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US20080105085A1 - Method Of Production Of High Purity Silver Particles - Google Patents

Method Of Production Of High Purity Silver Particles Download PDF

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Publication number
US20080105085A1
US20080105085A1 US11/664,640 US66464005A US2008105085A1 US 20080105085 A1 US20080105085 A1 US 20080105085A1 US 66464005 A US66464005 A US 66464005A US 2008105085 A1 US2008105085 A1 US 2008105085A1
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US
United States
Prior art keywords
silver
surfactants
surfactant
oxalate
group
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Abandoned
Application number
US11/664,640
Other languages
English (en)
Inventor
Insoo Kim
Chang Gun Lee
Sang Ho Kim
Charles E. Smith
Young Jin Kim
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
TOKUSEN U Inc SA
Tokusen USA Inc
Original Assignee
Tokusen USA Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Tokusen USA Inc filed Critical Tokusen USA Inc
Priority to US11/664,640 priority Critical patent/US20080105085A1/en
Assigned to TOKUSEN U.S.A., INC. reassignment TOKUSEN U.S.A., INC. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: SMITH, CHARLES E., JR., KIM, YOUNG JIN, KIM, SANG HO, LEE, CHANG GUN, KIM, INSOO
Publication of US20080105085A1 publication Critical patent/US20080105085A1/en
Abandoned legal-status Critical Current

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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F9/00Making metallic powder or suspensions thereof
    • B22F9/16Making metallic powder or suspensions thereof using chemical processes
    • B22F9/18Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds
    • B22F9/20Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds starting from solid metal compounds
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F9/00Making metallic powder or suspensions thereof
    • B22F9/16Making metallic powder or suspensions thereof using chemical processes
    • B22F9/30Making metallic powder or suspensions thereof using chemical processes with decomposition of metal compounds, e.g. by pyrolysis
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F9/00Making metallic powder or suspensions thereof
    • B22F9/16Making metallic powder or suspensions thereof using chemical processes
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F9/00Making metallic powder or suspensions thereof
    • B22F9/16Making metallic powder or suspensions thereof using chemical processes
    • B22F9/18Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2998/00Supplementary information concerning processes or compositions relating to powder metallurgy
    • B22F2998/10Processes characterised by the sequence of their steps
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B22CASTING; POWDER METALLURGY
    • B22FWORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2999/00Aspects linked to processes or compositions used in powder metallurgy

Definitions

  • the present invention relates to a method of forming silver particles by dispersing silver oxalate into an appropriate carrier and then applying heat at a temperature of 100° C. or higher to decompose the silver oxalate.
  • a number of methods have been developed to synthesize silver particles including, but not limited to, chemical reduction, photochemical, sonochemical and gas evaporation methods.
  • chemical reduction method is widely used due to the ease of production.
  • silver powder produced using the chemical reduction method can be contaminated by the reducing agent, the surfactant and impurity ions used during the reaction process, which can serve as a limiting factor in the field of electronics requiring high conductivity or in the field of bacteria resistance requiring high purity.
  • the object of the present invention is to synthesize high purity silver particles and colloids in a process that does not require either surfactants or reducing agents, or only a minimal amount of a surfactant.
  • this object is achieved by dispersing silver oxalates into an appropriate carrier and then thermally decomposing the silver oxalates at a temperature of 100° C. or higher to synthesize high purity silver particles and colloids.
  • the process of synthesizing silver particles and colloids by the method of the present invention comprises: (i) a silver oxalate synthesizing process; (ii) a process of dispersing silver oxalates into an appropriate carrier, for example, water, alcohol or the like, including a combination of more than one carrier; and (iii) a process of heating said silver oxalates dispersed into said carrier at a temperature of 100° C. or higher under a pressure greater than atmospheric pressure.
  • FIG. 1 is a microphotograph of silver particles obtained under the conditions described in Example 1.
  • FIG. 2 is a microphotograph of silver particles obtained under the conditions described in Example 2.
  • FIG. 3 is a microphotograph of silver particles obtained under the conditions described in Example 3.
  • FIG. 4 is a microphotograph of silver particles obtained under the conditions described in Example 4.
  • FIG. 5 is a microphotograph of silver particles obtained under the conditions described in Example 5.
  • FIG. 6 is a microphotograph of silver particles obtained under the conditions described in Example 6.
  • a method for the production of silver particles and colloids comprises three processes as follows: (i) a silver oxalate (Ag 2 C 2 o 4 ) synthesizing process; (ii) a process of dispersing silver oxalate into an appropriate carrier, for example, water, alcohol or the like, including a combination of more than one carrier; and (iii) a process of heating said silver oxalate dispersed into said carrier at a temperature of 100° C. or higher under a pressure greater than atmospheric pressure to form silver particle or colloids from the decomposition of the silver oxalate.
  • a silver oxalate Ag 2 C 2 o 4
  • a first solution of a water soluble silver compound and a second solution of an oxalate compound are mixed together to precipitate silver oxalates.
  • the silver compound may be AgNO 3 .
  • the oxalate compound may be sodium oxalate or oxalic acid.
  • the present invention is not, however, limited to these specific compounds but may include any two solutions of compounds that form silver oxalates upon mixing. After water cleaning processes, preferably two or more rounds of water cleaning processes, are performed to remove impure ions from the precipitated silver oxalate, the silver oxalate is used as the starting material for synthesizing silver powder or colloids.
  • the synthesized silver oxalate is dispersed into an appropriate carrier.
  • the silver oxalate is not dissolved to any substantial extent in the carrier, but is dispersed as solid particles by using ultrasonic treatment.
  • the appropriate carrier may include all types of carriers which can disperse silver oxalate to effectively deliver heat.
  • the carrier is selected to have properties that allow it to behave similarly to a surfactant so as to prevent agglomeration of the silver particles formed from the thermal decomposition of the silver oxalate.
  • alcohols consist of alkyl and hydroxyl groups. Generally, alkyl groups have hydrophobic properties and hydroxyl groups have hydrophilic properties. Organic materials having both hydrophobic and hydrophilic properties can play a role as a surfactant.
  • organic materials having higher carbon numbers tend to be dominantly hydrophobic and may therefore tend to lose the ability to act as a surfactant in the process of the present invention.
  • organic materials having higher numbers of carbon atoms have superior surfactant properties.
  • organic materials with a higher number of carbon atoms is observed to agglomerate silver particles.
  • organic materials with a higher number of carbon atoms do not mix well with water. Therefore, the present invention is limited to methyl, ethyl and propyl alcohols, which have a low number of carbon atoms. Water is also effective in the practice of the present invention.
  • the appropriate carrier may therefore consist of ethyl alcohol, methyl alcohol, propyl alcohol, water or a combination of more than one of the preceding.
  • the carriers selected for the practice of the present invention all have low boiling points: water (100° C.), methyl alcohol (64.65° C.), ethyl alcohol (78.3° C.), and propyl alcohol (82° C.). Accordingly, when the carrier with the dispersed silver oxalate is heated in a container at or above 100° C., the pressure is always above atmospheric pressure. Typical reaction pressures are about 1.86*10 5 N/m 2 when using water as the carrier and about 5.31*10 5 N/m 2 when using ethyl alcohol as the carrier.
  • the carbon dioxide gas evolved during the thermal decomposition of the silver oxalate and the carrier vapor may be evacuated as necessary but pressure drops of less than about 6.89*10 4 N/m 2 do not affect the quality of the silver particles.
  • the dispersed silver oxalate in the carrier is placed into a closed reactor to heat the dispersed silver oxalate and carrier up to at least 100° C. to synthesize silver powder or colloids of various form factors.
  • This method may optionally use surfactants in order to prevent coagulation or agglomeration of the silver particles.
  • Surfactants may be added to the water soluble silver or oxalate solutions used to produce silver oxalate, or may be added after the silver oxalate is produced by mixing the two solutions.
  • Surfactants used in this method may include anionic surfactants, cationic surfactants, amphoteric surfactants, nonionic surfactants, fluorochemical surfactants, and polymerizable surfactants, or combinations of the preceding, which may be added to aid in forming silver particles and to break down silver plates or prevent silver plates from coagulation.
  • Surfactants suitable for use in the present invention include PVP (polyvinyl pyrrolidone) and gelatine.
  • silver particles or colloids can be obtained by the method of the present invention, however, it is desirable to limit the amount of surfactant to no more than 80% of the weight of the silver. For example, if 10 grams of silver is placed into the reactor, the weight of the surfactant, such as PVP or gelatin, should be no more than 8 grams.
  • PVP polyvinyl pyrrolidone

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacture Of Metal Powder And Suspensions Thereof (AREA)
  • Colloid Chemistry (AREA)
US11/664,640 2004-10-14 2005-10-13 Method Of Production Of High Purity Silver Particles Abandoned US20080105085A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
US11/664,640 US20080105085A1 (en) 2004-10-14 2005-10-13 Method Of Production Of High Purity Silver Particles

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
US61887604P 2004-10-14 2004-10-14
US11/664,640 US20080105085A1 (en) 2004-10-14 2005-10-13 Method Of Production Of High Purity Silver Particles
PCT/US2005/036727 WO2006049831A1 (fr) 2004-10-14 2005-10-13 Procede de production de particules d'argent de haute purete

Publications (1)

Publication Number Publication Date
US20080105085A1 true US20080105085A1 (en) 2008-05-08

Family

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Family Applications (1)

Application Number Title Priority Date Filing Date
US11/664,640 Abandoned US20080105085A1 (en) 2004-10-14 2005-10-13 Method Of Production Of High Purity Silver Particles

Country Status (6)

Country Link
US (1) US20080105085A1 (fr)
EP (1) EP1819467A4 (fr)
JP (1) JP2008517153A (fr)
KR (1) KR100888559B1 (fr)
CN (1) CN101065205A (fr)
WO (1) WO2006049831A1 (fr)

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20080064592A1 (en) * 2004-10-14 2008-03-13 Insoo Kim Method for Synthesizing Nano-Sized Titanium Dioxide Particles
US20100226851A1 (en) * 2006-09-21 2010-09-09 Insoo Kim Low temperature process for producing nano-sized titanium dioxide particles
US20110088593A1 (en) * 2010-12-23 2011-04-21 Mansour Hemmati Silver dz nano-fluid composition for nano-fin formation and a method of producing the same
US9545668B2 (en) 2009-11-27 2017-01-17 Tokusen Kogyo Co., Ltd. Fine metal particle-containing composition
US20180096747A1 (en) * 2012-02-13 2018-04-05 Dowa Electronics Materials Co., Ltd. Spherical silver powder and method for producing same

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP4978242B2 (ja) * 2007-03-05 2012-07-18 昭栄化学工業株式会社 銀超微粒子の製造方法
TW201100185A (en) * 2009-05-01 2011-01-01 Du Pont Silver particles and a process for making them
JP5119362B2 (ja) * 2009-07-30 2013-01-16 国立大学法人京都大学 金属系ナノ粒子とそれを含んだ分散液及びその製造方法
KR20110113877A (ko) * 2010-04-12 2011-10-19 서울대학교산학협력단 균일한 크기를 가지는 은 나노입자의 대량 제조 방법
JP6182294B2 (ja) * 2011-01-28 2017-08-16 宣政 奥田 殺菌組成物及び医薬
FR2977178B1 (fr) * 2011-06-30 2014-05-16 Thales Sa Procede de fabrication d'un dispositif comprenant des brasures realisees a partir d'oxalate metallique
CN104884193B (zh) * 2012-08-30 2017-03-08 康宁股份有限公司 不含溶剂的银合成及由此制备的银产物
WO2014036270A1 (fr) 2012-08-31 2014-03-06 Corning Incorporated Procédés de récupération d'argent et produits en argent fabriqués au moyen de ces procédés
WO2014036261A1 (fr) 2012-08-31 2014-03-06 Corning Incorporated Synthèses d'argent à base de dispersions basse température et produits en argent fabriqués à partir de ces synthèses
TWI508799B (zh) * 2012-12-06 2015-11-21 China Steel Corp A Method for Synthesis of Silver Powder with Adjustable Particle Size
JP6157104B2 (ja) * 2012-12-14 2017-07-05 田中貴金属工業株式会社 銀化合物を製造するための銀前駆体及びその製造方法、並びに、銀化合物の製造方法
CN103602019B (zh) * 2013-11-15 2015-12-02 三河市京纳环保技术有限公司 一种新型大规模制备高透明塑料用含银无机抗菌母粒的方法

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US2426761A (en) * 1943-08-28 1947-09-02 Honorary Advisory Council Sci Preparation of silver catalysts
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US2426761A (en) * 1943-08-28 1947-09-02 Honorary Advisory Council Sci Preparation of silver catalysts
US3377160A (en) * 1964-12-31 1968-04-09 Allis Chalmers Mfg Co Process of making a high surface area silver catalyst
US3702259A (en) * 1970-12-02 1972-11-07 Shell Oil Co Chemical production of metallic silver deposits
US4186244A (en) * 1977-05-03 1980-01-29 Graham Magnetics Inc. Novel silver powder composition
US4463030A (en) * 1979-07-30 1984-07-31 Graham Magnetics Incorporated Process for forming novel silver powder composition
US5250101A (en) * 1991-04-08 1993-10-05 Mitsubishi Gas Chemical Company, Inc. Process for the production of fine powder
US5367328A (en) * 1993-10-20 1994-11-22 Lasermaster Corporation Automatic ink refill system for disposable ink jet cartridges
US5846511A (en) * 1995-06-19 1998-12-08 Korea Advanced Institute Of Science And Technology Process for preparing crystalline titania powders from a solution of titanium salt in a mixed solvent of water and alcohol
US5935608A (en) * 1996-04-15 1999-08-10 Nittetsu Mining Co., Ltd. Antibacterial titania and process for producing the same
US5973175A (en) * 1997-08-22 1999-10-26 E. I. Du Pont De Nemours And Company Hydrothermal process for making ultrafine metal oxide powders
US6114553A (en) * 1997-12-16 2000-09-05 Nippon Shokubai Co., Ltd. Silver catalyst for production of ethylene oxide, method for production thereof, and method for production of ethylene oxide
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US6001326A (en) * 1998-07-16 1999-12-14 Korea Atomic Energy Research Institute Method for production of mono-dispersed and crystalline TiO2 ultrafine powders for aqueous TiOCl2 solution using homogeneous precipitation
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US6706902B2 (en) * 2001-02-16 2004-03-16 Bayer Aktiengesellschaft Continuous process for the synthesis of nano-scale precious metal particles
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US20040151662A1 (en) * 2003-01-31 2004-08-05 Sumitomo Chemical Company, Limited Method for producing titanium oxide
US6969690B2 (en) * 2003-03-21 2005-11-29 The University Of North Carolina At Chapel Hill Methods and apparatus for patterned deposition of nanostructure-containing materials by self-assembly and related articles
US20060251573A1 (en) * 2004-03-19 2006-11-09 Musick Charles D Titanium dioxide nanopowder manufacturing process
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US7270695B2 (en) * 2004-04-01 2007-09-18 Dong-A University Synthesis of nanosized metal particles
US20050234178A1 (en) * 2004-04-16 2005-10-20 Andrews John W Metal peroxide films
US20050265918A1 (en) * 2004-06-01 2005-12-01 Wen-Chuan Liu Method for manufacturing nanometer scale crystal titanium dioxide photo-catalyst sol-gel
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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20080064592A1 (en) * 2004-10-14 2008-03-13 Insoo Kim Method for Synthesizing Nano-Sized Titanium Dioxide Particles
US20100226851A1 (en) * 2006-09-21 2010-09-09 Insoo Kim Low temperature process for producing nano-sized titanium dioxide particles
US8557217B2 (en) 2006-09-21 2013-10-15 Tokusen, U.S.A., Inc. Low temperature process for producing nano-sized titanium dioxide particles
US9545668B2 (en) 2009-11-27 2017-01-17 Tokusen Kogyo Co., Ltd. Fine metal particle-containing composition
US20110088593A1 (en) * 2010-12-23 2011-04-21 Mansour Hemmati Silver dz nano-fluid composition for nano-fin formation and a method of producing the same
US20180096747A1 (en) * 2012-02-13 2018-04-05 Dowa Electronics Materials Co., Ltd. Spherical silver powder and method for producing same

Also Published As

Publication number Publication date
EP1819467A4 (fr) 2010-01-20
WO2006049831A1 (fr) 2006-05-11
KR100888559B1 (ko) 2009-03-16
KR20070073775A (ko) 2007-07-10
JP2008517153A (ja) 2008-05-22
CN101065205A (zh) 2007-10-31
EP1819467A1 (fr) 2007-08-22

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