KR20160071912A - Process of synthesizing disilane - Google Patents

Process of synthesizing disilane Download PDF

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KR20160071912A
KR20160071912A KR1020140179692A KR20140179692A KR20160071912A KR 20160071912 A KR20160071912 A KR 20160071912A KR 1020140179692 A KR1020140179692 A KR 1020140179692A KR 20140179692 A KR20140179692 A KR 20140179692A KR 20160071912 A KR20160071912 A KR 20160071912A
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inert gas
synthesized
present
diacylene
disilane
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KR1020140179692A
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Korean (ko)
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강영남
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강영남
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    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F7/00—Compounds containing elements of Groups 4 or 14 of the Periodic Table
    • C07F7/02—Silicon compounds
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F7/00—Compounds containing elements of Groups 4 or 14 of the Periodic Table
    • C07F7/02—Silicon compounds
    • C07F7/08—Compounds having one or more C—Si linkages
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F7/00—Compounds containing elements of Groups 4 or 14 of the Periodic Table
    • C07F7/02—Silicon compounds
    • C07F7/08—Compounds having one or more C—Si linkages
    • C07F7/12—Organo silicon halides
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S516/00—Colloid systems and wetting agents; subcombinations thereof; processes of
    • Y10S516/01—Wetting, emulsifying, dispersing, or stabilizing agents

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  • Organic Chemistry (AREA)

Abstract

The present invention relates to a method for manufacturing disilane by filling a container including a catalyst with an inert gas, and conducting a reaction by adding a disilane precursor into the container. In the present invention, synthesized disilane is transported by using the inert gas, and can be separated and collected from the inert gas at a low temperature through a simple method. Thus, according to the present invention, the manufacturing method can manufacture a large quantity of disilane exceeding laboratory scale while securing safety, and thus is advantageous in a process.

Description

PROCESS OF SYNTHESIZING DISLLANE [0002]

The present invention relates to a process for producing diacylene, and more particularly, to a process for producing diacylene capable of mass production and ensuring safety.

As electronic technology has developed, many materials have been used in display devices such as computer chips, liquid crystal displays (LCD), and organic light emitting diodes (OLED) An insulating film such as an insulating film should be formed. Silicon-based inorganic materials such as silicon oxide (SiOx) and silicon nitride (SiNx) are widely used as such insulating film materials.

For example, in connection with the application of silicon-based inorganic materials to semiconductor devices and display devices, a chemical vapor deposition (CVD) process such as plasma enhanced chemical vapor deposition (PECVD) or thermal chemical vapor deposition (TCVD) A polycrystalline or amorphous silicon thin film can be produced by depositing a silane gas as a raw material on a suitable substrate such as a wafer or a substrate by a CVD (chemical vapor deposition) method. Conventionally, monosilane is mainly used as a raw silane gas. However, since the line width of a semiconductor device is becoming finer and smaller, it has been difficult to obtain such a line width of finely-used monosilane.

In recent years, disilane has been used instead of monosilane. The colorless gas of the formula Si 2 H 6 , molecular weight 62.22 g / mol, density 2.7 g / m 3, melting point -32 ° C, boiling point -4 ° C, is a disiliconethane, disilicon hexa hydrate hexahydride).

Dyssilane is used to form a thin film according to a CVD process in a semiconductor manufacturing process. The thin film can be deposited at a lower deposition temperature than that of monosilane, which is conventionally used, so that a thin film having a uniform thickness can be easily formed. In addition, the deposition rate of the diisocyanate is 4 to 5 times higher than that of the monosilane, so that the efficiency of the thin film deposition process can be secured. In particular, the thin film can be formed in a micronization process in which the line width of the semiconductor device is 20 nm .

As a method for producing conventional diacylenes, a method of purifying the diacylene present in monosilane has been mainly used by using a vapor phase method of condensing monosilane with hydrogen. However, the method of purifying the di-silane in the monosilane was low in yield and high in production cost.

Therefore, in the case of producing diacylene by the vapor-phase method, the amount of diacylene produced is remarkably small as compared with the amount of demand, so that the price is very high. In recent years, a lot of efforts have been made to meet demand and production has increased, but the price of dicyclene is still high because of the low yield and risk of production.

On the other hand, a method has been proposed in which hydrogen is added to monosilane to increase the amount of disilene, which is a by-product, to purify it. However, such a method requires a large-scale production facility and has a problem of low yield.

Also, a method has been proposed in which halogen is replaced with hydrogen in a dicylene substituted with a halogen using LiAlH 4 as a catalyst. Although this method has the advantage of high yield, the reactivity of the catalyst is so intense that there is a danger of explosion during the reaction, so safety facilities must be secured sufficiently. It is also possible to synthesize silane at the laboratory scale through this method, but there are many difficulties in mass production of silane.

Korean Patent No. 10-1231370 proposes an apparatus and a method for pyrolyzing monosilane to produce diacylene. In this patent, it is possible to produce high purity dicyclene, but since high temperature and pyrolysis pressure are required, the stability of the process and the safety of the manufacturing facility are not sufficiently secured.

DISCLOSURE Technical Problem The present invention has been made in order to solve the problems of the prior art described above, and it is an object of the present invention to provide a method of manufacturing a diaciline which can be produced on a large scale outside a laboratory scale.

It is still another object of the present invention to provide a method for producing di-silane which is safe in the process.

According to the present invention, there is provided a method for producing a catalyst, comprising: charging an inert gas into a container in which a catalyst is stored; Adding a substituted dicayene represented by the following formula (1) to a container filled with the catalyst and the inert gas to synthesize dicaylane; And collecting the synthesized di-silane.

[Chemical Formula 1]

R a Si 2 X 6-a

(Wherein R is a C 1 -C 10 alkoxy group, X is a halogen, and a is an integer of 0 to 6)

For example, in Formula 1, a may be 0 or 6.

In the above formula (1), R is a C 1 -C 5 alkoxy group, and X is fluorine or chlorine.

The inert gas may be selected from at least one of helium, neon, and argon.

In an exemplary embodiment, the catalyst may comprise a dialkoxy hydrogenated aluminum substituted with an alkoxy group of 1-5 carbon atoms.

Preferably, the step of collecting the synthesized disilane comprises the steps of: adding liquid nitrogen to the synthesized disilane and the vessel to which the inert gas has been transferred to remove the inert gas; And collecting the diacylene.

In the present invention, a diisocyanate precursor is added to a storage container filled with a carrier gas with an inert gas, and the by-product is purified using liquid nitrogen and dry ice.

As a result, not only the safety of the process can be ensured, but also the reaction stability at the time of synthesizing the di-silane can be ensured and a high yield can be secured. In addition, it has an advantage that a large amount of di-silane can be produced as an insulating film of a semiconductor device on an industrial scale.

BRIEF DESCRIPTION OF THE DRAWINGS Figure 1 schematically depicts an apparatus for producing a di-silane in accordance with an exemplary embodiment of the present invention.
2 is a flow chart schematically illustrating a process for producing a di-silane in accordance with an exemplary embodiment of the present invention.
FIG. 3 is a graph showing FT-IR analysis results for the diacylenes prepared according to the exemplary embodiment of the present invention. It can be seen that the dicylene was synthesized in all three repetitive processes. The bottom part shows the results of FT-IR analysis of the dicylene marketed by Mitsubishi, Japan.
Figure 4 is a graph showing the QMS analysis results for the diacylenes prepared according to the exemplary embodiment of the present invention, indicating that the dicylene was synthesized in all three iterative steps.

Hereinafter, the present invention will be described in more detail with reference to the accompanying drawings when necessary.

Figure 1 schematically depicts an apparatus 100 for making a diacilane in accordance with an exemplary embodiment of the present invention, Figure 2 illustrates a process for manufacturing a diacilane in accordance with an exemplary embodiment of the present invention. As shown in FIG.

As shown in these drawings, the method of synthesizing the diacylene according to the present invention includes a step of preparing a catalyst in the reaction part 110 (step S110), a step of supplying an inert gas to the reaction part 110 in which the catalyst is stored (S130) of adding a diacylene precursor material to the reaction part 110 filled with a catalyst and an inert gas (step S130), and a step of synthesizing diacereine and inert gas (Step S140) of transferring the gas and the inert gas to the first collecting part 120 and the second collecting part 130 using the transferring device (Step S 150). Also, if necessary, the collected di-silane can be stored and stored in a suitable storage unit 140 such as a storage tank.

A process for producing a diacilane capable of ensuring safety, stability, high yield and productivity capable of mass production according to an exemplary embodiment of the present invention will be described in detail.

First, a catalyst capable of converting a diacylene precursor into a diacerein is added and stored in a reaction unit 110 such as a reaction vessel (step S110). In particular, in connection with the present invention, the catalyst that can be used to convert the substituted disilane precursor to the di-silane is an aluminum-based catalyst.

For example, a conventionally used LiAlH 4 catalyst causes a violent reaction when converting from a di-silane precursor to a di-silane, thus requiring a safety facility. Thus, the aluminum-based catalyst that can be used in accordance with the preferred embodiment is dialkoxy hydrogenated aluminum which is substituted with an alkoxy group having 1-5 carbon atoms, such as diisobutoxy aluminum hydride ((i-Bu) 2 AlH).

According to the present invention, before reacting the diisocyanate precursor with the catalyst, a carrier gas is supplied to the reaction part 110 where the catalyst is stored, thereby filling and purifying the inside of the reaction part 110 (Step S120). When diisocyanate is synthesized and prepared from a precursor of a diisocyanate, a large amount of by-products are formed, so that the diisocyanate must be separated and collected. Generally, an electric furnace is used for separating the diacylene. Since the separation process using the electric furnace is very dangerous, the safety of the facility and the stability of the process may become a problem.

Therefore, in the present invention, in order to take advantage of the fact that the synthesized diisocyanate is transported to the collecting units 120 and 130 by using a carrier gas having no reactivity and the carrier gas can be safely separated from the synthesized di- The inside of the reaction part 110 is filled with the carrier gas before the silane precursor reacts with the catalyst. Preferably, an inert gas which is not reactive can be used as the carrier gas. For example, inert gases that can be used as carrier gases are helium (He), neon (Ne), argon (Ar), krypton (Kr), xenon (Xe) and radon (Rn). More preferably, an inert gas selected from at least one of helium, neon, and argon can be used in terms of cost and efficient delivery of the produced diacylene to another container.

A precursor material for synthesizing a diacerein is added to the reaction part 110 and a catalyst such as di-silane (Si 2 H 6 ) are synthesized (step S130). For example, the diacylene precursor material may be substituted with an alkoxy group and / or a halogen and may be represented by the following formula (1).

[Chemical Formula 1]

R a Si 2 X 6-a

(Wherein R is a C 1 -C 10 alkoxy group, X is a halogen, and a is an integer of 0 to 6)

Illustratively, R, which is an alkoxy group substituted in the diacylene precursor in Formula 1, may be a C 1 -C 5 alkoxy group. For example, in the above formula (1), R may include a methoxy group, an ethoxy group, a propoxy group, a butoxy group, and a pentoxy group in a straight chain or branched chain form. For example, when two or more alkoxy groups are substituted for the diacylene in the above formula (1), the respective alkoxy groups may be the same or different.

Meanwhile, the halogen substituted to the diacylene in the above formula (1) may be fluorine (F), chlorine (Cl), bromine (Br) or iodine (I) and combinations thereof. For example, when two or more halogens substituted on the diacylene are represented by the above formula (1), each substituted halogen may be the same atom or different atoms. Particularly halogen which may be substituted on the dicylene is fluorine and / or chlorine.

According to an exemplary embodiment, the diacylene precursor may be substituted only with halogen (in Formula 1, a is 0), or may be substituted with only an alkoxy group (a in Formula 1 is 6). For example, the dicylene precursor used in the exemplary embodiment of the present invention was HexaEthoxyDisilane (HEODS) or hexaChloro Disilane (HCDS).

The diisocyanate substituted with an alkoxy group and / or a halogen can be converted to a diacerein (Si 2 H 6 ) by converting the substituent into a hydrogen atom by a catalyst.

In the following Reaction Scheme 1, hexachlorodisilane or hexaethoxydisilane is used as a diacylene precursor to show the step of synthesizing and preparing dicylene.

[Reaction Scheme 1]

Figure pat00001

When the diacylene is synthesized from the diacylene precursor, synthesis material / by-product and carrier gas are transferred from the reaction part 110 to the first collecting part 120 using the transferring means (step S140).

According to an exemplary embodiment of the present invention, the collecting portion for collecting synthesized disilane and storing the synthesized disilane in the storage portion 140 is composed of two collecting portions. In the collecting units 120 and 130, the synthesized dicylins from the carrier gas and by-products are separated and collected (step S150).

As described above, the diacylene and other by-products synthesized in the reaction part 110 are transferred to the first collecting part 120 by means of transferring means (not designated) by the inert gas filled in the reaction part 110 do.

In the exemplary embodiment, the first collecting part 120 stores liquid nitrogen, and the internal temperature of the first collecting part 120 in which liquid nitrogen is stored is maintained at approximately -5 to -10 ° C. The inert gas, which is the carrier gas carrying the synthesized diacerein and other by-products, is separated and removed from the dicylin and other by-products synthesized by the liquid nitrogen stored in the first collecting part 120.

The synthesized dicylin and other by-products from which the carrier gas has been removed are conveyed to the second collecting part 130 through the conveying means. The second collecting part 130 is maintained at a temperature of -120 to -130 캜, and dry ice is stored. Therefore, among synthesized diacylenes and by-products transferred to the second collecting unit 130, the diacylene can be separated and separated from the by-products due to the dry ice. The synthesized di-silane collected in the second collecting part 130 is transferred to the storage part 140 and stored and stored for later processing.

BEST MODE FOR CARRYING OUT THE INVENTION Hereinafter, the present invention will be described in detail by way of illustrative examples. However, the present invention is not limited to the technical idea described in the following embodiments.

Example  One : From alkoxysilane Diisocyanate  synthesis

325 g (1.6 mol) of diisobutoxy aluminum hydroxide (i-Bu) 2 AlH as a catalyst was stirred in a reaction vessel equipped with three injection pipes and a discharge pipe at a temperature of 15 to 30 DEG C for a period of 0.5 hour . After the reaction vessel was evacuated, the reaction vessel was purged with helium as inert gas for 1.5 hours. 79 g (0.243 mol) of hexaethoxydisilane (HEODS) as a diacylene precursor was added to the reaction vessel and stirred at 50 to 60 캜 for 0.5 hour to synthesize dicylene. The synthesized di-silane and helium were transferred to a container containing liquid nitrogen, and helium was removed using liquid nitrogen. Subsequently, the synthesized dicylene was transferred to a container containing dry ice, and the synthesized dicylene was collected and stored using dry ice. The same procedure was repeated three times to synthesize the diacylene.

Example  2: Halogen substituted In diacylene Diisocyanate  synthesis

The procedure of Example 1 was repeated except that hexachlorodisilane (HCDS) was used as the diacylene precursor material in the same molar ratio (0.243 mol) to synthesize the diacylene.

Example  3: FT - IR  Analysis and QMS  analysis

FT-IR (Fourier transform infrared spectrometer) analysis and QMS (Quadruple mass spectrometer) analysis were performed on the diisocyanate synthesized three times repeatedly in Example 1.

FT-IR analysis results are as shown in the bar, these figures shown in Figure 3, the die silane all the compounds prepared in triplicate in accordance with the present invention is from less than 1000 ㎝ -1 inherent peak (paek) And is in agreement with the peak of the commercially available diisocyanate of Mitsubishi.

The results of the QMS analysis are shown in FIG. 4, respectively. The QMS analysis shows that the peaks of Si-H, SiH 2 and SiH 3 are shown at 27 to 32 and the peak of Si 2 H 6 is at 55 and 60.

Therefore, it is confirmed through FT-IR and QMS analysis that the safety of the reaction process is secured and the synthesis of the diacylene is performed at a high yield as compared with the conventional method of synthesizing the diacerein.

Although the present invention has been described based on the exemplary embodiments and examples of the present invention, the present invention is not limited to the technical ideas described in the above embodiments. On the contrary, those skilled in the art will appreciate that various modifications and changes may be made without departing from the scope of the present invention. It will be apparent, however, that the appended claims are intended to cover all such modifications and changes as fall within the true scope of the invention.


100: reaction system 110: reaction part (reaction vessel)
120: first collecting part 130: second collecting part
140: Storage section (storage tank)

Claims (6)

Filling the container with the inert gas;
Adding a dicylene precursor represented by the following formula (1) to a container filled with the catalyst and the inert gas to synthesize dicylene;
And collecting the synthesized disilane. ≪ RTI ID = 0.0 > 11. < / RTI >

[Chemical Formula 1]
R a Si 2 X 6 -a
(Wherein R is a C 1 -C 10 alkoxy group, X is a halogen, and a is an integer of 0 to 6)
The method according to claim 1,
Wherein a is 0 or 6 in the formula (1).
3. The method according to claim 1 or 2,
Wherein R is a C 1 -C 5 alkoxy group and X is fluorine or chlorine.
3. The method according to claim 1 or 2,
Wherein the inert gas is at least one selected from helium neon and argon.
3. The method according to claim 1 or 2,
Wherein the catalyst comprises a dialkoxy hydrogenated aluminum substituted with an alkoxy group having 1-5 carbon atoms.
3. The method according to claim 1 or 2,
Wherein the step of collecting the synthesized diisocyanate comprises the steps of adding liquid nitrogen to the synthesized diisocyanate and the vessel to which the inert gas has been transferred to remove the inert gas, ≪ / RTI > further comprising the step of collecting the diacerein.

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