JP2008077894A - Electrode active substance for nonaqueous type power storage device and its manufacturing method - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide an electrode active substance for a nonaqueous type power storage device with a small irreversible capacity and a capacity higher than that of graphite for active substances available as electrode materials for the nonaqueous type power storage devices. <P>SOLUTION: The problem is solved by the electrode material for the storage device using an electrode active substance for the nonaqueous type storage device which is a complex formed by baking carbonaceous materials bridged by -O-Si-O-. The complex is provided with a peak in the vicinity of 101.5 eV and in the vicinity of 103.5 eV in a Si2p spectrum for X-ray photoelectron spectroscopy and a ratio of strength between the peak A in the vicinity of 101.5 eV and the peak B in the vicinity of 103.5 eV is A/B=10/90 to 30/70. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

  The present invention relates to an electrode active material for a non-aqueous power storage device and a production method thereof. When the active material comprising the composite according to the present invention is used for an electrode for a non-aqueous power storage device, it has a low irreversible capacity and a high discharge capacity. Therefore, a non-aqueous power storage represented by a lithium ion secondary battery or an electric double layer capacitor Suitable for device applications.

  In recent years, with the miniaturization and mobile use of electronic devices, it is desired to increase the energy density of power storage devices. Lithium ion batteries and lithium polymer batteries have high voltage and high energy density among power storage devices, and are therefore used as power sources for mobile devices. As a constituent material of such a lithium ion battery, lithium cobaltate is usually used as an active material for the positive electrode, and a graphite-based carbon material such as natural graphite or artificial graphite is used for the negative electrode.

  However, since the theoretical capacity of graphite is 372 mAh / g, it is difficult to reach a higher capacity than this, and development of a material exhibiting a high capacity is desired. In response to this demand, silicon, tin, and the like are being developed as active materials suitable for the negative electrode exhibiting a high capacity, but when these materials occlude lithium ions, their volume changes greatly, Since cracks in the active material particles, poor contact between the active material and the current collector, and the like occur, there arises a problem that the charge / discharge cycle life is shortened.

As a method for solving such a problem, for example, it has been proposed to use SiO _x (0 <x <2) whose volume expansion coefficient during charging is lower than that of silicon as the active material of the negative electrode (Patent Document 1). However, when such an oxide is used, since the initial irreversible capacity is large although the discharge capacity is large, there is a problem that the positive electrode material has to be greatly increased, and the total amount of energy as a battery does not increase greatly. Arise. Therefore, a material having a small irreversible capacity and a higher capacity than graphite is demanded.
Japanese Patent No. 2999741

On the other hand, it contains graphite particles, amorphous carbon and silicon, the silicon content in terms of SiO ₂ is 40 to 80% by weight, the true density is 1.8 × 10 ³ kg / m ³ or more, the tap density Discloses a composite electrode material having a surface area of 0.8 × 10 ³ kg / m ³ or more and a specific surface area of 8 × 103 m ² / kg or less. And it is described that this composite electrode material has one peak in the vicinity of 102.5 to 107.5 eV in the Si2p spectrum of XPS (Patent Document 2).
JP 2002-231225 A

Further, a carbon compound containing 1 to 100% by weight of silicon based on carbon is disclosed in a carbon material fired at 800 ° C. to 1500 ° C. in an inert gas atmosphere using a phenol resin as a raw material (patent) Reference 3). However, the composite electrode materials and carbon compounds described above are still not sufficient from the viewpoint of total energy.
JP-A-11-322323

  Therefore, an object of the present invention is to provide an electrode active material for a non-aqueous storage device and a method for producing the same in an active material used for an electrode material of a non-aqueous storage device that has a small irreversible capacity and a higher capacity than graphite. There is.

  As a result of intensive investigations of a carbonaceous raw material crosslinked with —O—Si—O— by focusing on the fired composite, the present inventors have found that the Si2p spectrum by X-ray photoelectron spectroscopy is around 101.5 eV. And a composite having a peak in the vicinity of 103.5 eV and an intensity ratio (percentage) of peak A in the vicinity of 101.5 eV and peak B in the vicinity of 103.5 eV being A / B = 10/90 to 30/70 It has been found that the above object can be achieved by an electrode active material for a non-aqueous power storage device comprising the present invention, and has led to the present invention. That is, the present invention is an electrode active material for a non-aqueous power storage device comprising a composite obtained by firing a carbonaceous raw material crosslinked with —O—Si—O—, and in an Si2p spectrum by X-ray photoelectron spectroscopy, It has peaks in the vicinity of .5 eV and 103.5 eV, and the intensity ratio of peak A in the vicinity of 101.5 eV and peak B in the vicinity of 103.5 eV is A / B = 10/90 to 30/70. It is the electrode active material for non-aqueous power storage devices characterized.

  In another aspect of the present invention, a composite obtained by firing a carbonaceous raw material crosslinked with —O—Si—O— is further fired at 1400 to 1600 ° C. under pressure. It is a manufacturing method of the electrode active material for non-aqueous electrical storage devices which consists of.

  The electrode using the electrode active material for a non-aqueous storage device comprising the composite of the present invention has a small irreversible capacity and a higher capacity than graphite. Therefore, a lithium-ion battery or an electric double layer which is a non-aqueous storage device Suitable for capacitor electrodes.

  The composite of the present invention is obtained by firing a carbonaceous raw material crosslinked with —O—Si—O—, and the carbonaceous raw material crosslinked with —O—Si—O— is a silicon compound. And prepared from carbonaceous raw materials. Examples of the silicon compound include tetraalkoxysilane, alkyltrialkoxysilane which may have a functional group, oligomers thereof, and compounds derived by hydrolysis of terachlorosilane.

In particular, the general formula (I)
Si (OR) ₄ (I)
From the viewpoints of reactivity and crosslinkability, silicon compounds such as tetraalkoxysilane and / or oligomers thereof are preferred. Here, R is a hydrogen atom or an optionally substituted alkyl group or aryl group having 1 to 10 carbon atoms. Examples of the alkyl group include a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, an isobutyl group, a t-butyl group, an amyl group, an isoamyl group, a hexyl group, a cyclohexyl group, a heptyl group, an octyl group, and a cyclooctyl group. Examples of the aryl group include a phenyl group and a naphthyl group.

  Examples of the substituent include an alkyl group, aryl group, alkoxy group, carboxyl group, carbonyl group, alkoxycarbonyl group, carbonate group, amino group, amide group, oxirane group, isocyanate group, and thioisocyanate group.

  When tetraalkoxysilane is used as the silicon compound, tetraalkoxysilane may be used as it is or after hydrolysis. Further, it may be used after being oligomerized. Hydrolysis may be performed under either basic or acidic conditions. However, in consideration of operability and industrial stability, hydrolysis is preferably performed under acidic conditions.

  When the silicon compound is an oligomer, the oligomer is preferably a tetraalkoxysilane 3 to 100 mer, and a 3 to 50 mer is preferably used in consideration of operability and reactivity. The oligomer may be used as it is, or may be used after hydrolysis in consideration of compatibility with the polymer material. Hydrolysis may be performed under either basic or acidic conditions. However, in consideration of operability and industrial stability, hydrolysis is preferably performed under acidic conditions.

  The carbonaceous raw material crosslinked with —O—Si—O— is preferably a carbonaceous raw material obtained by a crosslinking reaction between a carbonaceous raw material and a hydrolyzate of tetraalkoxysilane. Such a carbonaceous raw material can be obtained by mixing and reacting a carbonaceous raw material with a silicon compound such as tetraalkoxysilane and / or an oligomer thereof.

  When mixing the silicon compound and the carbonaceous raw material, or when further adding a conductive material, use a solvent to ensure the dispersibility of the silicon compound and the carbonaceous raw material and the compatibility between the silicon compound and the carbonaceous raw material. Also good. Examples of such solvents include alcohols such as methanol, ethanol and isopropanol, quinoline, pyridine, toluene, benzene and tetrahydrofuran. When a solvent is used, the solvent may be distilled off when a silicon compound described later and a carbonaceous material are reacted.

  The carbonaceous raw material is not particularly limited as long as it is a material that becomes a carbide, such as a resole resin, a phenolic resin such as a novolac resin, a thermosetting resin such as an epoxy resin, a calixarene, a furan resin, a polyvinyl chloride, Examples thereof include polyvinylidene chloride, polyacrylonitrile, polyamide resin, polyimide resin, polyamideimide resin, synthetic pitch, petroleum pitch, coal pitch, and tars. Of these, thermosetting resins are preferred. These may be used alone or in combination of two or more.

  Among thermosetting resins, phenol resins and epoxy resins such as resole resin and novolak resin are preferable because they do not melt during carbonization, and phenol resin is more preferable in terms of carbonization yield. Of these, a novolac type phenol resin is preferable in consideration of operability and reactivity. When a phenol resin or an epoxy resin is used, a compound that reacts with these functional groups to form a crosslinked structure, that is, a polyhydric alcohol, a polyvalent epoxy compound, or the like may be used in combination.

  Examples of the polyhydric alcohols include aliphatic polyhydric alcohols such as ethylene glycol, glycerin, and polyvinyl alcohol, and aromatic polyhydric alcohols such as pyrocatechol, resorcinol, and hydroquinone. For example, aliphatic polyepoxy compounds such as glycerol polyglycidyl ether and trimethylolpropane polyglycidyl ether, and aromatic polyepoxy compounds such as bisphenol A type epoxy compounds can be used. Usually, such a crosslinking agent is used in the range of 1 to 40% by weight based on the raw material.

  When reacting the silicon compound with the carbonaceous raw material, an acid or base catalyst can be added. Examples of the base catalyst include alkali metal hydroxides such as lithium hydroxide, sodium hydroxide and potassium hydroxide, organic amines such as ammonia, monomethylamine and dimethylamine, and quaternary compounds such as tetramethylammonium hydroxide. Ammonium salts can be used. Examples of the acid catalyst include inorganic acids such as hydrochloric acid, sulfuric acid, nitric acid, perchloric acid, phosphoric acid and boric acid, organic sulfonic acids such as p-toluenesulfonic acid, formic acid, acetic acid, Organic monocarboxylic acids such as propionic acid and benzoic acid, and organic dicarboxylic acids such as oxalic acid, malonic acid, succinic acid, fumaric acid, phthalic acid, isophthalic acid and terephthalic acid can be used. In consideration of operability and industrial stability, it is desirable to carry out the reaction under acidic conditions. Among them, inorganic acids such as hydrochloric acid and nitric acid having a pKa value of 4 or less to promote the reaction, malonic acid, fumaric acid, etc. It is preferable to use an organic dicarboxylic acid such as an acid.

  The amount of carbonaceous material used is preferably 0.01 to 10 times the weight of the silicon compound. The amount is more preferably 0.02 to 1 times by weight, and further preferably 0.05 to 0.5 times by weight in consideration of the operability and the lithium occlusion amount of the obtained electrode material.

  When producing a carbonaceous raw material crosslinked with —O—Si—O—, it is preferable to add a conductive material (C) because the conductivity of the electrode material can be improved. Examples of such a conductive material include graphite such as natural graphite, artificial graphite, and expanded graphite, carbon black, carbon fiber, and carbon tube. Of these, graphite is preferable. Of the graphite, a flat plate material is preferable, and specific examples include flaky graphite and scaly graphite. The conductive material is preferably added so as to be 1 to 30% by mass in the composite.

  When a conductive material is added, there is no particular limitation as long as the dispersibility of the conductive material can be ensured. However, in order to obtain an active material with excellent conductivity, the surface of the conductive material is wetted with a carbonaceous material or a silicon compound. It is preferable to create a state. For example, a solution in which the conductive material is well dispersed can be obtained by mixing a silicon compound and a carbonaceous raw material to obtain a homogeneous solution, mixing the conductive material with this solution, and preferably performing vacuum degassing.

  A composite in which the silicon compound and the carbonaceous raw material are homogeneous is preferable because the cycle characteristics of the lithium ion secondary battery can be improved. From such a viewpoint, it is preferable to select a carbonaceous raw material that is compatible with the silicon compound as the carbonaceous raw material.

  The method for mixing the silicon compound and the carbonaceous raw material is not particularly limited as long as the homogeneity of the silicon compound in the carbonaceous raw material can be ensured, and may be mixed by a known method below the decomposition temperature of the carbonaceous raw material. Furthermore, when using a carbonaceous raw material having reactivity with a silicon compound, in order to obtain a composite having excellent homogeneity, the silicon compound and the carbonaceous raw material are mixed to form a homogeneous solution, and then the silicon compound and the carbonaceous raw material are mixed. It is preferable to react to form a precursor of a homogeneous composite.

  Homogeneous here means a state in which phase separation between the silicon compound and the carbonaceous raw material cannot be confirmed even when measured with a scanning electron microscope or a transmission electron microscope at an observation magnification of 5,000 to 100,000. To do. Such a reaction between the silicon compound and the carbonaceous raw material is performed in the range of 20 ° C. to 300 ° C. in consideration of the decomposition temperature of the carbonaceous raw material. A catalyst is preferably used in the reaction between the silicon compound and the carbonaceous raw material. Examples of the catalyst include an acid catalyst and a base catalyst, but an inorganic acid such as nitric acid and an organic acid such as fumaric acid are preferable in consideration of the persistence in the complex.

  In the present invention, when a silicon compound such as an alkoxysilane represented by the general formula (I) or an oligomer thereof is used as a silicon compound, the silicon compound and a carbonaceous raw material are reacted to form a composite precursor. Hydrolysis and dealcohol condensation can also be performed. The hydrolysis can be performed, for example, by charging the composite precursor into a stirring reactor and blowing an inert gas containing water vapor. The hydrolysis rate is not particularly limited as long as the silicon compound is not vaporized by heat treatment such as carbonization or thermal reduction of the composite precursor. Usually, hydrolysis is performed at a temperature below the decomposition temperature of the carbonaceous raw material in consideration of operability and safety, and is performed at room temperature to about 180 ° C.

  The composite precursor can be obtained by subjecting it to primary firing treatment and further firing treatment under pressure. The primary baking treatment is preferably performed at an ultimate temperature of 900 to 1400 ° C. in an inert gas atmosphere. If the firing temperature is too low, carbonization is not sufficient. A high temperature is not preferable because the silicon compound is volatilized. Nitrogen, argon, etc. can be used as the inert gas. The heating rate is usually 50 to 500 ° C./hour in consideration of operability.

  The pressurizing condition is not particularly limited as long as the pressure is higher than 0.1 MPa. However, even if the pressure is increased, the characteristics are not affected and only the cost is increased. Is desirable. If the firing treatment temperature under pressure is too low, the irreversible capacity increases, and if it is too high, the capacity decreases. Therefore, the temperature is 1400 to 1600 ° C., preferably 1450 to 1550 ° C. in an inert gas atmosphere. It is good to hold for about 12 minutes. Argon or the like can be used as the inert gas. Moreover, you may perform a primary baking process and the baking process under pressure continuously.

  The composite is formed on the electrode, but when the average particle diameter of the composite exceeds 50 μm, there may be a problem in terms of the smoothness of the electrode, and when the average particle system is less than 1 μm, Therefore, the composite may be pulverized and classified so that the average particle diameter of the composite is 1 μm to 50 μm, preferably 2 μm to 20 μm before or after the heat treatment. For the pulverization, a known mechanical pulverization apparatus may be used.

  Desirably, the composite is substantially homogeneous. The term “substantially homogeneous” refers to a state in which phase separation between silicon oxide and a conductive substance cannot be confirmed even when measured with a scanning electron microscope or a transmission electron microscope at an observation magnification of 5,000 to 100,000. .

  The electrode active material for a non-aqueous storage device of the present invention comprising such a composite has a peak A near 101.5 eV and a peak B near 103.5 eV in the Si2p spectrum of X-ray photoelectron spectroscopy (XPS). . In the present invention, the intensity ratio of peak A and peak B (peak intensity ratio) needs to be in the range of A / B = 10/90 to 30/70. When the peak intensity ratio is larger than 30/70, the capacity is lowered. On the other hand, when the peak intensity ratio is smaller than 10/90, although the capacity is high, the irreversible capacity is increased.

  The XPS measurement is performed under the conditions of excitation X-ray source: Mg—Kα ray, applied voltage: 15 kV, emission current: 10 mA, Pass Energy: 40 eV, and photoelectron detection angle: 90 ° with respect to the sample surface. As the reference peak, the peak of the largest peak among the carbon components in the complex observed in the C1s spectrum was set to 285 eV.

  The electrode active material comprising the composite of the present invention is kneaded with a conductive material, a binder or the like and molded to be used as an electrode material for an electricity storage device. Examples of the electrode material for an electricity storage device include a lithium battery, a lithium ion secondary battery, and a capacitor, and a negative electrode material for a lithium ion secondary battery is preferable.

  Such a conductive material is not particularly limited as long as it does not adversely affect battery performance. For example, carbon black, natural graphite (such as scale graphite, earthy graphite), artificial graphite, carbon whisker, carbon nano Examples thereof include carbons such as fibers, multi-wall type carbon fibers and carbon tubes, metals such as copper, silver and gold, and conductive ceramics.

  Examples of the binder usually include materials such as polyfluoroethylene, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, ethylene-propylene diene terpolymer, styrene butadiene rubber, and fluororubber.

  The composite obtained as described above is mixed with a binder and a conductive material, pressed into a mold or rolled into a sheet, and formed into a polarizable electrode by punching into a required shape. Can do. Moreover, after apply | coating the slurry which mixed the composite_body | complex, electroconductive material, the binder, and the solvent on the electrical power collector, it can also dry and roll-press as needed and shape | mold into a polarizable electrode. In that case, you may use organic compounds, such as alcohol and N-methylpyrrolidone, solvents, such as water, a dispersing agent, and various additives as needed. It is also possible to apply heat.

  The electrode made of the composite is preferably used as a negative electrode material for a lithium ion secondary battery. FIG. 1 is an example of a schematic view showing a cross section of the lithium ion secondary battery thus obtained. In FIG. 1, 1 is a positive electrode, 2 is a negative electrode, 3 and 4 are current collecting members, 5 is a separator, 6 and 7 are upper and lower lids, and 8 is a gasket. Hereinafter, the present invention will be described more specifically with reference to examples, but the present invention is not limited thereto.

Example 1
In a three-necked flask equipped with a thermometer and a cooler, 36.3 g of tetramethoxysilane oligomer (M-silicate 51, manufactured by Tama Chemical Industry Co., Ltd.) and a novolac type phenol resin (Register Top PSM-6200, manufactured by Gunei Chemical Co., Ltd.) 6.2 g was added and heated to 120 ° C. with stirring under a nitrogen stream to obtain a uniform mixed solution. Further, 5 g of graphite particles (GR-15 manufactured by Nippon Graphite Industry Co., Ltd.) and 0.5 g of fumaric acid were added while stirring, and the mixture was heated to 180 ° C. and stirred for 1 hour. Thereafter, the contents were transferred to a Brabender type kneader and kneaded at 180 ° C. for 3 hours under a nitrogen stream to obtain a composite precursor.

  Next, using a ceramic tube furnace, the temperature was raised to 400 ° C. at a rate of 100 ° C./hour in a nitrogen stream, held at that temperature for 1 hour, and then further raised to 900 ° C. at 100 ° C./hour. Held for 1 hour to carbonize and decompose the phenol resin and the silane compound, respectively. Furthermore, using a pressure firing apparatus (manufactured by Fuji Denpa Kogyo Co., Ltd., High Multi 5000), the temperature was raised to 1450 ° C. over 60 minutes under an argon pressure of 0.3 MPa, and then the composite was fired at the same temperature for 12 hours. Obtained. Measurement was performed with a transmission electron microscope (H-800NA type manufactured by Hitachi, Ltd.) at an observation magnification of 100,000, but phase separation between silicon oxide and carbonaceous material could not be confirmed. FIG. 2 shows an electron micrograph.

X-ray electron spectroscopy (XPS)
XPS analysis uses AXIS-HS manufactured by Shimadzu-Kratos, excitation X-ray source: Mg-Kα ray, applied voltage:
15 kV, emission current: 10 mA, Pass Energy: 40 eV, photoelectron detection angle: 90 ° with respect to the sample surface, the peak of the largest peak among the carbon components in the complex observed in the C1s spectrum Set to 285 eV. The XPS Si2p spectrum is shown in FIG. It has a peak A near 101.5 (eV) and a peak B near 103.6 (eV). The intensity ratio between peak A and peak B was 14/86. Since the peak intensity ratio varies to some extent as shown in Table 1, in Example 1, a sample was prepared with N = 3, and the measured peak intensity ratio and average value of peak positions were used. .

  To 90 parts by weight of the obtained active material, 5 parts by weight of polyvinylidene fluoride dissolved in N-methyl-2-pyrrolidone and 5 parts by weight of acetylene black were added and kneaded to prepare a slurry. This slurry was applied to a rolled copper foil to a thickness of 150 μm, dried at 80 ° C. for 1 hour, and then rolled to a thickness of about 100 μm by a rolling roll machine. A negative electrode was produced by vacuum drying at 80 ° C. for 12 hours.

A coin-type cell was produced under an argon atmosphere by using Li metal as a counter electrode, an ethylene carbonate / diethyl carbonate 3/7 (weight ratio) solution in which 1M LiPF ₆ was dissolved as an electrolyte, and a porous polyolefin separator as a separator. Charging was performed at a current density of 0.44 mA / cm ² and cut at 5 mV. The discharge was cut at 1.5 V with a current density of 0.44 mA / cm ² . The discharge capacity based on the negative electrode weight in the first cycle and the irreversible capacity (charge capacity value-discharge capacity value) are shown in Table 2. The discharge capacity value exceeds 372 mAh / g, which is the theoretical discharge capacity value of graphite. Yes.

Example 2
An active material was obtained in the same manner as in Example 1 except that the pressure firing temperature was changed to 1550 ° C. and the holding time was changed to 6 hours. A battery was prepared in the same manner as in Example 1, and the discharge capacity and irreversible capacity based on the negative electrode weight were measured. Table 2 shows the peak position, peak intensity ratio, discharge capacity based on the negative electrode weight in the first cycle, and irreversible capacity in the XPS Si2p spectrum.

Comparative Example 1
An active material was obtained in the same manner as in Example 1 except that no pressure was applied, the firing temperature was 1550 ° C., and the holding time was 6 hours. A battery was prepared in the same manner as in Example 1, and the discharge capacity and irreversible capacity based on the negative electrode weight were measured. Table 2 shows the peak position, peak intensity ratio, discharge capacity based on the negative electrode weight in the first cycle, and irreversible capacity in the XPS Si2p spectrum.

Comparative Example 2
An active material was obtained in the same manner as in Example 1 except that no pressure was applied, the firing temperature was 1200 ° C., and the holding time was 10 hours. A battery was prepared in the same manner as in Example 1, and the discharge capacity and irreversible capacity based on the negative electrode weight were measured. Table 2 shows the peak position, peak intensity ratio, discharge capacity based on the negative electrode weight in the first cycle, and irreversible capacity in the XPS Si2p spectrum.

Comparative Example 3
An active material was obtained in the same manner as in Example 1 except that the pressure firing temperature was 1750 ° C. and the holding time was 2 hours. A battery was prepared in the same manner as in Example 1, and the discharge capacity and irreversible capacity based on the negative electrode weight were measured. Table 2 shows the peak position, peak intensity ratio, discharge capacity based on the negative electrode weight in the first cycle, and irreversible capacity in the XPS Si2p spectrum.

  According to the present invention, an electrode active material for an electricity storage device and a method for manufacturing the electrode active material can be provided. Such an active material is suitable as an electrode material for an electricity storage device, and exhibits a low irreversible capacity and a discharge capacity higher than that of graphite, and thus is particularly preferably used as a negative electrode material for a lithium ion secondary battery.

It is the cross-sectional schematic of the lithium secondary battery which used the active material of this invention as the negative electrode material.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Positive electrode 2 Negative electrode 3 Current collecting member 4 Current collecting member 5 Separator 6 Upper lid 7 Lower lid 8 Gasket

Claims (8)

An electrode active material for a non-aqueous power storage device comprising a composite obtained by firing a carbonaceous raw material crosslinked with —O—Si—O—, and in the Si2p spectrum measured by X-ray photoelectron spectroscopy, around 101.5 eV and 103 A non-aqueous system having a peak in the vicinity of 0.5 eV and an intensity ratio of peak A in the vicinity of 101.5 eV and peak B in the vicinity of 103.5 eV is A / B = 10/90 to 30/70 Electrode active material for electricity storage devices. The carbonaceous raw material crosslinked with -O-Si-O- is a carbonaceous raw material obtained by a crosslinking reaction between a carbonaceous raw material and a hydrolyzate of tetraalkoxysilane. Electrode active material. The electrode active material for a non-aqueous power storage device according to claim 1 or 2, wherein the carbonaceous material is a thermosetting resin. The electrode active material for a non-aqueous power storage device according to claim 3, wherein the thermosetting resin is a novolac resin. A composite obtained by firing a carbonaceous raw material crosslinked with —O—Si—O— is further fired at 1400 to 1600 ° C. under pressure, and the electrode active for a non-aqueous power storage device comprising the composite A method for producing a substance. The carbonaceous raw material cross-linked with -O-Si-O- is a carbonaceous raw material obtained by a cross-linking reaction between a carbonaceous raw material and a hydrolyzate of tetraalkoxysilane. A method for producing an electrode active material. The method for producing an electrode active material for a non-aqueous power storage device according to claim 6 or 7, wherein the carbonaceous material is a thermosetting resin. The method for producing an electrode active material for a non-aqueous power storage device according to claim 8, wherein the thermosetting resin is a novolac resin.

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