CN117123791A - Preparation method of gold powder for matching low-temperature co-fired ceramics - Google Patents
Preparation method of gold powder for matching low-temperature co-fired ceramics Download PDFInfo
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- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 title claims abstract description 62
- 238000002360 preparation method Methods 0.000 title claims abstract description 19
- 239000000919 ceramic Substances 0.000 title claims abstract description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 35
- 239000008367 deionised water Substances 0.000 claims abstract description 32
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 32
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 26
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 26
- 150000001413 amino acids Chemical class 0.000 claims abstract description 24
- 239000010931 gold Substances 0.000 claims abstract description 19
- 229910052737 gold Inorganic materials 0.000 claims abstract description 19
- 239000007864 aqueous solution Substances 0.000 claims abstract description 14
- 239000002245 particle Substances 0.000 claims abstract description 14
- 238000005406 washing Methods 0.000 claims abstract description 13
- 230000001788 irregular Effects 0.000 claims abstract description 11
- 239000000843 powder Substances 0.000 claims abstract description 7
- 125000002883 imidazolyl group Chemical group 0.000 claims abstract description 5
- 239000008139 complexing agent Substances 0.000 claims abstract description 3
- 239000000243 solution Substances 0.000 claims description 54
- 238000006243 chemical reaction Methods 0.000 claims description 36
- 235000001014 amino acid Nutrition 0.000 claims description 23
- RAXXELZNTBOGNW-UHFFFAOYSA-N imidazole Natural products C1=CNC=N1 RAXXELZNTBOGNW-UHFFFAOYSA-N 0.000 claims description 18
- 238000003756 stirring Methods 0.000 claims description 18
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 15
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
- 239000002270 dispersing agent Substances 0.000 claims description 15
- DHMQDGOQFOQNFH-UHFFFAOYSA-N Glycine Chemical compound NCC(O)=O DHMQDGOQFOQNFH-UHFFFAOYSA-N 0.000 claims description 10
- -1 gold ion Chemical class 0.000 claims description 8
- 238000001035 drying Methods 0.000 claims description 6
- 239000004471 Glycine Substances 0.000 claims description 5
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 5
- 229910017604 nitric acid Inorganic materials 0.000 claims description 5
- 230000001376 precipitating effect Effects 0.000 claims description 5
- 239000006228 supernatant Substances 0.000 claims description 5
- 239000002202 Polyethylene glycol Substances 0.000 claims description 4
- HNDVDQJCIGZPNO-UHFFFAOYSA-N histidine Natural products OC(=O)C(N)CC1=CN=CN1 HNDVDQJCIGZPNO-UHFFFAOYSA-N 0.000 claims description 4
- 229920001223 polyethylene glycol Polymers 0.000 claims description 4
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 4
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 4
- WHUUTDBJXJRKMK-UHFFFAOYSA-N Glutamic acid Natural products OC(=O)C(N)CCC(O)=O WHUUTDBJXJRKMK-UHFFFAOYSA-N 0.000 claims description 3
- DBMJMQXJHONAFJ-UHFFFAOYSA-M Sodium laurylsulphate Chemical compound [Na+].CCCCCCCCCCCCOS([O-])(=O)=O DBMJMQXJHONAFJ-UHFFFAOYSA-M 0.000 claims description 3
- QZPSXPBJTPJTSZ-UHFFFAOYSA-N aqua regia Chemical compound Cl.O[N+]([O-])=O QZPSXPBJTPJTSZ-UHFFFAOYSA-N 0.000 claims description 3
- 235000013922 glutamic acid Nutrition 0.000 claims description 3
- 239000004220 glutamic acid Substances 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 3
- NWZSZGALRFJKBT-KNIFDHDWSA-N (2s)-2,6-diaminohexanoic acid;(2s)-2-hydroxybutanedioic acid Chemical compound OC(=O)[C@@H](O)CC(O)=O.NCCCC[C@H](N)C(O)=O NWZSZGALRFJKBT-KNIFDHDWSA-N 0.000 claims description 2
- HYZJCKYKOHLVJF-UHFFFAOYSA-N 1H-benzimidazole Chemical compound C1=CC=C2NC=NC2=C1 HYZJCKYKOHLVJF-UHFFFAOYSA-N 0.000 claims description 2
- BAXOFTOLAUCFNW-UHFFFAOYSA-N 1H-indazole Chemical compound C1=CC=C2C=NNC2=C1 BAXOFTOLAUCFNW-UHFFFAOYSA-N 0.000 claims description 2
- RIAHASMJDOMQER-UHFFFAOYSA-N 5-ethyl-2-methyl-1h-imidazole Chemical compound CCC1=CN=C(C)N1 RIAHASMJDOMQER-UHFFFAOYSA-N 0.000 claims description 2
- 239000004475 Arginine Substances 0.000 claims description 2
- QNAYBMKLOCPYGJ-REOHCLBHSA-N L-alanine Chemical compound C[C@H](N)C(O)=O QNAYBMKLOCPYGJ-REOHCLBHSA-N 0.000 claims description 2
- ODKSFYDXXFIFQN-BYPYZUCNSA-P L-argininium(2+) Chemical compound NC(=[NH2+])NCCC[C@H]([NH3+])C(O)=O ODKSFYDXXFIFQN-BYPYZUCNSA-P 0.000 claims description 2
- WHUUTDBJXJRKMK-VKHMYHEASA-N L-glutamic acid Chemical compound OC(=O)[C@@H](N)CCC(O)=O WHUUTDBJXJRKMK-VKHMYHEASA-N 0.000 claims description 2
- HNDVDQJCIGZPNO-YFKPBYRVSA-N L-histidine Chemical compound OC(=O)[C@@H](N)CC1=CN=CN1 HNDVDQJCIGZPNO-YFKPBYRVSA-N 0.000 claims description 2
- KDXKERNSBIXSRK-YFKPBYRVSA-N L-lysine Chemical compound NCCCC[C@H](N)C(O)=O KDXKERNSBIXSRK-YFKPBYRVSA-N 0.000 claims description 2
- COLNVLDHVKWLRT-QMMMGPOBSA-N L-phenylalanine Chemical compound OC(=O)[C@@H](N)CC1=CC=CC=C1 COLNVLDHVKWLRT-QMMMGPOBSA-N 0.000 claims description 2
- KZSNJWFQEVHDMF-BYPYZUCNSA-N L-valine Chemical compound CC(C)[C@H](N)C(O)=O KZSNJWFQEVHDMF-BYPYZUCNSA-N 0.000 claims description 2
- KDXKERNSBIXSRK-UHFFFAOYSA-N Lysine Natural products NCCCCC(N)C(O)=O KDXKERNSBIXSRK-UHFFFAOYSA-N 0.000 claims description 2
- 239000004472 Lysine Substances 0.000 claims description 2
- KZSNJWFQEVHDMF-UHFFFAOYSA-N Valine Natural products CC(C)C(N)C(O)=O KZSNJWFQEVHDMF-UHFFFAOYSA-N 0.000 claims description 2
- 235000004279 alanine Nutrition 0.000 claims description 2
- 235000009697 arginine Nutrition 0.000 claims description 2
- ODKSFYDXXFIFQN-UHFFFAOYSA-N arginine Natural products OC(=O)C(N)CCCNC(N)=N ODKSFYDXXFIFQN-UHFFFAOYSA-N 0.000 claims description 2
- GVGUFUZHNYFZLC-UHFFFAOYSA-N dodecyl benzenesulfonate;sodium Chemical compound [Na].CCCCCCCCCCCCOS(=O)(=O)C1=CC=CC=C1 GVGUFUZHNYFZLC-UHFFFAOYSA-N 0.000 claims description 2
- IKDUDTNKRLTJSI-UHFFFAOYSA-N hydrazine monohydrate Substances O.NN IKDUDTNKRLTJSI-UHFFFAOYSA-N 0.000 claims description 2
- 235000018977 lysine Nutrition 0.000 claims description 2
- 235000008729 phenylalanine Nutrition 0.000 claims description 2
- COLNVLDHVKWLRT-UHFFFAOYSA-N phenylalanine Natural products OC(=O)C(N)CC1=CC=CC=C1 COLNVLDHVKWLRT-UHFFFAOYSA-N 0.000 claims description 2
- 229940080264 sodium dodecylbenzenesulfonate Drugs 0.000 claims description 2
- 235000014393 valine Nutrition 0.000 claims description 2
- 239000004474 valine Substances 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims 8
- 238000000643 oven drying Methods 0.000 claims 1
- 230000001737 promoting effect Effects 0.000 claims 1
- 239000002253 acid Substances 0.000 abstract description 9
- 238000000034 method Methods 0.000 abstract description 8
- 238000005245 sintering Methods 0.000 abstract description 8
- 239000000758 substrate Substances 0.000 abstract description 4
- 239000005456 alcohol based solvent Substances 0.000 abstract description 3
- 239000003759 ester based solvent Substances 0.000 abstract description 3
- 239000012295 chemical reaction liquid Substances 0.000 abstract description 2
- 239000006179 pH buffering agent Substances 0.000 abstract 1
- 238000010438 heat treatment Methods 0.000 description 6
- 239000004020 conductor Substances 0.000 description 4
- 229910052573 porcelain Inorganic materials 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 3
- 239000011148 porous material Substances 0.000 description 3
- 238000005054 agglomeration Methods 0.000 description 2
- 230000002776 aggregation Effects 0.000 description 2
- 230000005670 electromagnetic radiation Effects 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 229920002873 Polyethylenimine Polymers 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 125000003277 amino group Chemical group 0.000 description 1
- 230000000712 assembly Effects 0.000 description 1
- 238000000429 assembly Methods 0.000 description 1
- 239000012752 auxiliary agent Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000006172 buffering agent Substances 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000010344 co-firing Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 230000000295 complement effect Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 239000006260 foam Substances 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 230000004807 localization Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000002107 nanodisc Substances 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 125000004433 nitrogen atom Chemical group N* 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000005416 organic matter Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000007639 printing Methods 0.000 description 1
- 238000004080 punching Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 238000006479 redox reaction Methods 0.000 description 1
- 238000002310 reflectometry Methods 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F9/00—Making metallic powder or suspensions thereof
- B22F9/16—Making metallic powder or suspensions thereof using chemical processes
- B22F9/18—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds
- B22F9/24—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds starting from liquid metal compounds, e.g. solutions
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F1/05—Metallic powder characterised by the size or surface area of the particles
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F1/05—Metallic powder characterised by the size or surface area of the particles
- B22F1/054—Nanosized particles
- B22F1/056—Submicron particles having a size above 100 nm up to 300 nm
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F1/06—Metallic powder characterised by the shape of the particles
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Nanotechnology (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Manufacture Of Metal Powder And Suspensions Thereof (AREA)
Abstract
The invention provides a preparation method of gold powder for matching low-temperature co-fired ceramics, which is used for preparing submicron irregular-morphology gold powder in chloroauric acid aqueous solution by a redox method. In the preparation process, amino acid is used as a gold ion complexing agent and a pH buffering agent of reaction liquid, micromolecular organic matters with weak reducibility and containing imidazole functional groups are used as a reducing agent, and means such as ethanol replacement of water in the powder are used after deionized water is used for washing the gold powder, so that submicron-level gold powder with irregular morphology and no caking is prepared. The gold powder prepared by the invention has the particle size ranging from 200nm to 900nm, good dispersibility in alcohol and ester solvents, compact film after sintering, capability of matching with imported and domestic various ceramics, and smooth substrate after sintering, and the warping degree is less than 0.1mm. The preparation method has high yield and convenient preparation process.
Description
Technical Field
The invention relates to the field of noble metal electronic paste, in particular to a preparation method of gold powder for matching low-temperature co-fired ceramics.
Background
The low-temperature co-fired ceramic (Low Temperature Co-fired Ceramic LTCC) is a high-density circuit with three-dimensional space complementary interference manufactured by punching, printing conductor paste, laminating and sintering, and is a mainstream technology of passive integration. The number of wiring layers is more, and the assembly density can be improved; components are easy to embed in the module, so that the module is multifunctional; the cavity with various structures is easy to form or is compatible with other wiring technologies, the application advantages of the multi-functional and hybrid multi-chip assembly are realized, and the multi-chip module is widely applied to various high-frequency communication assemblies. The conductors in LTCC are mainly gold and alloy powders. Gold has the characteristics of high conductivity, high heat conductivity, oxidation resistance, environmental corrosion resistance, excellent reflectivity of electromagnetic radiation and the like, is prepared into various functional conductor pastes, and can play a role in stabilizing under the conditions of high temperature, high humidity, high corrosiveness, electromagnetic radiation and the like, and is particularly applied to the fields of aviation, aerospace and the like.
The main manufacturers are Ferro and Dupont, ferro prepares gold inner electrode and pore size for LTCC, sheet powder is used for doping nanometer irregular particle gold powder, dupont prepares gold inner electrode and pore size for LTCC, submicron irregular particle gold powder is used, the two company size is well matched with raw porcelain, and sintered porcelain sheets are smooth and have no bubbles. The domestic related reports mainly include the preparation of micron-sized and nano-sized spherical gold powder and flake-doped spherical gold powder, and the gold powder is commonly used for preparing post-firing slurry, has poor matching with raw porcelain during co-firing, and is easy to foam or warp after sintering. The invention prepares gold powder with the shape and the particle size similar to that of the gold internal electrode for LTCC and the gold powder for pore size of Dupont company. At present, gold powder and gold conductor slurry for LTCC are mainly imported, and the preparation of the gold powder has good market application prospect and localization of key technology.
At present, the preparation of submicron irregular-morphology gold powder mainly comprises the following steps:
CN104275493a discloses a method for preparing gold nano-disc by using amino acid as reducing agent, gold powder is prepared by using amino acid as reducing agent, the main product is flake gold powder, chloroauric acid is low concentration 0.03mol/L, and the reaction time is 72h. Under the condition, the oxidation-reduction reaction period is long, and the prepared gold powder is small;
CN106112005a discloses a preparation method of monodisperse sheet gold powder, which uses anti-cycloxuic acid as reducer and linear polyethylenimine as auxiliary agent to prepare sheet gold powder. The preparation method can obtain irregular polygonal particle gold powder with submicron level of 500-800 nm, but the main product is sheet gold powder with the particle size of 4-6 mu m.
Disclosure of Invention
The invention aims to provide a preparation method of gold powder for matching low-temperature co-fired ceramics, and the prepared submicron irregular-morphology gold powder has the characteristics of uniform particle size, small specific surface area, no agglomeration and the like, and the warpage of a sintered substrate is less than 0.1mm, so that the gold powder can be applied to the low-temperature co-fired ceramics.
In order to achieve the above object, the present invention provides the following technical solutions:
the preparation method of the gold powder for matching the low-temperature co-fired ceramic comprises the following steps:
(1) Dissolving 99.99% gold sheet, removing nitric acid and excessive hydrochloric acid, and preparing into 1mol/L chloroauric acid (HAuCl) with deionized water 4 ) A solution;
(2) Dissolving dispersant in deionized water, wherein the mass ratio of dispersant (dispersant: HAuCl) 4 ) 1 to 5:100; volume ratio (deionized water: HAuCl) 4 Solution) 9:1;
(3) Dissolving amino acid in deionized water to obtain 1mol/L amino acid aqueous solution, and preparing into amino acid (amino acid: HAuCl) 4 ) 3:2;
(4) Dissolving reducer containing imidazole functional group in deionized water to prepare reducer solution with concentration of 1mol/L, wherein the mol ratio (reducer: HAuCl) 4 ) 2-3:2, heating the solution to 40 ℃;
(5) Under stirring, HAuCl prepared in step (1) 4 Pouring the solution into the dispersant solution prepared in the step (2), stirring for 15 minutes, and adding the amino acid prepared in the step (3)Adjusting the pH value of the aqueous solution to be 1.3-1.5 by using 0.1-1 mol/L HCl or NaOH solution, heating the reaction solution to 40 ℃, adding the aqueous solution of the reducing agent prepared in the step (4), and continuously stirring until the reaction is complete;
(6) Standing the reaction solution obtained in the step (5), precipitating, pouring out supernatant, repeatedly washing with deionized water for three times, washing with ethanol for 2 times, and drying in an oven at 80 ℃ to obtain submicron-level gold powder with irregular morphology.
In the step (5), adding a reducing agent solution into the reaction solution by pouring, wherein the temperature of the reaction solution and the reducing agent solution is 40 ℃;
in the step (5), about 1ml of the reaction solution was taken out, and the reaction was tested for completion using hydrazine hydrate. If the reaction liquid turns black or purple, continuing stirring for reaction; if the color of the reaction solution is not changed, the reaction is complete.
Preferably, the dispersing agent is one or more of polyvinylpyrrolidone (PVP, molecular weight 30000), sodium dodecyl sulfate, sodium dodecyl benzene sulfonate, polyethylene glycol and ethylphenyl polyethylene glycol.
Preferably, the amino acid is one or more of glycine, alanine, valine, phenylalanine, glutamic acid, lysine and arginine.
Preferably, the reducing agent is one or more of imidazole, 2-methyl-4-ethylimidazole, indazole, benzimidazole and histidine.
The invention has the following characteristics:
1. amino acid is used as a gold ion complexing agent and a pH regulator of the reaction solution. The amino group in the amino acid is complexed with gold ions, so that the reaction rate of the gold ions can be reduced, and other morphologies are avoided. The amino acid is an amphoteric substance, can be used as a buffering agent, maintains the pH value of the reaction solution, and promotes the reaction to be carried out stably;
2. the small molecular organic matter with weak reducibility and containing imidazole functional groups is used as a reducing agent to reduce chloroauric acid with strong oxidability, the reaction process is controllable, and single gold powder with irregular morphology is obtained, and no flaky or spherical powder is produced;
3. after washing the gold powder with deionized water, replacing water in the powder with ethanol, and drying to obtain non-caking gold powder, which is beneficial to dispersing the gold powder in an organic carrier;
4. the invention provides a preparation method of gold powder for matching low-temperature co-fired ceramics, wherein the gold powder is submicron powder with irregular morphology, and the particle size is in the range of 200-900 nm;
5. the gold powder prepared by the method has high yield, uniform particle size, no agglomeration, good dispersibility in alcohol and ester solvents, compact film after sintering, capability of matching with imported and domestic various porcelain materials, and smooth substrate after sintering, and warping degree of less than 0.1mm;
6. the preparation method is simple and convenient, the process is easy to control, the batch stability is high, the expansion is easy, and the environmental pollution is small.
In a word, the method can be used for preparing submicron irregular-morphology gold powder, the particle size is 200-900 nm, the particle size is not agglomerated, the dispersibility in alcohol and ester solvents is good, the film layer after sintering is compact, the method can be matched with various ceramic materials imported and produced in China, the substrate after sintering is smooth, and the warping degree is less than 0.1mm.
Drawings
FIG. 1 is a scanning electron micrograph of the gold powder prepared in example 1.
FIG. 2 is a scanning electron micrograph of the gold powder prepared in example 2.
Detailed Description
The method adopts the following raw materials with the purity: 99.99% gold flakes, deionized water, and the remaining chemical reagents were all analytically pure.
The preparation method comprises the following steps:
1. dissolving 99.99% gold sheet, removing nitric acid and excessive hydrochloric acid, and preparing into 1mol/L chloroauric acid (HAuCl) with deionized water 4 ) A solution;
2. dissolving dispersant in deionized water, wherein the mass ratio of dispersant (dispersant: HAuCl) 4 ) 1 to 5:100; volume ratio (deionized water: HAuCl) 4 Solution) 9:1;
3. dissolving amino acid in deionized water to obtain 1mol/L amino acid aqueous solution, and preparing into amino acid (amino acid: HAuCl) 4 ) 3:2;
4. will contain imidazole functionalityDissolving the reducer in deionized water to obtain reducer solution with concentration of 1mol/L, and mixing the reducer solution with the molar ratio (reducer: HAuCl) 4 ) 2-3:2, heating the solution to 40 ℃;
5. under stirring, HAuCl prepared in step (1) 4 Pouring the solution into the dispersant solution prepared in the step (2), stirring for 15 minutes, adjusting the pH value to be 1.3-1.5 by using 0.1-1 mol/L HCl or NaOH solution, adding the amino acid aqueous solution prepared in the step (3), heating the reaction solution to 40 ℃, adding the reducer aqueous solution prepared in the step (4), and continuously stirring until the reaction is complete;
6. standing the reaction solution obtained in the step (5), precipitating, pouring out supernatant, repeatedly washing with deionized water for three times, washing with ethanol for 2 times, and drying in an oven at 80 ℃ to obtain submicron-level gold powder with irregular morphology.
Example 1
1. Dissolving gold flake with purity of 99.99% 10g with aqua regia, removing nitric acid and excessive hydrochloric acid, preparing into 1mol/L chloroauric acid (HAuCl) with deionized water 4 ) A solution;
2. 0.2g of polyvinylpyrrolidone was dissolved in 450ml of deionized water with stirring;
3. 5.6g glycine was dissolved in 75ml deionized water;
4. 3.4g of imidazole was dissolved in 75ml of deionized water, molar ratio (imidazole: HAuCl) 4 ) 1:1, heated to 40 ℃.
5. Under stirring, HAuCl prepared in step (1) 4 Pouring the solution into the dispersant solution prepared in the step (2), stirring for 15 minutes, adjusting the pH value to be 1.3-1.5 by using 0.1-1 mol/L HCl or NaOH solution, adding the glycine aqueous solution prepared in the step (3), heating the reaction solution to 40 ℃, adding the reducer aqueous solution prepared in the step (4), and continuously stirring until the reaction is complete;
6. standing the reaction solution obtained in the step (5), precipitating, pouring out supernatant, repeatedly washing with deionized water for three times, washing with ethanol for 2 times, and drying in an oven at 80 ℃ to obtain submicron-level gold powder with irregular morphology.
Example 2
1. 10g of pure aqua regia is usedDissolving 99.99% gold sheet, removing nitric acid and excessive hydrochloric acid, and preparing into 1mol/L and about 50ml chloroauric acid (HAuCl) with deionized water 4 ) A solution;
2. 0.5g sodium dodecyl sulfate was dissolved in 450ml deionized water with stirring;
3. 11.02g of glutamic acid was dissolved in 75ml of deionized water;
4. 11.6g histidine was dissolved in 75ml deionized water, molar ratio (histidine: HAuCl) 4 ) 3:2, heated to 40 ℃.
5. Under stirring, HAuCl prepared in step (1) 4 Pouring the solution into the dispersant solution prepared in the step (2), stirring for 15 minutes, adjusting the pH value to be 1.3-1.5 by using 0.1-1 mol/L HCl or NaOH solution, adding the glycine aqueous solution prepared in the step (3), heating the reaction solution to 40 ℃, adding the reducer aqueous solution prepared in the step (4), and continuously stirring until the reaction is complete;
6. standing the reaction solution obtained in the step (5), precipitating, pouring out supernatant, repeatedly washing with deionized water for three times, washing with ethanol for 2 times, and drying in an oven at 80 ℃ to obtain submicron-level gold powder with irregular morphology.
As can be seen from fig. 1 and 2, example 2 increases the molar ratio of the reducing agent to chloroauric acid, and the particle size of the prepared gold powder particles is increased, compared to example 1. As the reducing agent containing imidazole functional groups, imidazole contains two nitrogen atoms, which can complex gold ions, reduce the reaction rate and prolong the grain size growth process, so that the grain size of the gold powder prepared in the embodiment 2 is increased.
Claims (10)
1. The preparation method of the gold powder for matching the low-temperature co-fired ceramic is characterized by comprising the following steps of:
(1) Dissolving 99.99% gold sheet with aqua regia, removing nitric acid and excessive hydrochloric acid, and preparing into 1mol/L HAuCl with deionized water 4 A solution;
(2) Dissolving dispersant in deionized water, dispersing dispersant and HAuCl 4 The mass ratio of (2) is 1-5: 100, deionized water and HAuCl 4 9:1 of the volume ratio of the solution;
(3) Dissolving amino acid in deionized water to obtain 1mol/L amino acid aqueous solution, and mixing amino acid with HAuCl 4 The molar ratio of (2) is 3:2;
(4) Dissolving reducer containing imidazole functional group in deionized water to prepare reducer solution with concentration of 1mol/L, and mixing reducer with HAuCl 4 The molar ratio of (2) to (3) to (2) is 2, and the temperature of the solution is properly increased;
(5) Under stirring, HAuCl prepared in step (1) 4 Pouring the solution into the dispersant solution prepared in the step (2), stirring for 15 periods of time, adding the amino acid aqueous solution prepared in the step (3), adjusting the pH value to be 1.3-1.4 by using HCl or NaOH solution with the concentration of 0.1-1 mol/L, properly raising the temperature of the solution, adding the reducer aqueous solution prepared in the step (4), and continuously stirring until the reaction is complete;
(6) Standing the reaction solution in the step (5), precipitating, pouring out supernatant, repeatedly washing with deionized water, washing with ethanol to replace water in the powder, and drying in an oven to obtain submicron-sized gold powder with irregular morphology and no caking.
2. The method of manufacturing according to claim 1, wherein: in the step (2), the amino acid is used as a gold ion complexing agent for reducing the reaction rate of gold ions and avoiding the generation of other morphologies.
3. The method of manufacturing according to claim 1, wherein: in step (2), the amino acid acts as a pH adjustor for the buffer and the reaction solution; for promoting stable reaction.
4. The method of manufacturing according to claim 1, wherein: the dispersing agent is one or more of polyvinylpyrrolidone, sodium dodecyl sulfate, sodium dodecyl benzene sulfonate, polyethylene glycol or ethylphenyl polyethylene glycol.
5. The method of manufacturing according to claim 1, wherein: the amino acid is one or more of glycine, alanine, valine, phenylalanine, glutamic acid, lysine or arginine.
6. The method of manufacturing according to claim 1, wherein: the reducing agent is one or more of imidazole, 2-methyl-4-ethylimidazole, indazole, benzimidazole or histidine.
7. The method of manufacturing according to claim 1, wherein: in step (4) and step (5), the solution temperature was raised to 40 ℃.
8. The method of manufacturing according to claim 1, wherein: in the step (5), about 1ml of the reaction solution is taken out, whether the reaction is complete or not is tested by using hydrazine hydrate, and if the reaction solution turns black or purple, the reaction is continuously stirred; if the color of the reaction solution is not changed, the reaction is complete.
9. The method of manufacturing according to claim 1, wherein: in the step (6), the deionized water is repeatedly washed for more than three times, and ethanol is used for washing for more than 2 times; the oven drying temperature was 80 ℃.
10. The preparation method of any one of claims 1 to 9, wherein the particle size of the prepared gold powder is 200nm to 900nm, and the warping degree is less than 0.1mm.
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| CN202310894323.9A CN117123791A (en) | 2023-07-20 | 2023-07-20 | Preparation method of gold powder for matching low-temperature co-fired ceramics |
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