JPS60131868A - Manufacture of silicic acid powder sphere - Google Patents

Abstract

(57) [Summary] This bulletin contains application data before electronic filing, so abstract data is not recorded.

Description

[Detailed Description of the Invention] The present invention relates to a method for producing a silicic acid substrate, more specifically,
There are few companies that contain uranium for filling fecal fat, which is used as a side-filling material for transistors, ICs, LSIs, etc. (This article relates to a method for producing siliceous primary spheres with good fluidity.

Conventionally, siliceous materials such as fused quartz and fused acid are known as fillers used in grease-resistant materials such as transistors, ICs, and LSIs.In particular, fused quartz is filled with epoxy, siligene, and polyester. *, jflll When blended with molding materials such as fats, it is attracting attention because it imparts excellent thermal properties and electrical customization workability.

However, recently, with the advancement of technology, half-four bodies have become more efficient, and the packaging materials are required to have higher performance, and the uranium used as the filler produces alpha particles when it disintegrates. Therefore, fillers with fewer uranium-containing groups are desired since they can cause soft errors in semiconductor products.

Fillers with low uranium content include those made from naturally occurring silica ore, bath-fused and pulverized, and synthetic fillers using halogenated silicon compounds as starting materials. (Unexamined Japanese Patent Application No. 57-187956, Unexamined Japanese Patent Application No. 58-15
(No. 1318), the production of natural products is at a limit, and Juhitai Koka, which is on the verge of collapse, cannot meet the increasing demand and supplies, and the quality is also stable. I'm worried about hoping for something of good quality.・ On the other hand, synthetic products have a very small particle size, which makes it difficult to fill the resin and have poor workability, so fine synthetic products are heated to over 1900'C and then rapidly cooled. A method has been proposed in which a vitrified product is crushed into pieces of about 200 μm or less to obtain an optical filler. (Japanese Patent Application Laid-Open No. 57-195151) However, although this method yields siliceous rice with a small uranium-containing layer, the pulverized product has an amorphous particle shape due to the pulverization process.
Increasing the loading of the resin reduces its fluidity, which impedes the pricking operation, and also leaves distortions during curing, which deteriorates the properties of the ten-damaged element.

There is also a proposal to improve this distortion by adjusting the particle size distribution of the optical material, but it is sufficient for resin filling, and four plus one is sufficient.

By granulating the powdered Ryoshina, which is used in the field of fire, and melting it directly into #1 spherules for flame use, it contains less uranium and improves the stability and fluidity when blended with Shikamo resin. The object of the present invention is to provide a method for manufacturing a silicate powder spherical body containing uranium and W in a small process, which allows a resin composition with excellent properties and low stress during molding to be obtained. In other words, the present invention is a synthetic silicon material with a uranium N magnetism of 10 ppb or less! ll! After granulating the powder into particles with a particle size of 5L and 10μ or less, the powder was granulated into powder. 11! Sprayed from the burner with the raw material and 17ooc
Heat treatment at a temperature above and cooling '4! J symptoms.

The invention will be further explained in detail below.

In the present invention, the synthetic silicon used as a raw material is hydrolyzed, modified by silane compounds and silane compounds that tend to occur together with halo r/silicon ratio 9, modified by 'J+ solution or alcohol present. It is produced by hydrolyzing it into alcoquid in finishing, and the ura/containing void is 1 [3 ppb or less,
It is preferably used that has a particle size of 0.01~U, about 5 μWL, and has a uranium residue of 1 Uppb or less. When inspecting raw materials, the uranium content in the raw materials must not exceed 101) I) b, and silicate powder spheres with a content of less than ppb cannot be expected.

In order to granulate these silicon negative wave powders of 1 (J (2) A method that utilizes the compression and sintering of horse chestnuts without using a binder (hereinafter referred to as the non-bonded abrasion granulation method) '41? It can be used and is granulated to a particle size of 500μ or less, preferably 200μ or less. If the particle size is larger than 500 μm, operation becomes difficult due to clogging of the burner, etc., and spherical shape and bath melting are also difficult to obtain.

The binders used in the bonding four-branching method include zero-purity water that contains virtually no uranium, organic bath media such as alcohol, ethyl silicate, colloidal silica, and polyvinyl alcohol (PVA). Specifically, the uranium-containing layer or those with less than i ppb are used for one history.

In addition, as a granulator used in the bonded abrasion granulation method, a known granulator can be used. Specifically, a drum-type granulator with uranium-containing lining (for example, urethane rubber), a rotary M-type FI granulator, or a spray dryer. Examples include injection type granulation equipment such as . All of these are preferable because they have the advantage that particles having a wide range of grain sizes can be stored relatively easily.

The amount of binder used varies depending on the speed of the granulator, but for example, in the case of a spray dryer, it is
If it is 0 weight or more (and the transfer type granulator is 70 weight,
It is preferable that the amount is less than or equal to 5 to 60%. Terera Wei 8! It is not necessary to dry the product, or if it is dried, it can be done at the same time as granulation or after granulation. .

In addition, in the non-bonding abrasion granulation method, each individual product, including a rotary kiln that uses a material with low concentration of hydrogen, such as uranium and high-purity silica containing less than 10 ppb F, is used. A heating furnace can be used.

One time during heating is 14 UL] (preferably 3 or less; is 12 L)
1 (below J゛CC (at temperatures other than the above, large particle sizes will be produced).The granulated product that has been granulated as described above is not desirable because it is below J゛CC (at temperatures other than the above). 1700' formed by injecting gas, TLL, and element from the burner from the upper part of the vertical furnace to the lower part of the furnace.
Instantly heat treated in 4 enclosures of U or higher. As the oT fuel gas, hydrogen, gropa/dethane, globylene, acetylene, etc. can be used for one cycle, but it is also possible to convert solid fuel such as kerosene or heavy oil into a gas stream and use it for one cycle.

Injected into the furnace = yr fuel injection and oxygen η speed is only to form a nice flame shape or atmosphere. In order to influence the formation rate or retention time, if the raw gas Q is 1t, the speed is preferably 40n.
It is preferable that it is t/paper or more. See you again! It is preferable that the li2 element is injected at a flow rate lower than the flow rate of the above-mentioned 1-Ij combustion gas.

Injecting at a flow rate other than the above is undesirable as grains may crack each other or the grains may not be perfectly separated by a millimeter.

The temperature of the atmosphere is the temperature at which the quartz wood melts into fused quartz. Specifically, it is 17 uoC or more, preferably 180 u to 260 U'' C. At the temperature of 17 uo C, it is completely melted. Unable to form fused silica.

The retention time of the silicic acid powder spheres in the furnace melting firefly is instantaneous and is less than 0.05 seconds. Thereafter, the silicic acid powder spherules are quenched together with the combustion exhaust gas through duct V3, etc., and cooled and separated using a cyclone, a bag filter, and a fruit machine. Note that the combustion νF gas is discharged through the blower.

The silicate powder spheroid obtained by the present invention has a particle size bU
Since the particle size is less than Oμ, when it is used once again as a resin cutter, it can be used as is, or it can be adjusted to obtain the desired grain size.

In addition, for particles with a particle size of 500μ or more, 1 containing this
If the disintegrating composition is used once more, problems may occur in work vehicles, such as clogging of pot-shaped dates, when manufacturing electronic parts to prevent millet. In addition, when using the combined cutting method, it is possible to obtain a product that undergoes the following one-sided modification and easily breaks up with bait fat.

As explained above, the present invention involves granulating synthetic silicon' According to the present invention, a spherical body that does not contain any impurities from the uranium cap is desired, so when mixed with resin, a molded body with good fluidity and low stress during molding can be obtained, and this can be used as a semiconductor. Using sealed VC can reduce soft errors.

In addition, in the method of saponification in the presence of bond cutting, the surface of the spherical bodies can be modified and K can be obtained, resulting in the formation of linseed fat, soybean oil, and soybean oil.

Hereinafter, a more specific explanation will be given using "l-yi θ=++ll".

Real sister l + I11 Japan Aerosol Co., Ltd. Fold product name [Aerosol] 1Lln
9U of pure water made by exchanging 55 ions to lts and distilling it further.
Add the volume of polyurethane rubber (Osaka Rubber Industries Co., Ltd.) and stir and mix with a mixer lined with lining to create a slurry with a solid content of 10 ljt%.This slurry is 1υKy/Hr.
The hot air temperature was approximately 3L at a supply rate of
A granulated product with a ratio of 100% under 9μ to 78.5μ under 44μ was obtained. This granulated product was heated with hydrogen gas at 50 Nm'/Hr (45-9m
/sec), 1 post-prime gas 15Nm3/Hr (8,
The product was melted in a bath at a temperature of 1850'O using a transparent quartz burner with a gas MArlt of 5m/sec) to melt the product. Product particle size outer pores, back/end, length')
The fl diameter comparison table shows. 450 light filler on the frame.
Door-Runovolac epoxy position (11i! (Cinoma Geyer's simple product name "gcN-1280J") 100 days, Phenol novolac stool fat (CH/Mageigy company's Ilb name rHT-94!,'OJ) 50ffi approval 3, - 1) Landisyl imidazole (hardening accelerating cutting) 2) Add 6 parts of carnauba wax, and mix with 30 parts.
After kneading for 0 minutes + iJJ, the mixture was cooled, solidified, and chopped. Flow to the end! ! l
In order to measure the properties and resin stress, this auxiliary crushed product was molded at a molding temperature of 160' and a cutting pressure of Q kg/mm''.The results are shown in the table.

Example 2: 100% silicon tetrachloride was added to 100% pure water and 200% pure water was distilled to 90% pure water at room temperature. Thereafter, washing with pure water is repeated until the - value becomes 6 to 7, followed by filtration. I was served! Heated in a 7JD heat furnace at a temperature of 700" (EK) and then fed to a rotary kiln lined with pure silica, with a particle size of 200μ or less, 98 μm, 44μ, 65.
A granulated product of 2% was prepared. This granulated product was heat treated under the same conditions as in Example 1.

100M parts of silica obtained by hydrolyzing silicon tetrachloride with oxygen and hydrogen gas is added by distillation to Hx -y
-/I/ 7 A/ Co-A/ 15 While blowing the LJ volume part, polyurethane rubber [Osaka Rubber Industries Co., Ltd. Granulated in a drum granulation stone with 8 lining, particle size 149μ'F92% 44μ
80.2% (7) It's a grain product and it's a family. This granulated product was heated with propane gas 10 Nm3/Hr (12,'orn/, s
ec ), [raw scrap 5Nm3/Hr (6-2rn/
sec ) with a gas composition of
! I cum.

A composition was prepared using the same formulation as C Shiori 1 1 bottle of Aerosol (4), trade name ``Aerosil'' 5゜ Tsukuobubu and Meikareli 1, and its (
I often performed 1J po.

Comparative Example 2 Nippon Aerosil <th) trade name "Aerosol" was placed in a high-purity silica crucible and heated to 1850'C with a transparent quartz burner using hydrogen gas once to melt it. Thereafter, the melt was collected, subjected to co-grinding using a ball mill lined with polyurethane rubber, and sieved to obtain a pulverized product.

Comparative Example 6 The same procedure as in Example 1 was carried out by a colleague, except that madder purity Indian silica stone was co-pulverized in a polyurethane-lined ball mill and adjusted to 200μ or less.

However, the troughs and easiness of the table were measured using the following method.

(1) Fluid side rectangle (spiral flow) Using a mold that complies with EMM engineering regulations, molding temperature: 160°C, molding pressure: 0
I did side leg at kg/1+1142. C inch] (2
) Uranium content by fluorophotometry. Cppbl +21 +*I Resistance 11 If0) Measurement of stress Resistor 11 If0) Resistor that changes ratio was molded into a cow conductor chig. It was die-bonded to the 14-bin IC frame and connected to the external electrode with a wire bond using Au. Initial resistance value (Ro) of confectionery +1111 f L
The resistance value (CR) after this confectionery was pierced with resin at 160°C and 7 [1 kg/an2 molding time of 6 minutes] was measured, and (R-Ro)/Ro was defined as the resin stress.

Claims (1)

[Claims] Synthetic silicon 1XtIl with uranium content of 10 ppb or less
+! After granulating the powder to a particle size of 500μ or less, it is injected from a burner together with a flammable gas and heated to 1700"C.
A method for manufacturing siliceous powder spherical bodies with a low urene content, which is patented by heat treatment at a temperature above and reduced to zero.