JP7100511B2 - Method for Producing Dialkenyl Magnesium, Solid Catalyst Component for Olefin Polymerization, Solid Catalyst for Olefin Polymerization and Method for Producing Olefin Polymer - Google Patents

Description

INDUSTRIAL APPLICABILITY The present invention relates to a method for producing a dialkenyl magnesium, particularly a method for producing a dialkenyl magnesium suitable as a carrier raw material for a catalyst component for olefin polymerization, and a solid catalyst component for olefin polymerization using the dialkenyl magnesium obtained by the method. The present invention relates to a solid catalyst for olefin polymerization and a method for producing an olefin polymer.

Conventionally, as a method for polymerizing olefins, there is an olefin polymerization catalyst composed of a solid catalyst component obtained by contacting a dialkenyl magnesium, a titanium halongen compound and an internal electron donating compound with each other, and an organic aluminum compound. Below, many methods for polymerizing olefins by polymerizing or copolymerizing olefins have been proposed.

In such a method for polymerizing olefins, the shape of the obtained polyolefin depends on the shape of the solid catalyst component used for the polymerization. Therefore, it is important to control the morphology (particle structure) of the solid catalyst component, and many studies have been conducted. Has been made.

Under such circumstances, in the polymerization of olefins, one requirement for controlling the shape of the polyolefin is that the particle size distribution index (SPAN = (D ₅₀ / (D ₉₀ − D ₁₀ )) is small.

Here, the particle structure of the solid catalyst component depends on the particle structure of dialkoxymagnesium, which is a carrier of the solid catalyst component. That is, in order to obtain a polyolefin having a small particle size distribution index (SPAN), dialkoxymagnesium having a small particle size distribution index (SPAN) is required.

As a method for producing dialkoxymagnesium having a small particle size distribution index (SPAN), for example, Patent Document 1 describes a reaction accelerator in a method in which metallic magnesium and alcohol are reacted in the presence of iodine as a reaction accelerator. It is disclosed that dialkoxymagnesium having an average particle size (D50) of 55 μm and a particle size distribution index (SPAN) of 0.78 can be obtained by adding iodine to the reaction system in a plurality of times.

International Publication No. 2013/0588193

However, in the production method of Patent Document 1, when dialkoxymagnesium having a large particle size having an average particle size of more than 50 μm is produced, dialkoxymagnesium having a small particle size distribution index (SPAN) can be obtained, but the average. In the case of producing dialkoxymagnesium having a small particle size, there is a problem that dialkoxymagnesium having a small particle size distribution index (SPAN) cannot be obtained.

Therefore, an object of the present invention is to provide a method for producing dialkoxymagnesium, which can obtain dialkoxymagnesium having a small particle size distribution index (SPAN).

In such a situation, as a result of repeated diligent studies, the present inventor has made the presence of cyclic dimethylpolysiloxane in the reaction system when reacting metallic magnesium with alcohol, so that the particle size distribution tends to be relatively wide. We have found that dialkoxymagnesium having a small particle size distribution index (SPAN) can be obtained in dialkoxymagnesium having a small diameter, and have completed the present invention.

That is, the present invention (1) is a method for producing dialkoxymagnesium, which is obtained by reacting metallic magnesium with an alcohol in the presence of a reaction accelerator to obtain dialkoxymagnesium.
Adding a surfactant before or during the reaction of the metallic magnesium with the alcohol,
The present invention provides a method for producing dialkoxymagnesium, which is characterized by the above.

The present invention (2) also provides the method for producing dialkoxymagnesium (1), wherein the surfactant is dimethylpolysiloxane having 1 to 30 Si—O units. Is.

Further, the present invention (3) provides the method for producing dialkoxymagnesium according to (1), wherein the surfactant is a fatty acid salt of a Group 1 element of the periodic table or an element of Group 2 of the periodic table. It is something to do.

Further, in the present invention (4), the dimethylpolysiloxane is used in the following general formula (1a):

(In the formula, n is an integer of 3 to 30.)
The present invention provides the method for producing dialkoxymagnesium (2), which is characterized by being a cyclic dimethylpolysiloxane represented by.

Further, in the present invention (5), the dimethylpolysiloxane is used in the following general formula (1b):

(In the formula, m is an integer from 1 to 30.)
The present invention provides the method for producing dialkoxymagnesium (2), which is characterized by being a chain dimethylpolysiloxane represented by.

Further, the present invention (6) is characterized in that the dimethylpolysiloxane represented by the general formula (1b) is a chain dimethylpolysiloxane in which m in the general formula (1b) is 1 to 10. (5) The method for producing dialkoxymagnesium is provided.

Further, the present invention (7) provides the method for producing dialkoxymagnesium (3), wherein the fatty acid salt of the Group 2 element of the periodic table is a fatty acid salt of magnesium or calcium. ..

Further, the present invention (8) provides a method for producing dialkoxymagnesium according to any one of (1) to (7), wherein the average particle size (D ₅₀ ) of the dialkoxymagnesium is 5 to 100 μm. It is something to do.

Further, the present invention (9) provides a method for producing dialkoxymagnesium according to any one of (1) to (8), wherein the average particle size (D ₅₀ ) of the metallic magnesium is 5 to 500 μm. It is a thing.

Further, in the present invention (10), the bulk density of the dialkoxymagnesium is 0.15 to 0.70 g / ml, and the particle size distribution index ((D ₅₀ / (D ₉₀ − D ₁₀ )) is 0. It is intended to provide the method for producing the dialkoxymagnesium according to any one of (1) to (9), which is 3 to 2.0.

Further, the present invention (11) provides a method for producing the dialkoxymagnesium according to any one of (1) to (9), wherein the Si content of the dialkoxymagnesium is 0.01 to 10% by mass. It is something to do.

Further, in the present invention (12), the dialkenylmagnesium (a) obtained by the method for producing the dialkenylmagnesium according to any one of (1) to (11), the titanium halogen compound (b), and the electron donating compound are provided. It provides a solid catalyst component for olefin polymerization, which is obtained by contacting with (c).

Further, in the present invention (13), the solid catalyst component for olefin polymerization of (A) and (12) and (B) the following general formula (2):
R ² _p AlQ _3-p (2)
(In the formula, R ² indicates an alkyl group having 1 to 4 carbon atoms, Q indicates a hydrogen atom or a halogen atom, and p is a real number of 0 <p ≦ 3. When a plurality of R ² are present, each R ² may be the same or different from each other, and when there are a plurality of Qs, each Q may be the same or different.)
The present invention provides a catalyst for polymerizing olefins, which comprises an organoaluminum compound represented by.

Further, the present invention (14) further provides (13) a catalyst for olefin polymerization, which comprises (C) an external electron donating compound.

Further, the present invention (15) provides a method for producing an olefin polymer, which comprises polymerizing olefins in the presence of any of the catalysts for polymerizing olefins (13) or (14). Is.

According to the present invention, it is possible to provide a method for producing dialkoxymagnesium, which can obtain dialkoxymagnesium having a small particle size distribution index (SPAN).

The method for producing dialkoxymagnesium of the present invention is a method for producing dialkoxymagnesium, which is obtained by reacting metallic magnesium with an alcohol in the presence of a reaction accelerator to obtain dialkoxymagnesium.
Adding a surfactant before or during the reaction of the metallic magnesium with the alcohol,
It is a method for producing dialkoxymagnesium, which is characterized by the above.

The shape of the metallic magnesium according to the method for producing dialkoxymagnesium of the present invention is not particularly limited, and examples thereof include granules, ribbons, and powders. Of these, as the metallic magnesium, powdery magnesium is preferable. The average particle size (D ₅₀ ) of the powdered metallic magnesium is 5 to 500 μm, preferably 10 to 500 μm, more preferably 10 to 400 μm, and particularly preferably 30 to 300 μm. The surface state of the metallic magnesium is not particularly limited, but it is preferable that a film such as magnesium oxide is not formed on the surface. The content of the fine powder component having an average particle size of less than 5 μm in the metallic magnesium is preferably 20% by mass or less, more preferably 10% by mass or less, particularly preferably 5% by mass or less, and the average particle size is 500 μm or more. The content of the crude powder component is preferably 10% by mass or less, more preferably 5% by mass or less.

The alcohol according to the method for producing dialkoxymagnesium of the present invention is not particularly limited, and for example, lower alcohols having 1 to 6 carbon atoms such as methanol, ethanol, propanol, butanol, and hexanol are preferable, and ethanol is particularly preferable. The water content of the alcohol is not particularly limited, but the smaller the water content is, the more preferable it is, and anhydrous alcohol or dehydrated alcohol having a water content of 200 ppm or less is particularly preferable.

In the method for producing dialkoxymagnesium of the present invention, metallic magnesium and alcohol are reacted in the presence of a reaction accelerator.

Examples of the reaction accelerator include halogens, alkyl halides, metal halides, acid halides, and the following general formula (6):
SiR ¹ _n X _(4-n) (6)
Examples thereof include silicon halide compounds represented by.

In the general formula (6), R ¹ is an alkyl group or an alkoxy group, preferably an alkyl group or an alkoxy group having 1 to 3 carbon atoms, and particularly preferably an alkyl group or an alkoxy group having 1 to 2 carbon atoms. It is the basis. X is a chlorine atom or a bromine atom, and X is preferably a chlorine atom. n is an integer of 0 to 3, preferably an integer of 0 to 2, and particularly preferably 0. When n is 2 or more, the plurality of R ^1s may be the same or different from each other. Further, when there are a plurality of X's, the plurality of X's may be the same or different from each other.

The silicon halide compound represented by the general formula (6) is preferably tetrafluorosilane, tetrachlorosilane, tetrabromosilane, or tetraiodosilane.

In the method for producing dialkoxymagnesium of the present invention, the molar ratio of the total amount of alcohol to the total amount of metallic magnesium (total amount of alcohol / total amount of metallic magnesium) is preferably 3 to 30, particularly preferably 5 to 20. .. When the molar ratio of the total amount of alcohol to the total amount of metallic magnesium is within the above range, the dialkoxy magnesium has a small amount of fine coarse powder, a good particle size distribution, and a high bulk density. When the metallic magnesium is added to the reaction system at one time, the total amount of the metallic magnesium means the addition amount at the time of adding the metallic magnesium at one time, and the metallic magnesium is divided into a plurality of reactions. When added to the system, the total amount of metallic magnesium refers to the total amount of multiple additions. When alcohol is added to the reaction system at one time, the total amount of alcohol refers to the amount of alcohol added at one time, and the alcohol is added to the reaction system in a plurality of times. If so, the total amount of alcohol refers to the total amount of multiple additions.

In the method for producing dialkoxymagnesium of the present invention, the molar ratio of the total amount of the reaction accelerator to the total amount of metallic magnesium (total amount of reaction accelerator / total amount of metallic magnesium) is preferably 0.001 to 0.1. Particularly preferably, it is 0.003 to 0.03. When the molar ratio of the total amount of the reaction accelerator to the total amount of metallic magnesium is in the above range, high-purity dialkoxymagnesium having a good particle size distribution and bulk density and a good shape can be obtained. When the metallic magnesium is added to the reaction system at one time, the total amount of the metallic magnesium means the addition amount at the time of adding the metallic magnesium at one time, and the metallic magnesium is divided into a plurality of reactions. When added to the system, the total amount of metallic magnesium refers to the total amount of multiple additions. When the reaction accelerator is added to the reaction system at one time, the total amount of the reaction accelerator means the amount of the reaction accelerator added at one time, and the reaction accelerator is added at a plurality of times. When added separately to the reaction system, the total amount of the reaction accelerator refers to the total amount of the multiple additions.

In the method for producing dialkoxymagnesium of the present invention, these reactions are carried out in a suspended state in which metallic magnesium is dispersed in alcohol while stirring metallic magnesium and alcohol. In the method for producing dialkoxymagnesium of the present invention, a reaction accelerator is mixed with alcohol in advance, and the alcohol containing the reaction accelerator is mixed with metallic magnesium, or metallic magnesium and alcohol are mixed. The reaction accelerator is introduced into the reaction system by adding the reaction accelerator to the suspension obtained by mixing, or by adding the reaction accelerator as it is without mixing with alcohol when the reaction accelerator is a liquid. Then, the metallic magnesium and the alcohol are reacted in the presence of a reaction accelerator.

In the method for producing dialkoxymagnesium of the present invention, the metallic magnesium and the alcohol may be introduced into the reaction system at one time, or may be introduced in a plurality of times. Hereinafter, the addition of metallic magnesium and alcohol to the reaction system in a plurality of times is also referred to as partial addition. That is, in the method for producing dialkoxymagnesium of the present invention, the reaction may be started using the total amount of metallic magnesium and alcohol from the beginning, or after the reaction is started using a part of metallic magnesium and alcohol. , The remaining metallic magnesium and alcohol may be added to the reaction system at one time or in multiple batches while the reaction is ongoing.

In the method for producing dialkoxymagnesium of the present invention, the reaction accelerator may be introduced into the reaction system at one time, or may be divided into a plurality of times. That is, in the method for producing dialkoxymagnesium of the present invention, the entire amount of the reaction accelerator may be mixed with the metallic magnesium and the alcohol, or after the metallic magnesium and the alcohol are mixed and before the reaction is started. , The entire amount of the reaction accelerator may be added, or after starting the reaction in the presence of a part of the reaction accelerator together with metallic magnesium and alcohol, the remaining reaction accelerator may be added while the reaction is being continued. , May be added to the reaction system at once or in multiple batches.

The reaction temperature in the method for producing dialkoxymagnesium of the present invention is not particularly limited as long as it is equal to or lower than the boiling point of the raw material mixture, and is preferably 30 to 100 ° C., particularly preferably 50 to 90 ° C., and the reaction time is set to. The reaction atmosphere is preferably in the range of 0.5 to 15 hours, particularly preferably 1 to 10 hours, and the reaction atmosphere is an inert gas atmosphere.

Then, in the method for producing dialkoxymagnesium of the present invention, the surfactant is added to the reaction system once or in a plurality of times before or during the reaction between the metallic magnesium and the alcohol. ..

The surfactant according to the method for producing dialkoxymagnesium of the present invention is not particularly limited, and any substance having a property of reducing the free interface energy is preferably used. The surfactant may be one kind or a combination of two or more kinds. The surfactant is preferably dimethylpolysiloxane having 1 to 30 Si—O units, a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table, and the like. The dimethylpolysiloxane having 1 to 30 Si—O units may be one kind or a combination of two or more kinds. Further, the fatty acid salt of the Group 1 element of the periodic table or the element of Group 2 of the periodic table may be one kind or a combination of two or more kinds.

As a dimethylpolysiloxane having 1 to 30 Si—O units, the general formula (1a):

(In the formula, n is an integer of 3 to 30.)
Examples thereof include cyclic dimethylpolysiloxane represented by.

Further, as the dimethylpolysiloxane having the number of Si—O units of 1 to 30, the following general formula (1b):

(In the formula, m is an integer from 1 to 30.)
Examples thereof include chain dimethylpolysiloxane represented by.

In the present invention, the fatty acid salt of the Group 1 element of the Periodic Table or the Element of Group 2 of the Periodic Table is a long-chain hydrocarbon group among the elements of Group 1 of the Periodic Table or the Elements of Group 2 of the Periodic Table and 5 or more carbon atoms. It is a compound composed of a monovalent carboxylic acid having. The elements of Group 1 of the periodic table are Li, Na, K, Rb, Cs, and Fr, except for H, and lithium, sodium, and potassium are preferable, and sodium or potassium is particularly preferable. The Group 2 element of the periodic table is Be, Mg, Ca, Sr, Ba or Ra, preferably beryllium, magnesium, calcium and strontium, and magnesium or calcium is particularly preferable. In particular, as the fatty acid salt of the Group 2 element of the periodic table, the fatty acid salt of magnesium changes to magnesium chloride at the time of preparation of the solid catalyst component like dialkoxymagnesium, so that it is not necessary to remove it from the antisystem. Preferred in terms of points.

That is, in the method for producing dialkoxymagnesium of the present invention, (i) before reacting metallic magnesium with alcohol, a surfactant is added to the reaction system, and then the reaction between metallic magnesium and alcohol is started. , The reaction between the metallic magnesium and the alcohol is carried out, or (ii) a surfactant is added during the reaction between the metallic magnesium and the alcohol, and the reaction between the metallic magnesium and the alcohol is continued.

In the cyclic dimethylpolysiloxane represented by the general formula (1a), in the general formula (1a), n is an integer of 3 to 30, preferably an integer of 3 to 20, and more preferably an integer of 3 to 10. Examples of the cyclic dimethylpolysiloxane represented by the general formula (1a) include decamethylcyclopentasiloxane, hexamethylcyclotrisiloxane, octamethylcyclotetrasiloxane, and dodecamethylcyclopentasiloxane. The cyclic dimethylpolysiloxane represented by the general formula (1a) may be one kind or a combination of two or more kinds within the range represented by the general formula (1a).

The amount of the cyclic dimethylpolysiloxane represented by the general formula (1a) added is 0.1% by mass or more, preferably 0.1 to 30% by mass, particularly preferably 0.1% by mass, based on the total amount of metallic magnesium used in the reaction. It is 0.5 to 20% by mass. When the cyclic dimethylpolysiloxane represented by the general formula (1a) is added to the reaction system at one time, the addition amount of the cyclic dimethylpolysiloxane represented by the general formula (1a) is once. Refers to the amount of addition when the cyclic dimethylpolysiloxane is added in the general formula (1a), and when the cyclic dimethylpolysiloxane represented by the general formula (1a) is added to the reaction system in a plurality of times, the cyclic dimethylpolysiloxane represented by the general formula (1a) is added. The amount of dimethylpolysiloxane added refers to the total amount of multiple additions. When the metallic magnesium is added to the reaction system at one time, the total amount of the metallic magnesium means the addition amount at the time of adding the metallic magnesium at one time, and the metallic magnesium is divided into a plurality of reactions. When added to the system, the total amount of metallic magnesium refers to the total amount of multiple additions.

Further, in the chain dimethylpolysiloxane represented by the general formula (1b), in the general formula (1b), m is an integer of 1 to 30, preferably an integer of 1 to 20, and more preferably an integer of 1 to 12. , Particularly preferably an integer of 1-10. Examples of the chain dimethylpolysiloxane represented by the general formula (1b) include hexamethyldisiloxane, octamethyltrisiloxane, decamethyltetrasiloxane, and dodecamethylpentasiloxane. In particular, when the solvent is distilled off after producing dialkoxymagnesium, it easily evaporates together with the solvent, so that the residual amount in dialkoxymagnesium is reduced and the purity of dialkoxymagnesium is increased. A chain dimethylpolysiloxane in which m is 1 to 6 is preferable. The chain dimethylpolysiloxane represented by the general formula (1b) may be one kind or a combination of two or more kinds within the range represented by the general formula (1b).

The boiling point of the chain dimethylpolysiloxane represented by the general formula (1b) is not particularly limited, but is preferably higher than the boiling point of the alcohol used for producing dialkoxymagnesium. The boiling point of the chain dimethylpolysiloxane represented by the general formula (1b) is preferably 80 ° C. or higher, more preferably 80 to 500 ° C., still more preferably 80 to 400 ° C., and particularly preferably 90 to 300 ° C. In particular, when dialkoxymagnesium obtained after the reaction is heat-dried, air-dried or vacuum-dried, it is easily removed together with alcohol, the residual amount of chain dimethylpolysiloxane in dialkoxymagnesium is reduced, and the purity of dialkoxymagnesium is reduced. The boiling point of the chain dimethylpolysiloxane represented by the general formula (1b) is preferably in the range of 90 to 250 ° C.

The amount of the chain dimethylpolysiloxane represented by the general formula (1b) added is 0.1% by mass or more, preferably 0.1 to 30% by mass, particularly preferably with respect to the total amount of metallic magnesium used in the reaction. Is 0.5 to 20% by mass. When the chain dimethylpolysiloxane represented by the general formula (1b) is added to the reaction system at one time, the addition amount of the chain dimethylpolysiloxane represented by the general formula (1b) is the same. It refers to the amount of addition when it is added once, and when the chain dimethylpolysiloxane represented by the general formula (1b) is added to the reaction system in a plurality of times, it is represented by the general formula (1b). The added amount of the chain dimethylpolysiloxane to be added refers to the total of the added amounts of a plurality of times. When the metallic magnesium is added to the reaction system at one time, the total amount of the metallic magnesium means the addition amount at the time of adding the metallic magnesium at one time, and the metallic magnesium is divided into a plurality of reactions. When added to the system, the total amount of metallic magnesium refers to the total amount of multiple additions.

In the method for producing dialkoxymagnesium of the present invention, (i) the cyclic dimethylpolysiloxane represented by the general formula (1a), general, is the surfactant according to the present invention before reacting the metallic magnesium with the alcohol. After adding the chain dimethylpolysiloxane represented by the formula (1b) or the fatty acid salt of the Group 1 element of the Periodic Table or the element of Group 2 of the Periodic Table to the reaction system, the reaction between the metallic magnesium and the alcohol is started. As a method for carrying out the reaction between the metallic magnesium and the alcohol, for example, a reaction accelerator and a surfactant according to the present invention (for example, a cyclic dimethylpolysiloxane represented by the general formula (1a), a general formula (1b). ) Is mixed with an alcohol containing a chain dimethylpolysiloxane or a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table) to start the reaction, and the metal magnesium and the alcohol are started. Method of reacting with; metallic magnesium, alcohol and a surfactant according to the present invention (for example, cyclic dimethylpolysiloxane represented by the general formula (1a), chain dimethylpolysiloxane represented by the general formula (1b)). Alternatively, a reaction accelerator is added to a suspension obtained by mixing with an element of Group 1 of the Periodic Table or a fatty acid salt of an element of Group 2 of the Periodic Table) to initiate the reaction, and the metal magnesium and alcohol are mixed. Examples thereof include a method for carrying out a reaction.

In the method for producing dialkoxymagnesium of the present invention, (ii) a cyclic dimethylpolysiloxane represented by the general formula (1a) during the reaction between the metallic magnesium and the alcohol, the general formula (1b). ) Is added (such as a chain dimethylpolysiloxane or a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table), and then the reaction between metallic magnesium and alcohol is continued, for example. , When the reaction is initiated with a portion of the total amount of metallic magnesium to be reacted and the remaining metallic magnesium is added to the reaction system in batches or in multiple batches during the reaction, or the rest. Between the divided addition and the divided addition of the metallic magnesium of the above, the surfactant according to the present invention (for example, cyclic dimethylpolysiloxane represented by the general formula (1a), chain dimethylpoly represented by the general formula (1b)). After adding siloxane or a fatty acid salt of Group 1 of the Periodic Table or Group 2 of the Periodic Table), the reaction between metallic magnesium and alcohol is continued; the reaction is started using the total amount of metallic magnesium to be reacted. , That is, during the period from the start of the reaction between the metallic magnesium and the alcohol to the end of the reaction, the surface active agent according to the present invention (for example, the cyclic dimethyl represented by the general formula (1a)). Polysiloxane, chain dimethylpolysiloxane represented by the general formula (1b), or a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table) is added, and then the reaction between metallic magnesium and alcohol is further added. The reaction is started with a part of the total amount of metallic magnesium to be reacted, and during the reaction, the remaining metallic magnesium is added to the reaction system in batches or in multiple batches. From the time when all the metallic magnesium is added to the time when the reaction between the metallic magnesium and the alcohol is completed, the surfactant according to the present invention (for example, the cyclic dimethylpolysiloxane represented by the general formula (1a)) , A chain dimethylpolysiloxane represented by the general formula (1b) or a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table) is added, and after the addition of the dimethylpolysiloxane according to the present invention, a metal is added. Examples thereof include a method of further continuing the reaction between magnesium and alcohol.

Of these methods, in terms of the smaller particle size distribution index (SPAN), the present period is from the time when the total amount of metallic magnesium, alcohol and reaction accelerator is added to the time when the reaction between metallic magnesium and alcohol is completed. The surfactant according to the invention (for example, cyclic dimethylpolysiloxane represented by the general formula (1a), chain dimethylpolysiloxane represented by the general formula (1b), Group 1 element of the Periodic Table, or Group 2 of the Periodic Table. The surface active agent according to the present invention (for example, cyclic dimethylpolysiloxane represented by the general formula (1a), chain dimethylpolysiloxane represented by the general formula (1b), or the periodic table) is added by adding an elemental fatty acid salt or the like. It is preferable to continue the reaction between the metallic magnesium and the alcohol after the addition of the group 1 element in the table or the fatty acid salt of the element in the group 2 in the periodic table, and the total amount of the metallic magnesium, the alcohol and the reaction accelerator has been added. Within 60 minutes from time to time, the surfactant according to the present invention (for example, cyclic dimethylpolysiloxane represented by the general formula (1a), chain dimethylpolysiloxane represented by the general formula (1b), or the first periodic table. A surface active agent according to the present invention (for example, cyclic dimethylpolysiloxane represented by the general formula (1a), represented by the general formula (1b)) is added by adding a group element or a fatty acid salt of a group 2 element of the periodic table. A method of further continuing the reaction between the metallic magnesium and the alcohol after the addition of the chain dimethylpolysiloxane or the fatty acid salt of the Group 1 element of the periodic table or the element of the Group 2 of the periodic table is particularly preferable.

After performing the method for producing the dialkoxymagnesium of the present invention, the obtained dialkoxymagnesium may be dried by a method such as heat drying, air flow drying or vacuum drying, or washed with an inert hydrocarbon compound. Removes alcohol from dialkoxymagnesium.

In the method for producing dialkoxymagnesium of the present invention, the cyclic dimethylpolysiloxane represented by the general formula (1a), for example, the surfactant according to the present invention, before or during the reaction between the metallic magnesium and the alcohol. By adding a chain dimethylpolysiloxane represented by the general formula (1b) or a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table) and reacting metallic magnesium with alcohol. Dialkoxymagnesium having a small particle size distribution index (SPAN) can be obtained. In particular, in the conventional method, in order to obtain dialkoxymagnesium having a small average particle size, the particle size distribution index (SPAN) becomes large when the reaction is carried out under the condition that the average particle size is small. On the other hand, in the method for producing dialkoxymagnesium of the present invention, before or during the reaction of metallic magnesium with alcohol, the surfactant according to the present invention (for example, cyclic dimethyl represented by the general formula (1a)) Polysiloxane, chain dimethylpolysiloxane represented by the general formula (1b), or a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table) is added to react metallic magnesium with alcohol. As a result, it is possible to obtain dialkoxymagnesium having a small particle size distribution index (SPAN) in dialkoxymagnesium having a relatively small particle size, which tends to have a wide particle size distribution. That is, in the method for producing dialkoxymagnesium of the present invention, it is possible to obtain dialkoxymagnesium having a small particle size and a small particle size distribution index (SPAN).

Further, in the method for producing dialkoxymagnesium of the present invention, dialkoxymagnesium having a high bulk density can be obtained.

The particle size distribution index (SPAN) (SPAN = (D ₉₀ -D ₁₀ ) / D ₅₀ ) of the dialkoxymagnesium obtained by the method for producing the dialkoxymagnesium of the present invention is 2.0 or less, preferably 1.5 or less. , Particularly preferably 1.0 or less. The average particle size (D ₅₀ ) of the dialkoxymagnesium obtained by the method for producing the dialkoxymagnesium of the present invention is not particularly limited, and is usually 5 to 100 μm, preferably 7 to 90 μm, more preferably 10 to 80 μm, and further. It is preferably 10 to 60 μm, and particularly preferably 10 to 50 μm.

In particular, the method for producing dialkoxymagnesium of the present invention can be obtained from the viewpoint that dialkoxymagnesium having a small particle size distribution index (SPAN) can be obtained in dialkoxymagnesium having a relatively small particle size, which tends to have a wide particle size distribution. The average particle size (D ₅₀ ) of dialkoxymagnesium is preferably 7 to 90 μm, more preferably 10 to 80 μm, still more preferably 10 to 60 μm, particularly preferably 10 to 50 μm, and the particle size distribution index (SPAN). Is 2.0 or less, preferably 1.5 or less, more preferably 1.0 or less, and particularly preferably 0.8 or less.

In the present invention, D ₁₀ , D ₅₀ , and D ₉₀ have integrated body integration factors in the particle size distribution obtained by measuring with a laser diffraction type particle size distribution measuring device (MICROTRAC HRA 9320-X100 manufactured by Nikkiso Co., Ltd.). Refers to the particle size (μm) corresponding to 10%, 50%, and 90%, respectively.

The purity of dialkoxymagnesium obtained by the method for producing dialkoxymagnesium of the present invention is such that a solid catalyst component for olefin polymerization is produced using dialkoxymagnesium obtained by the method for producing dialkoxymagnesium of the present invention. When polysiloxane is not added to the reaction system, the content is 99% by mass or more, more preferably 99 to 100% by mass, and particularly preferably 99.1 to 99.9% by mass. In the present invention, the purity of the dialkoxymagnesium is the purity of the dialkoxymagnesium after the solvent is removed, and after the solvent is removed, the halogen content in the dialkoxymagnesium indicates the purity of the dialkoxymagnesium. The content of the reaction accelerator is determined, the content of dimethylpolysiloxane in dialkoxymagnesium is determined from the Si content in dialkoxymagnesium, and the value is calculated by the following formula.
Dialkoxymagnesium purity (% by mass) = 100- {(reaction accelerator content (mass%) + (dimethylpolysiloxane content (mass%))}

Another object of the present invention is to enhance the steric regularity of the olefin polymer when producing the solid catalyst component for olefin polymerization by using the dialkoxy magnesium obtained by the method for producing the dialkoxy magnesium of the present invention. , When a surfactant is added to the reaction system for producing a solid catalyst component for olefin polymerization, the surfactant according to the present invention may remain in the dialkamic magnesium, and therefore the dialkoxymagnesium of the present invention may remain. The content of the surfactant according to the present invention in the dialkoxymagnesium obtained by the above-mentioned production method is not particularly limited, but is preferably 30% by mass or less, and particularly preferably 20% by mass or less. The content of the reaction accelerator in the dialkoxymagnesium obtained by the method for producing dialkoxymagnesium of the present invention is not particularly limited, but is preferably 5% by mass or less, and particularly preferably 3% by mass or less. In the present invention, after the solvent is removed, the content of the reaction accelerator in dialkoxymagnesium is determined from the halogen content in dialkoxymagnesium, and the Si content in dialkoxymagnesium is used in dialkoxymagnesium. The content of dimethylpolysiloxane according to the present invention is determined.

The bulk density of dialkoxymagnesium obtained by the method for producing dialkoxymagnesium of the present invention is preferably 0.15 to 0.70 g / ml, more preferably 0.20 to 0.60 g / ml, and particularly preferably 0. .20 to 0.50 g / ml.

The dialkoxymagnesium obtained by the method for producing dialkoxymagnesium of the present invention preferably does not contain alcohol, but has an alcohol content of 5% by mass or less, preferably 2% by mass or less, particularly preferably. Is acceptable as long as it is 1% by mass or less.

Dialkenylmagnesium obtained by carrying out the method for producing dialkenylmagnesium of the present invention is suitably used as dialkenylmagnesium as a raw material for producing a solid catalyst component for olefin polymerization. In particular, the dialkoxymagnesium obtained by the method for producing dialkoxymagnesium of the present invention is a raw material alkoxy for producing a solid catalyst component for producing a polyolefin having a small average particle size and a small particle size distribution index (SPAN). Suitable as magnesium.

The method for producing a solid catalyst component for olefin polymerization using the dialkenylmagnesium obtained by the method for producing dialkenylmagnesium of the present invention as a raw material is not particularly limited and may be appropriately selected.

For example, as a method for producing a solid catalyst component for olefin polymerization, the following production method can be mentioned.

The solid catalyst component for olefin polymerization of the present invention includes dialkenylmagnesium (a) obtained by the method for producing dialkenylmagnesium of the present invention, a titanium halogen compound (b), and an electron donating compound (c). It is a solid catalyst component for olefin polymerization, which is obtained by contacting with.

The details of the method for producing dialkoxymagnesium (a) according to the solid catalyst component for olefin polymerization of the present invention are as described above.

Examples of the titanium halogen compound (b) constituting the solid catalyst component for olefin polymerization of the present invention include one or more selected from known substances, and a tetravalent titanium halogen compound is preferable, and titanium tetrachloride is more preferable.

Examples of the electron donating compound (c) constituting the solid catalyst component for olefin polymerization of the present invention include one or more selected from known substances, and an organic compound having an oxygen atom or a nitrogen atom is preferable.

The electron donating compound (c) is preferably one or more selected from succinic acid ester, maleic acid ester, cyclohexene carboxylic acid ester, ether carboxylic acid ester, dicarbonate, and ether carbonate.

In the solid catalyst component for olefin polymerization of the present invention, the contents of titanium atom, magnesium atom, halogen atom and electron donating compound are not particularly specified.

In the solid catalyst component for olefin polymerization of the present invention, the content ratio of titanium atoms is preferably 0.5 to 8.0% by mass, more preferably 1.0 to 6.0% by mass. It is more preferably 1.0 to 4.0% by mass.

In the solid catalyst component for olefin polymerization of the present invention, the content ratio of magnesium atoms is preferably 10 to 70% by mass, more preferably 10 to 50% by mass, and 15 to 40% by mass. Is more preferable, and 15 to 25% by mass is further preferable.

In the solid catalyst component for olefin polymerization of the present invention, the content ratio of halogen atoms is preferably 20 to 90% by mass, more preferably 30 to 85% by mass, and 40 to 80% by mass. Is more preferable, and 45 to 75% by mass is further preferable.

In the solid catalyst component for olefin polymerization of the present invention, the total content of the electron donating compound (c) is preferably 0.5 to 30% by mass, more preferably 1 to 25% by mass. It is preferably 2 to 20% by mass, and more preferably 2 to 20% by mass.

In the solid catalyst component for olefin polymerization of the present invention, in order to exhibit the overall performance in a well-balanced manner, the titanium content is 1 to 4% by mass, the magnesium content is 15 to 25% by mass, and the halogen atom content is set. It is desirable that the content is 45 to 75% by mass and the content of the electron donating compound (c) is 2 to 20% by mass.

As a method for producing the solid catalyst component for olefin polymerization of the present invention, an alkoxymagnesium (a), a titanium halogen compound (b) and an electron donating compound (c) are used as an inert organic solvent having a boiling point of 50 to 150 ° C. Examples thereof include a method of contacting in the presence of (d).

Examples of the inert organic solvent (d) having a boiling point of 50 to 150 ° C. include one or more selected from toluene, xylene, ethylbenzene, heptane, octane, decane and the like. As the inert organic solvent (d) having a boiling point of 50 to 150 ° C., aromatic hydrocarbon compounds and aliphatic hydrocarbon compounds are generally used, but the solubility of impurities does not decrease during reactivity or washing after the reaction. If there is, an inert organic solvent other than aromatic hydrocarbons and saturated hydrocarbons may be used.

Further, when producing the solid catalyst component for olefin polymerization of the present invention, polysiloxane may be further added to the reaction system. As the polysiloxane, conventionally known ones are appropriately selected, but one or more selected from decamethylcyclopentasiloxane and dimethylpolysiloxane are preferable, and decamethylcyclopentasiloxane is more preferable.

The details of the method for preparing the solid catalyst component for olefin polymerization of the present invention are the same as the conventionally known method for preparing the solid catalyst component for olefin polymerization.

As described above, the solid catalyst component for olefin polymerization of the present invention includes dialkenylmagnesium (a), a titanium halogen compound (b), and electrons obtained by the method for producing dialkenylmagnesium of the present invention. It is obtained by contacting and reacting with the donor compound (c).

According to the present invention, there is provided a solid catalyst component for olefin polymerization capable of forming a polymer having a smooth particle surface, a large average particle size, a low fine powder amount, and a narrow particle size distribution under high polymerization activity. be able to.

The catalyst for olefin polymerization of the present invention comprises (A) the solid catalyst component for olefin polymerization of the present invention, and (B) the following general formula (2):
R ² _p AlQ _3-p (2)
(In the formula, R ² indicates an alkyl group having 1 to 4 carbon atoms, Q indicates a hydrogen atom or a halogen atom, and p is a real number of 0 <p ≦ 3. When a plurality of R ² are present, each R ² may be the same or different from each other, and when a plurality of Q's are present, each Q may be the same or different.) It is characterized by containing an organic aluminum compound represented by. It is a catalyst for olefin polymerization. Further, the catalyst for olefin polymerization of the present invention is, in addition to (A) the solid catalyst component for olefin polymerization of the present invention and (B) the organoaluminum compound represented by the general formula (2), further (C. ) External electron donating compounds can be included.

(A) The solid catalyst component for olefin polymerization of the present invention according to the catalyst for polymerizing olefins of the present invention is as described above.

The catalyst for olefin polymerization of the present invention is (B) the following general formula (2):
R ² _p AlQ _3-p (2)
(In the formula, R ² indicates an alkyl group having 1 to 4 carbon atoms, Q indicates a hydrogen atom or a halogen atom, and p is a real number of 0 <p ≦ 3. When a plurality of R ² are present, each R ² may be the same or different from each other, and when a plurality of Q's are present, each Q may be the same or different.) Contains an organic aluminum compound represented by.

The organic aluminum compound represented by the general formula (2) is not particularly limited, but R ² includes one or more selected from an ethyl group and an isobutyl group, and Q includes a hydrogen atom, a chlorine atom and a chlorine atom. One or more selected from bromine atoms can be mentioned, and p is preferably 2, 2.5 or 3, and particularly preferably 3.

Specific examples of such organic aluminum compounds include trialkylaluminum such as triethylaluminum, triisopropylaluminum, tri-n-butylaluminum, and triisobutylaluminum, alkylaluminum halides such as diethylaluminum chloride and diethylaluminum bromide, and diethyl. One or more selected from aluminum hydride and the like can be mentioned, and among them, one or more selected from halogenated alkylaluminum such as diethylaluminum chloride, or trialkylaluminum such as triethylaluminum, tri-n-butylaluminum and triisobutylaluminum is preferable. , Triethylaluminum and triisobutylaluminum are more preferred.

In the catalyst for olefin polymerization of the present invention, the external electron donating compound (C) is preferably a known external electron donating compound containing an oxygen atom or a nitrogen atom. The external electron donating compound (C) may be used alone or in combination of two or more.

In the catalyst for polymerizing olefins of the present invention, the external electron donating compound (C) is referred to as the following general formula (3):
R ³ _q Si (OR ⁴ ) _4-q (3)
(In the formula, R ³ is an alkyl group having 1 to 12 carbon atoms, a vinyl group, an alkenyl group having 3 to 12 carbon atoms, a cycloalkyl group having 3 to 12 carbon atoms, a cycloalkenyl group having 3 to 12 carbon atoms, and carbon. When an aromatic hydrocarbon group having 6 to 15 carbon atoms or an aromatic hydrocarbon group having 6 to 15 carbon atoms having a substituent is shown and a plurality of R ^3s are present, the plurality of R ^3s may be the same or different from each other. R ⁴ is an alkyl group having 1 to 4 carbon atoms, a vinyl group, an alkenyl group having 3 to 12 carbon atoms, a cycloalkyl group having 3 to 6 carbon atoms, an aromatic hydrocarbon group having 6 to 12 carbon atoms or a substituent. It represents an aromatic hydrocarbon group having 7 to 12 carbon atoms, and when a plurality of R ^4s are present, the plurality of R ^4s may be the same or different from each other. Q is an integer of 0 ≦ q ≦ 3. ) Is one or more selected from the organic silicon compounds represented by.

Further, in the catalyst for polymerizing olefins of the present invention, the external electron donating compound (C) is referred to as the following general formula (4):
(R ⁵ R ⁶ N) _s SiR ⁷ _4-s (4)
(In the formula, R ⁵ and R ⁶ are a hydrogen atom, an alkyl group having 1 to 20 carbon atoms, a vinyl group, an alkenyl group having 3 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, and 3 to 20 carbon atoms. R ⁵ and R ⁶ may be the same or different from each other, or may be bonded to each other to form a ring, and the R ⁵ R ⁶ N group may be represented by a cycloalkenyl group or an aryl group having 6 to 20 carbon atoms. When there are a plurality of R 5 R 6 N groups, the plurality of R ⁵ R ⁶ N groups may be the same or different from each other. R ⁷ has an alkyl group having 1 to 20 carbon atoms, a vinyl group, an alkenyl group having 3 to 12 carbon atoms, and a carbon number of carbon atoms. 1 to 20 alkoxy groups, vinyl oxy groups, alkenyloxy groups having 3 to 20 carbon atoms, cycloalkyl groups having 3 to 20 carbon atoms, cycloalkyloxy groups having 3 to 20 carbon atoms, aryl groups having 6 to 20 carbon atoms, Aminosilane representing an aryloxy group having 6 to 20 carbon atoms and having a plurality of R ^7s , the plurality of R ^7s may be the same or different from each other. S is an integer of 1 to 3). One or more selected from the compounds may be mentioned.

Examples of the organic silicon compound represented by the general formula (3) or the aminosilane compound represented by the general formula (4) include phenylalkoxysilane, alkylalkoxysilane, phenylalkylalkoxysilane, cycloalkylalkoxysilane, and alkyl (cycloalkyl). Alkoxysilane, (alkylamino) alkoxysilane, alkyl (alkylamino) alkoxysilane, cycloalkyl (alkylamino) alkoxysilane, tetraalkoxysilane, tetrakis (alkylamino) silane, alkyltris (alkylamino) silane, dialkylbis (alkyl) Examples thereof include amino) silane and trialkyl (alkylamino) silane.

Specific examples of the organic silicon compound represented by the general formula (3) or the aminosilane compound represented by the general formula (4) include n-propyltriethoxysilane, cyclopentyltriethoxysilane, phenyltrimethoxysilane, and phenyl. Triethoxysilane, t-butyltrimethoxysilane, diisopropyldimethoxysilane, isopropylisobutyldimethoxysilane, diisopentyldimethoxysilane, bis (2-ethylhexyl) dimethoxysilane, t-butylmethyldimethoxysilane, t-butylethyldimethoxysilane, di Cyclopentyldimethoxysilane, dicyclohexyldimethoxysilane, cyclohexylcyclopentyldimethoxysilane, cyclohexylmethyldimethoxysilane, tetraethoxysilane, tetrabutoxysilane, bis (ethylamino) methylethylsilane, bis (ethylamino) t-butylmethylsilane, bis (ethylamino) ) Dicyclohexylsilane, dicyclopentylbis (ethylamino) silane, bis (methylamino) (methylcyclopentylamino) methylsilane, diethylaminotriethoxysilane, bis (cyclohexylamino) dimethoxysilane, bis (perhydroisoquinolino) dimethoxysilane, bis One or more selected from (perhydroquinolino) dimethoxysilane, ethyl (isoquinolino) dimethoxysilane and the like can be mentioned, among which n-propyltriethoxysilane, phenyltrimethoxysilane, t-butylmethyldimethoxysilane and t-butylethyldimethoxy. Silane, diisopropyldimethoxysilane, isopropylisobutyldimethoxysilane, diisopentyldimethoxysilane, diphenyldimethoxysilane, dicyclopentyldimethoxysilane, cyclohexylmethyldimethoxysilane, tetramethoxysilane, tetraethoxysilane, t-butylmethylbis (ethylamino) silane, One or more selected from bis (ethylamino) dicyclohexylsilane, dicyclopentylbis (ethylamino) silane, bis (perhydroisoquinolino) dimethoxysilane, diethylaminotriethoxysilane and the like are preferable.

Further, in the catalyst for polymerizing olefins of the present invention, examples of the external electron donating compound (C) include ether compounds having two or more ether groups. As the ether compound having two or more ether groups, a 1,3-diether compound having a substituent at the 2-position is preferable. Examples of the 1,3-diether compound having a substituent at the 2-position include the following general formula (5);
R ⁶ -O-CH ₂ CR ⁷ R ⁸ CH ₂ -OR ⁹ (5)
(In the formula, R ⁷ and R ⁸ are a hydrogen atom, a halogen atom, an alkyl group having 1 to 12 carbon atoms, a vinyl group, an alkenyl group having 3 to 12 carbon atoms, a cycloalkyl group having 3 to 12 carbon atoms or a cycloalkenyl group. , An aromatic hydrocarbon group having 6 to 12 carbon atoms or a halogen-substituted aromatic hydrocarbon group, an aromatic hydrocarbon group having a substituent and having 7 to 12 carbon atoms, an alkylamino group having 1 to 12 carbon atoms or 2 carbon atoms. It represents a dialkylamino group of ~ 12, and may be the same or different, or may be bonded to each other to form a ring. R ⁶ and R ⁹ are an alkyl group having 1 to 12 carbon atoms, a vinyl group, and 3 carbon atoms. An alkenyl group of ~ 12, a cycloalkyl group having 3 to 6 carbon atoms, an aromatic hydrocarbon group having 6 to 12 carbon atoms or a halogen-substituted aromatic hydrocarbon group or an aromatic hydrocarbon having 7 to 12 carbon atoms having a substituent. It indicates a group and may be the same or different.)
Examples thereof include 1,3-diether compounds represented by.

Specific examples of the 1,3-diether compound represented by the general formula (5) include 2-isopropyl-2-isobutyl-1,3-dimethoxypropane and 2,2-diisobutyl-1,3-dimethoxy. Propane, 2-isopropyl-2-isopentyl-1,3-dimethoxypropane, 2,2-dicyclohexyl-1,3-dimethoxypropane, 2,2-bis (cyclohexylmethyl) 1,3-dimethoxypropane, 9,9- Examples thereof include bis (methoxymethyl) fluorene, among which 2-isopropyl-2-isobutyl-1,3-dimethoxypropane, 2-isopropyl-2-isopentyl-1,3-dimethoxypropane and 9,9-bis (methoxy) are used. Methyl) fluorene and the like can be mentioned. These compounds may be used alone or in combination of two or more.

In the catalyst for olefin polymerization of the present invention, (A) the solid catalyst component for olefin polymerization of the present invention, (B) the organic aluminum compound represented by the general formula (2), and (C) an external substance used as necessary. The content ratio of the electron donating compound is arbitrarily selected within the range in which the effect of the present invention can be obtained, and is not particularly limited, but per mole of the titanium atom in the solid catalyst component (A) for olefin polymerization. (B) The organic aluminum compound represented by the general formula (2) is preferably 1 to 2000 mol, more preferably 50 to 1000 mol. Further, the amount of (C) the external electron donating compound is preferably 0.002 to 10 mol, preferably 0.01 to 2 mol, per 1 mol of the organoaluminum compound represented by the general formula (2). It is more preferably present, and further preferably 0.01 to 0.5 mol.

The method for producing the olefin polymerization catalyst of the present invention is not particularly limited. For example, when (C) an external electron donating compound is used, (A) the solid catalyst component for olefin polymerization of the present invention, (B) general. Examples thereof include a method of producing a catalyst for olefin polymerization by contacting an organoaluminum compound represented by the formula (2) and an external electron donating compound (C) by a known method.
The order in which each of the above components is brought into contact is arbitrary, but for example, the following contact order can be exemplified.
(I) (A) Solid catalyst component for olefin polymerization of the present invention → (C) External electron donating compound → (B) Organoaluminium compound represented by the general formula (2) (ii) (B) General formula ( Organoaluminium compound represented by 2) → (C) External electron donating compound → (A) Solid catalyst component for olefin polymerization of the present invention (iii) (C) External electron donating compound → (A) The present invention Solid catalyst component for olefin polymerization → (B) Organoaluminium compound represented by the general formula (2) (iv) (C) External electron donating compound → (B) Organoaluminium compound represented by the general formula (2) → (A) Solid catalyst component for olefin polymerization of the present invention Of the above contact examples (i) to (iv), the contact example (ii) is preferable.
In the above contact examples (i) to (iv), "→" means the contact order, for example, "(A) solid catalyst component for olefin polymerization of the present invention → (B) general formula (2). The "organic aluminum compound represented → (C) external electron donating compound" is obtained by adding (B) an organic aluminum compound represented by the general formula (2) to (A) the solid catalyst component for olefin polymerization of the present invention. It means that (C) an external electron donating compound is added and brought into contact with each other.

The catalyst for olefin polymerization of the present invention comprises (A) a solid catalyst component for olefin polymerization of the present invention, (B) an organoaluminum compound represented by the general formula (2), and (C) an external electron donating compound. It may be contacted in the absence of olefins, or may be contacted (in the polymerization system) in the presence of olefins.

According to the present invention, it is possible to provide a catalyst for olefin polymerization having a smooth surface, a large average particle size, a low amount of fine powder, and a narrow particle size distribution.

The method for producing an olefin polymer of the present invention is characterized in that the olefins are polymerized in the presence of the catalyst for olefin polymerization of the present invention.

In the method for producing an olefin polymer of the present invention, the polymerization of olefins may be homopolymerization or copolymerization.

In the method for producing an olefin polymer of the present invention, examples of the olefins include one or more selected from ethylene, propylene, 1-butene, 1-pentene, 4-methyl-1-pentene, vinylcyclohexane and the like, and ethylene. , Propylene or 1-butene is preferred, with propylene being more preferred.

When polymerizing propylene, copolymerization with other olefins may be carried out, and block copolymerization of propylene and other α-olefins is preferable. The block copolymer obtained by block copolymerization is a polymer containing segments in which two or more kinds of monomer compositions change continuously, and is a monomer type, a comonomer type, a comonomer composition, a comonomer content, a comonomer arrangement, and a steric rule. It refers to a form in which two or more types of polymer chains (segments) having different primary structures such as sex are connected in one molecular chain. The olefins to be copolymerized are preferably α-olefins having 2 to 20 carbon atoms (excluding propylene having 3 carbon atoms), and specifically, ethylene, 1-butene, 1-pentene, 4-. Examples thereof include methyl-1-pentene and vinylcyclohexane, and one or more of these olefins may be used in combination. In particular, ethylene and 1-butene are preferably used.

In the method for producing an olefin polymer of the present invention, the polymerization of olefins can be carried out in the presence or absence of an organic solvent. Further, in the method for producing an olefin polymer of the present invention, the olefins to be polymerized can be used in either a gas state or a liquid state.

Regarding the polymerization of olefins, for example, in a reaction furnace such as an autoclave, the olefins are introduced in the presence of the catalyst for polymerizing the olefins of the present invention, and the olefins are polymerized under heating and pressure conditions. be able to.

In the method for producing an olefin polymer of the present invention, the polymerization temperature is usually 200 ° C. or lower, preferably 100 ° C. or lower, and more preferably 60 to 100 ° C. from the viewpoint of improving activity and stereoregularity. 70 to 90 ° C. is more preferable. In the method for producing an olefin polymer of the present invention, the polymerization pressure is preferably 10 MPa or less, more preferably 5 MPa or less. Further, either a continuous polymerization method or a batch type polymerization method can be used. Further, the polymerization reaction may be carried out in one stage or in two or more stages.

In the method for producing an olefin polymer of the present invention, when polymerizing olefins (hereinafter, appropriately referred to as the present polymerization), the constituent components of the catalyst for polymerizing the olefins of the present invention with respect to the olefins to be polymerized. Preliminary polymerization (hereinafter, appropriately referred to as prepolymerization) may be carried out by contacting a part or all of the above.

When performing the prepolymerization, the constituent components of the catalyst for olefin polymerization of the present invention and the contact order of the olefins are arbitrary, but the organic aluminum compound is first placed in the prepolymerization system set to an inert gas atmosphere or an olefin gas atmosphere. It is preferable to charge and then contact the solid catalyst component for olefin polymerization of the present invention, and then contact one or more olefins such as propylene. Alternatively, the organoaluminum compound is first charged into the prepolymerization system set to the inert gas atmosphere or the olefin gas atmosphere, then the external electron donating compound is contacted, and then the solid catalyst component for olefin polymerization of the present invention is contacted. After that, it is preferable to contact one or more olefins such as propylene. In the prepolymerization, the same olefins or monomers such as styrene can be used as in the main polymerization, and the prepolymerization conditions are the same as the above polymerization conditions.

By performing the above prepolymerization, the catalytic activity is improved, and it becomes easier to further improve the stereoregularity and particle properties of the obtained polymer.

According to the present invention, there is provided a method for producing an olefin polymer capable of producing a polymer having a smooth surface, a large average particle size, a low fine powder amount, and a narrow particle size distribution under high polymerization activity. can do.
The method for producing an olefin polymer according to the present invention is particularly applied to a process for producing a polyolefin by a vapor phase method.

Hereinafter, the present invention will be described in more detail with reference to examples, but this is merely an example and does not limit the present invention.

(Example 1)
<Manufacturing of diethoxymagnesium>
2.0 g of metal magnesium powder (average particle size 97 μm), absolute ethanol in a 1 L capacity four-necked flask equipped with an integrated gas meter, a dropping funnel, a stirrer and a reflux condenser, and the inside is filled with nitrogen gas. 76 g and 1.29 g (5.07 mmol) of iodine were charged and heated to the reflux temperature of ethanol in an oil bath to maintain the reflux state.
Then, a mixture of 5.8 g of metallic magnesium powder and 33 g of ethanol was added thereto in 4 portions every 6.5 minutes. After the total amount was added, 0.37 g (1.00 mmol) of decamethylcyclopentasiloxane was added, and the mixture was further heated under reflux for 1 hour to complete the reaction.
Then, the reaction solution was dried by a rotary evaporator to obtain 29.9 g of powdered diethoxymagnesium.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.84% by mass and the Si atom content was 0.70% by mass (8.53% by mass when converted to the decamethylcyclopentasiloxane content). Met. The results of the analysis and evaluation are shown in Table 1.

<Analysis of average particle size (D ₅₀ ) and SPAN>
Using a laser diffraction type particle size distribution measuring device (MICROTRAC HRA 9320-X100 manufactured by Nikkiso Co., Ltd.), dialkoxymagnesium is dispersed in anhydrous ethanol, automatic measurement is performed twice, the particle size distribution is measured, and the integrated volume fraction is integrated. The particle diameter (D ₁₀ ) with a rate of 10%, the particle diameter with an integrated volume fraction of 50% (D ₅₀ ), and the particle diameter with an integrated volume fraction of 90% (D ₉₀ ) were obtained, and the average values were calculated as D ₁₀ and D. It was set to ₅₀ and D ₉₀ . Then, the value of D ₅₀ obtained was used as the average particle size, and the SPAN was calculated from the obtained values of D ₁₀ , D ₅₀ and D ₉₀ by the following formula.
SPAN = (D ₉₀ -D ₁₀ ) / D ₅₀

<Purity of Dialkoxy Magnesium>
The purity (mass%) of the obtained dialkoxymagnesium was measured by an automatic drip device, an automatic drip device (manufactured by Mitsubishi Chemical Analytech Co., Ltd., model GT-200), and the halogen in the dialkoxy magnesium after removing the solvent. From the content (% by mass), the content (% by mass) of iodine used as a reaction accelerator in dialkoxymagnesium and the induction coupling plasma (ICP) emission spectroscopic analyzer, manufactured by Hitachi High-Tech Science Co., Ltd., model SPS- From the Si content (mass%) in dialkoxymagnesium after removing the solvent as measured by 3100, the content (mass%) of decamethylcyclopentasiloxane in dialkoxymagnesium was determined, and the following formula was used. Calculated.
Dialkoxymagnesium purity (% by mass) = 100-{(iodine content (% by mass)) + (decamethylcyclopentasiloxane content (% by mass))}

(Example 2)
Powdered diethoxymagnesium was prepared in the same manner as in Example 1 except that the amount of decamethylcyclopentasiloxane added was changed from 0.37 g (1.0 mmol) to 1.11 g (3.0 mmol). ..
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.73% by mass and the Si content was 1.84% by mass (4.85% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 3)
Powdered diethoxymagnesium was prepared in the same manner as in Example 1 except that the amount of decamethylcyclopentasiloxane added was changed from 0.37 g (1.0 mmol) to 3.33 g (9.0 mmol). ..
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.32% by mass and the Si content was 4.22% by mass (11.14% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 4)
After adding the entire amount of metallic magnesium powder, instead of adding 0.37 g (1.0 mmol) of decamethylcyclopentasiloxane, 2.0 g of metallic magnesium powder, 76 g of anhydrous ethanol and 1.3 g of iodine (5.08 mmol) were added. Powdered diethoxymagnesium was prepared in the same manner as in Example 1 except that 1.11 g (3.0 mmol) of decamethylcyclopentasiloxane was added at the time of charging.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.88% by mass and the Si content was 3.23% by mass (8.51% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 5)
After adding the entire amount of the metallic magnesium powder, instead of adding 0.37 g (1.0 mmol) of decamethylcyclopentasiloxane, decamethyl is added when the mixture of 5.8 g of the metallic magnesium powder and 33 g of ethanol is added in the fourth division. Powdered diethoxymagnesium was prepared in the same manner as in Example 1 except that 1.11 g (3.0 mmol) of cyclopentasiloxane was added.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.62% by mass and the Si content was 2.66% by mass (7.02% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 6)
Powdered diethoxymagnesium was prepared in the same manner as in Example 1 except that the same molar amount of hexamethylcyclotrisiloxane was added instead of adding 0.37 g (1.0 mmol) of decamethylcyclopentasiloxane. ..
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.54% by mass and the Si content was 2.43% by mass (6.41% by mass when converted to the hexamethylcyclotrisiloxane content). there were. The results are shown in Table 1.

(Example 7)
Powdered diethoxymagnesium was prepared in the same manner as in Example 1 except that the same molar amount of octamethylcyclotetrasiloxane was added instead of 0.37 g (1.0 mmol) of decamethylcyclopentasiloxane. ..
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.49% by mass and the Si content was 2.56% by mass (6.76% by mass when converted to the octamethylcyclotetrasiloxane content). there were. The results are shown in Table 1.

(Comparative Example 1)
A powdery diethoxymagnesium was prepared in the same manner as in Example 1 except that the decamethylcyclopentasiloxane was not added after the addition of the metallic magnesium powder.
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.61% by mass and the Si content was 0% by mass (0% by mass when converted to the decamethylcyclopentasiloxane content). The results are shown in Table 1.

(Example 8)
Example 1 except that the amount of decamethylcyclopentasiloxane added is 0.074 g (0.2 mmol) instead of 0.37 g (1.0 mmol). Similarly, powdered diethoxymagnesium was prepared.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 3.16% by mass and the Si content was 0.01% by mass (0.03% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 9)
Example 1 except that the amount of decamethylcyclopentasiloxane added is 0.185 g (0.5 mmol) instead of 0.37 g (1.0 mmol). Similarly, powdered diethoxymagnesium was prepared.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.94% by mass and the Si content was 0.18% by mass (0.48% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 10)
Example 1 except that the amount of decamethylcyclopentasiloxane added is 5.55 g (15.0 mmol) instead of 0.37 g (1.0 mmol). Similarly, powdered diethoxymagnesium was prepared.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 3.08% by mass and the Si content was 5.10% by mass (13.46% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 11)
Example 1 except that the amount of decamethylcyclopentasiloxane added is 7.40 g (20.0 mmol) instead of 0.37 g (1.0 mmol). Similarly, powdered diethoxymagnesium was prepared.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.88% by mass and the Si content was 5.60% by mass (14.78% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

(Example 12)
Example 1 except that the amount of decamethylcyclopentasiloxane added is 11.10 g (30.0 mmol) instead of 0.37 g (1.0 mmol). Similarly, powdered diethoxymagnesium was prepared.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.70% by mass and the Si content was 6.20% by mass (16.36% by mass when converted to the decamethylcyclopentasiloxane content). there were. The results are shown in Table 1.

１）金属マグネシウム合計量に対する環状ジメチルポリシロキサンの添加量
２）得られたジアルコキシマグネシウム中のＳｉ含有量

1) Addition of cyclic dimethylpolysiloxane to the total amount of metallic magnesium 2) Si content in the obtained dialkoxymagnesium

(Example 13)
2.0 g of metal magnesium powder (average particle size 97 μm), absolute ethanol in a 1 L capacity four-necked flask equipped with an integrated gas meter, a dropping funnel, a stirrer and a reflux condenser, and the inside is filled with nitrogen gas. 76 g and 1.29 g (5.07 mmol) of iodine were charged and heated to the reflux temperature of ethanol in an oil bath to maintain the reflux state.
Then, a mixture of 5.8 g of metallic magnesium powder and 33 g of ethanol was added thereto in 4 portions every 6.5 minutes. After the total amount was added, 0.37 g (0.63 mmol) of magnesium stearate was added, and the mixture was further heated under reflux for 1 hour to complete the reaction.
Then, the reaction solution was dried by a rotary evaporator to obtain powdered diethoxymagnesium. The results of the analysis and evaluation are shown in Table 2.

１）ジアルコキシマグネシウム調製時に添加したアルカリ土類金属脂肪酸塩の金属マグネシウム合計量に対する質量比

1) Mass ratio of alkaline earth metal fatty acid salt added at the time of preparation of dialkoxymagnesium to the total amount of metallic magnesium

(Example 14)
<Preparation of solid catalyst components for olefin polymerization>
A mixed solution was formed by charging 30 ml of titanium tetrachloride and 20 ml of toluene into a round bottom flask having a capacity of 500 ml, which was sufficiently replaced with nitrogen gas and equipped with a stirrer. Next, a suspension formed using 10 g of diethoxymagnesium obtained in Example 1 above, 50 ml of toluene and 3.3 ml (12.5 mmol) of di-n-butyl phthalate was brought to a solution temperature of 10 ° C. It was added to the retained mixed solution.
Then, the liquid temperature was raised from 10 ° C. to 90 ° C., and the reaction was carried out at 90 ° C. for 2 hours with stirring.
After completion of the reaction, the obtained solid product was washed 4 times with 100 ml of toluene at 90 ° C., 30 ml of titanium tetrachloride and 70 ml of toluene were newly added, the temperature was raised to 110 ° C., and the reaction was carried out with stirring for 2 hours. After completion of the reaction, the mixture was washed 10 times with 100 ml of n-heptane at 40 ° C. to obtain a solid catalyst component (A-1) for olefin polymerization.
The solid catalyst component (A-1) contained 14.2% by mass of a phthalic acid diester as an internal electron donating compound. Moreover, when the titanium content in this solid catalyst component was measured, it was 2.2% by weight.

<Formation of olefin polymerization catalyst and propylene polymerization>
In an autoclave with a stirrer having an internal volume of 2.0 liters completely replaced with nitrogen gas, 1.32 mmol of triethylaluminum, 0.13 mmol of cyclohexylmethyldimethoxysilane and the above solid catalyst component (A-1) were converted into titanium atoms. To form a catalyst for olefin polymerization, 0.0026 mmol was charged.
Next, 4 liters of hydrogen gas and 1.4 liters of liquefied propylene are charged into an autoclave, prepolymerized at 20 ° C. for 5 minutes, heated to 70 ° C., and polymerized at 70 ° C. for 1 hour. To obtain a propylene polymer. Table 3 shows the polymerization activity per 1 g of the solid catalyst component and the physical characteristics of the obtained polymer.

<Average particle size of polymer, particle size distribution index and amount of fine powder with particle size less than 75 μm>
The average particle size, particle size distribution index, and fine powder amount of less than 75 μm of the obtained polymer were measured under the following measurement conditions using a digital image analysis type particle size distribution measuring device (Camsizer, manufactured by Horiba Seisakusho Co., Ltd.). The volume-based integrated particle size distribution of the polymer was automatically measured.
(Measurement condition)
Funnel position: 6mm
Camera coverage area: Basic camera less than 3%, Zoom camera less than 10% Target coverage area: 0.5%
Feeder width: 40 mm
Feeder control level: 57, 40 seconds Measurement start level: 47
Maximum control level: 80
Control criteria: 20
Image rate: 50% (1: 2)
Particle size definition: Minimum value of Martin diameter measured n times for each particle SPHT (spherical) fitting: 1
Class upper limit: Select 50 points in the range of 32 μm to 4000 μm as a logarithmic scale.

(Comparative Example 2)
Preparation of a solid catalyst component for olefin polymerization, formation of an olefin polymerization catalyst, propylene polymerization and acquisition in the same manner as in Example 14 except that the diethoxymagnesium obtained in Comparative Example 1 was used as the diethoxymagnesium. The physical properties of the obtained polymer were evaluated. The results are shown in Table 3.

(Example 15)
<Manufacturing of diethoxymagnesium>
2.0 g of metal magnesium powder (average particle size 97 μm), absolute ethanol in a 1 L capacity four-necked flask equipped with an integrated gas meter, a dropping funnel, a stirrer and a reflux condenser, and the inside is filled with nitrogen gas. 76 g and 1.3 g (5.1 mmol) of iodine were charged and heated to the reflux temperature of ethanol in an oil bath to maintain the reflux state.
Then, a mixture of 5.8 g of metallic magnesium powder and 33 g of ethanol was added thereto in 4 portions every 6.5 minutes. After the total amount was added, 3.3 g (20 mmol) of hexamethyldisiloxane was added, and the mixture was further heated under reflux for 1 hour to complete the reaction.
Then, the reaction solution was dried by a rotary evaporator to obtain 27.8 g of powdered diethoxymagnesium.
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.9% by mass and the Si content was 0.13% by mass (0.77% by mass when converted to hexamethyldisiloxane content). rice field. The results of the analysis and evaluation are shown in Table 4.

(Example 16)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that the amount of hexamethyldisiloxane added was changed from 3.3 g (20 mmol) to 2.2 g (14 mmol).
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.9% by mass and the Si content was 0.09% by mass (0.51% by mass when converted to hexamethyldisiloxane content). rice field. The results are shown in Table 4.

(Example 17)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that the amount of hexamethyldisiloxane added was changed from 3.3 g (20 mmol) to 5.5 g (34 mmol).
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.7% by mass and the Si content was 0.22% by mass (1.28% by mass when converted to hexamethyldisiloxane content). rice field. The results are shown in Table 4.

(Example 18)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that the amount of hexamethyldisiloxane added was changed from 3.3 g (20 mmol) to 7.3 g (45 mmol).
Analysis of the obtained diethoxymagnesium revealed that the iodine content was 2.6% by mass and the Si content was 0.01% by mass (0.06% by mass when converted to hexamethyldisiloxane content). rice field. The results are shown in Table 4.

(Example 19)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that 3.3 g (8.5 mmol) of dodecamethylpentasiloxane was used instead of 3.3 g (20 mmol) of hexamethyldisiloxane.
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.4% by mass and the Si content was 0.65% by mass (3.6% by mass when converted to the polysiloxane content). The results are shown in Table 4.

(Example 20)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that 3.3 g of silicone oil (CasNo. 63148-62-9) was used instead of 3.3 g (20 mmol) of hexamethyldisiloxane. ..
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.3% by mass and the Si content was 0.09% by mass (0.52% by mass when converted to the polysiloxane content). The results are shown in Table 4.

(Example 21)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that 3.3 g (14 mmol) of octamethyltrisiloxane was used instead of 3.3 g (20 mmol) of hexamethyldisiloxane.
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.5% by mass and the Si content was 0.01% by mass (0.08% by mass when converted to the polysiloxane content). The results are shown in Table 4.

(Example 22)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that 3.3 g (11 mmol) of decamethyltetrasiloxane was used instead of 3.3 g (20 mmol) of hexamethyldisiloxane.
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.1% by mass and the Si content was 0.20% by mass (2.2% by mass when converted to the polysiloxane content). The results are shown in Table 4.

(Comparative Example 3)
Powdered diethoxymagnesium was prepared in the same manner as in Example 15 except that hexamethyldisiloxane was not added after the addition of the metallic magnesium powder.
When the obtained diethoxymagnesium was analyzed, the iodine content was 2.6% by mass and the Si content was 0% by mass. The results are shown in Table 4.

１）金属マグネシウム合計量に対する環状ジメチルポリシロキサンの添加量
２）得られたジアルコキシマグネシウム中のＳｉ含有量

1) Addition of cyclic dimethylpolysiloxane to the total amount of metallic magnesium 2) Si content in the obtained dialkoxymagnesium

(Example 23)
<Preparation of solid catalyst components for olefin polymerization>
A mixed solution was formed by charging 30 ml of titanium tetrachloride and 20 ml of toluene into a round bottom flask having a capacity of 500 ml, which was sufficiently replaced with nitrogen gas and equipped with a stirrer. Next, a suspension formed using 10 g of diethoxymagnesium obtained in Example 15 above, 50 ml of toluene and 3.3 ml (12.5 mmol) of di-n-butyl phthalate was brought to a solution temperature of 10 ° C. It was added to the retained mixed solution.
Then, the liquid temperature was raised from 10 ° C. to 90 ° C., and the reaction was carried out at 90 ° C. for 2 hours with stirring.
After completion of the reaction, the obtained solid product was washed 4 times with 100 ml of toluene at 90 ° C., 30 ml of titanium tetrachloride and 70 ml of toluene were newly added, the temperature was raised to 110 ° C., and the reaction was carried out with stirring for 2 hours. After completion of the reaction, the mixture was washed 10 times with 100 ml of n-heptane at 40 ° C. to obtain a solid catalyst component (A-2) for olefin polymerization.
The solid catalyst component (A-2) contained 14.2% by mass of phthalic acid diester as an internal electron donating compound. Moreover, when the titanium content in this solid catalyst component was measured, it was 2.2% by weight.
<Formation of olefin polymerization catalyst and propylene polymerization>
In an autoclave with a stirrer having an internal volume of 2.0 liters completely replaced with nitrogen gas, 1.32 mmol of triethylaluminum, 0.13 mmol of cyclohexylmethyldimethoxysilane and the above solid catalyst component (A-2) were converted into titanium atoms. To form a catalyst for olefin polymerization, 0.0026 mmol was charged.
Next, 4 liters of hydrogen gas and 1.4 liters of liquefied propylene are charged into an autoclave, prepolymerized at 20 ° C. for 5 minutes, heated to 70 ° C., and polymerized at 70 ° C. for 1 hour. To obtain a propylene polymer. Table 5 shows the polymerization activity per 1 g of the solid catalyst component and the physical properties of the obtained polymer.
<Average particle size of polymer, particle size distribution index and amount of fine powder with particle size less than 75 μm>
The average particle size, particle size distribution index, and fine powder amount of less than 75 μm of the obtained polymer were measured under the following measurement conditions using a digital image analysis type particle size distribution measuring device (Camsizer, manufactured by Horiba Seisakusho Co., Ltd.). The volume-based integrated particle size distribution of the polymer was automatically measured.
(Measurement condition)
Funnel position: 6mm
Camera coverage area: Basic camera less than 3%, Zoom camera less than 10% Target coverage area: 0.5%
Feeder width: 40 mm
Feeder control level: 57, 40 seconds Measurement start level: 47
Maximum control level: 80
Control criteria: 20
Image rate: 50% (1: 2)
Particle size definition: Minimum value of Martin diameter measured n times for each particle SPHT (spherical) fitting: 1
Class upper limit: Select 50 points in the range of 32 μm to 4000 μm as a logarithmic scale.

(Comparative Example 4)
As the diethoxymagnesium, the preparation of the solid catalyst component for olefin polymerization, the formation of the olefin polymerization catalyst, the propylene polymerization and the obtained were carried out in the same manner as in Example 23, except that the diethoxymagnesium obtained in Comparative Example 3 was used. The physical properties of the polymer were evaluated. The results are shown in Table 5.

Claims (13)

A method for producing dialkoxymagnesium, which is obtained by reacting metallic magnesium and alcohol in the presence of a reaction accelerator to obtain dialkoxymagnesium.
Adding a surfactant before or during the reaction of the metallic magnesium with the alcohol,
The surfactant is either dimethylpolysiloxane having 1 to 30 Si—O units or a fatty acid salt of a Group 1 element of the Periodic Table or an element of Group 2 of the Periodic Table.
A method for producing dialkoxymagnesium. The dimethylpolysiloxane is based on the following general formula (1a):

(In the formula, n is an integer of 3 to 30.)
The method for producing dialkoxymagnesium according to claim 1, wherein the cyclic dimethylpolysiloxane is represented by. The dimethylpolysiloxane is based on the following general formula (1b):

(In the formula, m is an integer from 1 to 30.)
The method for producing dialkoxymagnesium according to claim 1, wherein the chain dimethylpolysiloxane is represented by. The dialkoxymagnesium according to claim 3, wherein the dimethylpolysiloxane represented by the general formula (1b) is a chain dimethylpolysiloxane in which m in the general formula (1b) is 1 to 10. Manufacturing method. The method for producing dialkoxymagnesium according to claim 1, wherein the fatty acid salt is a fatty acid salt of magnesium or calcium. The method for producing dialkoxymagnesium according to any one of claims 1 to 5, wherein the average particle size (D ₅₀ ) of the dialkoxymagnesium is 5 to 100 μm. The method for producing dialkoxymagnesium according to any one of claims 1 to 6, wherein the average particle size (D ₅₀ ) of the metallic magnesium is 5 to 500 μm. The bulk density of the dialkoxymagnesium is 0.15 to 0.70 g / ml, and the particle size distribution index ((D ₉₀ − D ₁₀ ) / D ₅₀ ) is 0.3 to 2.0. The method for producing dialkoxymagnesium according to any one of claims 1 to 7. The method for producing dialkoxymagnesium according to any one of claims 1 to 8, wherein the Si content of the dialkoxymagnesium is 0.01 to 10% by mass. Contact the dialkoxymagnesium (a) obtained by the method for producing dialkoxymagnesium according to any one of claims 1 to 9, the titanium halogen compound (b), and the electron donating compound (c). A solid catalyst component for olefin polymerization, which is characterized by being obtained by subjecting the mixture. (A) The solid catalyst component for olefin polymerization according to claim 10, and (B) the following general formula (2):
R ² _p AlQ _3-p (2)
(In the formula, R ² indicates an alkyl group having 1 to 4 carbon atoms, Q indicates a hydrogen atom or a halogen atom, and p is a real number of 0 <p ≦ 3. When a plurality of R ² are present, each R ² may be the same or different from each other, and when there are a plurality of Qs, each Q may be the same or different.)
A catalyst for polymerizing olefins, which comprises an organoaluminum compound represented by. The catalyst for polymerizing olefins according to claim 11, further comprising (C) an external electron donating compound. A method for producing an olefin polymer, which comprises polymerizing olefins in the presence of the catalyst for polymerizing olefins according to any one of claims 11 or 12.