is an inorganic oxide. As particles whose part is an inorganic oxide, particles having an inorganic oxide on the surface are preferred. The "inorganic oxide particles" referred to in this specification are more preferably particles whose entire particle is an inorganic oxide.

[0128] Examples of particles partly made of an inorganic oxide (preferably particles having an inorganic oxide on their surface) include partially oxidized metal particles (preferably metal particles having at least a part of their surface oxidized). Metal particles can be partially oxidized (preferably at least a part of their surface) in the presence of oxygen. Therefore, "particles having an inorganic oxide on their surface," which is one form of inorganic oxide particles in the present invention, includes metal particles having at least a part of their surface oxidized.

[0129] Inorganic oxide particles other than metal particles (e.g., silica particles, alumina particles, titania particles, etc.) may be particles in which the entire particle is an inorganic oxide, or particles in which a part of the particle is an inorganic oxide (preferably, particles having an inorganic oxide on the surface). That is, taking silica particles as an example, the silica particles may be particles in which the entire particle is silica, or particles in which a part of the particle is silica (preferably, particles having silica on the surface).

[0130] The average particle size of the inorganic oxide particles can be appropriately set depending on the purpose. In terms of being able to further exhibit the effects of the present invention, the average particle size of the inorganic oxide particles is preferably 0.01 μm to 100 μm, and particularly preferably 0.1 μm to 10 μm.

[0131] The average particle size of the inorganic oxide particles is the average particle size in the volume-based particle size distribution, and is preferably measured by a laser diffraction scattering method.

[0132] In order to further enhance the effects of the present invention, the inorganic oxide particles are preferably inorganic oxide particles having functional groups on their surfaces. Examples of such functional groups include hydroxyl functional groups such as M-OH; oxygen functional groups containing ether functional groups such as MOM; nitrogen functional groups containing amine functional groups such as M-NH2 and M-NH-M; sulfur functional groups containing thiol functional groups such as M-SH and MSM; and silicon functional groups, boron functional groups, phosphorus functional groups, etc. (M conceptually represents the object to which the functional group binds, and represents any suitable object to which the functional group can bind, such as the inorganic oxide itself, for example, a metal element or organic group constituting the inorganic oxide.) These functional groups can be easily formed by surface-treating the inorganic oxide with various compounds. Among these, inorganic oxide particles are preferably inorganic oxide particles having oxygen functional groups on their surfaces.

[0133] When inorganic oxide particles having functional groups on their surfaces are used as the inorganic oxide, the functional groups present on the surfaces of the inorganic oxide particles can form bonds with the carbon material in the carbon-containing material. The carbon material region (carbon material-bonded region) contributing to such bonding is not the carbon material itself. Specifically, as shown in FIG. 1, an organic-inorganic composite (described in detail below) 100 in one preferred embodiment of the carbon-containing material is a carbon material 10 matrix in which a plurality of inorganic particles 20 (in this case, inorganic oxide particles) are dispersed. At the interface between the carbon material 10 and the inorganic particles 20, a carbon material region (carbon material-bonded region) 30 is present, where the carbon material forms bonds with the functional groups present on the surfaces of the inorganic particles 20. For example, if the carbon material is soluble in a solvent, treating the organic-inorganic composite 100 with a solvent that dissolves the carbon material can produce a core-shell particle (core portion: inorganic oxide particle, shell portion: carbon material-bonded region) 200, in which the surfaces of the inorganic particles 20 are coated with carbon material-bonded regions (solvent-insoluble regions) 30, as shown in FIG. 2. By removing the inorganic particles 20 as core portions from the core-shell particles 200 thus obtained, hollow carbon microparticles containing a carbon material can be obtained.

[0134] The inorganic oxide particles having functional groups on their surfaces are preferably at least one selected from the group consisting of silica particles, alumina particles, titania particles, magnesium oxide particles, polyacid particles, metal particles having at least a portion of their surface oxidized, composite oxide particles, and solid solution oxide particles. By using at least one selected from the group consisting of silica particles, alumina particles, titania particles, magnesium oxide particles, polyacid particles, metal particles having at least a portion of their surface oxidized, composite oxide particles, and solid solution oxide particles as the inorganic oxide particles having functional groups on their surfaces, the functional groups present on the surfaces of the inorganic oxide particles are more likely to form bonds with the carbon material.

[0135] The inorganic oxide particles having functional groups on their surfaces are more preferably polyacid particles. Examples of polyacids constituting the polyacid particles include isopolyacids and heteropolyacids. As mentioned above, when compound (A) is used, a carbonaceous material can be obtained without utilizing a catalytic effect. However, when polyacid particles are used as the inorganic oxide particles having functional groups on their surfaces, the catalytic effect of the strong acidity combined with the presence of the surface functional groups promotes a dehydration condensation reaction when the carbonaceous material is obtained, increasing the ratio of the total number of -OH groups and -O- groups to the total number of C-O bonds, and thus enabling a high structural control rate.

[0136] Any appropriate isopolyacid may be used as the isopolyacid as long as it does not impair the effects of the present invention. Examples of such isopolyacids include inorganic acids containing inorganic elements such as molybdenum, vanadium, tungsten, niobium, titanium, tantalum, chromium, manganese, rhenium, iron, ruthenium, cobalt, nickel, palladium, platinum, copper, silver, gold, tin, titanium, zirconium, rhodium, iridium, osmium, and zinc as the main component, and salts thereof. Representative examples include molybdic acid, vanadic acid, tungstic acid, niobic acid, titanic acid, and tantalic acid.

[0137] Any suitable heteropolyacid may be used as the heteropolyacid as long as it does not impair the effects of the present invention. Examples of such heteropolyacids include isopolyacids or metal salts thereof into which heteroatoms have been introduced. Examples of heteroatoms include oxygen, sulfur, phosphorus, ammonium, potassium, sodium, and silicon. The heteropolyacid may be a hydrate.

[0138] Specific examples of heteropolyacids include tungsten-based heteropolyacids obtained by introducing a heteroatom into a tungsten-containing isopolyacid, and molybdenum-based heteropolyacids obtained by introducing a heteroatom into a molybdenum-containing isopolyacid.

[0139] Examples of tungsten-based heteropolyacids include phosphotungstic acid, silicotungstic acid, cobaltotungstic acid, germanotungstic acid, borotungstic acid, phosphovanadotungstic acid, and phosphotungstomolybdic acid.

[0140] Examples of molybdenum heteropolyacids include phosphomolybdic acid, silicomolybdic acid, and phosphovanadomolybdic acid.

[0141] Any suitable inorganic nitride may be used as the inorganic nitride as long as it does not impair the effects of the present invention. Examples of such inorganic nitrides include boron nitride, carbon nitride, aluminum nitride, and gallium nitride, and boron nitride and aluminum nitride are preferred.

[0142] The inorganic nitride may be of only one type, or of two or more types.

[0143] In the present invention, like the inorganic oxides described above, inorganic nitride particles are preferred as the inorganic nitride, in that the effects of the present invention can be more effectively exhibited.

[0144] The average particle size of the inorganic nitride particles can be appropriately set depending on the purpose. In terms of being able to further exhibit the effects of the present invention, the average particle size of the inorganic nitride particles is preferably 0.01 μm to 100 μm, and particularly preferably 0.1 μm to 10 μm.

[0145] The average particle size of the inorganic nitride particles is the average particle size in the volume-based particle size distribution, and is preferably measured by a laser diffraction scattering method.

[0146] In order to further enhance the effects of the present invention, inorganic nitride particles are preferably inorganic nitride particles having functional groups on their surfaces. Examples of such functional groups include hydroxyl functional groups such as M-OH; oxygen functional groups containing ether functional groups such as MOM; nitrogen functional groups containing amine functional groups such as M-NH2 and M-NH-M; sulfur functional groups containing thiol functional groups such as M-SH and MSM; silicon functional groups, boron functional groups, phosphorus functional groups, etc. (M conceptually represents the object to which the functional group binds, and represents any suitable object to which the functional group can bind, such as the inorganic nitride itself, for example, a metal element or organic group constituting the inorganic nitride). These functional groups can be easily formed by, for example, surface-treating the inorganic nitride with various compounds.

[0147] When inorganic nitride particles having functional groups on their surfaces are used as the inorganic nitride, the functional groups present on the surfaces of the inorganic nitride particles can form bonds with the carbon material in the carbon-containing material. The region of the carbon material contributing to such bonding (carbon material-bonded region) is not the carbon material itself. That is, as with the inorganic oxide particles having functional groups on their surfaces, as shown in FIG. 1, an organic-inorganic composite 100 in one preferred embodiment of the carbon-containing material (details will be described later) is a matrix of carbon material 10 in which a plurality of inorganic particles 20 (in this case, inorganic nitride particles) are dispersed. At the interface between the carbon material 10 and the inorganic particles 20, a region of the carbon material (carbon material-bonded region) 30 is present, resulting from the carbon material forming bonds with the functional groups present on the surfaces of the inorganic particles 20. Then, for example, when the carbon material is soluble in a solvent, treating the organic-inorganic composite 100 with a solvent that dissolves the carbon material can produce core-shell particles (core portion: inorganic nitride particle, shell portion: carbon material-bonded region) 200 in which the surfaces of inorganic particles 20 are coated with carbon material-bonded regions (regions that are not dissolved by the solvent) 30, as shown in Fig. 2. Removing the inorganic particles 20 as core portions from the core-shell particles 200 thus obtained can produce hollow carbon microparticles containing the carbon material.

[0148] Any suitable inorganic sulfide can be used as the inorganic sulfide as long as it does not impair the effects of the present invention. Examples of such inorganic sulfides include copper sulfide, zinc sulfide, and cadmium sulfide.

[0149] The inorganic sulfide may be of only one type, or of two or more types.

[0150] In the present invention, inorganic sulfide particles are preferred as the inorganic sulfide, similar to the inorganic oxides described above, in that the effects of the present invention can be more effectively exhibited.

[0151] The average particle size of the inorganic sulfide particles can be appropriately set depending on the purpose. In terms of being able to further exhibit the effects of the present invention, the average particle size of the inorganic sulfide particles is preferably 0.01 μm to 100 μm, and particularly preferably 0.1 μm to 10 μm.

[0152] The average particle size of the inorganic sulfide particles is the average particle size in a volume-based particle size distribution, and is preferably measured by a laser diffraction scattering method.

[0153] In order to further enhance the effects of the present invention, the inorganic sulfide particles are preferably inorganic sulfide particles having functional groups on their surfaces. Examples of such functional groups include hydroxyl functional groups such as M-OH; oxygen functional groups containing ether functional groups such as MOM; nitrogen functional groups containing amine functional groups such as M-NH2 and M-NH-M; sulfur functional groups containing thiol functional groups such as M-SH and MSM; and silicon functional groups, boron functional groups, phosphorus functional groups, etc. (M conceptually represents the object to which the functional group is bonded, and represents any suitable object to which the functional group can be bonded, such as the inorganic sulfide itself, for example, a metal element or organic group constituting the inorganic sulfide.) These functional groups can be easily formed by surface-treating the inorganic sulfide with various compounds.

[0154] When inorganic sulfide particles having functional groups on their surfaces are used as the inorganic sulfide, the functional groups present on the surfaces of the inorganic sulfide particles can form bonds with the carbon material in the carbon-containing material. The region of the carbon material contributing to such bonding (carbon material-bonded region) is not the carbon material itself. That is, as with the inorganic oxide particles having functional groups on their surfaces, as shown in FIG. 1, an organic-inorganic composite 100 in one preferred embodiment of the carbon-containing material (details will be described later) is a carbon material 10 matrix containing a plurality of inorganic particles 20 (in this case, inorganic sulfide particles), and a carbon material region (carbon material-bonded region) 30 is present at the interface between the carbon material 10 and the inorganic particles 20, resulting from bonding between the carbon material and the functional groups present on the surfaces of the inorganic particles 20. Then, for example, when the carbon material is soluble in a solvent, treating the organic-inorganic composite 100 with a solvent that dissolves the carbon material can produce core-shell particles (core portion: inorganic nitride particle, shell portion: carbon material-bonded region) 200 in which the surfaces of inorganic particles 20 are coated with carbon material-bonded regions (regions that are not dissolved by the solvent) 30, as shown in Fig. 2. Removing the inorganic particles 20 as core portions from the core-shell particles 200 thus obtained can produce hollow carbon microparticles containing the carbon material.

[0155] Any suitable inorganic carbide can be used as long as it does not impair the effects of the present invention, such as silicon carbide, tungsten carbide, calcium carbide, etc.

[0156] The inorganic carbide may be of only one type or of two or more types.

[0157] In the present invention, like the inorganic oxides described above, inorganic carbide particles are preferred as the inorganic carbide, in that they can more effectively exhibit the effects of the present invention.

[0158] The average particle size of the inorganic carbide particles can be appropriately set depending on the purpose. In terms of being able to further exhibit the effects of the present invention, the average particle size of the inorganic carbide particles is preferably 0.01 μm to 100 μm, and particularly preferably 0.1 μm to 10 μm.

[0159] The average particle size of the inorganic carbide particles is the average particle size in the volume-based particle size distribution, and is preferably measured by a laser diffraction scattering method.

[0160] In order to further enhance the effects of the present invention, the inorganic carbide particles are preferably inorganic carbide particles having functional groups on their surfaces. Examples of such functional groups include hydroxyl functional groups such as M-OH; oxygen functional groups containing ether functional groups such as MOM; nitrogen functional groups containing amine functional groups such as M-NH2 and M-NH-M; sulfur functional groups containing thiol functional groups such as M-SH and MSM; and silicon functional groups, boron functional groups, phosphorus functional groups, etc. (M conceptually represents the target to which the functional group binds, and represents any suitable target to which the functional group can bind, such as the inorganic carbide itself, for example, a metal element or organic group constituting the inorganic carbide.) These functional groups can be easily formed by, for example, surface-treating the inorganic carbide with various compounds.

[0161] When inorganic carbide particles having functional groups on their surfaces are used as the inorganic carbide, the functional groups present on the surfaces of the inorganic carbide particles can form bonds with the carbon material in the carbon-containing material. The regions of the carbon material contributing to such bonds (carbon material-bonded regions) are not the carbon material itself. That is, as with the inorganic oxide particles having functional groups on their surfaces, as shown in FIG. 1, an organic-inorganic composite 100 in one preferred embodiment of the carbon-containing material (details will be described later) is a matrix of carbon material 10 in which a plurality of inorganic particles 20 (in this case, inorganic carbide particles) are dispersed. At the interface between the carbon material 10 and the inorganic particles 20, regions of the carbon material (carbon material-bonded regions) 30 are present, resulting from the carbon material forming bonds with the functional groups present on the surfaces of the inorganic particles 20. Then, for example, when the carbon material is soluble in a solvent, treating the organic-inorganic composite 100 with a solvent that dissolves the carbon material can produce core-shell particles (core portion: inorganic nitride particle, shell portion: carbon material-bonded region) 200 in which the surfaces of inorganic particles 20 are coated with carbon material-bonded regions (regions that are not dissolved by the solvent) 30, as shown in Fig. 2. Removing the inorganic particles 20 as core portions from the core-shell particles 200 thus obtained can produce hollow carbon microparticles containing the carbon material.

[0162] As the insoluble salt, any appropriate insoluble salt can be used as long as it does not impair the effects of the present invention. Such insoluble salts are preferably metal-containing salts that are insoluble in organic solvents, such as metal phosphates such as lithium iron phosphate and metal sulfates, and are preferably lithium iron phosphate.

[0163] The insoluble salt may be of only one kind or of two or more kinds.

[0164] The insoluble salt may be any salt as long as it is insoluble in the solvent used in the method for producing a carbonaceous material according to an embodiment of the present invention. For example, when a solvent is used in the step of mixing compound (A) with an inorganic substance, the inorganic substance may be insoluble in the solvent. In other words, an appropriate solvent that does not dissolve the inorganic substance may be selected depending on the inorganic substance. The same applies to the carbonaceous material removal step in the method for producing a carbonaceous material according to an embodiment of the present invention. Note that, when producing hollow carbon microparticles or the like, the method for producing a carbonaceous material according to an embodiment of the present invention preferably includes a step of dissolving an inorganic substance. However, even if such a step of dissolving an inorganic substance is included, an inorganic substance that is insoluble in the solvent may be selected in the step prior to the step. The insoluble salt means that it can be dissolved in a solvent under certain conditions, but is insoluble in the solvent in the production method that can achieve the effects of the present invention. Furthermore, the insoluble salt is preferably in the form of particles, and the preferred range of the average particle size is the same as that of the oxide.

[0165] When at least one type selected from the group consisting of silica particles and polyacid particles is used as the inorganic oxide particles having functional groups on their surfaces, the functional groups present on the surfaces of the inorganic oxide particles are more likely to form bonds with the carbon material, and the resulting carbon material-containing material preferably has the following aspect (4) in particular.

[0166] (4) In IR analysis, preferably, 1660 cm -1 ~1800cm -1 In the IR analysis of carbon-containing materials, no peak due to C=O stretching vibration is observed between 1660 cm -1 ~1800cm -1 When no peak due to C═O stretching vibration is observed between these, the structure of the carbonaceous material can be more precisely controlled.

[0167] 2. Representative Examples of Methods for Producing Carbon-Containing Materials A wide variety of carbonaceous materials can be produced by the method for producing a carbonaceous material of the present invention, and they can take various shapes such as particulate and non-particulate (for example, fibrous, thin film, etc.). Particulate shapes are preferred.

[0168] As described above, when inorganic substances of various shapes such as particulate inorganic substances (inorganic particles) and non-particulate inorganic substances (for example, fibrous inorganic substances, thin film inorganic substances, etc.) are used as the inorganic substance, a wide variety of carbon material-containing materials can be obtained depending on the respective shapes. Particulate inorganic substances (inorganic particles) are preferred as the inorganic substance.

[0169] When inorganic particles are used, the method for producing a carbonaceous material of the present invention can typically produce a clumped carbonaceous material containing a large number of inorganic particles. In this case, a particulate carbonaceous material can be obtained by crushing or the like. Furthermore, by adjusting the blending ratio of compound (A) and the inorganic substance, the method for producing a carbonaceous material of the present invention can sometimes produce a particulate carbonaceous material.

[0170] When a fibrous inorganic substance is used, the method for producing a carbonaceous material of the present invention can produce fibrous core-shell fibers instead of core-shell particles, which will be described later. Also, when a fibrous inorganic substance is used, the method for producing a carbonaceous material of the present invention can produce tubular hollow carbonaceous materials instead of hollow carbon microparticles, which will be described later.

[0171] When a thin film of an inorganic substance is used, a layered carbon material-containing material can be obtained by the method for producing a carbon material-containing material of the present invention. Furthermore, by further subjecting such a layered carbon material-containing material to the heating step (II), the carbon material removing step, the inorganic substance removing step, etc., which will be described later, various thin film carbon materials can be obtained.

[0172] In the carbonaceous material that can be produced by the method for producing a carbonaceous material of the present invention, the film thickness of the carbonaceous material portion can be controlled to be used for various purposes. For example, the film thickness of such a carbonaceous material portion can be described as a typical specific embodiment. (Aspect 1) A film thickness of a carbon material portion in a carbon material-containing material obtained by removing all carbon materials other than the carbon material that strongly interacts with the outermost surface of an inorganic material and is present on the surface of the inorganic material through a carbon material removal step; (Embodiment 2) The film thickness of the carbon material portion of the carbon material-containing material in a state in which all or part of the carbon material portion of the carbon material-containing material remains, Examples include:

[0173] More specifically, the carbon material portion in the above (Aspect 1) is a carbon material portion that strongly interacts with the outermost surface of the inorganic substance, obtained by removing all carbon materials (typically, soluble carbon materials) other than the carbon material that strongly interacts with the outermost surface of the inorganic substance through the carbon material removal step. The film thickness of such a carbon material portion is thin, and although it depends on the structure of the carbon material, it is preferably 0.3 nm to 10 nm, and more preferably 0.4 nm to 3 nm. By controlling the film thickness of the carbon material portion within this range, the carbon component that strongly interacts with the inorganic substance can be fully utilized in various applications.

[0174] In the above (Aspect 1), typically, the film thickness of the carbon material portion is thin, but it is also possible to adjust the thickness without any upper limit by using an appropriate carbon material removal method.

[0175] The film thickness of the carbon material portion in (Aspect 2) above is typically thicker than the film thickness of the carbon material portion in (Aspect 1) above, but to better function as a carbon material film, it is preferably 100 μm or less, more preferably 50 μm or less, even more preferably 10 μm or less, and most preferably 1 μm or less. In (Aspect 2) above, if the film thickness of the carbon material portion is controlled within this range, it can fully function as a film.

[0176] The film thickness of the carbon material portion can be appropriately controlled by the type of raw material compound (for example, compound (A)) used in the method for producing the carbon-containing material and the production conditions.

[0177] The thickness of the carbon material portion can be confirmed by various analytical methods, such as a method of direct observation using an electron microscope (Method A) or a method of estimating the amount of carbon calculated by elemental analysis or thermogravimetric analysis from the macroscopic surface area of ​​the inorganic material (excluding the surface area of ​​a microstructure into which organic molecules cannot penetrate, as in the present invention) and the density of the carbon material (Method B).

[0178] More specifically, the above-mentioned (Method A) can be exemplified by a method in which a cross section of a carbon material-containing sample is observed using a transmission electron microscope or a scanning electron microscope, preferably a transmission electron microscope or a scanning electron microscope equipped with an energy dispersive X-ray analyzer.

[0179] In the above (Method B), the macroscopic surface area of ​​the inorganic substance can be estimated from the shape of the carbon material-containing material serving as the sample and the shape of the inorganic substance contained therein.

[0180] In the above (Method A), for example, when the sample is a particle, it is preferable to measure the thickness of each particle contained in the sample at three or more locations and use the simple average value as the film thickness of the particle, and more preferably, it is preferable to measure the film thickness of 10 or more particles and use the simple average value as the average film thickness of the sample. It is preferable that the film thickness (average film thickness) obtained in this way falls within the desired film thickness range that is desired to be controlled, for example.

[0181] In the above (Method B), the analyzed film thickness can be regarded as the average film thickness of the sample. It is preferable that the film thickness analyzed by this (Method B) falls within the desired film thickness range that is desired to be controlled, for example.

[0182] Representative embodiments of such carbon material-containing materials include organic-inorganic composites, carbon material-containing particles, etc. Examples of carbon material-containing particles include core-shell particles, highly carbonized core-shell particles, hollow carbon microparticles, highly carbonized hollow carbon microparticles, etc. Hereinafter, representative and specific carbon material-containing materials and their manufacturing methods will be described.

[0183] 2-1. Manufacturing method of organic-inorganic composite One embodiment of the carbon material-containing material obtained by the production method of the present invention is an organic-inorganic composite.

[0184] The organic-inorganic composite can typically be obtained by a heating step (I) in which a composition containing a compound (A) and an inorganic substance is heated so that a condensation reaction between the same molecules and / or different molecules occurs upon heating.

[0185] The organic-inorganic composite contains a carbon material and an inorganic substance. The carbon material can be typically produced by heating a composition containing a compound (A) and an inorganic substance, in a heating step (I) in which the compound (A) undergoes a condensation reaction between the same molecules and / or different molecules upon heating. The explanation in 1-2. Inorganic substance can be used for the term "inorganic substance."

[0186] The carbon material may be of only one type or may be of two or more types, and the inorganic material may be of only one type or may be of two or more types.

[0187] The content of the carbon material in the organic-inorganic composite is preferably 0.01% by mass to 99.99% by mass, and particularly preferably 0.1% by mass to 99.9% by mass. If the content of the carbon material in the organic-inorganic composite is within the above range, the organic-inorganic composite can be produced industrially under mild conditions, and hollow carbon microparticles and the like can be produced industrially using the organic-inorganic composite as a material. The content of these carbon materials can be easily adjusted to any desired ratio by various removal processes, etc., as described below, depending on the desired physical properties.

[0188] The content of the inorganic substance in the organic-inorganic composite is preferably 0.01% by mass to 99.99% by mass, and particularly preferably 0.1% by mass to 99.9% by mass. If the content of the inorganic substance in the organic-inorganic composite is within the above range, the organic-inorganic composite can be industrially produced under mild conditions, and hollow carbon microparticles and the like can be industrially produced using the organic-inorganic composite as a material. The content of these inorganic substances can be easily adjusted to any desired ratio by various removal processes, etc., as described below, depending on the desired physical properties.

[0189] In the organic-inorganic composite, the ratio of all carbon-oxygen bonds, i.e., the total amount of C-C bonds, C=C bonds, C-H bonds, and C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), to the total amount of C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), as determined by C1s XPS analysis, is preferably 10% or more, more preferably 20% or more, and even more preferably 25% or more. The upper limit of this ratio is preferably 35% or less. In the organic-inorganic composite, if the ratio of the total amount of C-O bonds and C=O bonds to the total amount of C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds as determined by C1s XPS analysis is within the above range, the organic-inorganic composite can be a novel carbon-containing material with various physical properties such as solubility, unlike conventionally known simple carbon materials.

[0190] In the organic-inorganic composite, the ratio of the total amount of ether-derived CO bonds (i.e., CO-C bonds) and alcohol-derived CO bonds (i.e., C-OH bonds) to the total amount of all carbon-oxygen bonds, i.e., CO bonds (including alcohol-derived CO bonds, ether-derived CO bonds, epoxy-derived CO bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.) determined by C1s XPS analysis is preferably 50% or more, more preferably 60% or more, even more preferably 65% ​​or more, particularly preferably 70% or more, and most preferably 75% or more. The upper limit of the above ratio is preferably 90% or less. In the organic-inorganic composite, if the ratio of the total amount of ether-derived CO bonds and alcohol-derived CO bonds to the total amount of CO bonds and C=O bonds determined by C1s XPS analysis is within the above range, the organic-inorganic composite can increase the structural control rate of the carbon material portion and the structure can be controlled more precisely. In other words, the lower the ratio of C=O bonds resulting from the decomposition reaction, the more the decomposition reaction is suppressed, and such organic-inorganic composites can be said to be carbon-containing materials with a more precisely controlled structure.

[0191] In the organic-inorganic composite, the ratio of the total amount of ether-derived CO bonds (i.e., CO-C bonds) and alcohol-derived CO bonds (i.e., C-OH bonds) to the total amount of all bonds, i.e., C-C bonds, C-H bonds, C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), and C-O bonds (including carbonyl-derived C-O bonds, carboxyl-derived C-O bonds, ester-derived C-O bonds, lactone-derived C-O bonds, etc.), as determined by C1s XPS analysis, is preferably 15% or more, more preferably 17% or more, and even more preferably 20% or more. The upper limit of this ratio is preferably 30% or less. In the carbon material-containing material, if the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of all bonds as determined by C1s XPS analysis is within the above range, the organic-inorganic composite can be said to be an organic-inorganic composite with a more precisely controlled structure.

[0192] The organic-inorganic composite is particularly preferably a composite in which, according to C1sXPS analysis, the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, and C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.) is the ratio of the total amount of all carbon-oxygen bonds, i.e., C-O bonds and C=O bonds, is within the above range, and, according to C1sXPS analysis, the total amount of all carbon-oxygen bonds, i.e., C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.) is the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) is within the above range. In such an embodiment, the organic-inorganic composite can further increase the solubility of the carbon material portion and can further increase the structural control rate of the carbon material portion. Furthermore, in such an embodiment, the structure of the organic-inorganic composite can be controlled more precisely.

[0193] The organic-inorganic composite is particularly preferably a composite in which, according to C1sXPS analysis, the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, and C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), the ratio of the total amount of all carbon-oxygen bonds, i.e., C-O bonds and C=O bonds, is within the above range, and, according to C1sXPS analysis, the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, and C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.), and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.), the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) is within the above range. In such an embodiment, the organic-inorganic composite can further increase the solubility of the carbon material portion and can further increase the structural control rate of the carbon material portion. Furthermore, in such an embodiment, the structure of the organic-inorganic composite can be controlled more precisely.

[0194] The organic-inorganic composite is most preferably such that the ratio of all carbon-oxygen bonds, i.e., the total amount of C-C bonds, C=C bonds, C-H bonds, and C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) and C=O bonds (including carbonyl-derived C=O bonds, carboxyl-derived C=O bonds, ester-derived C=O bonds, lactone-derived C=O bonds, etc.) to the total amount of all bonds, i.e., C-C bonds, C=C bonds, C-H bonds, and C-O bonds (including alcohol-derived C-O bonds, ether-derived C-O bonds, epoxy-derived C-O bonds, etc.) by C1sXPS analysis, i.e., the total amount of C=O bonds and C=O bonds, is within the above range, and In this embodiment, the ratio of the total amount of ether-derived C-O bonds (i.e., C-O-C bonds) and alcohol-derived C-O bonds (i.e., C-OH bonds) to the total amount of C=O bonds (including C=O bonds derived from alcohols, C=O bonds derived from ether ...

[0195] The organic-inorganic composite preferably has a peak at 1660 cm in IR analysis. -1 ~1800cm -1 In the IR analysis of the organic-inorganic composite, no peak due to C=O stretching vibration is observed between 1660 cm -1 ~1800cm -1When no peak due to C═O stretching vibration is observed between these, the structure of the organic-inorganic composite can be controlled more precisely.

[0196] In IR analysis of organic-inorganic composites, -1 ~1800cm -1 The reason why the structure of the organic-inorganic composite can be controlled more precisely when no peak due to C=O stretching vibration is observed between these two peaks is thought to be as follows. That is, when an organic-inorganic composite is formed using the compounds and manufacturing method described below, the aromatic skeleton and oxygen functional groups remain in the product after the reaction due to the condensation reaction. At this time, if the aromatic structure is maintained (in other words, if the structure is controlled), it is thought that the C-O bond of the ether bridge or the C-O bond derived from the alcohol, as well as the oxygen functional groups, will undergo elimination condensation, resulting in the formation of a C-C bond in which the aromatic skeleton bonds together. On the other hand, if an undesired decomposition reaction occurs and the aromatic skeleton structure is cleaved, a C=O bond resulting from the decomposition reaction will be generated. Therefore, in IR analysis, -1 ~1800cm -1 The absence of a peak due to C=O stretching vibration between 1700 cm and 1700 cm indicates that the decomposition reaction is suppressed, and such an organic-inorganic composite can be said to be a carbon material-containing material with a more precisely controlled structure. -1 ~1800cm -1 The range is.

[0197] When the organic-inorganic composite is subjected to TG-DTA analysis under an air atmosphere at a temperature increase from 40°C at a rate of 10°C / min, the oxidation onset temperature indicated by the DTA rise temperature is preferably 200°C or higher, more preferably 250°C or higher, and most preferably 300°C or higher. When the organic-inorganic composite is subjected to TG-DTA analysis under an air atmosphere at a temperature increase from 40°C at a rate of 10°C / min, the oxidation onset temperature indicated by the DTA rise temperature is within the above range. If this temperature is within the above range, the carbon material-containing material of the present invention has high oxidation stability, i.e., the structure is controlled and the skeletal structure is maintained, resulting in high oxidation resistance (decomposition resistance). If skeletal cleavage occurs, such as the generation of C=O bonds, the stability of the skeletal structure may decrease, and the oxidation resistance (decomposition resistance) may be reduced.

[0198] As described above, the organic-inorganic composite, which is one embodiment of the carbon-containing material obtained by the production method of the present invention, contains a carbon material and an inorganic substance. The organic-inorganic composite, which is one embodiment of the carbon-containing material obtained by the production method of the present invention, contains a "carbon material" as described above. Typically, as described above, the organic-inorganic composite can be produced by heating a composition containing a compound (A) and an inorganic substance, in which a condensation reaction between identical molecules and / or different molecules occurs upon heating. The following explanation of the "carbon material" contained in the organic-inorganic composite, which is one embodiment of the carbon-containing material obtained by the production method of the present invention, can be used to explain the "carbon material" mentioned in the previous section "1. Production method of a carbon-containing material," the "carbon material" mentioned in the section "2. Representative examples of production methods for carbon-containing materials" other than this "2-1. Production method of an organic-inorganic composite," and the "carbon material" mentioned in the section "3. Carbon-containing material."

[0199] The presence of carbon components in carbon materials can be easily confirmed by C1s XPS analysis. Furthermore, carbon materials preferably have a honeycomb structure (graphene structure) derived from benzene rings within their structure. The presence or absence of the graphene structure can be confirmed by Raman spectroscopy (Non-Patent Document 4).

[0200] The total content of metal impurities in carbon materials is typically preferably 0.1 atomic % or less, more preferably 0.01 atomic % or less, and particularly preferably substantially zero, relative to 100 atomic % of carbon atoms. This can be confirmed by analyzing the carbon material using X-ray fluorescence elemental analysis (XRF). Furthermore, when a carbon material-containing material (an organic-inorganic composite in this section) is analyzed using X-ray fluorescence elemental analysis (XRF), the content of metal components other than the metal components contained in the inorganic matter constituting the carbon material-containing material (an organic-inorganic composite in this section) is preferably 0.1 atomic % or less, more preferably 0.01 atomic % or less, and particularly preferably substantially zero, relative to 100 atomic % of carbon atoms. For example, when a carbon material-containing material (an organic-inorganic composite in this section) using alumina as the inorganic matter is analyzed using X-ray fluorescence elemental analysis (XRF), if the only metal component contained in the alumina is aluminum, the content of metal components other than aluminum is preferably 0.1 atomic % or less, more preferably 0.01 atomic % or less, and particularly preferably substantially zero, relative to 100 atomic % of carbon atoms.

[0201] Carbon materials essentially contain carbon as a constituent element, but may contain elements other than carbon. Such elements other than carbon are preferably at least one element selected from oxygen, hydrogen, nitrogen, sulfur, fluorine, chlorine, bromine, and iodine, more preferably at least one element selected from oxygen, hydrogen, nitrogen, and sulfur, even more preferably at least one element selected from oxygen, hydrogen, and nitrogen, and particularly preferably at least one element selected from oxygen and hydrogen. When the total amount of elements other than hydrogen constituting the carbon material is taken as 100 atomic %, carbon preferably accounts for 60 atomic % or more, more preferably 70 atomic % or more, and even more preferably 75 atomic % or more. Furthermore, elements other than carbon are preferably 10 atomic % or more. By ensuring that the proportions of each element fall within these ranges, the carbon material can exhibit good solubility. These properties can be confirmed by quantifying the carbon material using X-ray photoelectron spectroscopy (C1sXPS). Furthermore, when a carbon material-containing material (organic-inorganic composite in this section) is quantified by X-ray photoelectron spectroscopy (C1sXPS), when the total amount of elements other than those contained in the inorganic matter constituting the carbon material-containing material (organic-inorganic composite in this section) is taken as 100 atomic %, carbon is preferably 60 atomic % or more, more preferably 70 atomic % or more, and even more preferably 75 atomic % or more. Furthermore, elements other than carbon are preferably 10 atomic % or more. For example, when a carbon material-containing material (organic-inorganic composite in this section) using phosphotungstic acid as the inorganic matter is analyzed by X-ray photoelectron spectroscopy (C1sXPS), phosphorus and tungsten are detected, but it is preferable that the ratio of the amount of carbon to the total amount of elements other than the amount of oxygen (excluding hydrogen) constituting the phosphotungstic acid calculated from the phosphorus, tungsten, and phosphorus and tungsten contents, and the ratio of elements other than carbon, fall within the above ranges.

[0202] The carbon material is preferably soluble in the solvent.

[0203] Here, when a carbon material is soluble in a solvent, it means that the carbon material has superior solubility in a solvent compared to conventional carbon materials and can be easily handled.

[0204] The carbon material can be preferably soluble in a solvent in the following manner. (Embodiment 1) An embodiment in which the entire carbon material is soluble in a solvent, i.e., an embodiment in which the carbon material consists only of a component (component A) that is soluble in a solvent. (Embodiment 2) An embodiment in which a portion of the carbon material dissolves in a solvent. That is, an embodiment in which the carbon material comprises a component (component A) that dissolves in a solvent and a component (component B) that does not dissolve in the solvent. In this case, component B includes a portion that interacts with an inorganic substance and does not dissolve.

[0205] In the present invention, "soluble in a solvent" means an embodiment in which the component is soluble in any solvent, and preferred examples of the solvent include N,N-dimethylformamide, N,N-dimethylacetamide, N-methylpyrrolidone, dimethyl sulfoxide, acetone, methyl ethyl ketone, methyl isobutyl ketone, tetrahydrofuran, methanol, ethanol, 2-propanol, butanol, chloroform, dichloromethane, etc. That is, a preferred embodiment is one in which the component is soluble in at least one solvent selected from the group consisting of N,N-dimethylformamide, N,N-dimethylacetamide, N-methylpyrrolidone, dimethyl sulfoxide, acetone, methyl ethyl ketone, methyl isobutyl ketone, tetrahydrofuran, methanol, ethanol, 2-propanol, butanol, chloroform, and dichloromethane. More preferably, the composition contains a component that is soluble in at least one solvent selected from the group consisting of N,N-dimethylformamide, N,N-dimethylacetamide, N-methylpyrrolidone, dimethyl sulfoxide, and chloroform. Even more preferably, the composition contains a component that is soluble in at least one solvent selected from the group consisting of N,N-dimethylformamide and N-methylpyrrolidone. Particularly preferably, the composition contains a component that is soluble in N-methylpyrrolidone.

[0206] One embodiment in which the carbon material is soluble in the solvent is, for example, an embodiment in which the carbon material comprises a carbon-based compound that is soluble in the solvent.

[0207] To determine whether a material is soluble in a solvent, for example, a carbonaceous material (in this case, an organic-inorganic composite) is mixed with the solvent to a concentration of 0.001% by mass, followed by ultrasonic treatment for 1 hour. The resulting liquid is then passed through a PTFE filter paper (pore size 0.45 μm). The liquid that passes through the filter paper is then examined to determine whether it contains a carbonaceous compound. If the liquid that passes through the filter paper contains a carbonaceous compound, the carbonaceous material is determined to contain a carbonaceous compound that is soluble in the solvent. For example, a GL Chromatodisc (Model 13P) manufactured by GL Sciences Inc. can be used as the PTFE filter paper.

[0208] The carbon material preferably has (i) a G band (generally 1550 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~1650cm -1 Therefore, the carbon material exhibits a peak in the G band (generally in the range of 1550 cm ) in the Raman spectrum obtained by Raman spectroscopy. -1 ~1650cm -1 A peak in the range of 0.01 to 0.10 indicates that the carbon material has a graphene structure or a structure similar to that of graphene. The stronger and sharper the G band, the better the graphene structure or a structure similar to that of graphene.

[0209] The carbon material preferably has (ii) a D band (generally around 1300 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~1400cm -1 Carbon materials with structures derived from defects in the graphene structure exhibit a peak in the D band (generally in the range of 1300 cm ) in the Raman spectrum obtained by Raman spectroscopy. -1 ~1400cm -1 Therefore, the carbon material exhibits a peak in the D band (generally in the range of 1300 cm ) in the Raman spectrum obtained by Raman spectroscopy. -1 ~1400cm -1The presence of a peak within the range of (a) to (d) indicates that the carbon material contains a functional group or has a structure derived from defects in the graphene structure or a structure similar to a structure derived from defects in the graphene structure. A lower intensity of the D band indicates a cleaner graphene structure or a structure similar to a graphene structure. Furthermore, the presence of the D band indicates that the carbon-containing material obtained by the production method of the present invention has a functional group, which can increase its solubility in a solvent.

[0210] The carbon material preferably has (i) a G band (generally 1550 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~1650cm -1 (ii) a peak in the D band (generally in the range of 1300 cm ) in the Raman spectrum obtained by Raman spectroscopy; -1 ~1400cm -1 The peak is within the range of

[0211] The carbon material preferably has (iii) a G′ band (generally 2650 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~2750cm -1 Therefore, the carbon material exhibits a peak in the G′ band (generally in the range of 2650 cm ) in the Raman spectrum obtained by Raman spectroscopy. -1 ~2750cm -1 The presence of a peak in the G' band (within the range of 1 / 2 sq. m) indicates that the carbon material has a graphene structure or a structure similar to that of graphene. The intensity of the G' band is strongest when the graphene structure is a single layer and gradually decreases as the number of layers in the graphene structure increases. However, even if the intensity of the G' band gradually decreases as the number of layers in the graphene structure increases, the peak can still be observed. Therefore, the presence of a peak in the G' band indicates that the carbon material has a graphene structure or a structure similar to that of graphene. The G' band is sometimes called the 2D band.

[0212] The carbon material preferably has (i) a G band (generally 1550 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~1650cm -1 (ii) a peak in the D band (generally in the range of 1300 cm ) in the Raman spectrum obtained by Raman spectroscopy; -1 ~1400cm -1 (iii) a peak in the G′ band (generally 2650 cm ) in the Raman spectrum obtained by Raman spectroscopy; -1 ~2750cm -1 The peak is within the range of

[0213] The carbon material preferably exhibits (iv) a D+D′ band (generally around 2800 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~3000cm -1 Carbon materials with structures derived from defects in the graphene structure exhibit a peak in the D+D′ band (generally in the range of 2800 cm ) in the Raman spectrum obtained by Raman spectroscopy. -1 ~3000cm -1 Therefore, the carbon material exhibits a peak in the D+D′ band (generally in the range of 2800 cm ) in the Raman spectrum obtained by Raman spectroscopy. -1 ~3000cm -1 The presence of a peak within this range (in the range of ) indicates that the carbon material contains functional groups or has a structure derived from defects in the graphene structure or a structure similar to a structure derived from defects in the graphene structure. If the intensity of the D+D' band is low, it can be said that the carbon material has a cleaner graphene structure or a structure similar to a graphene structure. The D+D' band is also sometimes called the D+G band. Furthermore, the presence of the D+D' band also indicates that the carbon-containing material obtained by the production method of the present invention has functional groups, which can increase its solubility in solvents.

[0214] The carbon material preferably has (i) a G band (generally 1550 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~1650cm -1 (ii) a peak in the D band (generally in the range of 1300 cm ) in the Raman spectrum obtained by Raman spectroscopy; -1 ~1400cm -1 (iii) a peak in the G′ band (generally 2650 cm ) in the Raman spectrum obtained by Raman spectroscopy; -1 ~2750cm -1 (iv) a peak in the D+D′ band (generally in the range of 2800 cm ) in the Raman spectrum obtained by Raman spectroscopy; -1 ~3000cm -1 The peak is within the range of

[0215] The carbon material preferably comprises a carbon-based compound that is soluble in the solvent.

[0216] In one embodiment, the carbon material may, for example, (i) exhibit a G band (generally 1550 cm ) in a Raman spectrum obtained by Raman spectroscopy. -1 ~1650cm -1 (ii) a peak in the D band (generally in the range of 1300 cm ) in the Raman spectrum obtained by Raman spectroscopy; -1 ~1400cm -1 The carbon-based compounds exhibit peaks in the range of 100 to 1500 nm and are soluble in the solvent.

[0217] When a carbon material contains a functional group and also has defects in a part of the graphene structure, these defects can contribute to the solubility of the carbon material in a solvent.

[0218] As described above, the carbon material has a graphene structure or a structure similar to a graphene structure, unlike conventionally known carbon materials, and has better solubility in solvents (for example, more components of the carbon material dissolve in solvents, or more types of solvents in which the carbon material can be dissolved).

[0219] The molecular weight of the carbon-based compound contained in the carbon material is preferably 1,000 to 1,300,000, more preferably 5,000 to 1,000,000, even more preferably 10,000 to 700,000, particularly preferably 15,000 to 500,000, and most preferably 20,000 to 300,000. When the molecular weight of the carbon-based compound contained in the carbon material is within the above range, combined with the characteristic (i) above, the solubility of the carbon material in solvents is improved (e.g., more components of the carbon material dissolve in solvents, or the number of solvents in which the carbon material can be dissolved increases). If the molecular weight of the carbon-based compound contained in the carbon material exceeds 1,300,000, the solubility of the carbon material in solvents may be reduced. If the molecular weight of the carbon-based compound contained in the carbon material is less than 1,000, the characteristics of the carbon material may be diminished. These molecular weights can be analyzed using the methods described below.

[0220] The content of the carbon-based compound in the carbon material is preferably 50% by mass to 100% by mass, more preferably 70% by mass to 100% by mass, even more preferably 90% by mass to 100% by mass, particularly preferably 95% by mass to 100% by mass, and most preferably substantially 100% by mass. When the content of the carbon-based compound in the carbon material is within the above range, combined with the above features (i) and (ii), the solubility of the carbon material in solvents becomes more excellent (for example, more components of the carbon material dissolve in solvents, or more types of solvents in which the carbon material can be dissolved).

[0221] The carbon material preferably exhibits a peak within a range of 20° to 30° in an XRD spectrum chart obtained by XRD analysis. That is, in one preferred embodiment, the carbon material has a structure in which graphene structures are stacked (a graphene stacked structure). By having a stacked structure, the carbon material can become stronger and more stable.

[0222] More preferred forms of the carbon material are those which have any one of the above forms (i) to (iv) or a combination thereof; (i) and (ii), (i), (ii) and (iii), or (i), (ii), (iii) and (iv) in a Raman spectrum obtained by Raman spectroscopic analysis, and which exhibit a peak within a range of 20° to 30° in an XRD spectrum chart obtained by XRD analysis.

[0223] The carbon material may preferably exist in a bulk state. Generally, the properties of a substance in a bulk state are the intrinsic properties of that substance. That is, the basic properties of the substance, such as the boiling point, melting point, viscosity, and density, can be determined for the substance in a bulk state. The physical properties of a substance refer to the properties of the bulk portion. Examples of bulk states include particles, pellets, and films. Examples of particle states include powder. Preferably, the film is a free-standing film.

[0224] 2-2. Manufacturing method of carbon material-containing particles One embodiment of the carbon material-containing material obtained by the production method of the present invention is carbon material-containing particles. Typical examples of the carbon material-containing particles include core-shell particles, highly carbonized core-shell particles, hollow carbon fine particles, and highly carbonized hollow carbon fine particles.

[0225] <2-2-1. Manufacturing method of core-shell particles> Core-shell particles can be produced by the method for producing a carbon-containing material of the present invention, which includes a carbon material removal step after the heating step (I), in which at least a portion of the carbon material generated by heating compound (A) is removed. That is, after producing an organic-inorganic composite, which is one embodiment of a carbon-containing material, through the heating step (I), the core-shell particles can be produced by subjecting the organic-inorganic composite to a carbon material removal step in which at least a portion of the carbon material contained in the composite is removed. In the carbon material removal step, the organic-inorganic composite is treated with a solvent that dissolves the carbon material contained in the composite. As a result, as shown in FIG. 2, core-shell particles 200 (core portion: inorganic particle, shell portion: carbon material-bonded region) can be obtained, in which the surface of inorganic particle 20 is coated with a carbon material-bonded region (region insoluble in the solvent) 30. Such core-shell particles are also carbon-containing materials.

[0226] Examples of the solvent include N,N-dimethylformamide, N,N-dimethylacetamide, N-methylpyrrolidone, dimethyl sulfoxide, acetone, methyl ethyl ketone, methyl isobutyl ketone, tetrahydrofuran, methanol, ethanol, 2-propanol, butanol, chloroform, and dichloromethane. Preferred are N,N-dimethylformamide, N,N-dimethylacetamide, N-methylpyrrolidone, dimethyl sulfoxide, and chloroform, more preferred are N,N-dimethylformamide and N-methylpyrrolidone, and particularly preferred is N-methylpyrrolidone.

[0227] <2-2-2. Method for producing highly carbonized core-shell particles> Highly carbonized core-shell particles can be produced by the method for producing a carbon material-containing material of the present invention, which includes a heating step (II) after the heating step (I) and the subsequent carbon material removal step, in which further heating is performed. That is, the above-mentioned core-shell particles (core portion: inorganic particles, shell portion: carbon material bonding region) are further heated. This heating step (II) can highly carbonize the shell portion. This makes it possible to obtain highly carbonized core-shell particles (core portion: inorganic particles, shell portion: highly carbonized material). High carbonization can improve the strength and heat resistance of the obtained carbon material or carbon material composite. Highly carbonized core-shell particles are also carbon material-containing materials.

[0228] The heating temperature in the heating step (II) may be within a range that the inorganic components of the core can withstand, but specific heating temperatures are preferably 500° C. to 3000° C., more preferably 600° C. to 2500° C., and most preferably 700° C. to 2000° C. By adjusting the heating temperature in the heating step (II) to within the above range, the shell portion can be effectively highly carbonized.

[0229] The heating time in the heating step (II) is preferably 0.1 to 120 hours, more preferably 0.5 to 100 hours, even more preferably 1 to 50 hours, and most preferably 2 to 24 hours. By adjusting the heating time within the above range, the shell portion can be effectively highly carbonized.

[0230] <2-2-3. Manufacturing method of hollow carbon microparticles> The hollow carbon microparticles can be produced by including an inorganic substance removal step of removing inorganic substances after the heating step (I) in the method for producing a carbon material-containing material of the present invention (Production Form 1). That is, the hollow carbon microparticles can be produced by producing an organic-inorganic composite, which is one embodiment of the carbon material-containing material, through the heating step (I), and then subjecting the organic-inorganic composite to an inorganic substance removal step of removing inorganic substances contained in the organic-inorganic composite.

[0231] Hollow carbon microparticles can also be produced by including an inorganic substance removal step of removing inorganic substances after the heating step (I) and the subsequent carbon material removal step in the method for producing a carbon material-containing material of the present invention (Production Form 2). That is, core-shell particles, which are one embodiment of the carbon material-containing material, are produced through the heating step (I) and the subsequent carbon material removal step, and then the core-shell particles are subjected to the inorganic substance removal step of removing inorganic substances contained in the core-shell particles.

[0232] The inorganic substance can be removed in the inorganic substance removal step using a solvent that dissolves the inorganic substance without dissolving the carbon material. While there are no particular limitations on the solvent with the above-described solubility characteristics, aqueous solvents are preferred. The reason why aqueous solvents are preferred is that the carbon material contained in the carbon material-containing material produced by the production method of the present invention is poorly soluble in water, while many inorganic substances are soluble in water (particularly acidic water or basic water). Examples of aqueous solvents include acidic aqueous solutions such as sulfuric acid, hydrochloric acid, and nitric acid; and basic aqueous solutions such as sodium hydroxide, potassium hydroxide, and ammonia. Furthermore, the temperature in the removal step is not particularly limited, but is preferably 0°C to 150°C, more preferably 20°C to 100°C, in order to effectively utilize the solubility characteristics of the aqueous solvent. Furthermore, the physical treatment in the removal step is not particularly limited, but is preferably standing, stirring, ultrasonic treatment, or shearing operation, more preferably stirring, ultrasonic treatment, or shearing operation, in order to effectively utilize the removability.

[0233] <2-2-4. Manufacturing method of highly carbonized hollow carbon particles> Highly carbonized hollow carbon microparticles can be produced by the method for producing a carbon material-containing material of the present invention, which further includes a heating step (II) after the heating step (I) and the subsequent inorganic substance removal step. That is, the hollow carbon microparticles obtained in the above-mentioned production form 1 are further heated. This heating step (II) can highly carbonize the carbon material portion. This makes it possible to obtain highly carbonized hollow carbon microparticles. High carbonization can improve the strength and heat resistance of the obtained carbon material or carbon material composite. Highly carbonized hollow carbon microparticles are also carbon material-containing materials.

[0234] Highly carbonized hollow carbon microparticles can also be produced by the method for producing a carbon material-containing material of the present invention, which further comprises a heating step (II) after the heating step (I), the subsequent carbon material removal step, and the subsequent inorganic matter removal step. That is, the hollow carbon microparticles obtained in the above-mentioned Production Form 2 are further heated. This heating step (II) can highly carbonize the carbon material portion.

[0235] ≪≪3. Carbon-containing materials≫≫ The carbonaceous material of the present invention is a carbonaceous material containing a carbonaceous material and an inorganic substance, in which at least a portion of the carbonaceous material and at least a portion of the inorganic substance are bonded by a covalent bond.

[0236] In the carbon-containing material of the present invention, at least a portion of the carbon material and at least a portion of the inorganic material are covalently bonded. Preferably, at least a portion of the carbon material is covalently bonded to at least a portion of the outermost surface of the inorganic material. More preferably, at least a portion of the carbon material is covalently bonded to at least a portion of the outermost surface of an inorganic particle.

[0237] In the description of the carbon material-containing material of the present invention, the explanations in <<1. Method for producing a carbon material-containing material>> and <<2. Representative examples of methods for producing a carbon material-containing material>> can be used for the “carbon material” and “inorganic substance”.

[0238] The carbon material-containing material of the present invention can be produced by any appropriate method, and preferably by the method for producing a carbon material-containing material of the present invention.

[0239] The carbon material-containing material of the present invention can be of a wide variety, and can take various forms such as particulate and non-particulate (for example, fibrous, thin film, etc.). The particulate form is preferred.

[0240] As explained above in <<1. Manufacturing method for carbon material-containing material>> and <<2. Representative example of manufacturing method for carbon material-containing material>>, when inorganic substances of various shapes such as particulate inorganic substances (inorganic particles) and non-particulate inorganic substances (for example, fibrous inorganic substances, thin film-like inorganic substances, etc.) are used as the inorganic substance, a wide variety of carbon material-containing materials can be obtained depending on the respective shapes. Particulate inorganic substances (inorganic particles) are preferred as the inorganic substance.

[0241] As explained above in <<1. Method for Producing a Carbon Material-Containing Material>> and <<2. Representative Examples of Methods for Producing a Carbon Material-Containing Material>>, when inorganic particles are used, a representative example of the carbon material-containing material of the present invention is a clumped carbon material-containing material containing a large number of inorganic particles. In this case, a particulate carbon material-containing material can be obtained by crushing or the like. A particulate carbon material-containing material can also be obtained by adjusting the blending ratio of compound (A) and the inorganic material. When a fibrous inorganic material is used, examples of the carbon material-containing material of the present invention include fibrous core-shell fibers and tubular hollow carbon materials. Furthermore, when a thin-film inorganic material is used, examples of the carbon material-containing material of the present invention include laminated carbon material-containing materials. Furthermore, by further subjecting such laminated carbon material-containing materials to the aforementioned heating step (II), carbon material removal step, inorganic material removal step, etc., various thin-film carbon materials can be obtained.

[0242] Representative embodiments of the carbon material-containing material of the present invention include organic-inorganic composites and carbon material-containing particles, such as the carbon material-containing materials obtained by the production methods described in <<2. Representative Examples of Production Methods of Carbon Material-Containing Materials>>. Examples of the carbon material-containing particles include core-shell particles, highly carbonized core-shell particles, hollow carbon microparticles, and highly carbonized hollow carbon microparticles.

[0243] The carbon material-containing material of the present invention is preferably 13 C-NMR analysis shows a peak between 125 ppm and 135 ppm. 13 In the C-NMR analysis, the presence of a peak between 125 ppm and 135 ppm means that the carbonaceous material contains a carbonaceous material that contains at least sp2 carbon.

[0244] The carbon material-containing material of the present invention is preferably 13 C-NMR analysis shows a peak between 140 ppm and 160 ppm. 13 In C-NMR analysis, the presence of a peak between 140 ppm and 160 ppm indicates the presence of a C-O bond. 13 In C-NMR analysis, the presence of a peak between 140 ppm and 160 ppm typically means that the outermost surface of the inorganic material contains an "oxygen-containing group" (for example, an oxygen-containing group derived from an inorganic oxide, a metal hydroxyl group, etc.), and that the oxygen is covalently bonded to the carbon of the carbon material.

[0245] The carbon material-containing material of the present invention is 29 In the case where a peak due to a CO-Si bond is observed in the Si-NMR analysis, this means that at least a part of the carbon material and at least a part of the Si-containing inorganic material are covalently bonded together, typically to at least a part of the outermost surface of the silica particle.

[0246] In the carbon material-containing material of the present invention, regarding the film thickness of the carbon material portion, the content described in the item of <<<2. Representative examples of the method for producing the carbon material-containing material>>> may be incorporated.

Example

[0247] Hereinafter, the present invention will be specifically described with reference to examples, but the present invention is not limited to these examples. Unless otherwise specified, "parts" means "parts by mass" and "%" means "% by mass". Also, in this specification, "mass" may be read as "weight". However, the % in the part related to C1sXPS in this specification means atomic %.

[0248] <Raman spectroscopy analysis> Raman spectroscopy analysis was performed using the following apparatus and conditions. Measuring apparatus: Micro Raman (JASCO NRS-3100) Measurement conditions: Using a 532 nm laser, objective lens 20 times, CCD capture time 1 second, integration 64 times (resolution = 4 cm-1) In Raman analysis, the G' band and the D+D' band may appear overlapping, and the D+D' band may be analyzed as a broad peak with a shoulder in particular. In this case, the inflection point of the shoulder peak is regarded as the peak of the G' band.

[0249] <XRD analysis> XRD measurement was performed using a fully automatic horizontal X-ray diffractometer (manufactured by Rigaku, SMART LAB) under the following conditions. CuKα1 line: 0.15406 nm Scanning range: 10° - 90° X-ray output setting: 45 kV - 200 mA Step size: 0.020° Scan speed: 0.5° min -1 -4° min -1 In addition, XRD measurement was performed while maintaining an inert atmosphere by loading the sample into an airtight sample stage in a glove box.

[0250] <C1s XPS Analysis> The C1s XPS measurement was carried out under the following conditions using a photoelectron spectrometer (AXIS-ULTRA, manufactured by Shimadzu Corporation). Source: Mg (dual node) Emission: 10 mA Anode: 10 kV Analyzer: Pass Energy: 40 Measurement range: C1s: 296 - 270 eV Number of integrations: 10 times Analysis conditions: The peaks derived from the C1s orbital were separated at the energies described below for each functional group, and the ratio was calculated from each area. The types of functional groups were (1) -COO-, lactone, and some ketones @ 288.3 eV, (2) C=O and epoxy group @ 286.2 eV, (3) C-OH and C-O-C @ 285.6 eV, (4) 6-membered cyclic C=C @ 284.3 eV, (5) C-C, C-H, and 5-membered cyclic C=C @ 283.6 eV, separated into 5 peaks. However, for ratio calculation, (4) and (5) were calculated together. The % in the part related to C1s XPS means atomic %. In the table, the ratios of the peaks corresponding to (1), (2), and (3) are indicated by (A), (B), and (C) respectively, and the total ratio of the peaks corresponding to (4) and (5) is indicated by (D).

[0251] <TG-DTA Analysis> The TG-DTA analysis was carried out under the following apparatus and conditions. Measuring apparatus: Simultaneous thermal gravimetric analyzer (manufactured by Seiko Instruments Inc., TG / DTA6200) The determination of the condensation reaction temperature of compound (A) was carried out as follows. (1) When using one kind of compound as compound (A), the TG-DTA analysis of compound (A) was carried out under a nitrogen gas atmosphere, heating from 40 °C at a heating rate of 10 °C / min, and the peak top temperature on the lowest temperature side of DTA was determined as the condensation reaction temperature (T °C) of compound (A). (2) When using a mixture of two or more compounds as compound (A), the TG-DTA analysis of the mixture was carried out under a nitrogen gas atmosphere, starting from 40 °C and heating at a rate of 10 °C / min. The peak top temperature on the lowest temperature side of the DTA was determined as the condensation reaction temperature (T °C) of compound (A) (a mixture of two or more compounds). (3) However, when compound (A) as a single compound or a mixture of two or more compounds contains impurities such as solvents, moisture, or water of hydration, etc., a DTA peak (sometimes referred to as an impurity peak) associated with the desorption of the impurity may be observed at a lower temperature than the condensation reaction temperature. In such cases, the above impurity peak was ignored and the condensation reaction temperature of the compound (A) was determined. Specifically, after ignoring the above impurity peak, the peak top temperature on the lowest temperature side of the DTA was determined as the condensation reaction temperature of the compound (A). The oxidation start temperature of the organic-inorganic composite was carried out under an air atmosphere, starting from 40 °C and heating at a rate of 10 °C / min, and was estimated from the rising temperature of the DTA, specifically the rising temperature on the lowest temperature side of the DTA.

[0252] <IR analysis> FT-IR analysis was carried out under the following apparatus and conditions. Measuring apparatus: Fourier transform infrared spectrophotometer (FT / IR-4200 manufactured by JASCO Corporation) Measurement conditions: Diffuse reflectance (DRIFT) method, MCT detector, resolution 4 cm-1, integration number 128 times Sample conditions: A sample prepared by mixing the sample and KBr at a weight ratio of 1:50 was used.

[0253] < 13 C-NMR and 29 Si-NMR measurement> 13 C-NMR and 29 The measurements of C-NMR and Apparatus: Bruker Avance NEO 400MHz / 263GHz 9.4T DNP system Probe: 2ch 3.2mm DNP probe Sample tube: 3.2 mm sapphire rotor + Teflon insert + zirconia cap Measured temperature: 105 K - 107 K Magic angle spinning (MAS): 10 kHz Pulse program: CP(1H- 13 C, 1H- 29 Si) CP contact time: 3 ms Sample preparation conditions: 40 mg sample + 20 μL TEKPol / 1,1,2,2-tetrachloroethane (16 mM)

[0254] <Measurement of molecular weight> The molecular weight was measured using gel permeation chromatography (GPC, HLC-8220GPC manufactured by Tosoh Corporation). Each carbon material was mixed with N,N-dimethylformamide (containing 0.1% LiBr) to a concentration of 0.02% by mass, ultrasonicated for 1 hour, pretreated by passing through a PTFE filter paper (0.45 μm), and then the filtrate was used with N,N-dimethylformamide (containing 0.1% LiBr) as the eluent to calculate the molecular weight in terms of polystyrene. The maximum molecular weight in the carbon material was calculated from the rising point of the peak.

[0255] <Measurement of thermal conductivity properties (thermal diffusivity, thermal conductivity)> The thermal diffusivity as a thermal conductivity property was measured in the film thickness direction using M3 type 2 manufactured by Aphase Co., Ltd. The thermal conductivity as a thermal conductivity property was calculated from the specific heat × density × thermal diffusivity of the film.

[0256] <SPS sintering> SPS sintering was carried out under the following equipment and conditions. Equipment: Shintaland LABOX-125C manufactured by Shintaland Co., Ltd. Atmosphere: Under vacuum Heating: 10 °C / min (heating from ~5 Pa) Sintering temperature: 610 °C Holding time: 5 minutes Pressurization: 50 MPa (from heating to sintering) Cooling: Unpressurized and natural cooling

[0257] <Measurement of powder resistance> The powder resistance was measured by drilling a 1cm square hole in a 4mm Teflon plate, filling the hole with powder, and sandwiching it between copper electrodes on both sides. The equipment used was a Tektronix 6517BJ high resistivity meter, and the measurement was performed at an applied voltage of 10V.

[0258] [Example 1]: Phloroglucinol + silica particles + 250°C x 1 hour Phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C): theoretical specific surface area 750 m 2 Silica particles (manufactured by Fuji Silysia Chemical Ltd., product name "Q-10HT60315", specific surface area 259 m) were used so that the ratio of layers was 1.5. 2 / g) and mixed thoroughly. The resulting mixture was vacuum sealed in a quartz ampoule and then heated for 1 hour in an electric furnace preheated to 250°C. As a result, an organic-inorganic composite (1) containing a carbon material (1A) and an inorganic oxide (1B) was obtained. The organic-inorganic composite (1) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (1) are shown in Figure 3 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (1) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 26%, the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 62%, and the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 16%. This indicates a high degree of structural control. When phloroglucinol was analyzed by TG-DTA under a nitrogen gas atmosphere with a temperature increase rate of 10°C / min, the weight ratio (M500 / M50) of the weight M500 at a temperature of 500°C to the initial weight M50 at a temperature of 50°C was 0.49. This indicates that phloroglucinol can remain sufficiently present on the inorganic oxide even after carbonization. The results of the DTA analysis of the obtained organic-inorganic composite (1) in a TG-DTA analysis are shown in Figure 4. According to Figure 4, when the organic-inorganic composite (1) was subjected to TG-DTA analysis under the condition of a temperature rise from 40°C at 10°C / min in an air atmosphere, the oxidation onset temperature indicated by the DTA rise temperature was 200°C. This shows that the oxidation resistance is high. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (1) are shown in Figure 5. According to Figure 5, in the IR spectrum of the organic-inorganic composite (1), a peak at 1660 cm due to the C=O structure is observed. -1 ~1800cm -1 There is no peak and the structure is highly controlled. Furthermore, the Raman spectrum of the obtained organic-inorganic composite (1) is shown in FIG. -1 , 1590cm -1 , 2650cm -1 , 2835cm -1 , it was found that the carbon material (1A) was a carbon material containing a carbon-based compound having a graphene structure and a structure in which the graphene structures were stacked. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0259] [Example 2] Phloroglucinol + alumina particles + 250°C x 1 hour Silica particles were replaced with alumina particles (JRC-ALO7, a free sample distributed by the Catalysis Society of Japan, specific surface area 180 m 2 The same procedure as in Example 1 was carried out except that the amount of the inorganic oxide (2A) was changed to ( / g), and an organic-inorganic composite (2) containing a carbon material (2A) and an inorganic oxide (2B) was obtained. The organic-inorganic composite (2) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (2) are shown in Figure 3 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (2) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 29%, the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 59%, and the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 17%. This indicates a high degree of structural control. The results of the DTA analysis of the obtained organic-inorganic composite (2) in a TG-DTA analysis are shown in Figure 4. According to Figure 4, when the organic-inorganic composite (2) was subjected to TG-DTA analysis in an air atmosphere under the condition of a temperature increase from 40°C at a rate of 10°C / min, the oxidation onset temperature indicated by the DTA rise temperature was 230°C. This indicates that the oxidation resistance is high. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (2) are shown in Figure 5. According to Figure 5, in the IR spectrum of the organic-inorganic composite (2), a peak at 1660 cm due to the C=O structure is observed. -1 ~1800cm -1 The structural control rate by C1sXPS is high, but the structural control rate by FT-IR analysis is somewhat low. Furthermore, the Raman spectrum of the obtained organic-inorganic composite (2) is shown in FIG. -1 , 1585cm -1 , 2650cm -1 , 2835cm -1 It was found that the carbon material (2A) was a carbon material containing a carbon-based compound having a graphene structure and a structure in which the graphene structures were stacked. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0260] [Example 3] Phloroglucinol + titania particles + 250°C x 1 hour Silica particles were replaced with titania particles (JRC-TIO-4(2), a free sample distributed by the Catalysis Society of Japan, with a specific surface area of ​​50 m). 2 The same procedure as in Example 1 was carried out except that the amount of the carbon material (3A) was changed to ( / g), and an organic-inorganic composite (3) containing a carbon material (3A) and an inorganic oxide (3B) was obtained. The organic-inorganic composite (3) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (3) are shown in Figure 3 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (3) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 27%. The ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 56%. The ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 15%. This indicates a high degree of structural control. The results of the DTA analysis of the obtained organic-inorganic composite (3) in a TG-DTA analysis are shown in Figure 4. According to Figure 4, when the organic-inorganic composite (3) was subjected to TG-DTA analysis under the condition of a temperature rise from 40°C at 10°C / min in an air atmosphere, the oxidation onset temperature indicated by the DTA rise temperature was 200°C. This indicates that the oxidation resistance is high. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (3) are shown in Figure 5. According to Figure 5, in the IR spectrum of the organic-inorganic composite (3), there is a peak at 1660 cm due to the C=O structure.-1 ~1800cm -1 The structural control rate by C1sXPS is high, but the structural control rate by FT-IR analysis is somewhat low. Furthermore, the Raman spectrum of the obtained organic-inorganic composite (3) is shown in Figure 6. -1 , 1580cm -1 , 2650cm -1 , 2820cm -1 It was found that the carbon material (3A) was a carbon material containing a carbon-based compound having a graphene structure and a structure in which the graphene structures were stacked. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0261] [Example 4] Phloroglucinol + heteropoly acid particles (HPW) + 250°C x 1 hour Silica particles were used as heteropolyacid particles, and HPW (12-tungsto(VI) phosphate n-hydrate, manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., specific surface area 278 m) was used. 2 The same procedure as in Example 1 was carried out except that the amount of the carbon material (4A) was changed to (4B / g), and an organic-inorganic composite (4) containing a carbon material (4A) and an inorganic oxide (4B) was obtained. The organic-inorganic composite (4) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (4) are shown in Figure 3 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (4) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 29%, the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 76%, and the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 22%. This indicates a high degree of structural control. The results of the DTA analysis of the obtained organic-inorganic composite (4) in a TG-DTA analysis are shown in Figure 4. According to Figure 4, when the organic-inorganic composite (4) was subjected to TG-DTA analysis under the condition of a temperature rise from 40°C at 10°C / min in an air atmosphere, the oxidation onset temperature indicated by the DTA rise temperature was 300°C. This indicates that the oxidation resistance is high. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (4) are shown in Figure 5. According to Figure 5, in the IR spectrum of the organic-inorganic composite (4), a peak at 1660 cm originating from the C=O structure is observed. -1 ~1800cm -1 There is no peak and the structure is highly controlled. Furthermore, the Raman spectrum of the obtained organic-inorganic composite (4) is shown in FIG. -1 , 1585cm -1 , 2650cm -1 , 2810cm -1 From the peak at , it was found that the carbon material (4A) has a graphene structure and is a carbon material containing a carbon-based compound with a structure in which the graphene structures are stacked. Furthermore, when the molecular weight of the carbon material (4A) portion was measured, the weight average molecular weight was 8,000 and the maximum molecular weight was 50,000. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0262] [Example 5] Phloroglucinol + heteropoly acid particles (HPMo) + 250°C x 1 hour The same procedure as in Example 1 was carried out except that the silica particles were changed to heteropolyacid particles HPMo (12-molybdo(VI)phosphate n-hydrate, manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.), and an organic-inorganic composite (5) containing a carbon material (5A) and an inorganic oxide (5B) was obtained. The organic-inorganic composite (5) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (5) are shown in Figure 7 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (5) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 27%, the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 63%, and the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 17%. This indicates a high degree of structural control. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (5) are shown in Figure 8. According to Figure 8, in the IR spectrum of the organic-inorganic composite (5), a peak at 1660 cm originating from the C=O structure is observed. -1 ~1800cm -1 There is no peak and the structure is highly controlled. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0263] [Example 6] Phloroglucinol + heteropoly acid particles (HSiW) + 250°C x 1 hour The same procedure as in Example 1 was carried out except that the silica particles were changed to heteropolyacid particles HSiW (silicotungstic acid, manufactured by Nippon Shinkinzoku Co., Ltd.), and an organic-inorganic composite (6) containing a carbon material (6A) and an inorganic oxide (6B) was obtained. The organic-inorganic composite (6) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (6) are shown in Figure 7 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (5) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 29%, the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 72%, and the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 21%. This indicates a high degree of structural control. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (6) are shown in Figure 8. According to Figure 8, in the IR spectrum of the organic-inorganic composite (6), a peak at 1660 cm originating from the C=O structure is observed. -1 ~1800cm -1 There is no peak and the structure is highly controlled. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0264] [Example 7] Phloroglucinol + heteropoly acid particles (HPVMo) + 250°C x 1 hour The same procedure as in Example 1 was carried out except that the silica particles were changed to heteropolyacid particles HPVMo (phosphovanadomolybdic acid, manufactured by Nippon Shinkinzoku Co., Ltd.), and an organic-inorganic composite (7) containing a carbon material (7A) and an inorganic oxide (7B) was obtained. The organic-inorganic composite (7) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (7) are shown in Figure 7 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (7) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 29%, the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 55%, and the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 16%. This indicates a high degree of structural control. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (7) are shown in Figure 8. According to Figure 8, in the IR spectrum of the organic-inorganic composite (7), a peak at 1660 cm originating from the C=O structure is observed. -1 ~1800cm -1 There is no peak and the structure is highly controlled. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0265] [Example 8] Phloroglucinol + heteropoly acid particles (HPWMo) + 250°C x 1 hour The same procedure as in Example 1 was carried out except that the silica particles were changed to heteropolyacid particles HPWMo (phosphotungstomolybdic acid, manufactured by Nippon Shinkinzoku Co., Ltd.), and an organic-inorganic composite (8) containing a carbon material (8A) and an inorganic oxide (8B) was obtained. The organic-inorganic composite (8) was dispersed in NMP (N-methylpyrrolidone), and the solubility of the carbon component was confirmed by the above-mentioned method, and it was found to be soluble in the solvent. The results of the C1s XPS analysis of the obtained organic-inorganic composite (8) are shown in Figure 7 (XPS spectrum (C1s)) and Table 1. Table 1 shows that the organic-inorganic composite (8) is an organic-inorganic composite containing a carbon material and an inorganic oxide. The ratio of the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 27%, the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon-oxygen bonds (C-O bonds and C=O bonds) was 70%, and the ratio of the total amount of ether-derived C-O bonds and alcohol-derived C-O bonds to the total amount of all carbon bonds (C-C bonds, C=C bonds, C-H bonds, C-O bonds, and C=O bonds) was 19%. This indicates a high degree of structural control. Furthermore, the results of IR analysis of the obtained organic-inorganic composite (8) are shown in Figure 8. According to Figure 8, in the IR spectrum of the organic-inorganic composite (8), a peak at 1660 cm originating from the C=O structure is observed. -1 ~1800cm -1 There is no peak and the structure is highly controlled. As described above, according to the production method of the present invention, a carbonaceous material that is soluble in a solvent and has a precisely controlled structure can be produced simply under mild conditions.

[0266] [Example 9]: Phloroglucinol + silica particles + 300°C x 3 hours, hollow carbon microparticles 300 mg of phloroglucinol (manufactured by Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 3 g of isopropyl alcohol, to which 1000 mg of spherical silica microparticles (manufactured by Nippon Shokubai Co., Ltd., average particle size: 0.19 μm) were added and thoroughly mixed by ultrasonic treatment. The isopropyl alcohol was removed from the resulting mixture by vacuum drying at room temperature, and the remaining lumps were crushed and then heated at 300°C for 3 hours. As a result, an organic-inorganic composite (9) containing a carbon material (9A) and an inorganic oxide (9B) was obtained. The Raman spectrum of the organic-inorganic composite (9) is shown in Figure 9. -1 , 1600cm -1 , 2700cm -1 , 2890cm -1 From the peak at , it was found that the carbon material (9A) is a carbon material containing a carbon-based compound having a graphene structure and a structure in which the graphene structures are stacked. Furthermore, when the molecular weight of the carbon material (9A) portion was measured, the weight average molecular weight was 200,000 and the maximum molecular weight was 1,100,000. The obtained organic-inorganic composite (9) was treated with N-methylpyrrolidone (NMP), which removed the carbon material (9A) and gave core-shell particles (9) (core: inorganic oxide particle, shell: carbon material bonding region) in which the surface of the inorganic oxide (9B) was coated with a carbon material bonding region. The core-shell particles (9) were further calcined at 700°C for 1 hour. This resulted in the carbonization of the carbon material in the shell portion, resulting in highly carbonized core-shell particles (9). An SEM photograph of the highly carbonized core-shell particles (9) is shown in Figure 10, and a Raman spectrum of the surface of the highly carbonized core-shell particles (9) is shown in Figure 11. Figures 10 and 11 show that the surface (shell portion) of the highly carbonized core-shell particles (9) is composed of a highly carbonized carbon material without losing its shape. Highly carbonized core-shell particles (9) 13 C-NMR and 29 The results of the Si-NMR analysis are shown in Figures 12 and 13. 13 C-NMR confirmed a peak at 129 ppm and a shoulder peak from 140 ppm to 160 ppm. This is thought to be due to the presence of sp2 carbon (129 ppm) and the bond between oxygen atoms on the inorganic surface and carbon atoms derived from the carbon material (140 ppm to 160 ppm). In Comparative Example 3 described below, sp2 carbon was not formed, and sp3 carbon was predominant, which is thought to be hidden by the solvent peak. In addition, 29From the Si-NMR, peaks derived from Si-O-C bonds were confirmed in comparison with the raw material silica spherical microparticles and Comparative Example 3 described below, which revealed that covalent bonds were formed between carbon atoms derived from the carbon material and atoms on the outermost surface of the inorganic material. As described above, since the covalent bond was only with the outermost surface of the inorganic material, the peak intensity was small and could be confirmed as a shoulder peak. The powder resistivity of the highly carbonized core-shell particles (9) was measured and found to be 3 × 10 5 The powder resistivity of the raw material spherical silica particles was 10 14 Since the conductivity is on the order of Ωcm, it was found that by using core-shell particles, the conductivity can be improved by about nine orders of magnitude. The thickness of the carbon portion of the highly carbonized core-shell particles (9) was estimated by TG-DTA analysis. The estimation method involved heating the raw material spherical silica microparticles and the highly carbonized core-shell particles (9) in an air atmosphere from room temperature to 1000°C at a rate of 10°C / min to combust the carbon components, and then analyzing the amount of carbon by taking the difference between the raw material spherical silica microparticles and the highly carbonized core-shell particles (9). According to the above method, the carbon content of the highly carbonized core-shell particles (9) was determined to be 1.39% by mass. Assuming a diameter of the spherical silica particles of 0.19 μm and a density of the carbon component of 2, the average thickness of the carbon component was calculated to be 0.49 nm. 500 mg of core-shell particles (9) were ultrasonically cleaned in a 10% aqueous sodium hydroxide solution for 5 hours and then filtered to obtain 20 mg of hollow carbon microparticles (9). The filtrate was colorless and transparent, and considering the amount removed, only the carbon component remained, and the inorganic components inside were removed. This suggests that the formation of hollow carbon microparticles (9) with a hollow structure was achieved.

[0267] [Example 10]: Phloroglucinol + copper particles + 300°C x 2 hours, highly carbonized core-shell particles 1 g of phloroglucinol (manufactured by Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, to which 20 g of copper particles (manufactured by ECKA Granules Germany GmbH, particle size: 95 vol% or more of 36 μm or less) were added, and the mixture was thoroughly mixed by ultrasonic treatment. Acetone was removed from the resulting mixture by vacuum drying at room temperature, and the remaining lumps were crushed and then heated at 300°C for 2 hours. As a result, an organic-inorganic composite (10) containing a carbon material (10A) and an inorganic oxide (10B) was obtained. The obtained organic-inorganic composite (10) was treated with DMF (N,N-dimethylformamide), thereby removing the carbon material (10A) and obtaining core-shell particles (10) (core: inorganic oxide particle, shell: carbon material bonding region) in which the surface of the inorganic oxide (10B) was coated with a carbon material bonding region. The core-shell particles (10) were further calcined at 700°C for 1 hour. This resulted in the carbonization of the carbon material in the shell portion, resulting in highly carbonized core-shell particles (10). The Raman spectrum of the surface of the highly carbonized core-shell particles (10) is shown in Figure 14. Figure 14 shows that the surface (shell portion) of the highly carbonized core-shell particles (10) is composed of a highly carbonized carbon material without losing its shape.

[0268] [Example 11]: Phloroglucinol + aluminum particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of aluminum particles (ECKA Granules Germany GmbH, D50 = 5 μm) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain an aluminum particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (11) containing a carbon material (11A) and an inorganic oxide (11B). The obtained organic-inorganic composite (11) was subjected to ultrasonic treatment in DMF (N,N-dimethylformamide), and the excess carbon material (10A) was removed by filtration and purified to obtain core-shell particles (11) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (11B) was coated with a carbon material binding region. The core-shell particles (11) were further calcined at 600°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, resulting in highly carbonized core-shell particles (11). The Raman spectrum of the surface of the highly carbonized core-shell particles (11) is shown in Figure 15. Figure 15 shows that the surface (shell portion) of the highly carbonized core-shell particles (11) is composed of a highly carbonized carbon material without losing its shape. The obtained highly carbonized core-shell particles (11) were also sintered by SPS to produce an aluminum-carbon alloy sintered body. For comparison, raw aluminum particles were also sintered by SPS to produce an aluminum sintered body. The Vickers hardness of each sintered body was measured, and the results are shown in Figure 16. It was found that the strength (hardness) of sintered bodies produced by the carbon coating technology of the present invention can be increased. In other words, the carbon-containing material obtained by the production method of the present invention can be used to impart strength to sintered bodies (as a strength improver for sintered bodies).

[0269] [Example 12]: Phloroglucinol + barium titanate particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of barium titanate particles (Fujifilm Wako Pure Chemical Industries, Ltd.) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain a barium titanate particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This resulted in an organic-inorganic composite (12) containing a carbon material (12A) and an inorganic oxide (12B). The obtained organic-inorganic composite (12) was subjected to ultrasonic treatment in DMF (N,N-dimethylformamide), and the excess carbon material (12A) was removed by centrifugation for purification, yielding core-shell particles (12) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (12B) was coated with a carbon material binding region. The core-shell particles (12) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (12). The Raman spectrum of the surface of the highly carbonized core-shell particles (12) is shown in Figure 17. Figure 17 shows that the surface (shell portion) of the highly carbonized core-shell particles (12) is composed of a highly carbonized carbon material without losing its shape.

[0270] [Example 13]: Phloroglucinol + strontium titanate particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of strontium titanate particles (Aldrich) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain a strontium titanate particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (13) containing a carbon material (13A) and an inorganic oxide (13B). The obtained organic-inorganic composite (13) was sonicated in DMF (N,N-dimethylformamide), and the excess carbon material (13A) was removed by centrifugation for purification, yielding core-shell particles (13) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (13B) was coated with a carbon material binding region. The core-shell particles (13) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (13). The Raman spectrum of the surface of the highly carbonized core-shell particles (13) is shown in Figure 18. Figure 18 shows that the surface (shell portion) of the highly carbonized core-shell particles (13) is composed of a highly carbonized carbon material without losing its shape.

[0271] [Example 14]: Phloroglucinol + lithium niobate particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (manufactured by Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of lithium niobate particles (manufactured by Aldrich) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain a lithium niobate particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (14) containing a carbon material (14A) and an inorganic oxide (14B). The obtained organic-inorganic composite (14) was subjected to ultrasonic treatment in DMF (N,N-dimethylformamide), and the excess carbon material (14A) was removed by filtration and purified to obtain core-shell particles (14) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (14B) was coated with a carbon material binding region. The core-shell particles (14) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (14). The Raman spectrum of the surface of the highly carbonized core-shell particles (14) is shown in Figure 19. Figure 19 shows that the surface (shell portion) of the highly carbonized core-shell particles (14) is composed of a highly carbonized carbon material without losing its shape.

[0272] [Example 15]: Phloroglucinol + silicon particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (manufactured by Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, to which 2 g of silicon particles (manufactured by YY) was added. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain a silicon particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (15) containing a carbon material (15A) and an inorganic oxide (15B). The obtained organic-inorganic composite (15) was sonicated in DMF (N,N-dimethylformamide), and the excess carbon material (14A) was removed by centrifugation for purification, yielding core-shell particles (15) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (15B) was coated with a carbon material binding region. The core-shell particles (15) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, resulting in highly carbonized core-shell particles (15). The Raman spectrum of the surface of the highly carbonized core-shell particles (15) is shown in Figure 20. Figure 20 shows that the surface (shell portion) of the highly carbonized core-shell particles (15) is composed of a highly carbonized carbon material without losing its shape.

[0273] [Example 16]: Phloroglucinol + boron nitride particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of boron nitride particles (Showa Denko) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain a boron nitride particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (16) containing a carbon material (16A) and an inorganic oxide (16B). The obtained organic-inorganic composite (16) was sonicated in DMF (N,N-dimethylformamide), and the excess carbon material (16A) was removed by filtration for purification, yielding core-shell particles (16) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (16B) was coated with a carbon material binding region. The core-shell particles (16) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (16). The Raman spectrum of the surface of the highly carbonized core-shell particles (16) is shown in Figure 21. Figure 21 shows that the surface (shell portion) of the highly carbonized core-shell particles (16) is composed of a highly carbonized carbon material without losing its shape.

[0274] [Example 17]: Phloroglucinol + alumina particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of alumina particles (Showa Denko) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain an alumina particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (17) containing a carbon material (17A) and an inorganic oxide (17B). The obtained organic-inorganic composite (16) was sonicated in DMF (N,N-dimethylformamide), and the excess carbon material (16A) was removed by filtration and purified to obtain core-shell particles (17) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (17B) was coated with a carbon material binding region. The core-shell particles (17) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, resulting in highly carbonized core-shell particles (17). The Raman spectrum of the surface of the highly carbonized core-shell particles (17) is shown in Figure 22. Figure 22 shows that the surface (shell portion) of the highly carbonized core-shell particles (17) is composed of a highly carbonized carbon material without losing its shape. In addition, the obtained high-carbonized core-shell particles (17) and raw alumina were mixed in DMF at a volume ratio of 1:2 (PMMA: polymethyl methacrylate (PMMA): raw alumina particles) and PMMA: high-carbonized core-shell particles (17) in DMF, and then dried to obtain PMMA / alumina and PMMA / high-carbonized core-shell particles (17). Analysis of the thermal conductivity properties in the film thickness direction revealed that the use of high-carbonized core-shell particles (17) resulted in improved thermal conductivity, as shown in Table 2. The specific heat and density were calculated from the mixing ratio and were 920 J / kg K and 3000 kg / m, respectively. 3That is, the organic-inorganic composite of the present invention can be used for improving thermal conductivity (thermal conductivity improver).

[0275] [Example 18]: Phloroglucinol + magnesium oxide particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of magnesium oxide particles (MgO, Ube Industries, Ltd.) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain a magnesium oxide particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (18) containing a carbon material (18A) and an inorganic oxide (18B). The obtained organic-inorganic composite (18) was sonicated in DMF (N,N-dimethylformamide), and the excess carbon material (18A) was removed by centrifugation for purification, yielding core-shell particles (18) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (18B) was coated with a carbon material binding region. The core-shell particles (18) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (18). The Raman spectrum of the surface of the highly carbonized core-shell particles (18) is shown in Figure 23. Figure 23 shows that the surface (shell portion) of the highly carbonized core-shell particles (18) is composed of a highly carbonized carbon material without losing its shape.

[0276] [Example 19]: Phloroglucinol + aluminum nitride particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of aluminum nitride particles (Tokuyama) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain an aluminum nitride particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This yielded an organic-inorganic composite (19) containing a carbon material (19A) and an inorganic oxide (19B). The obtained organic-inorganic composite (19) was sonicated in DMF (N,N-dimethylformamide), and the excess carbon material (19A) was removed by centrifugation for purification, yielding core-shell particles (19) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (19B) was coated with a carbon material binding region. The core-shell particles (19) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, resulting in highly carbonized core-shell particles (19). The Raman spectrum of the surface of the highly carbonized core-shell particles (19) is shown in Figure 24. Figure 24 shows that the surface (shell portion) of the highly carbonized core-shell particles (19) is composed of a highly carbonized carbon material without losing its shape.

[0277] [Example 20]: Phloroglucinol + lithium iron phosphate particles + 300°C x 2 hours, highly carbonized core-shell particles 0.2 g of phloroglucinol (manufactured by Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 200 g of acetone, and 2 g of lithium iron phosphate particles (manufactured by Toshima Manufacturing Co., Ltd.) was added thereto. The mixture was thoroughly mixed by ultrasonic treatment and dried to obtain a lithium iron phosphate particle-phloroglucinol mixture. This mixture was calcined in a Kugelrohr at 300°C for 2 hours under a nitrogen atmosphere. This resulted in an organic-inorganic composite (20) containing a carbon material (20A) and an inorganic oxide (20B). The obtained organic-inorganic composite (20) was subjected to ultrasonic treatment in DMF (N,N-dimethylformamide), and the excess carbon material (20A) was removed by centrifugation for purification, yielding core-shell particles (20) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of the inorganic oxide (20B) was coated with a carbon material binding region. The core-shell particles (20) were further calcined at 700°C for 2 hours. This resulted in the carbonization of the carbon material in the shell portion, resulting in highly carbonized core-shell particles (20). The Raman spectrum of the surface of the highly carbonized core-shell particles (20) is shown in Figure 25. Figure 25 shows that the surface (shell portion) of the highly carbonized core-shell particles (20) is composed of a highly carbonized carbon material without losing its shape.

[0278] [Example 21]: Phloroglucinol + silica particles + 250°C x 2 hours, highly carbonized core-shell particles, different solvents 1 g of phloroglucinol (manufactured by Tokyo Chemical Industry Co., Ltd., melting point: 220°C, condensation reaction temperature: 330°C) was dissolved in 30 g of acetone, to which 10 g of spherical silica particles (manufactured by Nippon Shokubai Co., Ltd., average particle size: 0.19 μm) were added and thoroughly mixed by ultrasonic treatment. Acetone was removed from the resulting mixture by vacuum drying at room temperature, and the remaining lumps were crushed and then heated at 250°C for 2 hours. As a result, an organic-inorganic composite (21) containing a carbon material (21A) and an inorganic oxide (21B) was obtained. The Raman spectrum of the organic-inorganic composite (21) is shown in Figure 26. It was found that the carbon material (21A) is a carbon material containing a carbon-based compound having a graphene structure and a structure in which the graphene structures are stacked. The obtained organic-inorganic composite (21) was subjected to ultrasonic treatment in acetone, and the excess carbon material (21A) was removed by centrifugation for purification, thereby obtaining core-shell particles (21) (core portion: inorganic oxide particle, shell portion: carbon material binding region) in which the surface of the inorganic oxide (21B) was coated with a carbon material binding region. The core-shell particles (21) were further calcined at 700°C for 1 hour. This resulted in a high carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (21). The Raman spectrum of the surface of the highly carbonized core-shell particles (21) is shown in Figure 27.

[0279] [Example 22]: Phloroglucinol + boron nitride + 250°C x 2 hours, highly carbonized core-shell particles, different solvents Except for using boron nitride as the raw material, organic-inorganic composite (22), core-shell particles (22), and highly carbonized core-shell particles (22) were obtained in the same manner as in Example 21. The Raman spectra of organic-inorganic composite (22) and highly carbonized core-shell particles (22) are shown in Figures 28 and 29. As can be seen from Examples 21 and 22, it was found that it is possible to change the solvent used by adjusting the firing temperature or other operations.

[0280] [Example 23]: Hexahydroxytriphenylene + silica particles + 350°C x 2 hours, highly carbonized core-shell particles, different raw materials 1 g of 2,3,6,7,10,11-hexahydroxytriphenylene (manufactured by Tokyo Chemical Industry Co., Ltd., melting point: none, condensation reaction temperature: 430°C) was dissolved in 30 g of DMF, to which 10 g of spherical silica particles (manufactured by Nippon Shokubai Co., Ltd., average particle size: 0.19 μm) were added and thoroughly mixed by ultrasonic treatment. DMF was removed from the resulting mixture using an evaporator, and the remaining aggregates were crushed and then heated at 350°C for 2 hours. As a result, an organic-inorganic composite (23) containing a carbon material (23A) and an inorganic oxide (23B) was obtained. The Raman spectrum of the organic-inorganic composite (23) is shown in Figure 30. -1 , 1590cm -1 , 2700cm -1 , 2895cm -1 It was found that the carbon material (23A) was a carbon material containing a carbon-based compound having a graphene structure and a structure in which the graphene structures were stacked. The obtained organic-inorganic composite (23) was subjected to ultrasonic treatment in DMF, and the excess carbon material (23A) was removed by centrifugation for purification, thereby obtaining core-shell particles (23) (core portion: inorganic oxide particle, shell portion: carbon material binding region) in which the surface of the inorganic oxide (23B) was coated with a carbon material binding region. The core-shell particles (23) were further calcined at 700°C for 1 hour. This resulted in a high carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (23). The Raman spectrum of the surface of the highly carbonized core-shell particles (23) is shown in Figure 31.

[0281] [Example 24]: (+)-Catechin + silica particles + 250°C x 2 hours, highly carbonized core-shell particles, different raw materials 1 g of (+)-catechin hydrate (Tokyo Chemical Industry Co., Ltd., melting point: none, condensation reaction temperature: 270°C) was dissolved in 30 g of acetone, to which 10 g of silica spherical particles (Nippon Shokubai Co., Ltd., average particle size: 0.19 μm) were added and thoroughly mixed by ultrasonic treatment. Note that because this catechin is a hydrate, the condensation reaction temperature in TGDTA was confirmed by ignoring the dehydration peak and instead determining the temperature at which condensation proceeds after dehydration. Acetone was removed from the resulting mixture by vacuum drying at room temperature, and the remaining lumps were crushed and then heated at 250°C for 2 hours. As a result, an organic-inorganic composite (24) containing a carbon material (24A) and an inorganic oxide (24B) was obtained. The Raman spectrum of the organic-inorganic composite (24) is shown in Figure 32. -1 , 15cm -1 , 27cm -1 , 28cm -1 It was found that the carbon material (24A) was a carbon material containing a carbon-based compound having a graphene structure and a structure in which the graphene structures were stacked. The obtained organic-inorganic composite (24) was subjected to ultrasonic treatment in DMF, and the excess carbon material (24A) was removed by centrifugation for purification, yielding core-shell particles (24) (core: inorganic oxide particle, shell: carbon material binding region) in which the surface of inorganic oxide (24B) was coated with a carbon material binding region. The core-shell particles (24) were further calcined at 700°C for 1 hour. This resulted in a high carbonization of the carbon material in the shell portion, yielding highly carbonized core-shell particles (24). The Raman spectrum of the surface of the highly carbonized core-shell particles (24) is shown in Figure 33.

[0282] Comparative Example 1 Organic-inorganic composite (C1) was obtained by the method described in Example 9, except that the heating temperature was 170°C. However, no signal from the carbon material was observed by Raman analysis, and only fluorescence derived from low molecular weight compounds was confirmed. In other words, it was found that phloroglucinol was not sufficiently carbonized.

[0283] Comparative Example 2 Organic-inorganic composite (C2) was obtained by the method described in Example 23, except that the heating temperature was 270 ° C. However, no signal from the carbon material was observed by Raman analysis, and only fluorescence derived from low molecular weight compounds was confirmed. In other words, it was found that hexahydroxytriphenylene was not sufficiently carbonized.

[0284] Comparative Example 3 The spherical silica particles used in Example 9 were baked at 700°C for 2 hours in a nitrogen atmosphere and then coated with carbon in the gas phase using a quick carbon coater (SC-701CT, manufactured by Sanyu Electronics Co., Ltd.). The presence of carbon was confirmed by Raman analysis. 13 C-NMR and 29The results of the Si-NMR analysis are shown in Figures 12 and 13. Compared with Example 9, the particles obtained in Comparative Example 3 had carbon present on the surface, but it was not sp2 carbon, and there was no Si-O-C bond, so it was found that the carbon was not present on the surface of the particles via a covalent bond (of course, no bond was confirmed in the raw material silica spherical microparticles either). Comparing the results of Comparative Example 3 with those of the Examples, it was found that the present invention can provide a carbonaceous material in which the surface of an inorganic substance is firmly coated with sp2 carbon components via covalent bonds.

[0285] [Reference example 1] Organic-inorganic composite (R1) was obtained by the method described in Example 9, except that the heating temperature was set to 520° C. However, the carbon component was insoluble in NMP (N-methylpyrrolidone), and subsequent treatment was impossible.

[0286] From the above examples, it was found that the production method of the present invention can easily produce a carbonaceous material that is soluble in a solvent or a carbonaceous material that has a precisely controlled structure under mild conditions, and that the present invention can provide such a carbonaceous material.

[0287] [Table 1]

[0288] [Table 2] [Industrial Applicability]

[0289] The carbonaceous material obtained by the production method of the present invention and the carbonaceous material of the present invention can be effectively used as materials for industrially producing carbon-coated inorganic particles and hollow carbon microparticles, which are lightweight and have excellent lubricity, electrical conductivity, thermal conductivity, and antioxidant properties and are useful as fillers, etc. Potential uses include as a solid lubricant, as a lubricating additive for lubricating oils, as a conductive additive for inorganic materials and organic materials such as resins, as an antistatic agent, a strength imparting agent, a friction reducer, and a thermal conductivity imparting agent. [Explanation of symbols]

[0290] 10 Carbon materials 20 Inorganic particles 30 Carbon material bonding region 100 Organic-inorganic composites 200 core-shell particles

Claims

1. A method for producing a carbonaceous material, comprising: The method includes a heating step (I) of heating a composition containing a compound (A) that undergoes a condensation reaction between identical molecules and / or different molecules upon heating, and an inorganic substance, the compound (A) is a compound in which one neutral molecule is formed from two or more groups by the condensation reaction and is eliminated, and the compound (A) is a compound having three or more phenolic hydroxyl groups in the molecule; the inorganic substance is at least one selected from the group consisting of inorganic oxides, inorganic nitrides, inorganic carbides, metal phosphates, and metal sulfates; the heating temperature in the heating step (I) is (T-150)°C or higher and (T+50)°C or lower, when the condensation reaction temperature of the compound (A) is T°C; the carbon material of the carbon material-containing material has a graphene structure or a structure similar to a graphene structure; A method for producing a carbonaceous material.

2. 2. The method for producing a carbon material-containing material according to claim 1, further comprising, after the heating step (I), a carbon material removing step of removing at least a part of the carbon material produced by heating the compound (A).

3. The method for producing a carbon material-containing material according to claim 2 , further comprising a heating step (II) of heating the carbon material-containing material after the carbon material removing step.

4. The method for producing a carbonaceous material according to claim 1 , further comprising, after the heating step (I), an inorganic substance removing step of removing the inorganic substance.

5. The method for producing a carbonaceous material according to claim 4 , further comprising a heating step (II) of heating the material after the inorganic substance removing step.

6. The method for producing a carbon-containing material according to claim 1 , wherein the compound (A) has a molecular weight of 500 or less.

7. The method for producing a carbon-containing material according to claim 1 , wherein the condensation reaction temperature of the compound (A) is 450° C. or lower.

8. The method for producing a carbon-containing material according to claim 7 , wherein the condensation reaction temperature of the compound (A) is 400° C. or lower.

9. 9. The method for producing a carbon-containing material according to any one of claims 1 to 8, wherein, when compound (A) is subjected to TG-DTA analysis under a nitrogen gas atmosphere at a temperature rising condition from 40°C at a rate of 10°C / minute, the weight ratio (M500 / M50) of a weight M500 at a temperature of 500°C to an initial weight M50 at a temperature of 50°C is 0.2 or more.

10. The method for producing a carbonaceous material-containing material according to claim 1 , wherein the condensation reaction is promoted by an acid catalyst.

11. The condensation reaction (a) -H group and -OH group to H ２ condensation reaction with the formation and elimination of O; (b) a condensation reaction between an —H group and an —OR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate ROH; (c) a condensation reaction of a -H group with a -X group (where X is a halogen or CN) to form and eliminate HX; (d) -H group and -NH ２ From the group NH ３ and elimination of (e) RNH from a —H group and a —NHR group (R is any suitable substituted or unsubstituted alkyl group). ２ and elimination of (f) -H group and -NR １ R ２ Group (R １ , R ２ is any suitable substituted or unsubstituted alkyl group) and R １ R ２ condensation reaction with the formation and elimination of NH (g) -H group and -SH group to form H ２ condensation reaction with the formation and elimination of S; (h) a condensation reaction between an -H group and an -SR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RSH; (i) a condensation reaction between an -H group and an -OOCR group (where R is any suitable substituted or unsubstituted alkyl group) to form and eliminate RCOOH; (j) -H group and -OSO(OH) group to form H ２ SO ３ and elimination of (k) -H group and -OSO ２ R group (R is any suitable substituted or unsubstituted alkyl group) and RSO ２ a condensation reaction in which (OH) is formed and eliminated; (l) -H group and -OSO ２ (OR) group (R is any suitable substituted or unsubstituted alkyl group) to form ROSO ３ condensation reactions with the formation and elimination of H, and (m) -H group and -OSO ２ (OH) group to H ２ SO ４ and elimination of The method for producing a carbon-containing material according to any one of claims 1 to 10, wherein the carbon-containing material is at least one selected from the group consisting of:

12. The method for producing a carbon-containing material according to claim 1 , wherein the inorganic oxide is an inorganic oxide particle having a functional group on the surface thereof.

13. 13. The method for producing a carbon-containing material according to claim 12, wherein the inorganic oxide particles are at least one selected from the group consisting of silica particles, alumina particles, titania particles, magnesium oxide particles, polyacid particles, metal particles at least a portion of whose surface is oxidized, composite oxide particles, and solid solution oxide particles.

14. 14. The method for producing a carbon-containing material according to claim 13, wherein the metal constituting the polyacid particles is at least one selected from the group consisting of molybdenum, vanadium, tungsten, niobium, titanium, and tantalum.

15. The method for producing a carbonaceous material according to claim 1 , wherein the inorganic oxide has a decomposition temperature of 800° C. or higher.

16. A carbon material-containing material containing a carbon material and an inorganic substance, at least a portion of the carbon material and at least a portion of the inorganic material are bonded by a covalent bond; the carbon material has a graphene structure or a structure similar to a graphene structure, The inorganic substance is an inorganic oxide having a metal hydroxyl group on the outermost surface. Carbon-containing materials.

17. １３ The carbon-containing material according to claim 16, which exhibits a peak between 125 ppm and 135 ppm in C-NMR analysis.

18. １３ The carbon-containing material according to claim 17, which exhibits a peak between 140 ppm and 160 ppm in C-NMR analysis.

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