Graphitic or carbonaceous moldings and processes for producing the same

Claim 2

A process for producing a carbonaceous or graphitic composite molding comprising a filler of at least one material in powder form selected from the group consisting of graphitic carbon, carbonaceous carbon, metals, metal compounds and other inorganic compounds qualified as a filler to a carbonaceous or graphitic molding derived from a mesophase-containing pitch, which comprises the four steps of: (1) suspending a filler comprising at least one material in powder form selected from the group consisting of graphitic carbon, carbonaceous carbon, metals, and metal compounds or other inorganic compounds qualified as a filler to a carbonaceous or graphitic molding in a tar containing a mesophase pitch precursor; (2) heating said suspension system to evaporate the light distillates contained in the tar by blowing of an inert gas into the suspension or by subjecting the suspension to a reduced pressure and subjecting said mesophase pitch precursor to heat treatment at 350° to 500° C. to obtain a carbonaceous precursor having a mesophase-containing pitch containing 30 to 80% by weight of quinoline insolubles, 40% or more of mesophase content, an upper limit of 400° C. and a carbonization yield at 1,000° C. of at least 70% by weight; (3) molding said carbonaceous precursor into a green molding containing mesophase-containing pitch; and (4) providing said green molding for carbonization or graphitization reaction in an inert atmosphere to form a carbonaceous or graphitic composite.

Claim 3

A process according to claim 1 wherein 5 to 1,000 parts by weight of the filler comprising said materials are used per 100 parts of the tar in the step (1).

Claim 4

A process according to claim 1 wherein the filler is selected from the group consisting of powders of graphite, carbon black, carbon black plated with metal, silica-alumina, γ-alumina, α-alumina, silicon carbide, silicon nitride, boron nitride, metals and mixtures thereof.

Claim 5

A process according to claim 1 wherein the carbonaceous filler in the step (1) is carbon black which is used in an amount of 10 to 500 parts by weight per 100 parts by weight of the mesophase-containing pitch.

Claim 6

A process according to claim 1 wherein heating is carried out at a temperature of 400° to 500° C. in the step (2).

Claim 7

A process according to claim 1 wherein the mesophase-containing pitch formed in the step (2) contains 20 to 70% by weight of quinoline solubles.

Claim 8

A process according to claim 1 wherein molding is carried out at a temperature not higher than the softening point of the mesophase-containing pitch in the step (3).

Claim 9

A process according to claim 1 wherein molding is carried out at a temperature higher than the softening point of the mesophase-containing pitch and up to 400° C. in the step (3).

Claim 10

A process according to claim 1 wherein carbonization or graphitization in the step (4) comprises heating said green molding in an inert atmosphere until carbonization or graphitization of the mesophase-containing pitch occurs.

Claim 11

A process according to claim 1 wherein the filler in the step (1) is a mixture of carbon black and copper powder, and the heating in the step (4) is carried out at 1,000° to 1,500° C. to produce a graphitic molding.

Claim 12

The process according to claim 1 in which the inorganic compound is selected from the group consisting of silica-alumina, alumina, silicon carbide and silicon nitride.

Claim 13

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase-containing pitch, which comprises the four steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension system at 350° to 550° C. while blowing an inert gas thereinto or subjecting said system to reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the surface of graphite particles; (3) pressure molding said carbonaceous precursor at 400° to 800° C. into a green molding; (4) carbonizing or graphitizing said green molding in an inert atmosphere; and the mesophase-containing pitch having 30 to 80% by weight of quinoline insolubles, 40% or more of mesophase content, an upper limit of melting temperature of 400° C. and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 14

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase-containing pitch, which comprises the four steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension system at 350° to 550° C. while blowing an inert gas thereinto or subjecting said system to reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the surface of graphite particles; (3) pressure molding said carbonaceous precursor at 400° to 800° C. into a green molding; (4) carbonizing or graphitizing said green molding in an inert atmosphere; and the mesophase-containing pitch having 30 to 80% by weight of quinoline insolubles, 40% or more of mesophase content, an upper limit of melting temperature of 400° C. and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 15

A process according to claim 12 wherein the amount of the tar relative to the graphite powder in the step (1) is so selected that the amount of the mesophase pitch formed on the graphite powder will be 3 to 3,000 parts by weight per 100 parts by weight of the graphite.

Claim 16

A process according to claim 13 wherein the amount of the tar relative to the graphite powder in the step (1) is so selected that the amount of the mesophase pitch formed on the graphite powder will be 3 to 50 parts by weight per 100 parts by weight of the graphite.

Claim 17

A process according to claim 12 wherein the heating in the step (2) is carried out at 400° to 500° C.

Claim 18

A process according to claim 12 wherein the content of the quinoline solubles in the mesophase pitch in the step (2) is 0 to 50%.

Claim 19

A process according to claim 12 wherein the heating in the step (3) is carried out at a temperature of 500° C. or higher.

Claim 20

A process according to claim 12 wherein the pressure molding in the step (3) is carried out under a pressure of 10 to 3,000 kg/cm 2 (gauge).

Claim 21

A process according to claim 12 wherein the step (4) comprises heating to a temperature of 800° C. or higher at a heat elevation speed of 1° to 1,500° C./hour.

Claim 22

A process according to claim 12 wherein the step (4) comprises heating to a temperature of 800° C. or higher at a heat elevation speed of 1° to 1,500° C./hour. and further to a temperature around 3,000° C. at a heat elevation speed of 150° to 3,000° C./hour.

Claim 23

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase pitch, which comprises the three steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension at 350° to 550° C. while blowing an inert gas thereinto or subjecting said suspension to a reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the graphite particles; and (3) pressure molding said carbonaceous precursor at 800° to 3,000° C.; and the mesophase-containing pitch having 30 to 80% by weight of quinoline insolubles, 40% or more of mesophase content, an upper limit of melting temperature of 400° C. and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 24

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase pitch, which comprises the three steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension at 350° to 550° C. while blowing an inert gas thereinto or subjecting said suspension to a reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the graphite particles; and (3) pressure molding said carbonaceous precursor at 800° to 3,000° C.; and the mesophase-containing pitch having 30 to 80% by weight of quinoline insolubles, 40% or more of mesophase content, an upper limit of melting temperature of 400° C. and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 25

A process according to claim 21 wherein the amount of the tar relative to the graphite powder in the step (1) is so selected that the amount of the mesophase pitch formed on the graphite powder will be 3 to 150 parts by weight per 100 parts by weight of the graphite.

Claim 26

A process according to claim 21 wherein the amount of the tar relative to the graphite powder in the step (1) is so selected that the amount of the mesophase pitch formed on the graphite powder will be 5 to 50 parts by weight per 100 parts by weight of the graphite.

Claim 27

A process according to claim 21 wherein the heating in the step (2) is carried out at 400° to 500° C.

Claim 28

A process according to claim 21 wherein the pressure molding in the step (3) is carried out by heating and pressurizing the carbonaceous precursor obtained in the step (2) without preliminary calcination.

Claim 29

A process according to claim 21 wherein the heating is carried out up to a desired temperature between 800° and 3,000° C. at a speed of 150° to 3,000° C./hour, and the pressurization is carried out under a pressure of 50 to 2,000 kg/cm 2 (gauge).

Claim 30

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase-containing pitch, which comprises the four steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension system at 350° to 550° C. while blowing an inert gas thereinto or subjecting said system to reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the surface of graphite particles; (3) pressure molding said carbonaceous precursor at 400° to 800° C. into a green molding; (4) carbonizing or graphitizing said green molding in an inert atmosphere; and the mesophase-containing pitch containing 50 to 100% by weight of quinoline insolubles and having a 40% or more mesophase content, an upper limit of melting temperature of 400° C., and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 31

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase-containing pitch, which comprises the four steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension system at 350° to 550° C. while blowing an inert gas thereinto or subjecting said system to reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the surface of graphite particles; (3) pressure molding said carbonaceous precursor at 400° to 800° C. into a green molding; (4) carbonizing or graphitizing said green molding in an inert atmosphere; and the mesophase-containing pitch containing 50 to 100% by weight of quinoline insolubles and having a 40% or more mesophase content, an upper limit of melting temperature of 400° C., and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 32

The process of claim 27 wherein a graphitic molding is produced which has a specific resistivity of 5.0 mΩ·cm. or less and a flexural strength of 200 kg./cm. 2 or higher, and, when carbonized at 1,000° C., undergoes a volume change of 3% or less and a weight change of 3% or less.

Claim 33

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase pitch, which comprises the three steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension at 350° to 550° C. while blowing an inert gas thereinto or subjecting said suspension to a reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the graphite particles; and (3) pressure molding said carbonaceous precursor at 800° to 3,000° C.; and the mesophase-containing pitch containing 50 to 100% by weight of quinoline insolubles and having a 40% or more mesophase content, an upper limit of melting temperature of 400° C., and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 34

A process for producing a carbonaceous composite molding comprising graphitic carbon and a carbonaceous or graphitic material derived from a mesophase pitch, which comprises the three steps of: (1) suspending graphite powder in a tar containing a mesophase pitch precursor; (2) heating the resulting suspension at 350° to 550° C. while blowing an inert gas thereinto or subjecting said suspension to a reduced pressure thereby to obtain a carbonaceous precursor having mesophase pitch formed on the graphite particles; and (3) pressure molding said carbonaceous precursor at 800° to 3,000° C.; and the mesophase-containing pitch containing 50 to 100% by weight of quinoline insolubles and having a 40% or more mesophase content, an upper limit of melting temperature of 400° C., and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 35

A process for producing a carbonaceous or graphitic composite molding comprising a filler of at least one material in powder form selected from the group consisting of graphitic carbon, carbonaceous carbon, metals, metal compounds and other inorganic compounds qualified as a filler to a carbonaceous or graphitic molding derived from a mesophase-containing pitch, which comprises the four steps of: (1) suspending a filler comprising at least one material in powder form selected from the group consisting of graphitic carbon, carbonaceous carbon, metals, and metal compounds or other inorganic compounds qualified as a filler to a carbonaceous or graphitic molding in a tar containing a mesophase pitch precursor; (2) heating said suspension system to evaporate the light distillates contained in the tar by blowing of an inert gas into the suspension or by subjecting the suspension to a reduced pressure and subjecting said mesophase pitch precursor to heat treatment at 350° to 500° C. to obtain a carbonaceous precursor having a mesophase-containing pitch formed on the surface of said material; (3) molding said carbonaceous precursor into a green molding containing mesophase-containing pitch; and (4) providing said green molding for carbonization or graphitization reaction in an inert atmosphere to form a carbonaceous or graphitic composite; and the mesophase-containing pitch precursor contains 30 to 80% by weight of quinoline insolubles and in which the mesophase-containing pitch has a 40% or more mesophase content, an upper limit of melting temperature of 400° C. and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 36

A process for producing a carbonaceous or graphitic composite molding comprising a filler of at least one material in powder form selected from the group consisting of graphitic carbon, carbonaceous carbon, metals, metal compounds and other inorganic compounds qualified as a filler to a carbonaceous or graphitic molding derived from a mesophase-containing pitch, which comprises the four steps of: (1) suspending a filler comprising at least one material in powder form selected from the group consisting of graphitic carbon, carbonaceous carbon, metals, and metal compounds or other inorganic compounds qualified as a filler to a carbonaceous or graphitic molding in a tar containing a mesophase pitch precursor; (2) heating said suspension system to evaporate the light distillates contained in the tar by blowing of an inert gas into the suspension or by subjecting the suspension to a reduced pressure and subjecting said mesophase pitch precursor to heat treatment at 350° to 500° C. to obtain a carbonaceous precursor having a mesophase-containing pitch formed on the surface of said material; (3) molding said carbonaceous precursor into a green molding containing mesophase-containing pitch; and (4) providing said green molding for carbonization or graphitization reaction in an inert atmosphere to form a carbonaceous or graphitic composite; and the mesophase-containing pitch precursor contains 30 to 80% by weight of quinoline insolubles and in which the mesophase-containing pitch has a 40% or more mesophase content, an upper limit of melting temperature of 400° C. and a carbonization yield at 1,000° C. of at least 70% by weight.

Claim 37

The process of claim 30, wherein a graphitic composite is produced which has a specific resistivity of 5.0 mΩ·cm. or less and a flexural strength of 200 kg./cm. 2 or higher, and, when carbonized at 1,000° C., undergoes a volume change of 3% or less and a weight change of 3% or less.