JP6381738B1 - Paste-like metal particle composition, bonding method, and electronic device manufacturing method - Google Patents

Abstract

Disclosed is a paste-like metal particle composition that becomes a sintered product having excellent adhesive strength after a thermal cycle test when heated between metal members, a method for firmly joining metal members, a semiconductor element, a lead frame, or a circuit Provided is a method for manufacturing an electronic device in which a substrate is firmly bonded. SOLUTION: Heat-sinterable metal particles having an average particle size of 0.01 to 10 μm, surface-coated with a non-powdered fatty acid, a polymer dispersant or an organic amine, a volatile dispersion medium, and a powdered fatty acid A paste-like metal particle composition in which the metal particles sinter when heated at 100 ° C. to 300 ° C., and metal members by heating and sintering the paste-like metal particle composition between metal members And a method of manufacturing an electronic device in which the paste-like metal particle composition is interposed between a semiconductor element and a lead frame or a circuit board, and the semiconductor element and the lead frame or the circuit board are bonded by heating and sintering. . [Selection] Figure 2

Description

The present invention relates to a paste-like metal particle composition, a bonding method, and a method for manufacturing an electronic device. Specifically, it is a paste-like metal particle composition comprising sinterable metal particles surface-coated with a surface coating agent, a dispersion medium, and a fatty acid powdered at 25 ° C., and the coating agent, the dispersion medium and the Fatty acid is volatilized or decomposed, and the sinterable metal particles are sintered to form a solid metal having voids, and a metal using the paste-like metal particle composition The present invention relates to a method for joining manufactured members and a method for manufacturing an electronic device in which a semiconductor element and a lead frame or a wiring substrate are joined by the paste-like metal particle composition.

Conductive pastes and heat conductive pastes prepared by dispersing fine particles of metal such as silver, copper and nickel in a curable resin composition are cured by heating to form conductive films and heat conductive films. Since it is formed, the formation of conductive circuits on printed circuit boards, the formation of various electronic components such as resistors and capacitors and the electrodes of various display elements, the formation of conductive films for electromagnetic wave shielding, capacitors, resistors, diodes, and memories Bonding and adhesion of chip components such as arithmetic elements (CPU) to substrates, formation of solar cell electrodes, especially solar cell electrodes that cannot be processed at high temperature using amorphous silicon semiconductors, multilayer ceramic capacitors, multilayer ceramic inductors, multilayers Application to the formation of external electrodes of chip-type ceramic electronic components such as ceramic actuators is known (Patent Document 1: Japanese Patent Laid-Open No. 2004-260688). 003-55701).

However, the conductive film and the heat conductive film are composed of metal particles and a cured resin, and the cured resin is electrically insulating and has low thermal conductivity, so there is a limit to the size of the conductivity and thermal conductivity. .
In recent years, due to higher performance of chip parts, the amount of heat generated from the chip parts has increased, and improvement in thermal conductivity as well as electrical conductivity is required.

In Patent Document 2 (WO2007 / 034833), a paste-like silver particle composition comprising a silver particle in which at least a part of the surface of silver is coated with a higher fatty acid or a derivative thereof and a volatile dispersion medium is made of a plurality of metals. A joining method characterized in that the volatile dispersion medium is volatilized by heating at a temperature of 100 ° C. or higher and 400 ° C. or lower, and the silver particles are sintered to join a plurality of metal members. And a joining method in which the plurality of metal members are electrodes on a metal-based substrate or an electrically insulating substrate and a metal portion of an electronic component or an electrical component.
However, depending on the material of the metal member to be joined, there is a problem that the adhesive strength after the thermal cycle test is insufficient.

Patent Document 3 (Japanese Patent Application Laid-Open No. 2010-18832) includes (A) copper particles having an average particle size of more than 0.1 μm and 50 μm or less, and the amount of organic substances covering the surface is 5.0% by weight or less. And (B) a paste-like material comprising a volatile dispersion medium, which is heated at 70 ° C. or more and 400 ° C. or less in an oxidizing gas atmosphere containing oxygen gas, whereby the volatile dispersion medium is volatilized and copper. A bonding agent for a metal member, characterized in that the particles (A) are sintered to each other and have adhesiveness to a metal member that has been in contact during the sintering; The volatile dispersion medium (B) is volatilized and the copper particles (A) are sintered together by heating between 70 ° C. and 400 ° C. in an oxidizing gas atmosphere containing oxygen gas. A reducing gas atmosphere containing hydrogen gas after joining a plurality of metal members. Characterized by heating at 70 ° C. or higher 400 ° C. or less at method of producing a metal member assembly is disclosed. Examples of organic substances include high and medium fatty acids; high and medium fatty acid metal salts, high and medium fatty acid esters, high and medium fatty acid derivatives such as high and medium fatty acid amides; and high and medium alkylamines such as decylamine and dodecylamine. Has been.

However, depending on the material of the metal member to be joined, there is a problem that the adhesive strength after the thermal cycle test is insufficient.

JP 2003-55701 A WO2007 / 034833 JP 2010-18832 A

As a result of earnest research to develop a paste-like metal particle composition free from the above-mentioned problems, the present inventors have determined from sinterable metal particles surface-coated with a surface coating agent, a volatile dispersion medium, and a specific fatty acid powder. When the paste-like metal particle composition is interposed between metal members to be joined and heated to sinter the sinterable metal particles, the adhesive strength, particularly the adhesive strength after the thermal cycle test, is excellent. As a result, the present invention has been reached.

An object of the present invention is to paste metal particles having excellent adhesion strength, particularly adhesion strength after a thermal cycle test, when the sintered metal particles are sintered by being interposed between metal members to be joined and heated. Providing a bonding method with excellent adhesion strength, particularly after thermal cycle testing, by providing the composition and heating and sintering the paste-like metal particle composition between metal members Another object of the present invention is to provide a highly reliable electronic device manufacturing method in which a semiconductor element and a lead frame or a circuit board are firmly bonded.

This purpose is
[1] (A) The average particle size coated with a coating agent selected from the group consisting of solid, semi-solid or liquid fatty acids, polymer dispersants and organic amines at 25 ° C. is 0.01 to 10 μm. Sinterable metal particles which are
(B) a volatile dispersion medium;
(C) A paste-like metal particle composition comprising a fatty acid powdered at 25 ° C.
[2] Fatty acid (C) in powder form at 25 ° C. is a saturated fatty acid having 10 to 22 carbon atoms that has passed through a sieve having an opening of 150 μm, and 100 parts by mass of the sinterable metal particles (A) The paste-like metal particle composition according to [1], which is 0.01 to 5 parts by mass.
[3] The paste-like metal particle composition according to [1] or [2], wherein the material of the sinterable metal particles (A) is gold, silver, copper, platinum, palladium, or an alloy thereof.
[4] The volume resistivity of the heat-sintered material at 100 ° C. or higher and 300 ° C. or lower of the paste-like metal particle composition is 1 × 10 ⁻⁵ Ω · cm or less and the thermal conductivity is 100 W / m · The paste-like metal particle composition according to [1], [2] or [3], which is K or more.

[5] (A) The average particle size of the surface coated with a coating agent selected from the group consisting of solid, semi-solid or liquid fatty acids, polymer dispersants and organic amines at 25 ° C. is 0.01 to 10 μm. Sinterable metal particles which are
(B) a volatile dispersion medium;
(C) A paste-like metal particle composition comprising a powdered fatty acid at 25 ° C.
By interposing between the metal member (D1) and the metal member (D2) and heating at 100 ° C. or more and 300 ° C. or less, the sintered product of the sinterable metal particles (A) is made of metal. The joining method characterized by joining a member (D1) and metal members (D2).
[6] Powdered fatty acid (C) at 25 ° C. is a saturated fatty acid having 10 to 22 carbon atoms that has passed through a sieve having an opening of 150 μm, and 100 parts by mass of the sinterable metal particles (A) The bonding method according to [5], which is 0.01 to 5 parts by mass.
[7] The joining method according to [5] or [6], wherein the material of the sinterable metal particles (A) is gold, silver, copper, platinum, palladium, or an alloy thereof.
[8] The material of the metal member (D1) is gold, silver, copper, platinum, palladium or an alloy thereof, and the material of the metal member (D2) is gold or an alloy of gold, [5] , [6] or [7].
[9] The metal member (D1) is a metal part of a lead frame or a circuit board, and the metal member (D2) is a metal part of a semiconductor element, according to any one of [5] to [8] Joining method.
[10] The volume resistivity of the sintered product between the sinterable metal particles (A) is 1 × 10 ⁻⁵ Ω · cm or less, and the thermal conductivity is 100 W / m · K or more. 5. The joining method according to any one of [9].

[11] (A) Sinterability having an average particle size of 0.01 to 10 μm coated with a coating selected from the group consisting of non-powdered fatty acids, polymer dispersants and organic amines at 25 ° C. Metal particles,
(B) a volatile dispersion medium;
(C) A paste-like metal particle composition consisting of a fatty acid powdered at 25 ° C. is interposed between a metal part of a semiconductor element and a circuit board having a lead frame or metal part, and then 100 ° C. or more and 300 ° C. or less. A method of manufacturing an electronic device comprising: joining a metal part of a semiconductor element and a metal part of a lead frame or a circuit board as a sintered product of the sinterable metal particles (A) by heating at .
[12] Fatty acid (C) in powder form at 25 ° C. is a saturated fatty acid having 10 to 22 carbon atoms that has passed through a sieve having an opening of 150 μm, and is 100 parts by mass of sinterable metal particles (A). The manufacturing method of the electronic device as described in [11] which is 0.01-5 mass parts.
[13] The method for manufacturing an electronic device according to [11] or [12], wherein the material of the sinterable metal particles (A) is gold, silver, copper, platinum, palladium, or an alloy thereof.
[14] The material of the metal part of the lead frame or the circuit board is gold, silver, copper, platinum, palladium, or an alloy thereof, and the material of the metal part of the semiconductor element is gold or an alloy of gold, [11] A method for manufacturing an electronic device according to [12] or [13].
[15] The volume resistivity of the sintered product of the sinterable metal particles (A) is 1 × 10 ⁻⁵ Ω · cm or less, and the thermal conductivity is 100 W / m · K or more. [11] The method for manufacturing an electronic device according to any one of [14]. Achieved by;

In the paste-like metal particle composition defined in claim 1 of the present invention, the volatile dispersion medium and the fatty acid are volatilized or volatilized by volatilization or decomposition, and the sinterable metal particles (A) are sintered to each other by heating. It becomes a solid metal having excellent adhesion strength to a manufactured member, in particular, adhesion strength after a thermal cycle test.

[11] (A) The average particle size coated with a coating agent selected from the group consisting of solid, semi-solid or liquid fatty acids, polymer dispersants and organic amines at 25 ° C. is 0.01 to 10 μm. Sinterable metal particles which are
(B) a volatile dispersion medium;
(C) A paste-like metal particle composition consisting of a fatty acid powdered at 25 ° C. is interposed between a metal part of a semiconductor element and a circuit board having a lead frame or metal part, and then 100 ° C. or more and 300 ° C. or less. A method of manufacturing an electronic device comprising: joining a metal part of a semiconductor element and a metal part of a lead frame or a circuit board as a sintered product of the sinterable metal particles (A) by heating at .
[12] Fatty acid (C) in powder form at 25 ° C. is a saturated fatty acid having 10 to 22 carbon atoms that has passed through a sieve having an opening of 150 μm, and is 100 parts by mass of sinterable metal particles (A). The manufacturing method of the electronic device as described in [11] which is 0.01-5 mass parts.
[13] The method for manufacturing an electronic device according to [11] or [12], wherein the material of the sinterable metal particles (A) is gold, silver, copper, platinum, palladium, or an alloy thereof.
[14] The material of the metal part of the lead frame or the circuit board is gold, silver, copper, platinum, palladium, or an alloy thereof, and the material of the metal part of the semiconductor element is gold or an alloy of gold, [11] A method for manufacturing an electronic device according to [12] or [13].
[15] The volume resistivity of the sintered product of the sinterable metal particles (A) is 1 × 10 ⁻⁵ Ω · cm or less, and the thermal conductivity is 100 W / m · K or more. [11] The method for manufacturing an electronic device according to any one of [14]. Achieved by;

According to the method for manufacturing an electronic device defined in claim 11 of the present invention, the semiconductor element and the lead frame or the circuit board are firmly bonded, and the adhesive strength after the thermal cycle test is excellent, so that the electronic device has high reliability. Can be manufactured.

It is a top view about the test body for bonding strength measurement in an Example. It is sectional drawing in the XX line of the test body shown in FIG.

The paste-like metal particle composition of the present invention is (A) an average surface-coated with a coating agent selected from the group consisting of solid, semi-solid or liquid fatty acids, polymer dispersants and organic amines at 25 ° C. Sinterable metal particles having a particle size of 0.01 to 10 μm;
(B) a volatile dispersion medium;
(C) It consists of a fatty acid powdered at 25 degreeC. When this paste-like metal particle composition is heated at 100 ° C. or more and 300 ° C. or less, the volatile dispersion medium (B) and the powdered fatty acid (C) are volatilized or volatilized at 25 ° C., and the sinterable metal A sintered product of the particles (A), that is, a solid metal having voids.

(A) fatty acid which is solid, semi-solid or liquid at 25 ° C., (b) a polymeric dispersant having an acidic functional group and / or a basic functional group, and (c) a coating selected from the group consisting of organic amines The sinterable metal particles (A) having an average particle size of 0.01 to 10 μm whose surface is coated with an agent are not limited as long as they are metal particles having heat sinterability, but are preferable in terms of heat sinterability. Is selected from silver, gold, copper, platinum and palladium particles, more preferably silver particles. These metal alloy particles or other metal particles whose surfaces are coated with these metals may be used, or two or more kinds of these metal particles may be used in combination.

The sinterable metal particles (A) are preferably produced by a reduction method of a metal salt (wherein the metal is preferably selected from the group consisting of silver, copper, gold, platinum and palladium). is there. For example, in the case of silver particles, the reduction method usually involves mixing and reacting an aqueous silver nitrate solution and aqueous ammonia to obtain an aqueous silver ammine complex solution, which is then contacted with an aqueous solution of hydroquinone, anhydrous potassium sulfite or ammonium and gelatin. An example is a method in which silver powder is reduced and precipitated, filtered, the residue is washed with water, and dried by heating. Alternatively, silver nitrate aqueous solution and aqueous ammonia are mixed and reacted to obtain a silver ammine complex aqueous solution, which is contacted with an organic reducing agent (hydroquinone, ascorbic acid, glucose, etc.), particularly hydroquinone aqueous solution, to reduce silver powder. Examples are methods of precipitation, filtration, washing and drying.

The filtration residue contains ammonia, hydroquinone, anhydrous potassium sulfite or ammonium, and gelatin. Since ammonia, hydroquinone, anhydrous potassium sulfite, ammonium, and gelatin adhere to the silver particle surface, it is usually washed repeatedly with clean water. Thus, sinterable metal particles having an average particle diameter of preferably 0.01 to 10 μm can be obtained. Alternatively, the filtration residue contains ammonia and an organic reducing agent, particularly hydroquinone, and ammonia and an organic reducing agent, particularly hydroquinone, are attached to the surface of the silver particles, so it is usually repeatedly washed with clean water and methanol. Thus, sinterable metal particles having an average particle diameter of preferably 0.01 to 10 μm can be obtained.

When the metal of the metal particles is selected from the group consisting of copper, gold, platinum and palladium, sinterable metal particles are produced by a similar method using a metal nitrate, a metal sulfate, etc. Can do.

The sinterable metal particles (A) thus produced, particularly the sinterable silver particles, are usually spherical or granular.
The flaky sinterable silver particles (A) can be easily produced by physically hitting the silver particles with a rotary drum device such as a ball mill together with the ceramic sinterable silver particles. At this time, in order to reduce or prevent the aggregation of silver particles, a trace amount of higher fatty acid having 10 or more carbon atoms, metal salt of higher fatty acid, higher fatty acid ester, etc. may be added.

The average particle size of the sinterable metal particles (A) is a volume-based integrated fraction 50% value of the particle size distribution measured using a laser diffraction / scattering particle size distribution measuring device, that is, the median diameter (D50 value). is there.
If the average particle diameter of the sinterable metal particles (A) exceeds 10 μm, the sinterability between the sinterable metal particles (A) may be reduced, so that the sinterable metal particles (A) are 10 μm or less and 5 μm or less. preferable. In addition, when it is less than 0.01 μm, the surface activity is too strong and the storage stability of the paste-like metal particle composition may be lowered, so that it is 0.01 μm or more, and preferably 0.1 μm or more.

The shape of the sinterable metal particles (A) in the paste-like metal particle composition of the present invention is not limited, and is spherical, granular, flakes (pieces), needles, squares, dendritics, irregular shapes, tears Examples include drops, plates, ultrathin plates, hexagonal plates, columns, rods, porous, fibers, lump, spongy, kernel, round, etc. Preferably there is. For example, the classification described in JIS Z 2500 can be used as the shape.

Two or more kinds of these sinterable metal particles (A) may be used in combination.
As a combination example, a combination of granular silver particles and spherical silver particles (for example, a combination of granular silver particles having a small average particle diameter and spherical silver particles having a large average particle diameter, a spherical silver particle having a small average particle diameter and an average Combined use of granular silver particles having a large particle size), combined use of silver particles having a small average particle size and silver particles having a large average particle size (for example, spherical silver particles having a small average particle size and spherical silver particles having a large average particle size) And a combination of a spherical silver particle having a small average particle diameter and a granular silver particle having a large average particle diameter), and a spherical or granular copper particle.
The blending ratio is not limited, but the former and the latter are preferably in the mass ratio of 5:95 to 90:10 in terms of the adhesion strength to the metal member, particularly the adhesion strength after the thermal cycle test. 8:92 to 70:30 is more preferable.

In order to prevent aggregation of the sinterable metal particles (A), at least a part of the surface of the sinterable metal particles (A) is preferably coated with a specific organic substance. Examples of such organic substances include (a) a non-powdered fatty acid at 25 ° C., (b) a polymer dispersant having an acidic functional group and / or a basic functional group, and (c) an organic amine.
The non-powdered fatty acid (a) at 25 ° C. is solid, semi-solid or liquid at 25 ° C., but is not powdery.

The solid, semi-solid or liquid fatty acid (a) at 25 ° C. is usually added during the production process of the sinterable metal particles (A), for example, by the reduction method. Thus, since the sinterable metal particles (A) are completed by repeatedly washing with clean water and methanol, for example, the fatty acid simply attached to the surface of the sinterable metal particles (A) is removed. However, only those that adhere firmly to the surface or associate with the surface remain. Therefore, in mixing in producing the paste-like metal particle composition of the present invention, the paste-like metal particle composition of the present invention is not easily detached from the surface of the sinterable metal particles (A). It is clearly different from the fatty acid (C) powdered at 25 ° C. intentionally added.

As fatty acid (a) solid, semi-solid or liquid at 25 ° C., pentanoic acid (valeric acid), hexanoic acid (caproic acid), heptanoic acid (enanthic acid), octanoic acid (having 5 or more carbon atoms) Caprylic acid), nonanoic acid (pelargonic acid), decanoic acid (capric acid), dodecanoic acid (lauric acid), tetradecanoic acid (myristic acid), pentadecanoic acid, hexadecanoic acid (palmitic acid), heptadecanoic acid (margaric acid), octadecane Acid (stearic acid), 12-hydroxyoctadecanoic acid (12-hydroxyoleic acid), eicosanoic acid (arachidic acid), docosanoic acid (behenic acid), tetracosanoic acid (lignoceric acid), hexacosanoic acid (serotic acid), octacosanoic acid ( Monovalent linear saturated fatty acids such as montanic acid; 2-pens having 14 or more carbon atoms Monovalent branched saturated fatty acids such as lunananoic acid, 2-hexyldecanoic acid, 2-heptyldodecanoic acid and isooleic acid; palmitoleic acid, oleic acid, isooleic acid, elaidic acid, linoleic acid, linolenic acid, ricinoleic acid, gadrenic acid, Examples thereof include monovalent unsaturated fatty acids such as erucic acid and cerakoleic acid.

Oxalic acid, malonic acid, succinic acid, maleic acid, fumaric acid, oxydiacetic acid (diglycolic acid), glutaric acid, adipic acid, pimelic acid, speric acid, azelaic acid, sebacic acid having 2 or more carbon atoms Polyhydric aliphatic carboxylic acids such as phthalic acid, isophthalic acid and terephthalic acid may be used in combination with the non-powdered fatty acid (a) at 25 ° C.
A preferable blending amount of the polyvalent aliphatic carboxylic acid or the polyvalent aromatic carboxylic acid is 10% by mass or less of the non-powdered fatty acid (a) at 25 ° C.

In addition, you may use together the alkali metal salt of fatty acid, and the ester of fatty acid with non-powdered fatty acid (a) at 25 degreeC. Examples of the alkali metal salt of fatty acid include sodium salt, potassium salt and lithium salt of fatty acid. Examples of fatty acid esters include fatty acid alkyl esters (for example, methyl esters and ethyl esters) and fatty acid phenyl esters. The alkyl group of these alkyl esters preferably has 1 to 6 carbon atoms.
A preferable blending amount is 10% by mass or less of the non-powdered fatty acid (a) at 25 ° C.

(B) The polymer dispersant having an acidic functional group and / or a basic functional group usually has a weight average molecular weight of 1,000 or more. The weight average molecular weight (Mw) is a polystyrene equivalent weight average molecular weight measured by gel permeation chromatography (carrier: tetrahydrofuran).

Examples of the acidic functional group include a carboxyl group, an acid anhydride group, a sulfo group (sometimes referred to as a sulfonic acid group), a thiol group, a phosphoric acid group, an acidic phosphoric acid ester group, and a phosphonic acid group. A carboxyl group, a phosphate group or an acidic phosphate group is preferred. The acidic phosphate group is one in which a part of the phosphorus-bonded hydroxyl group is alkoxylated. Examples of the alkoxy group include lower alkoxy groups such as a methoxy group, an ethoxy group, and a propoxy group. The number of carbon atoms of the lower alkoxy group is preferably 1-8.
Examples of the basic functional group include an amino group, an imino group (= NH), an ammonium base, and a heterocyclic group having a basic nitrogen atom, but an amino group, an ammonium base (for example, a tertiary ammonium base, A quaternary ammonium base). The amino group may be any of a primary amino group (—NH ₂ ), a secondary amino group (—NHR), and a tertiary amino group (—NRR ′). R and R ′ are an alkyl group, a phenyl group, an aralkyl group and the like, and preferably have 1 to 8 carbon atoms.

The acid value of the polymer dispersant having an acidic functional group and / or a basic functional group is preferably 5 to 300 mgKOH / g, and more preferably 10 to 200 mgKOH / g. Further, the amine value of the polymer dispersant is preferably 5 to 300 mgKOH / g, more preferably 10 to 200 mgKOH / g.
The acid value represents the acid value per 1 g of the solid content of the polymer dispersant, and can be determined by potentiometric titration according to JIS K 0070. The amine value represents the amine value per gram of the polymer dispersant solid content, and is a value converted to an equivalent of potassium hydroxide after being obtained by potentiometric titration using a 0.1N hydrochloric acid aqueous solution.

As a polymer dispersant having a commercially available acidic functional group and / or basic functional group, SOLSPERSE24000 (acid value: 24 mgKOH / g, amine value: 47 mgKOH / g), SOLSPERSE32000 (acid value: 15 mgKOH / g, amine value: 180 mgKOH) / G) (manufactured by Lubrizol, Ltd.) (SOLSPERSE is a registered trademark of Lyubrizol Limited).

DISPERBYK-106 (acid value: 132 mgKOH / g, amine value: 74 mgKOH / g), DISPERBYK-130 (acid value: 2 mgKOH / g, amine value: 190 mgKOH / g), DISPERBYK-140 (acid value: 73 mgKOH / g) , Amine value: 76 mgKOH / g), DISPERBYK-142 (acid value: 46 mgKOH / g, amine value: 43 mgKOH / g), DISPERBYK-145 (acid value: 76 mgKOH / g, amine value: 71 mgKOH / g), DISPERBYK-180 (Acid value: 94 mgKOH / g, amine value: 94 mgKOH / g), DISPERBYK-187 (acid value: 35 mgKOH / g, amine value: 35 mgKOH / g), DISPERBYK-191 (acid value: 30 mgKOH / g, amine value: 20 mgKOH) / G), DISPERBYK-2001 (acid value: 19 mgKOH / g, amine value: 29 mgKOH / g), DISPERBYK-2010 (acid value: 20 mgKOH / g, a DISPERBYK-2020 (acid value: 37 mgKOH / g, amine value: 36 mgKOH / g), DISPERBYK-2020N (acid value: 36 mgKOH / g, amine value: 36 mgKOH / g), DISPERBYK-2025 ( Acid value: 38 mgKOH / g, amine value: 37 mgKOH / g), DISPERBYK-102 (acid value: 101 mgKOH / g), DISPERBYK-174 (acid value: 22 mgKOH / g), DISPERBYK-2096 (acid value: 40 mgKOH / g) , DISPERBYK-2150 (amine value: 57 mgKOH / g), etc. Disperbic series products [BIC Chemie Japan Co., Ltd. sales] (DISPERBYK is a registered trademark of Bik-Hemi Geselsyaft Mitto Beschlenktel Huffung) .

Further, BYK-9076 (acid value: 38 mgKOH / g, amine value: 44 mgKOH / g), BYK-9077 (amine value: 48 mgKOH / g), ANTI-TERRA-U (acid value: 24 mgKOH / g, amine value: 19 mgKOH) / G), ANTI-TERRA-U100 (acid value: 50 mgKOH / g, amine value: 35 mgKOH / g), ANTI-TERRA-204 (acid value: 41 mgKOH / g, amine value: 37 mgKOH / g), ANTI-TERRA- Bic series products such as 205 (acid value: 40 mg KOH / g, amine value: 37 mg KOH / g), ANTI-TERRA-250 (acid value: 46 mg KOH / g, amine value: 41 mg KOH / g), anti-terra series products [Bic Chemie ・Products sold by Japan Co., Ltd.] (BYK and ANTI-TERRA are registered trademarks of Beik-Hemmy Geselsyaft Mits Beschlenktel Huffung).

Disparon series products such as Dispalon DA-234 (acid value: 16 mg KOH / g, amine value: 20 mg KOH / g), Disparon DA-325 (acid value: 14 mg KOH / g, amine value: 20 mg KOH / g) [Enomoto Kasei Disparon is a registered trademark of Enomoto Kasei Co., Ltd.); Azisper PB-821 (acid value: 17 mg KOH / g, amine value: 10 mg KOH / g), Azisper PB-822 (acid value: 14 mg KOH / g, Amine value: 17 mg KOH / g), Azisper PB-881 (acid value: 17 mg KOH / g, amine value: 17 mg KOH / g), Azisper PN-411 (acid value: 6 mg KOH / g, Azisper PA-111 (acid value: 35 mg KOH / g) g) Ajisper series products such as [Ajinomoto Fine Techno [Ajispur is a registered trademark of Ajinomoto Co., Inc.].

Examples of (c) organic amines include primary, secondary or tertiary alkylamines, alkylamidoamines, N-alkylethanolamines, N-alkylmorpholines, and other organic amine compounds.

Examples of primary, secondary or tertiary alkylamines include dipropylamine, dibutylamine, hexylamine, cyclohexylamine, heptylamine, octylamine, nonylamine, decylamine, dodecylamine and other alkyl monoamines, ethylenediamine, N, N- Dimethylethylenediamine, N, N′-dimethylethylenediamine, N, N-diethylethylenediamine, N, N′-diethylethylenediamine, 1,2-propanediamine, 1,3-propanediamine, 2,2-dimethyl-1,3- Propanediamine, N, N-dimethyl-1,3-diaminopropane, N, N′-dimethyl-1,3-diaminopropane, N, N-diethyl-1,3-diaminopropane, 1,4-diaminobutane, 1,5-diamino-2-methylpentane, , 6-diaminohexane, N, N'-dimethyl-1,6-diaminohexane, 1,7-diamino heptane, 1,8-alkyldiamine diamino octane, and the like. Examples include trialkylamines such as tripropylamine and tributylamine.

(A) a solid, semi-solid or liquid fatty acid at 25 ° C., (b) a polymer dispersant having an acidic functional group and / or a basic functional group, and (c) an organic amine (nitrogen-containing organic compound). The sinterability of the sinterable metal particles (A) having an average particle diameter of 0.01 to 10 μm and surface-coated with a coating agent selected from the group was the same manufacturer, the same production method, and the same production conditions. However, even if there is such lot fluctuation, stable sinterability can be obtained by adding the fatty acid (C) that is powdered at 25 ° C.

The paste-like metal particle composition of the present invention comprises (a) a solid, semi-solid or liquid fatty acid at 25 ° C., (b) a polymer dispersant having an acidic functional group and / or a basic functional group, (c) Organic amine (sinterable metal particles (A) having an average particle size of 0.01 to 10 μm and coated with a coating agent selected from the group consisting of nitrogen-containing organic compounds, volatile dispersion medium (B) and 25 It is a mixture comprising a fatty acid (C) that is powdered at 0 ° C., and the sinterable metal particles (A) and the fatty acid (C) that is powdered at 25 ° C. are made into a paste by the action of the volatile dispersion medium (B). By making it into a paste, it can be easily discharged from a needle or nozzle, and is particularly suitable for screen printing and printing application using a metal mask, although the thickness of the paste-like metal particle composition after printing is not limited, 2mm or more It is preferably 1 mm or less, more preferably 5 to 500 μm, and particularly preferably 20 to 200 μm.The volatile dispersion medium (B) is used instead of the non-volatile dispersion medium for heating. When the sinterable metal particles (A) are sintered by the above, if the dispersion medium is volatilized in advance, the sinterable metal particles (A) are easy to sinter. This is because conductivity and adhesiveness are improved.

Such a volatile dispersion medium (B) is preferably one that does not alter the surface of the sinterable metal particles (A), and its viscosity is not limited, but is preferably 0.1 to 1000 mP · s. More preferably, it is -500 mP * s. When the viscosity is less than 0.1 mP · s, the volatility becomes extremely high, making it difficult to prepare a paste-like metal particle composition, and (a) a non-powdered fatty acid at 25 ° C., (b) an acidic functional group and / or Or a polymer dispersant having a basic functional group, (c) a sinterable metal particle having a mean particle size of 0.01 to 10 μm and coated with a coating agent selected from the group consisting of organic amines (A) The sinterability between them may decrease.

As the volatile dispersion medium (B), water; water, ethyl alcohol, propyl alcohol, butyl alcohol, pentyl alcohol, hexyl alcohol, heptyl alcohol, octyl alcohol, nonyl alcohol, decyl alcohol, benzyl alcohol, cyclohexanol, terpineol, etc. Volatile polyhydric alcohols such as ethylene glycol, propylene glycol, hexanediol and octanediol; volatile aliphatic hydrocarbons such as lower n-paraffins and lower isoparaffins; volatile aromatic hydrocarbons such as toluene and xylene; Acetone, methyl ethyl ketone, methyl isobutyl ketone, cyclohexanone, diacetone alcohol (4-hydroxy-4-methyl-2-pentanone), 2-octanone, isophorone (3,5 Volatile ketones such as 5-trimethyl-2-cyclohexen-1-one) and dibutyl ketone (2,6-dimethyl-4-heptanone); volatile acetates such as ethyl acetate and butyl acetate; Volatile aliphatic carboxylic acid esters such as methyl butyrate, methyl hexanoate, methyl octoate, methyl decanoate; volatile ethers such as tetrahydrofuran, methyl cellosolve, propylene bricol monomethyl ether, methyl methoxybutanol, butyl carbitol; Volatile silicone oil and volatile organic modified silicone oil are exemplified, and polybutene, polyvinyl alcohol, polyethylene glycol, cyclohexanedimethanol (a mixture of cis and trans), bornylcyclohexanol, isobornyl Hexanol, bornyl phenol, isobornyl phenol is exemplified. Two or more kinds of volatile dispersion media (B) may be used in combination, and the compatibility of the volatile dispersion media is not limited.

Fatty acid (C) powdered at 25 ° C. contained in the paste-like metal particle composition of the present invention is a component that is intentionally used, and is a surface coating agent component originally contained in the sinterable metal particles (A). Are different. The powdered fatty acid (C) at 25 ° C. does not hinder the sintering of the sinterable metal particles (A) when the paste-like metal particle composition of the present invention is heated. When the paste-like metal particle composition is used for joining metal members, there is an effect of improving the joining strength. In particular, when the material of the metal member includes gold or a gold alloy, the effect is remarkable.

It goes without saying that the fatty acid (C) in powder form at 25 ° C. is in powder form even at less than 25 ° C. The powdered fatty acid (C) at 25 ° C. is heated by frictional heat during mixing with the sinterable metal particles (A) and the volatile dispersion medium (B) in a mixer. It is preferable that

The fatty acid (C) powdered at 25 ° C. is preferably a saturated fatty acid that is solid at 25 ° C., and is preferably a saturated fatty acid having 10 to 22 carbon atoms in the molecular formula. Examples of such fatty acid (C) include capric acid, lauric acid, myristic acid, pentadecylic acid, palmitic acid, margaric acid, stearic acid, tuberculostearic acid, aragdic acid, and behenic acid. More preferred are lauric acid, myristic acid, pentadecylic acid, palmitic acid, margaric acid and stearic acid.

The powdered fatty acid (C) at 25 ° C. is preferably in the form of a fine powder that has passed through a sieve having an opening of 150 μm because of dispersibility in the paste-like metal particle composition of the present invention. When the fatty acid (C) in powder form is fine at 25 ° C., the paste-like metal particle composition of the present invention can be easily and stably discharged from a needle or nozzle that is a fine discharge port, and screen printing, metal In the printing application with a mask, the flatness of the printed surface is excellent. In addition, even if it is a powdery fatty acid (C) whose mesh opening does not pass through 150 μm, it may be used as long as it is not contrary to the object of the present invention.

As the sieve having an opening of 150 μm, a commercially available one can be used. Examples of such sieves include those specified in JIS Z 8801, or those specified in ISO R40 / 3 series.

It is preferable that the compounding quantity of a powdered fatty acid (C) at 25 degreeC is 0.01-5 mass parts with respect to 100 mass parts of said sinterable metal particles (A). When the amount is less than 0.01 parts by mass, the effect of adding the fatty acid powder (C) at 25 ° C. is small. For this reason, it is more preferably 0.05 parts by mass or more, particularly 0.1 parts by mass. It is preferable that the amount exceeds. On the other hand, if it exceeds 5 parts by mass, the sinterability of the sinterable metal particles (A) may be hindered, so that it is preferably 3 parts by mass or less, and preferably 2.2 parts by mass or less. More preferred.

The state of the powdered fatty acid (C) at 25 ° C. in the paste-like metal particle composition of the present invention is the temperature of the paste-like metal particle composition, the solubility in the volatile dispersion medium (B), the fatty acid (C However, at 25 ° C., it is preferable that at least a part of the powdered fatty acid (C) exists at 25 ° C. in the form of powder. This presence can be easily confirmed visually or with an optical microscope.

The paste-like metal particle composition of the present invention has a solid volatile dispersion medium such as pyrogallol, p-methylbenzyl alcohol, o-methyl at 25 ° C. as long as the effect of the present invention is not adversely affected and the effect is not impaired. Alcohols such as benzyl alcohol, sil-3,3,5-trimethylcyclohexanol, 1,4-cyclohexanedimethanol, 1,4-cyclohexanediol, pinacol; hydrocarbons such as biphenyl, naphthalene, durene; dibenzoylmethane A small amount of ketones such as chalcone and acetylcyclohexane may be blended.

In addition, the paste-like metal particle composition of the present invention is powdered at 25 ° C. unless the sinterable metal particles (A), the volatile dispersion medium (B), and the effect of the present invention are impaired. A small amount of additives such as metal particles or non-metallic powders, metal oxides, metal compounds, metal complexes, thixotropic agents, stabilizers, sintering accelerators, etc., other than the fatty acid (C) in the form of a powder .

The paste-like metal particle composition of the present invention can be produced by mixing the sinterable metal particles (A), the volatile dispersion medium (B) and the powdered fatty acid (C) at 25 ° C. In order to improve the dispersibility of the powdered fatty acid (C) at 25 ° C. in the paste-like metal particle composition, the sinterable metal particles (A) and the volatile dispersion medium (B) were previously mixed to form a paste. Later, it is preferable to add and mix the powdered fatty acid (C) at 25 ° C. In this case, the mixing temperature is preferably not higher than the melting point of the powdered fatty acid (C) at 25 ° C. so that sintering between the sinterable metal particles (A) does not proceed, and is not higher than 30 ° C. It is more preferable.

When the paste-like metal particle composition of the present invention is heated at 100 ° C. or higher and 300 ° C. or lower, preferably 150 ° C. or higher and 250 ° C. or lower in an atmosphere described later, (a) a non-powdered fatty acid at 25 ° C., (b) Polymer dispersing agent having acidic functional group and / or basic functional group, (c) Sinterability having an average particle size of 0.01 to 10 μm coated with a coating selected from the group consisting of organic amines The surface coating agent of the metal particles (A), the volatile dispersion medium (B) and the powdered fatty acid (C) are volatilized or volatilized at 25 ° C., and the sinterable metal particles (A) are sintered together. Thus, it becomes a solid metal having voids.

The heating time is sufficient for the surface coating agent, the volatile dispersion medium (B), and the powdered fatty acid (C) to volatilize or decompose at 25 ° C., so that the sinterable metal particles (A) are sintered together. It's time. Although the time sufficient for sintering of the sinterable metal particles (A) varies depending on the type and particle size of the sinterable metal particles (A), the heating temperature, the atmosphere during heating, etc., it is difficult to specify. For example, 5 minutes to 3 hours. Of course, the time is not limited.

The paste-like metal particle composition of the present invention can be used as a bonding agent between a plurality of metal members. After the paste-like metal particle composition is applied to the metal member (D1) by spraying, screen printing or stencil printing, and the metal member (D2) is brought into close contact, it is 100 ° C. or higher and 300 ° C. or lower, preferably 150 ° C. By heating at 250 ° C. or lower, the volatile dispersion medium (B) and the fatty acid (C) in powder form at 25 ° C. are volatilized or decomposed and volatilized, and sintering between the sinterable metal particles (A) is performed. Thus, the metal member (D1) and the metal member (D2) can be firmly joined. Sinterable metal particles having an average particle diameter of 0.01 to 10 μm and coated with a coating agent selected from the group consisting of fatty acid (a), polymer dispersant (b) and organic amine (c) (A ), The surface coating agent of the sinterable metal particles (A) is preferably volatilized or decomposed to volatilize.

In the paste-like metal particle composition of the present invention, (a) a non-powdered fatty acid at 25 ° C., (b) a polymer dispersant having an acidic functional group and / or a basic functional group, (c) an organic amine (including Amount of surface coating agent of sinterable metal particles (A) having an average particle size of 0.01 to 10 μm and coated with a coating material selected from the group consisting of nitrogen organic compounds), volatile dispersion medium (B ) And the amount of fatty acid (C) powdered at 25 ° C. can be easily measured by thermogravimetric analysis (TGA) or the like. Many TGA devices are commercially available.

The metal member (D1) and the metal member (D2) may be the same or different in material, shape, size, surface treatment, etc., and such materials include gold, silver, copper, platinum, Palladium or an alloy thereof is exemplified, but gold, silver, or an alloy thereof is preferable. The metal member (D1) and the metal member (D2) are plated with gold, silver, copper, platinum, palladium, or an alloy thereof on the surface of a sheet or plate such as iron or nickel as a base material. It may be given. Examples of the shape of the metal member (D1) and the metal member (D2) include a sheet shape, a flat plate shape, a block shape, and a chip shape.

When the metal member (D1) is a metal part of a lead frame or a circuit board and the metal member (D2) is a metal part of a semiconductor element, the electronic device joined in this way is a lead frame or a circuit. Since the thermal conductivity, electrical conductivity, and adhesion strength of the bonding layer between the metal portion of the substrate and the metal portion of the semiconductor element are excellent, especially the adhesion strength after the thermal cycle test, the electronic device, particularly the semiconductor device There is an effect that the stability of characteristics is excellent.

Atmosphere in heating the paste-like metal particle composition of the present invention, the oxidizing gas containing air or oxygen, but reducing gas containing hydrogen gas is exemplified, preferably an oxidizing gas containing air or oxygen . If readily oxidizable copper particles or metal member (D1, D2) comprises copper, preferably a reducing gas containing hydrogen gas, also after the sintering of copper particles in an oxidizing gas, reducing gas You may reduce in.

(A) non-powdered fatty acid at 25 ° C., (b) polymer dispersant having acidic functional group and / or basic functional group, (c) coated with a coating selected from the group consisting of organic amines Sintered metal particles (A) having an average particle diameter of 0.01 to 10 μm are sintered, that is, a solid metal having voids is excellent in conductivity and thermal conductivity. ing. Specifically, the volume resistivity is preferably 1 × 10 ⁻⁵ Ω · cm or less, and the thermal conductivity is preferably 100 W / m · K or more.

As described above, the paste-like metal particle composition of the present invention has excellent conductivity and heat conductivity (heat dissipation) in the sintered product, and is excellent in the metal member that was in contact during sintering. It has excellent adhesion strength, especially after thermal cycle test, so it can be used for bonding and coating on metal parts of semiconductor elements, metal parts of chip parts, lead frames, electrodes on circuit boards, etc. It can be suitably used as an agent. Therefore, it is useful for manufacturing electronic components, electronic devices, electrical components, electrical devices, etc., and bonding of chip components such as capacitors and resistors to circuit boards; semiconductor devices such as light emitting diodes, laser diodes, memories, IGBTs, and CPUs It is useful for joining a metal part and a metal part of a lead frame or a circuit board; joining a high heat generating CPU chip and a cooling plate.

A light-emitting diode element is also referred to as an LED chip, and a light-emitting diode device, which is a kind of electronic device, has an LED chip bonded (bonded) to a lead frame or a circuit board, and the paste-like metal particle composition of the present invention is a bonding material. It can be used as (bonding agent). The material of the metal part of the light emitting diode element, the lead frame, and the metal part of the circuit board to be joined by the paste-like metal particle composition of the present invention has light resistance, heat resistance, etc., and has high connection reliability, gold, Silver, copper, palladium, platinum, and alloys of these metals are preferable, or plating with these metals or alloys of these metals is preferable. The form of the light emitting diode device is not limited, and examples thereof include a shell type, a flat type, a chip type, and an array.

As a compound semiconductor constituting the light emitting diode element, GaAlAs, GaInP, GaAsP, AlGaInP, GaP, InGaN, GaN, AlN, or the like can be used, depending on the target emission peak wavelength. Note that the wavelength of light emitted from the light emitting diode element usually has a certain range, and the emission peak wavelength is a wavelength showing the highest emission intensity among them. The emission peak wavelength can be easily known by measuring the emission spectrum with a spectrophotometer. Moreover, the light emission amount and the light emission peak wavelength can be changed by selecting the ratio of each component.

Light-emitting diode elements generate a large amount of heat with light emission, and may emit ultraviolet rays that have the property of decomposing organic substances, so the use of adhesives containing organic substances such as epoxy resins that are easily degraded by heat and ultraviolet rays It is not preferred, and the paste-like metal particle composition of the present invention which does not substantially contain an organic substance in the sintered product of the paste-like metal particle composition can be suitably used.

Further, the sintered product of the paste-like metal particle composition of the present invention is preferably silver, gold, copper, platinum, palladium, or an alloy thereof, and has excellent adhesion to a metal member that was in contact during sintering. In addition to a CPU that operates at a high frequency and generates a large amount of heat, it operates at a high voltage of several hundred to several thousand volts and has a large amount of heat generated. Power semiconductor elements (power semiconductor elements) whose operating temperature also becomes high, for example, transistors such as MOSFET (field effect transistor), IGBT (insulated gate bipolar transistor), LTT (light trigger thyristor), GTO (gate turn-off thyristor), It can be suitably used for joining a thyristor such as a triac and a lead frame or a circuit board.
The power semiconductor element is generally preferably a nitride semiconductor element such as aluminum nitride, gallium nitride, or indium nitride that can operate at a high temperature.

Examples and comparative examples of the present invention will be given. In Examples and Comparative Examples, “parts” means “parts by mass”, and the average particle size is a volume-based integrated fraction 50% value of particle size distribution measured using a laser diffraction scattering type particle size distribution measuring device, that is, Mean the median diameter (D50 value). The heating in Examples and Comparative Examples is heating in a forced circulation oven, and the atmosphere in the forced circulation oven is air unless otherwise noted.
Silver particles and copper particles in Examples, Comparative Examples, and Reference Examples are silver particle manufacturer products and copper particle manufacturer products. However, granular silver particles having an average particle diameter of 1 μm in Example 4, Example 5, Comparative Example 5 and Comparative Example 6 are those of Japanese Patent Application No. 2012-201391 (Japanese Patent Application Laid-Open No. 2014-55332), which is an in-house application. It was produced by itself according to the example.
The preparation operations and the like in the examples, comparative examples, and reference examples are all at room temperature (about 25 ° C.) in the atmosphere.
The amount of the coating material of the sinterable metal particles (A), the presence or absence of a powdery coating material on the surface, the dischargeability of the paste-like metal particle composition, the volume resistivity and the thermal conductivity of the sintered product produced by heating. And the adhesive strength of the joined body joined by heating and the adhesive strength after the thermal cycle test were measured by the following methods. The measurement is a measurement at room temperature (about 25 ° C.) in the atmosphere unless otherwise specified.

[Sinterable metal particles (A) having an average particle size of 0.01 to 10 μm and coated with a coating agent selected from the group consisting of non-powdered fatty acid, polymer dispersant and organic amine at 25 ° C. Coating amount]
Using a differential thermothermal gravimetric simultaneous measurement device (DTG-60AH type, manufactured by Shimadzu Corporation), the sinterable metal particles (A) were heated from room temperature (about 25 ° C.) to 500 ° C. at a temperature rising rate of 10 ° C./min The temperature was raised, and the weight loss rate of the sinterable metal particles (A) was calculated as the coating amount. When the sinterable metal particles were copper particles, the temperature was measured in nitrogen gas instead of in the atmosphere.

[Sinterable metal particles (A) having an average particle size of 0.01 to 10 μm and coated with a coating agent selected from the group consisting of non-powdered fatty acid, polymer dispersant and organic amine at 25 ° C. Presence or absence of powdery coating on the surface of
The surface of the sinterable metal particles was observed for the presence of a powdery surface coating agent with an optical microscope having a magnification of 10 times.

[Dischargeability of paste-like metal particle composition]
A 5 ml syringe (EFD, Inc.) is filled with 3 ml of a paste-like metal particle composition, and a metal needle (made by Musashi Engineering Co., Ltd.) having an inner diameter of 0.14 mm and a length of 15 mm is attached, and pressure is applied at intervals of 1 second. Whether or not clogging occurs in the metal needle until the entire amount was discharged was examined by repeatedly discharging with and without pressurization of 200 kPa. If clogging did not occur even after discharging the entire amount, it was judged that there was no clogging. When clogging occurred before the entire amount was discharged, it was judged that clogging occurred.

[Volume resistivity of heated sintered product]
A paste-like metal particle composition was applied onto a glass plate having a width of 50 mm, a length of 50 mm, and a thickness of 2.0 mm using a 2 mm thick metal mask having an opening having a width of 10 mm and a length of 10 mm. The plate-like sintered product was heated for a predetermined time in the forced circulation oven. When the sinterable metal particles were copper particles, they were further heated at 200 ° C. for 10 minutes in a forming gas that was a mixed gas of 10% by volume of hydrogen gas and 90% by volume of nitrogen gas.
The volume resistivity (unit: Ω · cm) of the plate-like sintered product peeled from the glass plate was measured by a method according to JIS K 7194.

[Thermal conductivity of the sintered material]
A paste-like metal particle composition was applied onto a glass plate having a width of 50 mm, a length of 50 mm, and a thickness of 2.0 mm using a 2 mm thick metal mask having an opening having a width of 10 mm and a length of 10 mm. The plate-like sintered product was heated for a predetermined time in the forced circulation oven. When the sinterable metal particles were copper particles, they were further heated at 200 ° C. for 10 minutes in a forming gas that was a mixed gas of 10% by volume of hydrogen gas and 90% by volume of nitrogen gas.
The plate-shaped sintered product peeled from the glass plate was measured for thermal conductivity (unit: W / m · K) by a laser flash method.

[Adhesive strength of joined body]
On a silver-plated substrate (silver purity 99.99%) having a width of 25 mm, a length of 70 mm, and a thickness of 1.0 mm, four openings with a width of 2.5 mm and a length of 2.5 mm are provided at intervals of 10 mm. The paste-like metal particle composition was applied using a 100 μm thick metal mask. A gold-plated silicon chip (gold-plated chip) having a width of 2.5 mm, a length of 2.5 mm, and a thickness of 1 mm is mounted on the applied paste-like metal particle composition, and then placed in a forced circulation oven at 200 ° C. The silver-plated substrate and the gold-plated chip were joined by heating for 1 hour to sinter the sinterable metal particles in the paste-like metal particle composition. When the sinterable metal particles were copper particles, they were further heated at 200 ° C. for 10 minutes in a forming gas that was a mixed gas of 10% by volume of hydrogen gas and 90% by volume of nitrogen gas.

The side of the gold-plated chip having a width of 2.5 mm, a length of 2.5 mm, and a thickness of 1 mm of the test specimen for measuring the adhesive strength thus obtained was pressed at a speed of 23 mm / min by an adhesive strength tester, The load at the time of shear fracture was used as the adhesive strength (unit: MPa).

[Adhesive strength after thermal cycle test of joined body]
A test for adhesion strength measurement prepared in the same manner as described in [Joint strength of bonded body] is a thermal cycle test in which a cycle of standing at −40 ° C. for 30 minutes and standing at + 125 ° C. for 30 minutes is one cycle. After 100 cycles, the adhesive strength was measured in the same manner as described in [Adhesive strength of bonded body].

[Reference Example 1]
After crushing stearic acid (made by Wako Pure Chemical Industries, Ltd.), which is a solid fatty acid having 18 carbon atoms at 25 ° C., in a mortar, it is coarsened by a standard sieve defined in JIS Z 8801 with an opening of 150 μm. Was removed to obtain powdered stearic acid.

[Reference Example 2]
Capric acid (manufactured by Wako Pure Chemical Industries, Ltd.), a saturated fatty acid having 10 carbon atoms, which is solid at 25 ° C., is crushed in a mortar and then coarsely granulated with a standard sieve according to JIS Z 8801 having an opening of 150 μm. Was removed to obtain powdered capric acid.

[Reference Example 3]
After pulverizing myristic acid (made by Wako Pure Chemical Industries, Ltd.), which is a solid fatty acid having 14 carbon atoms at 25 ° C., in a mortar, coarse particles are formed using a standard sieve according to JIS Z 8801 with an opening of 150 μm. Was removed to obtain powdered myristic acid.

[Reference Example 4]
After crushing diglycolic acid having two solid carboxyl groups at 25 ° C. (manufactured by Wako Pure Chemical Industries, Ltd.) in a mortar, coarse particles are removed with a standard sieve of JIS Z 8801 having an opening of 150 μm, Powdered diglycolic acid was used.

[Example 1]
Using a mixer with a stirring blade, it was produced by a reduction method of silver nitrate, which is sinterable silver particles (A1), and the average particle diameter was 1.0 μm, and the surface was coated with solid stearic acid ( The amount of stearic acid is 0.5% by mass) 50 parts of granular silver particles (no powdered stearic acid on the surface), sinterable silver particles (A2), produced by the silver nitrate reduction method Spherical silver particles having an average particle diameter of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) (having no powdery stearic acid on the surface) 50 parts and 11 parts of octanediol (manufactured by Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B), are stirred and mixed at room temperature (about 25 ° C.). Stearic acid (C) 0.15 part is added, room temperature (about 25 ° C.) The paste Jogin particle composition was prepared by uniformly mixing.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. Moreover, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was high and the adhesiveness after the thermal cycle test was also high.
The above results are summarized in Table 1. This paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, and can firmly join the metal member (D1) and the metal member (D2).

[Example 2]
Using a mixer with a stirring blade, it was produced by the reduction method of silver nitrate, which is sinterable silver particles (A1), the average particle size was 0.08 μm, and the surface was coated with octanoic acid (octanoic acid is Liquid at 25 ° C., octanoic acid amount is 1.0% by mass) 10 parts of spherical silver particles, sinterable silver particles (A2), produced by the reduction method of silver nitrate, the average particle diameter is 90 parts of spherical silver particles (no powdery stearic acid on the surface) having a surface of 2.0 μm and having a surface coated with solid stearic acid (the amount of stearin is 0.7% by mass), and After 13 parts of octanediol (manufactured by Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B), is stirred and mixed at room temperature (about 25 ° C.), the powdered capric acid (C) prepared in Reference Example 2 is used. Add 2.0 parts and mix evenly at room temperature (about 25 ° C). The door-shaped silver particles composition was prepared.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. Moreover, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was high and the adhesiveness after the thermal cycle test was also high.
The above results are summarized in Table 1. This paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, and can firmly join the metal member (D1) and the metal member (D2).

[Example 3]
Using a mixer with a stirring blade, it was produced by the reduction method of copper sulfate, which is sinterable copper particles (A1), the average particle diameter was 1.0 μm, and the surface was coated with oleic acid (oleic acid Is a liquid at 25 ° C., and the amount of oleic acid is 0.9% by mass.) 20 parts of spherical copper particles, sinterable silver particles (A2), produced by the reduction method of silver nitrate and having an average particle size of 80 parts of spherical silver particles (no stearic acid powder on the surface) having a surface of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass), and After stirring 11 parts of α-terpineol (Wako Pure Chemical Industries, Ltd.), which is a volatile dispersion medium (B), and mixing at room temperature (about 25 ° C.), powdered stearic acid prepared in Reference Example 1 (C) Add 0.4 parts and mix uniformly at room temperature (about 25 ° C) Silver particles, copper particles composition was prepared.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle / copper particle composition were measured, and the volume resistivity and thermal conductivity of the sintered silver particles / copper particles were measured. The rate was high. Moreover, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was high and the adhesiveness after the thermal cycle test was also high.
The above results are summarized in Table 1. This paste-like silver particle / copper particle composition has high conductivity and thermal conductivity of the sintered product, and can firmly join the metal member (D1) and the metal member (D2).

[Comparative Example 1]
Using a mixer with a stirring blade, it was produced by a reduction method of silver nitrate, which is sinterable silver particles (A1), and the average particle diameter was 1.0 μm, and the surface was coated with solid stearic acid ( The amount of stearic acid is 0.5% by mass) 50 parts of granular silver particles (no powdered stearic acid on the surface), the sintered silver particles (A2) are produced by the silver nitrate reduction method, Spherical silver particles having an average particle diameter of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) (having no powdery stearic acid on the surface) A paste-like silver particle composition was prepared by uniformly mixing 50 parts and 11 parts of octanediol (manufactured by Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B), at room temperature (about 25 ° C.).

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. However, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was low and the adhesiveness after the thermal cycle test was also low.
The above results are summarized in Table 3. Although this paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, the metal member (D1) and the metal member (D2) cannot be bonded firmly.

[Comparative Example 2]
Using a mixer equipped with a stirring blade, the average particle size was 1.0 μm and the surface was coated with solid stearic acid, which was produced by a reduction method of silver nitrate, which is sinterable silver particles (A1). (The amount of stearic acid is 0.5% by mass) 50 parts of granular silver particles (no powdered stearic acid on the surface), sinterable silver particles (A2), manufactured by the silver nitrate reduction method Spherical silver particles having an average particle diameter of 2.0 μm and having a surface coated with solid stearic acid (the amount of stearic acid is 0.7% by mass) (having no powdered stearic acid on the surface) ) 50 parts and 11 parts of octanediol (manufactured by Kyowa Hakko Chemical Co., Ltd.) which is a volatile dispersion medium (B) are stirred and mixed at room temperature (about 25 ° C.), and then 25 ° C. having 18 carbon atoms. And 0.2 part of oleic acid (C) which is a liquid unsaturated fatty acid And, to prepare a paste Jogin particle composition by uniformly mixing at room temperature (about 25 ° C.).

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. However, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was low and the adhesiveness after the thermal cycle test was also low.
The above results are summarized in Table 3. Although this paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, the metal member (D1) and the metal member (D2) cannot be bonded firmly.

[Comparative Example 3]
Using a mixer with a stirring blade, it was produced by a reduction method of silver nitrate, which is sinterable silver particles (A1), and the average particle diameter was 1.0 μm, and the surface was coated with solid stearic acid ( The amount of stearic acid is 0.5% by mass) 50 parts of granular silver particles (no powdered stearic acid on the surface), the sintered silver particles (A2) are produced by the silver nitrate reduction method, Spherical silver particles having an average particle diameter of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) (having no powdery stearic acid on the surface) 50 parts and 11 parts of octanediol (manufactured by Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B), are stirred and mixed at room temperature (about 25 ° C.), and then at 25 ° C. having 8 carbon atoms. Add 0.2 part of octanoic acid, a liquid saturated fatty acid, and add room temperature ( It was prepared a paste Jogin particle composition were uniformly mixed at 25 ° C.).

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. However, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was low and the adhesiveness after the thermal cycle test was also low.
The above results are summarized in Table 3. Although this paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, the metal member (D1) and the metal member (D2) cannot be bonded firmly.

[Comparative Example 4]
Using a mixer with a stirring blade, it was produced by a reduction method of silver nitrate, which is sinterable silver particles (A1), and the average particle diameter was 1.0 μm, and the surface was coated with solid stearic acid ( The amount of stearic acid is 0.5% by mass) 50 parts of granular silver particles (no powdered stearic acid on the surface), the sintered silver particles (A2) are produced by the silver nitrate reduction method, Spherical silver particles having an average particle diameter of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) (having no powdery stearic acid on the surface) After 50 parts and 11 parts of octanediol (Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B), were stirred and mixed at room temperature (about 25 ° C.), the powdery powder prepared in Reference Example 4 was used. Add 0.5 parts of diglycolic acid and uniformly at room temperature (about 25 ° C) Mixing the paste Jogin particle composition was prepared.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. However, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was low and the adhesiveness after the thermal cycle test was also low.
The above results are summarized in Table 4. Although this paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, the metal member (D1) and the metal member (D2) cannot be bonded firmly.

[Example 4]
By using a mixer equipped with a stirring blade, manufactured by the reduction method of silver nitrate, which is sinterable silver particles (A1), the average particle size is 1.0 μm, and the surface is Big Chemie Japan Co., Ltd., which is a polymer dispersant Granular silver particles coated with DISPERBYK-2020 (acid value: 37 mg KOH / g, amine value: 36 mg KOH / g) manufactured by the company (DISPERBYK-2020 amount is 0.3% by weight) 50 parts by weight (without molecular dispersant), sinterable silver particles (A2), manufactured by the silver nitrate reduction method, the average particle size is 2.0 μm, and the surface is coated with solid stearic acid 50 parts of spherical silver particles (the amount of stearic acid is 0.7% by mass) (no powdered stearic acid on the surface) and octanediol (Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B) Stir 11 parts (made by company) at room temperature (about 25 ° C) After mixing, 0.2 parts of the powdery stearic acid (C) prepared in Reference Example 1 was added and uniformly mixed at room temperature (about 25 ° C.) to prepare a paste-like silver particle composition.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. Moreover, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was high and the adhesiveness after the thermal cycle test was also high.
The above results are summarized in Table 2. This paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, and can firmly join the metal member (D1) and the metal member (D2).

[Example 5]
1,2-Sintered silver particles (A1) using a mixer with stirring blades, manufactured by a reduction method of silver nitrate, having an average particle diameter of 1.0 μm and a surface being a nitrogen-containing organic compound 50 parts of granular silver particles coated with propanediamine (1,2-propanediamine is liquid at 25 ° C. and the amount of 1,2-propanediamine is 0.3% by mass), sinterable silver particles ( A2) spherical silver particles produced by the silver nitrate reduction method, having an average particle diameter of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) 50 parts (without powdery stearic acid on the surface) and 11 parts of octanediol (manufactured by Kyowa Hakko Chemical Co., Ltd.) which is a volatile dispersion medium (B) are stirred and mixed at room temperature (about 25 ° C.) After that, the powdered stearic acid prepared in Reference Example 1 C) was added 0.2 parts to prepare a paste Jogin particle composition by uniformly mixing at room temperature (about 25 ° C.).

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. Moreover, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was high and the adhesiveness after the thermal cycle test was also high.
The above results are summarized in Table 2. This paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, and can firmly join the metal member (D1) and the metal member (D2).

[Example 6]
Using a mixer with a stirring blade, it was produced by a reduction method of silver nitrate, which is sinterable silver particles (A1), and the average particle diameter was 1.0 μm, and the surface was coated with solid stearic acid ( The amount of stearic acid is 0.5% by mass) 50 parts of granular silver particles (no powdered stearic acid on the surface), the sintered silver particles (A2) are produced by the silver nitrate reduction method, Spherical silver particles having an average particle diameter of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) (having no powdery stearic acid on the surface) 50 parts and 11 parts of octanediol (produced by Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B), were stirred and mixed at room temperature (about 25 ° C.), and then the powdery powder prepared in Reference Example 3 was used. Add 0.15 parts of myristic acid (C), room temperature (about 25 ° C) The paste Jogin particle composition was prepared by uniformly mixing.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. Moreover, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was high and the adhesiveness after the thermal cycle test was also high.
The above results are summarized in Table 2. This paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, and can firmly join the metal member (D1) and the metal member (D2).

[Comparative Example 5]
By using a mixer equipped with a stirring blade, manufactured by the reduction method of silver nitrate, which is sinterable silver particles (A1), the average particle size is 1.0 μm, and the surface is Big Chemie Japan Co., Ltd., which is a polymer dispersant Granular silver particles coated with DISPERBYK-2020 (acid value: 37 mg KOH / g, amine value: 36 mg KOH / g) manufactured by the company (DISPERBYK-2020 amount is 0.3% by weight) 50 parts without a molecular dispersant), manufactured by the reduction method of silver nitrate which is sinterable silver particles (A2), the average particle diameter is 2.0 μm, and the surface is coated with solid stearic acid ( 50 parts of spherical silver particles (which do not have powdery stearic acid on the surface) and octanediol (Kyowa Hakko Chemical Co., Ltd.) which is a volatile dispersion medium (B) 11 parts) uniformly mixed at room temperature (about 25 ° C) The pasty silver particle composition was prepared.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. However, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was low and the adhesiveness after the thermal cycle test was also low.
The above results are summarized in Table 4. Although this paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, the metal member (D1) and the metal member (D2) cannot be bonded firmly.

[Comparative Example 6]
1,2-Sintered silver particles (A1) using a mixer with stirring blades, manufactured by a reduction method of silver nitrate, having an average particle diameter of 1.0 μm and a surface being a nitrogen-containing organic compound 50 parts of granular silver particles coated with propanediamine (1,2-propanediamine is liquid at 25 ° C. and the amount of 1,2-propanediamine is 0.3% by mass), sinterable silver particles ( A2) spherical silver produced by the silver nitrate reduction method, having an average particle size of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) 50 parts of particles (no powdery stearic acid on the surface) and 11 parts of octanediol (Kyowa Hakko Chemical Co., Ltd.), a volatile dispersion medium (B), are uniformly mixed at room temperature (about 25 ° C) Thus, a paste-like silver particle composition was prepared.

Next, when the volume resistivity and thermal conductivity of the paste-like silver particle composition were measured, and the sintered silver particles were measured, the ejection properties were excellent, the volume resistivity was low, and the thermal conductivity was high. However, when the adhesive strength of the joined body by this composition and the adhesive strength after the thermal cycle test were measured, the adhesiveness was low and the adhesiveness after the thermal cycle test was also low.
The above results are summarized in Table 4. Although this paste-like silver particle composition has high conductivity and thermal conductivity of the sintered product, the metal member (D1) and the metal member (D2) cannot be bonded firmly.

[Reference Example 5]
Using a mixer with a stirring blade, it was produced by a reduction method of silver nitrate, which is sinterable silver particles (A1), and the average particle diameter was 1.0 μm, and the surface was coated with solid stearic acid ( The amount of stearic acid is 0.5% by mass) 50 parts of granular silver particles (having no powdered stearic acid on the surface), manufactured by the reduction method of silver nitrate which is sinterable silver particles (A2), average Spherical silver particles having a particle diameter of 2.0 μm and coated with solid stearic acid on the surface (the amount of stearic acid is 0.7% by mass) (having no powdery stearic acid on the surface) 50 And 11 parts of octanediol (produced by Kyowa Hakko Chemical Co., Ltd.), which is a volatile dispersion medium (B), are stirred and mixed at room temperature (about 25 ° C.), and then the maximum particle size can be crushed in a mortar. Powdered stearin containing many coarse particles of 0.5 mm or more (C) 6 parts was added to prepare a paste Jogin particle composition by uniformly mixing at room temperature (about 25 ° C.).

Next, when the dischargeability of the paste-like silver particle composition was measured, clogging occurred during discharge. The above results are summarized in Table 5.

When the paste-like metal particle composition of the present invention is heated, the volatile dispersion medium (B) and the powdered fatty acid (C) are volatilized at 25 ° C., and the sinterable metal particles (A) are sintered together. Since the metal member (D1) and the metal member (D2) are firmly bonded and the adhesive strength after the thermal cycle test is excellent, it is useful for bonding between a plurality of metal members. In particular, it is useful for joining a metal part of a semiconductor element and a metal part of a lead frame or a circuit board. Since the bonding portion between the semiconductor element and the lead frame has excellent adhesion strength after the thermal cycle test, it is useful for manufacturing highly reliable electronic parts and electronic devices.

A Test specimen for measuring adhesive strength 1 Silver substrate 2 Paste-like metal particle composition (solid metal having voids after heating and sintering)
3 Au plated silicon chip or silver chip

Claims (15)

(A) A baked product having an average particle size of 0.01 to 10 [mu] m coated with a coating selected from the group consisting of solid, semi-solid or liquid fatty acids, polymer dispersants and organic amines at 25 [deg.] C Coherent metal particles,
(B) a volatile dispersion medium;
(C) A paste-like metal particle composition comprising a fatty acid powdered at 25 ° C. Fatty acid (C) in a powder form at 25 ° C. is a saturated fatty acid having 10 to 22 carbon atoms that has passed through a sieve having an opening of 150 μm. For 100 parts by mass of the sinterable metal particles (A), The paste-like metal particle composition according to claim 1, which is 0.01 to 5 parts by mass. The paste-like metal particle composition according to claim 1 or 2, wherein a material of the sinterable metal particles (A) is gold, silver, copper, platinum, palladium, or an alloy thereof. The paste metal particle composition has a volume resistivity of 1 × 10 ⁻⁵ Ω · cm or less and a thermal conductivity of 100 W / m · K or more at 100 ° C. or more and 300 ° C. or less. The paste-like metal particle composition according to claim 1, claim 2 or claim 3. (A) A baked product having an average particle size of 0.01 to 10 [mu] m coated with a coating selected from the group consisting of solid, semi-solid or liquid fatty acids, polymer dispersants and organic amines at 25 [deg.] C Coherent metal particles,
(B) a volatile dispersion medium;
(C) A paste-like metal particle composition comprising a powdered fatty acid at 25 ° C.
By interposing between the metal member (D1) and the metal member (D2) and heating at 100 ° C. or more and 300 ° C. or less, the sintered product of the sinterable metal particles (A) is made of metal. The joining method characterized by joining a member (D1) and metal members (D2). Fatty acid (C) in a powder form at 25 ° C. is a saturated fatty acid having 10 to 22 carbon atoms that has passed through a sieve having an opening of 150 μm. For 100 parts by mass of the sinterable metal particles (A), The bonding method according to claim 5, wherein the bonding method is 0.01 to 5 parts by mass. The joining method according to claim 5 or 6, wherein a material of the sinterable metal particles (A) is gold, silver, copper, platinum, palladium, or an alloy thereof. The material of the metal member (D1) is gold, silver, copper, platinum, palladium or an alloy thereof, and the material of the metal member (D2) is gold or an alloy of gold. The joining method according to claim 6 or claim 7. The joining according to any one of claims 5 to 8, wherein the metal member (D1) is a metal part of a lead frame or a circuit board, and the metal member (D2) is a metal part of a semiconductor element. Method. The volume resistivity of the sintered product of the sinterable metal particles (A) is 1 × 10 ⁻⁵ Ω · cm or less, and the thermal conductivity is 100 W / m · K or more. The joining method according to claim 9. (A) A baked product having an average particle size of 0.01 to 10 [mu] m coated with a coating selected from the group consisting of solid, semi-solid or liquid fatty acids, polymer dispersants and organic amines at 25 [deg.] C Coherent metal particles,
(B) a volatile dispersion medium;
(C) A paste-like metal particle composition consisting of a fatty acid powdered at 25 ° C. is interposed between a metal part of a semiconductor element and a circuit board having a lead frame or metal part, and then 100 ° C. or more and 300 ° C. or less. A method of manufacturing an electronic device comprising: joining a metal part of a semiconductor element and a metal part of a lead frame or a circuit board as a sintered product of the sinterable metal particles (A) by heating at . The powdered fatty acid (C) at 25 ° C. is a saturated fatty acid having 10 to 22 carbon atoms that has passed through a sieve having an opening of 150 μm, and is 0.1% relative to 100 parts by mass of the sinterable metal particles (A). The manufacturing method of the electronic device of Claim 11 which is 01-5 mass parts. The method of manufacturing an electronic device according to claim 11 or 12, wherein a material of the sinterable metal particles (A) is gold, silver, copper, platinum, palladium, or an alloy thereof. 12. The material of the metal part of the lead frame or the circuit board is gold, silver, copper, platinum, palladium, or an alloy thereof, and the material of the metal part of the semiconductor element is gold or a gold alloy. 14. A method for manufacturing an electronic device according to claim 12 or claim 13. The volume resistivity of the sintered product of the sinterable metal particles (A) is 1 × 10 ⁻⁵ Ω · cm or less, and the thermal conductivity is 100 W / m · K or more. The method for manufacturing an electronic device according to claim 14.

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