TW201634708A - Bonding composition - Google Patents

Abstract

Provided is a bonding composition that contains tin, silver, and iridium, with the tin being the primary component, and contains 0.5-11.0 mass% of the silver.

Description

Bonding composition

The present invention relates to a composition for bonding.

The bonding composition which can be used for joining a bonding material containing a metal or an oxide or the like in the joining portion has been studied from the past. In particular, it is difficult to bond the material to be joined including the oxide in the joint portion, and therefore, the bonding composition which can be joined even when the joint portion of the material to be joined contains an oxide is continuously studied.

For example, Patent Document 1 discloses a solder alloy for oxide bonding, which comprises, by mass%, Ag: 2.0 to 15.0%, Al: more than 0.1 to 6.0%, and the balance containing Sn and unavoidable impurities.

[Previous Technical Literature] [Patent Literature]

Patent Document 1: Japanese Patent No. 4669877

However, in recent years, when joining materials to be joined, it is required to exhibit a bonding composition having a higher bonding strength. Therefore, even in the solder alloy for oxide bonding disclosed in Patent Document 1, there is a problem that the joint strength is insufficient.

The present invention has been made in view of the problems of the prior art described above, and it is an object of the invention to provide a bonding composition having high bonding strength.

In order to solve the above problems, the present invention provides a bonding composition containing tin, silver, and antimony, containing tin as a main component, and containing 0.5% by mass or more and 11.0% by mass or less of the above. silver.

According to an aspect of the present invention, a bonding composition having a high bonding strength can be provided.

12‧‧‧Combination Composition Department

14‧‧‧ Pressing fixture

22‧‧‧ soldering iron

23‧‧‧ soldering iron

31, 33‧‧‧ Sodium Calcium Glass Substrate

32‧‧‧Combination Composition Department

111, 112‧‧‧ Soda-lime glass substrate

131, 132‧‧‧ Support fixtures

211, 212‧‧‧Combination Composition Department

331‧‧‧ hole

A‧‧‧square arrow

Fig. 1 is a schematic explanatory view showing a three-point bending test for evaluating joint strength in Examples and Comparative Examples.

Fig. 2 (A) to (C) are explanatory views showing the procedure for producing a test piece for a three-point bending test.

Fig. 3 is a schematic explanatory view showing a leak test piece for evaluating the vacuum sealing property of the joint surface in the examples and the comparative examples.

In the following, the embodiments of the present invention are described with reference to the drawings, but the present invention is not limited to the embodiments described below, and various changes and substitutions may be made to the embodiments described below without departing from the scope of the invention.

In the present embodiment, first, a configuration example of one of the bonding compositions will be described.

The bonding composition of the present embodiment contains tin, silver, and antimony, and contains tin as a main component and contains 0.5% by mass or more and 11.0% by mass or less of silver.

Hereinafter, each component which can be contained in the bonding composition of the present embodiment will be described.

(tin)

As described above, the bonding composition of the present embodiment contains tin (Sn) as a main component. Tin can alleviate the difference in thermal expansion between the material to be joined and the composition for bonding. Further, tin has a lower The effect of the melting temperature of the composition for bonding.

In addition, it is contained as a main component in the composition for bonding, for example, it means that the component for bonding is the most containing component by mass ratio, and it is preferable to contain 60 mass % or more of components in the composition for bonding. .

In particular, the content of tin in the composition for bonding is, for example, more preferably 84% by mass or more, still more preferably 92% by mass or more.

When the content of tin in the composition for bonding is 84% by mass or more, the thermal expansion difference between the material to be joined and the composition for bonding is moderated, and the melting temperature of the composition for bonding is lowered. Shows a particularly high effect.

The upper limit of the content of tin in the composition for bonding is not particularly limited, and is, for example, preferably 99% by mass or less, and more preferably 98% by mass or less.

As described above, the bonding composition of the present embodiment contains silver and bismuth in addition to tin. Further, by including these components, the bonding strength of the bonding composition can be particularly improved. Further, in addition to silver or strontium, any of the following components may be added. Therefore, in order to sufficiently ensure the content of the components other than the tin, the content of tin is preferably 99% by mass or less as described above.

(silver)

As described above, the bonding composition of the present embodiment contains silver.

When the composition for bonding contains silver, even when the joint portion of the material to be joined contains an oxide, a high joint strength can be exhibited.

This is because silver can be combined with oxygen, so that by containing silver, the bonding property or wettability with the oxide contained in the joint portion of the material to be joined can be improved.

In addition, when the bonding composition is combined with oxygen to form an oxide film, the bonding to the material to be bonded is hindered. However, it is considered that silver bonded to oxygen does not become an oxide film and is mainly included in the bonding combination. Inside the object. Further, when the composition for bonding contains silver, it is possible to suppress the formation of an oxide film by the bonding composition itself.

Further, the bonding composition of the present embodiment may contain tin as a main component as described above. However, since tin is a relatively soft metal, sufficient bonding strength cannot be obtained if only tin is used. On the other hand, in the bonding composition of the present embodiment, tin and silver are contained at the same time, and tin and silver can form an intermetallic compound, thereby improving the bonding strength of the bonding composition.

The content of silver in the bonding composition of the present embodiment is 0.5% by mass or more. The content of silver in the bonding composition of the present embodiment is preferably 1.0% by mass or more, and more preferably 1.5% by mass or more.

The reason for this is that when the content of silver in the composition for bonding is 0.5% by mass or more, as described above, tin and silver can form a sufficient amount of the intermetallic compound to improve the bonding strength of the bonding composition.

Moreover, the upper limit of the content of silver in the bonding composition of the present embodiment is 11.0% by mass or less. The upper limit of the content of silver in the bonding composition of the present embodiment is preferably 10.0% by mass or less, and more preferably 8.5% by mass or less.

The reason is that, as described above, tin and silver can form an intermetallic compound, and although the intermetallic compound of tin and silver is hard, it has a brittle characteristic, and if the content of the intermetallic compound is excessively increased, the joint strength is reversed. Reduce the situation. Therefore, it is preferable to set the content of silver to 11.0% by mass or less, and the intermetallic compound does not excessively increase in the composition for bonding.

(iridium)

As described above, the bonding composition of the present embodiment contains ruthenium.

The inventors of the present invention have made an effort to further study the composition of the bonding composition which can further improve the bonding strength when the material to be joined is joined. Then, it was found that the airtightness or the joint strength can be improved by containing iridium (Ir) which has not been used as a constituent material of the composition for bonding.

Moreover, according to the study by the inventors of the present invention, the composition for bonding contains ruthenium, and also has a tendency to reduce the melting of the bonding composition in order to bond the materials to be joined. The effect of the voids. The reason for this is that the surface tension of the molten metal obtained by melting the bonding composition can be reduced by adding antimony to the composition for bonding, and the entrainment of gas or the alloy contained in the composition for bonding can be reduced. The crystal grains are fine.

When a void is formed when the bonding composition is melted, the bonding area is lowered. However, the bonding composition of the present embodiment containing ruthenium suppresses generation of voids, so that generation of a leak path can be reduced, and airtightness can be improved. Further, a sufficient joint area can be secured, and the joint strength can be improved.

In the case where the bonding composition is melted to bond the material to be joined, the bonding composition of the prior art has an oxide film which is an oxide film formed on the surface of the bonding composition. As described above, when an oxide film is formed on the surface of the composition for bonding, it is difficult to coat the bonding composition or bond with the material to be bonded. Therefore, when the bonding composition is melted, applied, and bonded to the material to be joined, an ultrasonic iron which can be heated while applying ultrasonic vibration is used in order to destroy the film of the oxide.

On the other hand, according to the composition for bonding containing ruthenium according to the present embodiment, it is possible to suppress the occurrence of an oxide film on the surface of the composition for melting when the composition for bonding is melted. Therefore, the bonding composition can be coated or bonded to the material to be joined by using a soldering iron having only a heating function instead of the above-described ultrasonic soldering iron. Alternatively, when the bonding composition is heated in contact with the material to be joined, the bonding composition can be wet-diffused and bonded to the material to be joined without using a soldering iron. Therefore, the controllability of a processing apparatus such as a soldering iron when the bonding composition is melted and applied to the material to be joined is lowered, and workability can be improved.

The content of the ruthenium of the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 0.001% by mass or more. The content of the ruthenium in the composition for bonding of the present embodiment is preferably 0.005% by mass or more, and more preferably 0.008% by mass or more.

The reason for this is that the bonding strength can be sufficiently improved when the material to be joined is joined by the bonding composition by setting the content of cerium to 0.001% by mass or more. Moreover, the reason for this is that it is particularly effective in suppressing the bonding of the bonding composition to bond the material to be joined. The generation of a gap or the generation of an oxide film is preferred.

The upper limit of the content of the ruthenium of the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 1.0% by mass or less. The upper limit of the content of cerium in the bonding composition of the present embodiment is preferably 0.8% by mass or less, and more preferably 0.5% by mass or less.

The reason for this is that if the content of cerium exceeds 1.0% by mass, the melting point of the bonding composition may increase.

Moreover, according to the study by the inventors of the present invention, when the content of ruthenium is 1.0% by mass or less, it is possible to more reliably suppress oxidation of the surface of the composition for bonding when it is melted as described above. Membrane.

The tin, silver, and antimony contained in the bonding composition of the present embodiment have been described. However, the bonding composition of the present embodiment may further contain an optional component. Any component will be described below.

(aluminum)

The bonding composition of the present embodiment may further contain aluminum (Al).

When the bonding composition is melted, the aluminum contained in the bonding composition tends to be an oxide. Therefore, when the joint portion of the material to be joined contains an oxide, the oxide of the joint portion and the bonding composition are easily bonded, and the wettability of the joint composition and the joint portion containing the oxide is improved, and the wettability can be improved. A higher joint strength.

The content of aluminum in the bonding composition of the present embodiment is not particularly limited, and may be, for example, 0.001% by mass or more. The content of aluminum in the bonding composition of the present embodiment is preferably 0.01% by mass or more, and more preferably 0.03% by mass or more.

When the content of aluminum in the composition for bonding is 0.001% by mass or more, the wettability of the oxide contained in the joint portion of the material to be joined and the composition for bonding can be particularly improved, and the joint strength can be improved. .

In addition, the upper limit of the content of aluminum in the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 0.8% by mass or less. Aluminum of the bonding composition of the present embodiment The upper limit of the content is preferably 0.5% by mass or less, more preferably 0.3% by mass or less.

The reason for this is that aluminum has a tendency to form an oxide when the composition for bonding is melted as described above, and when the content of aluminum exceeds 0.8% by mass, the composition for bonding is melted in the composition for bonding. Overproduction of oxides.

When an oxide is excessively generated in the composition for bonding, for example, the oxide is deposited on the surface of the composition for bonding to form an oxide film. When an oxide film is formed on the surface of the composition for bonding, the bonding strength with the material to be joined is lowered, or the entire bonding composition is made porous due to solidification shrinkage, and the airtightness of the joined portion of the material to be joined is lowered. Hey.

Moreover, when the material to be joined is melted and joined, aluminum may be separated from the composition for bonding to form an aluminum layer. However, when the content of aluminum in the composition for bonding is 0.8% by mass or less, even if an aluminum layer is formed, the joint strength is hardly affected. Therefore, the content of aluminum is preferably 0.8% by mass or less.

Further, in the bonding composition of the present embodiment, the following cerium and aluminum may be contained at the same time. In the case where both are contained at the same time, it is preferably 1.8% by mass or less in total.

In addition, the bonding composition of the present embodiment may contain one or more metals selected from the group consisting of germanium (Ge), nickel (Ni), copper (Cu), and magnesium (Mg) as other optional components. Each component will be described below.

(germanium)

As described above, the bonding composition of the present embodiment may further contain ruthenium.

When the bonding composition is melted, the enthalpy contained in the bonding composition tends to be an oxide. Therefore, when the joint portion of the material to be joined contains an oxide, the oxide of the joint portion and the bonding composition are easily bonded, and the wettability of the joint composition and the joint portion containing the oxide is improved, and the wettability can be improved. A higher joint strength.

The content of the ruthenium of the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 0% by mass or more. The content of the ruthenium of the composition for bonding of the present embodiment is preferably 0.01. More than % by mass.

In addition, the upper limit of the content of the ruthenium of the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 1.0% by mass or less. The upper limit of the content of cerium in the bonding composition of the present embodiment is preferably 0.8% by mass or less, more preferably 0.6% by mass or less.

The reason for this is that when the content of cerium exceeds 1.0% by mass, when the bonding composition is melted, an oxide is excessively generated in the bonding composition. The reason for this is that if an oxide is excessively generated in the composition for bonding, for example, the oxide is deposited on the surface of the composition for bonding to form an oxide film, thereby hindering bonding to the object to be bonded.

(nickel)

As described above, the bonding composition of the present embodiment may contain nickel (Ni).

When the bonding composition is melted, the nickel contained in the bonding composition tends to be an oxide. Therefore, when the joint portion of the material to be joined contains an oxide, the oxide of the joint portion and the bonding composition are easily bonded, and the wettability of the joint composition and the joint portion containing the oxide is improved, and the wettability can be improved. A higher joint strength.

The content of nickel in the bonding composition of the present embodiment is not particularly limited, and may be, for example, 1.0% by mass or less, preferably 0.5% by mass or less.

This is because when the material to be joined is melted and joined, nickel is separated from the composition for bonding to form a nickel layer. However, when the content of nickel is 1.0% by mass or less, a nickel layer which affects the joint strength is hardly formed. Therefore, the content of nickel is preferably in the range of 1.0% by mass or less.

The lower limit of the content of nickel in the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 0% by mass or more.

(copper)

As described above, the bonding composition of the present embodiment may contain copper (Cu).

When the composition for bonding contains copper, the melting point of the composition for bonding can be lowered. Moreover, the reason is that the composition for bonding can be improved by the copper containing the composition for bonding. The wettability of the bonding material exerts a high bonding strength.

The content of copper in the bonding composition of the present embodiment is not particularly limited, and may be, for example, 0.1% by mass or less.

The reason for this is that copper has an effect of lowering the melting point of the composition for bonding as described above. However, if the content of copper is too large, the melting point of the composition for bonding may increase. Therefore, by setting the content of copper to 0.1% by mass or less, it is possible to more reliably prevent the melting point of the bonding composition from rising.

The lower limit of the content of the copper in the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 0% by mass or more.

(magnesium)

As described above, the bonding composition of the present embodiment may contain magnesium (Mg).

When the composition for bonding is melted, the magnesium contained in the composition for bonding tends to be an oxide. Therefore, when the joint portion of the material to be joined contains an oxide, the oxide of the joint portion and the bonding composition are easily bonded, and the wettability of the joint composition and the joint portion containing the oxide is improved, and the wettability can be improved. A higher joint strength.

The content of magnesium in the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 0.5% by mass or less, preferably 0.3% by mass or less.

The reason for this is that since magnesium is a metal which is easily corroded, if the content of magnesium is too large, the composition for bonding itself becomes brittle. By setting the content of magnesium to 0.5% by mass or less, it is possible to more reliably suppress the occurrence of corrosion, which is preferable.

The lower limit of the magnesium content of the composition for bonding of the present embodiment is not particularly limited, and may be, for example, 0% by mass or more.

The components which may be contained in the bonding composition of the present embodiment have been described so far, but are not limited thereto. Further, the bonding composition of the present embodiment may contain, for example, an unavoidable component which is produced when the composition for bonding is prepared. The unavoidable component is not particularly limited. Wherein, it contains a selected from the group consisting of Fe, Co, Cr, V, Mn, When an element of one or more of Sb, Pb, Bi, Zn, As, and Cd is an unavoidable component, the content of the above element is preferably 0.2% by mass or less, more preferably 0.05% by mass or less in total.

The reason for this is that the element has an effect of lowering the wettability of the composition for bonding to the material to be joined, and by setting the total content of the elements to 0.2% by mass or less, it is possible to suppress the bonding composition from being bonded to the material. Wettability is reduced.

In addition, when Ga, P, and B are caused to cause voids, when one or more elements selected from the group consisting of Ga, P, and B are contained as an unavoidable component, the content thereof is preferably 0.05% by mass or less in total. More preferably, it is 0.01% by mass or less in total.

Further, the bonding composition of the present embodiment may further contain oxygen.

When the oxygen in the bonding composition contains an oxide in the joint portion of the material to be joined, it is a component that promotes bonding between the bonding composition and the bonding portion containing the oxide.

The state of the oxygen contained in the bonding composition is not particularly limited. For example, oxygen is preferably contained in a form of being melted in the metal material. This is because the interface between the bonding composition and the material to be bonded is smoothed by the gradient of the oxygen concentration between the oxide of the joined portion of the bonding material and the metal in the bonding composition, and the bonding interface is made firm. .

The method of containing oxygen in the composition for bonding is not particularly limited, and examples thereof include a method of melting and producing a composition for bonding in an oxygen-containing atmosphere, or a bonding operation with a material to be joined in an oxygen-containing atmosphere. method.

Further, it is preferable that the bonding composition before bonding the material to be joined satisfies the content of oxygen in the bonding composition described below. Therefore, it is preferred to adjust the oxygen concentration by a method of melting and producing the composition for bonding in an oxygen-containing atmosphere.

In particular, it is more preferable that the content of oxygen satisfies the following range in any of the bonding compositions before bonding the bonding materials and the bonding composition after bonding.

The content of oxygen in the composition for bonding is not particularly limited, and for example, it can be set to 0.0001 The amount is at least %, preferably 0.0007 mass% or more.

The reason for this is that the effect of improving the joint strength can be sufficiently exhibited by setting the content of oxygen to 0.0001% by mass or more.

The upper limit of the content of the oxygen in the composition for bonding is not particularly limited, and may be, for example, 2% by mass or less, preferably 1% by mass or less.

The reason for this is that if the amount of oxygen contained in the composition for bonding is too large, precipitation of oxides tends to occur on the surface or inside of the metal material, and the bonding strength is rather lowered. Therefore, as described above, the content of oxygen in the composition for bonding is preferably 2% by mass or less.

In addition, the content of oxygen in the composition for bonding herein means the content of oxygen contained in the composition for bonding. In other words, when an oxide film is formed on the surface of the composition for bonding, the oxygen content in the bonding composition after removing the oxide film is shown.

When the amount of oxygen in the composition for bonding is measured, the method for removing the oxide film is not particularly limited, and for example, it can be removed by treating the surface of the composition for bonding with an acid or the like.

Although the bonding composition of the present embodiment has been described, the bonding material to be bonded by the bonding composition of the present embodiment is not particularly limited, and can be used for bonding various bonding materials. Examples of the material to be joined include a metal, an oxide, and the like, and can be used for bonding metals, bonding of oxides, and bonding of metals and oxides.

In particular, when the oxide is contained in the joint portion of the material to be joined, it is difficult to exhibit sufficient joint strength, but the joint composition of the present embodiment can exhibit high joint strength. Therefore, the bonding composition of the present embodiment can be preferably used in the case where the material to be joined including the oxide in the joint portion is joined.

In addition, the oxide to be contained in the joint portion of the material to be joined is not particularly limited, and for example, it is preferably one or more selected from the group consisting of glass, chromium oxide, and aluminum oxide. Chrome oxygen A compound comprising chromium oxide formed on the surface of stainless steel. Further, the aluminum oxide includes a passivation film formed on the surface of the aluminum metal or alumina.

[Examples]

The specific examples are described below, but the present invention is not limited to the examples.

First, the evaluation methods of the bonding compositions produced in the following examples and comparative examples will be described.

(joint strength)

A test piece in which two glass plates were joined by the bonding composition prepared in each of the following Examples and Comparative Examples was prepared, and the test piece was subjected to a three-point bending test to measure the joint strength (unit: N/mm ^{2 ).} ).

The specific test sequence will be described using Figs. 1 and 2 . Fig. 1 is a cross-sectional view schematically showing a test piece which is parallel to a plane in which the lamination directions of two glass sheets constituting the test piece are parallel. 2 is an explanatory view showing a procedure for producing a test piece shown in FIG. 1. 1 and 2, the same components are denoted by the same reference numerals.

As shown in Fig. 1, in the three-point bending test, the joints of the joining composition portion 12 including the bonding composition were joined by using the two soda-lime glass substrates 111 and 112 at positions shifted from each other and having a length of 5 mm. A test piece. Further, the supporting jigs 131 and 132 support the bottom surface of the joined test piece, and the load is applied in the direction of the arrow A in the direction of the square arrow A on the upper surface side and the succeeding portion of the joined test piece by the pressing jig 14 . Point bending test.

The three-point bending test measures the load when the two glass plates are separated or the test piece is broken by measuring the peeling of the succeeding portion. Further, the measured value is the bonding strength of the bonding composition to be used.

The load evaluation test machine used MODEL-1308 manufactured by Aikoh Engineering Co., Ltd.

Here, the procedure for producing the test piece shown in Fig. 1 will be described with reference to Fig. 2 .

As shown in Fig. 2(A), two sheets of soda lime glass substrates 111 and 112 each having a thickness of 5 mm, a length of 30 mm, and a width of 30 mm were prepared. Then, the bonding composition prepared in each of the examples and the comparative examples was heated to 300 ° C by a soldering iron 22 and applied to a bonding portion (length 5 mm × width 30 mm) provided along one side of the soda lime glass substrates 111 and 112. The bonding composition portions 211 and 212 are formed.

Thereafter, each of the soda lime glass substrates 111 and 112 and the applied bonding composition are cooled to the extent that the bonding composition does not flow, specifically, even the front side of the soda lime glass substrates 111 and 112 When the back surface is reversed, the composition for bonding does not flow to the extent that it solidifies. Further, at this time, the bonding composition was cooled to 160 ° C or lower.

Next, as shown in FIG. 2(B), the front surface and the back surface of the soda lime glass substrate 111 are reversed, and the bonding composition portions 211 and 212 which are applied to the succeeding portions of the soda lime glass substrates 111 and 112 are formed in contact with each other. . The soda lime glass substrates 111 and 112 were heated to 300 ° C in this state.

After heating, the soda lime glass substrate and the bonding composition were cooled, and the bonding composition was solidified to prepare a test piece shown in Fig. 1 .

In addition, there is a test piece in which the bonding composition portions 211 and 212 which are applied to the succeeding portions of the soda lime glass substrates 111 and 112 are brought into contact with each other and heated, and applied to each of the soda lime glass substrates. The bonding composition portions 211 and 212 are also not integrated. This is because an extremely thin oxide film is formed on the surfaces of the bonding composition portions 211 and 212. In the examples and the comparative examples 1 and 3, the soldering iron 23 was inserted between the bonding composition portions formed on each of the soda lime glass substrates 111 and 112, as shown in Fig. 2(C). By the slight contact, the oxide film formed on the surfaces of the bonding composition portions 211 and 212 can be easily broken, and the integrated bonding composition portion 12 can be obtained. However, in Comparative Examples 2, 4, and 5, even if the bonding composition portions 211 and 212 which are applied to the succeeding portions of the soda lime glass substrates 111 and 112 are brought into contact with each other, heated, and the soldering iron is brought into contact, coating is performed. The bonding composition portions 211 and 212 formed on each of the soda lime glass substrates are not joined but are not integrated. The reason for this is presumed to be that a strong oxide film which cannot be destroyed by a soldering iron having only a heating function which does not have an ultrasonic shock function is formed on the surface of the bonding composition portions 211 and 212.

(air tightness test)

The method of the airtightness test will be described using FIG. Fig. 3 is a perspective view showing a test piece of a gas tightness test (leak test).

Soda-lime glass substrates 31 and 33 having a thickness of 5 mm × a length of 50 mm × 50 mm were prepared. Further, the monosodium calcium glass substrate 33 is formed in advance at a central portion of 3 mm. Hole 331. Then, the bonding composition prepared in each of the examples and the comparative examples was applied to a soda lime glass substrate so as to have a width of about 2 mm along the periphery of one of the soda lime glass substrates 31 and 33, that is, the four sides. It was heated and coated by a soldering iron so as to become 300 °C.

Then, the soda lime glass substrate and the applied bonding composition are cooled, and the bonding composition does not flow, specifically, the front and back sides of the soda lime glass substrates 31 and 33 are reversed. In this case, the composition for bonding does not flow to the extent that it solidifies. Further, at this time, the bonding composition was cooled to 160 ° C or lower.

Next, the soda-lime glass substrates 31 and 33 are superposed so that the surfaces on which the bonding composition is applied face each other. At this time, the bonding compositions applied to the respective soda lime glass substrates are placed in contact with each other. Then, the soda lime glass substrates 31 and 33 were heated to 300 ° C to be joined. Thereafter, the test piece is joined to the soda-lime glass substrate 31 and the soda-lime glass substrate 33 by the bonding composition portion 32 formed of the bonding composition as shown in FIG.

Further, since a stainless steel sheet having a thickness of 0.35 mm was provided as a spacer between the soda lime glass substrate 31 and the soda lime glass substrate 33, the test piece was a container having a space of 0.35 mm in height.

Moreover, even if the soda lime glass substrate is superimposed and heated, the bonding composition applied to each of the soda lime glass substrates is not integrated, and the soldering iron can be inserted between the bonding compositions. The way it is lightly contacted and integrated. However, in the comparative example In 2, 4, and 5, when the soda-lime glass substrates were superposed and the bonding compositions were joined to each other, even if the soldering irons were brought into contact, they could not be joined in the same manner as in the case of the three-point bending test.

Then, with respect to the obtained container, a leak detector (HELIOT 700 manufactured by ULVAC Co., Ltd.) was used, and the space was vacuum-degassed, and helium gas (He) was blown to each of the joint portions, and the amount of leakage was measured.

It was judged to be acceptable when the measured leak amount was 1.0 × 10 ^-11 (Pa ‧ m ³ /s) or less. Further, when the measured leak amount exceeded 1.0 × 10 ^-11 (Pa ‧ m ³ /s), it was judged to be unacceptable. In addition, the qualified expression in Table 1 is ○, and the unqualified expression is ×.

(Measurement of oxygen content in the composition for bonding)

The oxygen content contained in the bonding compositions of Examples 1 to 4, Example 8, Example 16, and Example 25 was measured in the following order (1) to (3).

(1) 0.5 g of a small piece of the composition for bonding prepared was prepared as a sample for analysis.

(2) Chemical etching is performed in order to eliminate the influence of the oxide film contained on the surface of the small piece of the bonding composition prepared in (1).

Specifically, a small piece containing the bonding composition and a beaker diluted with twice the hydrochloric acid were placed in a water bath and heated at 80 ° C for 12 minutes. Thereafter, decantation was carried out using deaerated water, followed by decantation using ethanol.

(3) The oxygen concentration was measured for the sample of the bonding composition after the oxide film was removed in (2). The measurement was carried out using an oxygen-hydrogen analyzer (Model: ROH-600, manufactured by LECO Corporation).

Hereinafter, the bonding compositions of the respective examples and comparative examples will be described.

[Example 1]

Sn, Ag, and Ir were weighed and mixed so that each component contained in the composition for bonding was a composition of Table 1, and then melted, and then poured into a mold to prepare a bonding composition.

Then, the bonding strength test was carried out on the bonding composition to be produced. Air tightness test and determination of oxygen content. The results are shown in Table 1.

In addition, the content of Sn in Table 1 is described as "the rest", and the content obtained by subtracting the content of the components other than Sn shown in Table 1 from 100% by mass is the content of Sn. The same applies to the examples and comparative examples other than the first embodiment.

[Example 2 to Example 25]

In the case of producing the composition for bonding, each of the components shown in Table 1 was weighed and mixed so as to have the composition of Table 1, and the same components as in Example 1 were used. The composition for bonding was prepared and evaluated. Further, the measurement of the oxygen content in the bonding composition was also carried out for Examples 2 to 4, Example 8, Example 16, and Example 25.

The evaluation results are shown in Table 1.

[Comparative Example 1 to Comparative Example 5]

In the case of the production of the composition for the bonding, the composition for bonding was prepared and evaluated in the same manner as in Example 1 except that the respective components were weighed and mixed in the composition of Table 1.

The results are shown in Table 1.

According to the results shown in Table 1, it was confirmed that the contents of Examples 1 to 25 containing Sn, Ag, and Ir and containing Sn as a main component and the content of Ag being 0.5% by mass or more and 11.0% by mass or less were not Comparative Examples 1 to 5 having 0.5% by mass or more or 11% of Ir showed no high bonding strength. In particular, in Comparative Examples 2, 4 and 5, a strong oxide film was formed on the surface of the composition for bonding. Therefore, as described above, in the case of producing a test piece, a soldering iron having only a heating function which does not have an ultrasonic shock function is used, and an oxide film formed on the surface is attempted to be broken, but it is not even possible to bond, and a sample cannot be produced.

According to the bonding strength of the bonding compositions of Examples 1 to 25 and the bonding strength of the bonding compositions of Comparative Examples 1 to 5, the bonding compositions of Examples 1 to 25 were confirmed. Among them, the bonding strength can be improved by containing Sn, Ag, and Ir.

Further, according to the airtight test results of the first embodiment, the second embodiment, and the third to the second embodiments, it was confirmed that the content of Ag was 1.5% by mass or more, and the joint strength was improved. Air tightness.

Further, in the evaluation of the oxygen content in the composition for bonding, the results of Example 1 were 0.0004% by mass, the Example 2 was 0.0077% by mass, the Example 3 was 0.0224% by mass, and the Example 4 was 0.0073% by mass. Example 8 The content was 0.0006 mass%, the amount of the example 16 was 0.0003 mass%, and the example 25 was 0.0009 mass%, and the content of oxygen was 0.0001 mass% or more. In addition, the joint strength was confirmed to be sufficiently higher than the values of Comparative Example 1 to Comparative Example 5.

Although the bonding composition has been described in the embodiment and the examples, the present invention is not limited to the above-described embodiments and examples. Various changes and modifications can be made without departing from the spirit and scope of the invention.

This application claims the priority of Japanese Patent Application No. 2015-020550, filed on February 4, 2015, to the Japan Patent Office, and the entire contents of Japanese Patent Application No. 2015-020550 is incorporated into this International Application. .

12‧‧‧Combination Composition Department

14‧‧‧ Pressing fixture

111, 112‧‧‧ Soda-lime glass substrate

131, 132‧‧‧ Support fixtures

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Claims (7)

A composition for bonding containing tin, silver, and antimony, and containing tin as a main component and containing 0.5% by mass or more and 11.0% by mass or less of the above silver. The composition for bonding according to claim 1, which contains 0.001% by mass or more and 1.0% by mass or less of the above hydrazine. The bonding composition according to claim 1 or 2, which contains 0.001% by mass or more and 0.8% by mass or less of aluminum. The bonding composition according to any one of claims 1 to 3, which contains 0% by mass or more and 1.0% by mass or less of yttrium, 0% by mass or more and 1.0% by mass or less of nickel, 0% by mass or more and 0.1% by mass. The following copper, 0% by mass or more and 0.5% by mass or less of magnesium. The bonding composition according to any one of claims 1 to 4, wherein the content of oxygen is 0.0001% by mass or more and 2% by mass or less. The bonding composition according to any one of claims 1 to 5, which is used when joining the material to be joined in which the bonding portion contains an oxide. The bonding composition according to claim 6, wherein the oxide is one or more selected from the group consisting of glass, chromium oxide, and aluminum oxide.