Polymetalosilazane and process for preparing same

Claim 2

A novel polymetalosilazane having a metal/silicon atomic ratio of 0.001 to 3 and a number average molecular weight of about 200 to about 500,000, which is obtained by reacting a polysilazane having a number average molecular weight of about 100 to about 50,000, which has a main skeleton consisting substantially of units represented by the following general formula (I): ##STR20## wherein each R 1 , R 2 and R 3 is independently selected from the group consisting of a hydrogen atom, an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, a group other than the above-mentioned groups in which the atom bonded directly to the silicon atom is a carbon atom, an alkylsilyl group, an alkylamino group and an alkoxy group, with the proviso that at least one of R 1 , R 2 and R 3 is a hydrogen atom, with a metal alkoxide represented by the following general formula (II): M(OR.sup.4).sub.n (II) wherein M stands for at least one metal selected from the group consisting of metals of groups IIA and III through V of the Periodic Table, R 4 's which may be the same or different stand for a hydrogen atom or an alkyl group having 1 to 20 carbon atoms or aryl group, with the proviso that at least one of R 4 's is the above-mentioned alkyl group or aryl group, and n stands for the valency of the metal M.

Claim 3

A polymetalosilazane according to claim 1, wherein each R 1 , R 2 and R 3 in said formula (I) is independently selected from the group consisting of a hydrogen atom, an alkyl group having 1 to 5 carbon atoms, an alkenyl group having 2 to 6 carbon atoms, a cycloalkyl group having 5 to 7 carbon atoms, an aryl group, an alkylsilyl group having 1 to 4 carbon atoms, an alkyl-amino group having 1 to 5 carbon atoms, and an alkoxy group having 1 to 5 carbon atoms, with the proviso that at least one of R 1 , R 2 and R 3 is a hydrogen atom.

Claim 4

A polymetalosilazane according to claim 2, wherein each R 1 , R 2 and R 3 in said formula (I) is independently selected from the a group consisting of a hydrogen atom, and methyl, ethyl, vinyl, allyl, methylamino, ethylamino, methoxy and ethoxy groups, with the proviso that at least one of R 1 , R 2 and R 3 is a hydrogen atom.

Claim 5

A polymetalosilazane according to claim 1, wherein one of R 1 and R 2 is a hydrogen atom.

Claim 6

A polymetalosilazane according to claim 4, wherein said polysilazane is represented by the following composition formula: (R.sup.2 SiHNH).sub.x [R.sup.2 SiH).sub.1.5 N].sub.1-x where 0.4<x<1.

Claim 7

A polymetalosilazane according to claim 1, wherein each of R 1 , R 2 and R 3 is a hydrogen atom.

Claim 8

A polymetalosilazane according to claim 6, wherein said polysilazane is represented the following composition formula: ##STR21## where a+b+c=1.

Claim 9

A polymetalosilazane according to claim 1, wherein M in said formula (II) stands for at least one metal selected from the group consisting of the groups III and IV of the Periodic Table.

Claim 10

A polymetalosilazane according to claim 8, wherein M in said formula (II) stands for at least one metal selected from the group consisting of Ti, Al and Zr.

Claim 11

A polymetalosilazane according to claim 8, wherein M in said formula (II) stands for at least one metal selected from the group consisting of B and Y.

Claim 12

A polymetalosilazane according to claim 1, wherein the R 4 's in said formula (II) may be the same or different and are selected from the group consisting of a hydrogen atom, an alkyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, with the proviso that at least one R 4 is one of the above-mentioned alkyl and aryl groups.

Claim 13

A polymetalosilazane according to claim 11, wherein the R 4 's in said formula (II) may be the same or different and are selected from the group consisting of a hydrogen atom, methyl, ethyl, n-propyl, i-propyl, n-butyl, i-butyl, t-butyl, phenyl, benzyl and tolyl groups, with the proviso that at least one R 4 is not a hydrogen atom.

Claim 14

A polymetalosilazane according to claim 1 wherein said polymetalosilazane has a number average molecular weight of about 400 to 300,000.

Claim 15

A polymetalosilazane according to claim 1, wherein the metal/silicon atomic ratio of about 0.001 to 2.5.

Claim 16

A polymetalosilazane according to claim 1, wherein said metal/silicon atomic ratio of 0.01 to 2.0.

Claim 17

A process for the preparation of a polymetalo-silazane, which comprises reacting a polysilazane having a number average molecular weight of about 100 to about 50,000, which has a skeleton consisting substantially of units represented by the following general formula (I): ##STR22## wherein the R 1 , R 2 and R 3 is independently selected from the group consisting of a hydrogen atom, an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group a atom other than the above-mentioned groups, in which the group bonded directly to the silicon atom is a carbon atom, an alkylsilyl group, an alkylamino group and an alkoxy group, with the proviso that at least one of R 1 , R 2 and R 3 is a hydrogen atom, with a metal alkoxide represented by the following general formula (II): M(OR.sup.4).sub.n (II) wherein M stands for at least one metal selected from the group consisting of metals of groups IIA and III through V of the Periodic Table, R 4 's which may be the same or different stand for a hydrogen atom or an alkyl group having 1 to 20 carbon atoms or aryl group, with the proviso that at least one of R 4 's is the above-mentioned alkyl group or aryl group, and n stands for the valency of M, to obtain a novel polymetalosilazane having a metal/silicon atomic ratio of from 0.001 to 3 and a number average molecular weight of about 200 to about 500,000.

Claim 18

A process for the preparation of a polymetalo-silazane, which comprises reacting a polysilazane having a number average molecular weight of about 100 to about 50,000, which has a skeleton consisting substantially of units represented by the following general formula (I): ##STR22## wherein the R 1 , R 2 and R 3 is independently selected from the group consisting of a hydrogen atom, an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group a atom other than the above-mentioned groups, in which the group bonded directly to the silicon atom is a carbon atom, an alkylsilyl group, an alkylamino group and an alkoxy group, with the proviso that at least one of R 1 , R 2 and R 3 is a hydrogen atom, with a metal alkoxide represented by the following general formula (II): M(OR.sup.4).sub.n (II) wherein M stands for at least one metal selected from the group consisting of metals of groups IIA and III through V of the Periodic Table, R 4 's which may be the same or different stand for a hydrogen atom or an alkyl group having 1 to 20 carbon atoms or aryl group, with the proviso that at least one of R 4 's is the above-mentioned alkyl group or aryl group, and n stands for the valency of M, to obtain a novel polymetalosilazane having a metal/silicon atomic ratio of from 0.001 to 3 and a number average molecular weight of about 200 to about 500,000.

Claim 19

A process according to claim 16, wherein each R 1 , R 2 and R 3 in said formula (I) is independently selected from the group consisting of a hydrogen atom, an alkyl group having 1 to 5 carbon atoms, an alkenyl group having 2 to 6 carbon atoms, a cycloalkyl group having 5 to 7 carbon atoms, an aryl group, an alkylsilyl group having 1 to 4 carbon atoms, an alkylamino group having 1 to 5 carbon atoms, and an alkoxy group having 1 to 5 carbon atoms, with the proviso that at least one of R 1 , R 2 and R 3 is a hydrogen atom.

Claim 20

A process according to claim 17, wherein R 1 , R 2 and R 3 in said formula (I) independently stand for one of the group consisting of a hydrogen atom, and methyl, ethyl, vinyl, allyl, methylamino, ethylamino, methoxy and ethoxy groups, with the proviso that at least one of R 1 , R 2 and R 3 is a hydrogen atom.

Claim 21

A process according to claim 16, wherein one of R 1 and R 2 is a hydrogen atom.

Claim 22

A process according to claim 19, wherein said polysilazane is represented by the following composition formula: (R.sup.2 SiHNH).sub.x [(RSiH).sub.1.5 N].sub.1-x where 0.4<x<1.

Claim 23

A process according to claim 16, wherein each of R 1 , R 2 and R 3 is a hydrogen atom.

Claim 24

A process according to claim 19, wherein said polysilazane is represented by the following chemical formula: ##STR23## where a+b+c=1.

Claim 25

A process according to claim 16, wherein M in said formula (II) stand for at least one metal selected from the group consisting of the groups III and IV of the Periodic Table.

Claim 26

A process according to claim 23, wherein M in said formula (II) stand for at least one metal selected from the group consisting of Ti, Al and Zr.

Claim 27

A process according to claim 23, wherein M in said formula (II) stands for at least one metal selected from the group consisting of B and Y.

Claim 28

A process according to claim 16, wherein R 4 's in said formula (II) may be the same or different and stand for one of the group consisting of a hydrogen atom, an alkyl group having 1 to 10 carbon atoms and an aryl group having 6 to 10 carbon atoms, with the proviso that at least one of R 4 's is the above-mentioned alkyl group or aryl group.

Claim 29

A process according to claim 16 wherein R 4 's in said formula (II) may be the same or different and stand for a hydrogen atom, and methyl, ethyl, n-propyl, i-propyl n-butyl, i-henol, t-butyl, phenyl, benzyl and tolyl groups, with the proviso that at least one of R 4 's is not a hydrogen atom.

Claim 30

A process according to claim 16, wherein said mixing ratio of polysilazane/metal alkoxide is such that the M/Si atomic ratio is from 0.01 to 5.

Claim 31

A process according to claim 28, wherein said mixing ratio of polysilazane/metal alkoxide is such that the M/Si atomic ratio is from 0.05 to 2.5.