EP3527678A1 - Legierung auf gold-kupfer-basis, ihr herstellungsverfahren und ihre verwendung - Google Patents

Legierung auf gold-kupfer-basis, ihr herstellungsverfahren und ihre verwendung Download PDF

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Publication number
EP3527678A1
EP3527678A1 EP18156884.1A EP18156884A EP3527678A1 EP 3527678 A1 EP3527678 A1 EP 3527678A1 EP 18156884 A EP18156884 A EP 18156884A EP 3527678 A1 EP3527678 A1 EP 3527678A1
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EP
European Patent Office
Prior art keywords
alloy
gold
copper
palladium
tin
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.)
Granted
Application number
EP18156884.1A
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English (en)
French (fr)
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EP3527678B1 (de
Inventor
Fanny LALIRE
Frédéric DIOLOGENT
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.)
Richemont International SA
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Richemont International SA
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Publication date
Application filed by Richemont International SA filed Critical Richemont International SA
Priority to EP18156884.1A priority Critical patent/EP3527678B1/de
Priority to PCT/EP2019/053325 priority patent/WO2019158481A1/fr
Publication of EP3527678A1 publication Critical patent/EP3527678A1/de
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C5/00—Alloys based on noble metals
    • C22C5/02—Alloys based on gold
    • G—PHYSICS
    • G04—HOROLOGY
    • G04B—MECHANICALLY-DRIVEN CLOCKS OR WATCHES; MECHANICAL PARTS OF CLOCKS OR WATCHES IN GENERAL; TIME PIECES USING THE POSITION OF THE SUN, MOON OR STARS
    • G04B37/00—Cases
    • G04B37/22—Materials or processes of manufacturing pocket watch or wrist watch cases

Definitions

  • the present invention relates to an alloy based on gold and copper.
  • This alloy pink (4N) or red (5N and 6N), can be used in particular in the fields of jewelery and watchmaking.
  • Gold has always been mixed with other metals in order to modify its properties. Depending on the nature of the metal or metals introduced and their amounts, it is possible in particular to modulate the rigidity or the color of the gold.
  • an alloy comprising 75% by weight of gold, 12.5% of copper and 12.5% of silver corresponds to yellow gold.
  • An alloy comprising 75% gold, 20% copper and 5% agent corresponds to pink gold.
  • an alloy (Au750 Pd125 Ag30 Cu95) comprising for example 75% gold, 30% silver, 125% of palladium and 95% of copper corresponds to the gray gold.
  • the color of the alloy can be determined by the CIE L * a * b * color space, the CIE being the International Commission on Illumination.
  • conventional gold or red gold or red gold alloys correspond to zones 4N, 5N and 6N of the figure 2 .
  • this alloy is subject to a fading phenomenon over time by yellowing. This phenomenon corresponds to the corrosion of the copper and to the increase of the gold metal concentration on the surface of the alloy.
  • the document JP 10 245646 discloses an 18-carat pink gold alloy comprising between 15.0 and 23.0% by weight of copper and between 0.3 and 5.0% of palladium.
  • the document WO 2015/038636 discloses an alloy not containing tin. This alloy comprises 12.7 to 14.7% silver, 9.3 to 11.3% copper, 0.5 to 2% palladium, the balance being gold.
  • the present invention presents an alternative through the development of a gold-based alloy limiting or eliminating copper corrosion, and thus the phenomenon of discoloration over time.
  • the Applicant has developed a gold-based alloy for solving the discoloration problems of alloys of the prior art through the presence of specific amounts of several metals.
  • This alloy is non-tarnishing and non-discoloring over time, which provides an undeniable advantage in areas such as jewelery and watchmaking avoiding returns of articles related to this issue.
  • the CIE L * a * b * coordinates may in particular be obtained by means of a conventional spectrophotometer, by measuring the reflectance properties as a function of the illumination wavelength.
  • the alloy according to the invention is pink (4N) or red (5N and 6N). It is preferably located in one of the zones 4N, 5N or 6N of the CIE L * a * b * color space, or in an intermediate zone between the 4N, 5N or 6N zones ( figure 2 ).
  • the alloy according to the invention corresponds to the zone 5N.
  • Zones 4N 5N and 6N are advantageously defined according to ISO 8654 and this, in accordance with the practice of the skilled person.
  • the alloys Au752Cu158Ag78Pd4Sn8, Au752Cu210Ag22Pd5Sn11 and Au752Cu233Ag2Pd10Sn3 correspond to particular embodiments of the invention.
  • the quantity of each element is expressed in tenths of mass percentage.
  • the Au752Cu158Ag78Pd4Sn8 alloy therefore consists of 752 ⁇ of gold, 158 ⁇ of copper, 78 ⁇ of silver, 4 ⁇ of palladium and 8 ⁇ of tin.
  • the alloy according to the invention is free of nickel, chromium, niobium, hafnium and yttrium.
  • the alloy according to the invention can be made of gold, copper, silver, palladium and tin.
  • the sum of the percentages of the metals gold, copper, silver, palladium and tin is equal to 100.
  • the alloy according to the invention comprises 2% or less of titanium. In other words, it comprises between 0% and 2% of titanium.
  • the alloy according to the invention may comprise titanium, advantageously between 0.05% and 2% by weight relative to the mass of the alloy, more advantageously between 0.1% and 2%. and even more preferably between 0.8 and 1.5%.
  • the alloy according to the invention can thus be made of gold, copper, silver, palladium, tin, and titanium.
  • the sum of the percentages of the metals gold, copper, silver, palladium, tin and titanium is equal to 100.
  • the mass percentage of gold in the alloy is between 75% and 77.5%, advantageously between 75% and 75.5%.
  • the quantities of elements are expressed as a percentage by weight or as a percentage by mass percentage (ppm) relative to the mass of the alloy.
  • ppm percentage by mass percentage
  • Value ranges include terminals.
  • the value range "between 75% and 77.5%” includes 75% and 77.5% values.
  • the description discloses all possible combinations between the terminals of the different ranges of values.
  • the disclosure of the ranges 10% to 24%, advantageously 15% to 22% includes in particular the ranges 10% to 15%, 10% to 22%, 15% to 24% or 22% to 24%.
  • the alloy according to the invention has a homogeneous composition. Indeed, its various elements are distributed homogeneously within the alloy. This alloy necessarily includes the following five elements: gold, silver copper, palladium is tin. It may comprise a total of 13 elements: gold, copper, silver, palladium, tin, titanium, ruthenium, rhenium, iron, iridium, cobalt, vanadium and molybdenum.
  • Copper makes it possible to obtain the pink (4N) or red (5N and 6N) color of the alloy.
  • the corrosion in time of the copper of the alloy causes a color change, the alloy gradually changing from pink / red to yellow.
  • the mass percentage of copper in the alloy is between 10% and 24%, advantageously between 15% and 22%.
  • Silver makes it possible to fix the copper within the alloy.
  • silver has the disadvantage of whitening the alloy away from the color areas of interest.
  • the mass percentage of silver in the alloy is between 0.1% and 10.0%, advantageously between 1% and 4%.
  • palladium can limit or stop discoloration by acting on the corrosion of copper. However, it also has a whitening effect of the alloy. Thus, too much palladium can interfere with obtaining a pink (4N) or red (5N and 6N) color alloy. It is therefore important to limit the amount of palladium (1.1%) so as not to deviate from the areas of color of interest.
  • the mass percentage of palladium in the alloy is between 0.1% and 1.1%, advantageously between 0.3% and 0.8%.
  • Tin reduces the corrosion of copper, but to a lesser extent than palladium.
  • synergistic effects between tin and palladium appear to exist in terms of optimizing corrosion resistance.
  • tin does not exhibit the undesirable whitening effect of palladium.
  • the mass percentage of tin in the alloy is between 0.1% and 2.0%, advantageously between 0.5% and 1.5%.
  • the alloy according to the invention has a compromise between silver, palladium and tin to obtain the required properties not only in terms of color but also for use in watchmaking or jewelery.
  • titanium also reduces the phenomenon of discoloration while having a negligible impact on the color of the alloy. This effect is observed when the titanium represents between 0.05% and 2% by weight of the alloy, more particularly when the titanium advantageously represents 0.05 to 0.5% by weight of the alloy.
  • Titanium makes it possible to slow down the kinetics of ordering in the alloy according to the invention, and this, in order to optimize the stability of the alloy during the different stages of the manufacturing process (deformation, heat treatments, soldering, etc.). .). This effect is particularly observed when the titanium represents between 0.05% and 2% by weight of the alloy, more particularly when the titanium advantageously represents 1.5 to 2% by weight of the alloy.
  • titanium partially replaces palladium.
  • the elements titanium, tin, indium and germanium slow down the phenomenon of discoloration / de-alloying (selective dissolution of certain elements) existing in 18-carat pink and red gold.
  • the alloy according to the invention comprises 0.2% or less of at least one grain refining element (Ru, Re, Fe, Ir, Co, V, Mo). In other words, it includes between 0% and 0.2% of at least one grain refining element.
  • at least one grain refining element Ru, Re, Fe, Ir, Co, V, Mo.
  • the alloy according to the invention may also comprise at least one grain refining element.
  • the grain refiner is 0.2% or less based on the mass of the alloy, more preferably 0.1% or less. In general, when it is present, the grain refiner represents at least 0.001% by weight relative to the mass of the alloy (ie 10 ppm). It is a member selected from the group consisting of ruthenium, rhenium, iron, iridium, cobalt, vanadium, molybdenum and mixtures thereof. Elements such as ruthenium, rhenium or iron guarantee the fineness of the grain, without significantly modifying the hardness, nor affect the color.
  • the alloy according to the invention consists of 97.8% by mass or more of the elements gold, copper, silver, palladium and tin.
  • the alloy according to the invention comprises between 97.8% and 100% by weight of the elements gold, copper, silver, palladium and tin.
  • step a the respective percentages of the metals correspond to the percentages of the final alloy. This step is performed conventionally, according to the techniques known to those skilled in the art.
  • Step b) consists of melting the various metals so as to form a homogeneous mixture. This step is advantageously carried out by heating the mixture until the desired temperature is reached.
  • the temperature rise kinetics (° C / min) generally not being important, the setting of alloy is advantageously carried out in a crucible, for example with induction heating.
  • Cooling step c) makes it possible to freeze the structure of the alloy. It advantageously consists in carrying out a thermal quenching in air or in water.
  • the alloys obtained in these two ways have similar hardness properties, which provides an additional advantage.
  • the alloy according to the invention can be used (deformation, heat treatment, brazing %) without its mechanical properties and its color being altered.
  • the alloy thus obtained can then be shaped.
  • the shaping is carried out by cold or hot deformation, then by machining, for example by means of a cutting tool or by electro-erosion or by means of of a laser.
  • the shaping can be performed by additive manufacturing.
  • the alloy is previously converted into powder form.
  • Also part of the present invention is the use of this gold alloy in the field of jewelery; the use of this gold alloy in the field of watchmaking; jewelery articles comprising or consisting of this gold alloy; timepieces comprising or consisting of this gold alloy.
  • the hardness (measured on the raw casting structures) of these alloys according to the invention is similar, whether they have been obtained after thermal quenching or after quenching in air, which is not always the case with alloys not corresponding to the composition according to the invention.
  • the figure 4 shows the difference in hardness ( ⁇ hardness) between water-quenched alloys and quenched alloys, as a function of time.
  • pellets having a diameter of 15 mm and a thickness of 2 mm were prepared.
  • the diameter is at least 10 mm, which corresponds to the size of the sensor.
  • Table 2 Aging tests of the alloys according to the invention.
  • Fog NaCl (50 ⁇ 5 g / L) observations after 1, 3 and 7 days after 24 and 48 hours after 24 and 48 hours after 24
  • the alloy according to the invention solves the problems related to the discoloration of the alloy under normal conditions of use.
  • the figure 5 shows that the INV-3 alloy of Table 1 has a small color change over time, compared to a conventional Au750Ag45Cu205 alloy after aging for several days (synthetic sweat, bath or salt spray).
  • the figures 1 and 3 show the color change for alloys not forming part of the invention.
  • the figure 1 highlights the decrease in the phenomenon of discoloration over time when part of the copper is substituted by palladium.
  • the bleaching effect of palladium is highlighted by the figure 2 . Indeed, the more the alloy contains palladium, the more it moves away from the 6N color zone.
  • the figure 3 highlights the decrease in the phenomenon of discoloration over time in the presence of palladium and a member selected from germanium, indium, tin and titanium relative to an Au750Cu205Ag45 type alloy.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Physics & Mathematics (AREA)
  • General Physics & Mathematics (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Adornments (AREA)
EP18156884.1A 2018-02-15 2018-02-15 Legierung auf gold-kupfer-basis, ihr herstellungsverfahren und ihre verwendung Active EP3527678B1 (de)

Priority Applications (2)

Application Number Priority Date Filing Date Title
EP18156884.1A EP3527678B1 (de) 2018-02-15 2018-02-15 Legierung auf gold-kupfer-basis, ihr herstellungsverfahren und ihre verwendung
PCT/EP2019/053325 WO2019158481A1 (fr) 2018-02-15 2019-02-11 Alliage a base d'or et de cuivre, son procede de preparation et son utilisation

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP18156884.1A EP3527678B1 (de) 2018-02-15 2018-02-15 Legierung auf gold-kupfer-basis, ihr herstellungsverfahren und ihre verwendung

Publications (2)

Publication Number Publication Date
EP3527678A1 true EP3527678A1 (de) 2019-08-21
EP3527678B1 EP3527678B1 (de) 2021-06-02

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EP18156884.1A Active EP3527678B1 (de) 2018-02-15 2018-02-15 Legierung auf gold-kupfer-basis, ihr herstellungsverfahren und ihre verwendung

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WO (1) WO2019158481A1 (de)

Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH10245646A (ja) 1997-03-07 1998-09-14 Seiko Epson Corp 金合金、装飾部材、携帯時計及び装飾部材の製造方法
US5919320A (en) * 1997-11-17 1999-07-06 Leach & Garner Company Nickel-free white gold alloy with reversible hardness characteristics
GB2447620A (en) * 2007-03-21 2008-09-24 Sarah J Corbridge Alloys of gold which contain tin
JP2008308757A (ja) * 2007-05-15 2008-12-25 Raapisu:Kk 装飾用および歯科用金合金
EP2776597A1 (de) 2011-11-08 2014-09-17 The Swatch Group Research and Development Ltd. Golduhr oder schmuckstück
WO2015038636A1 (en) 2013-09-10 2015-03-19 Apple Inc. Crystalline gold alloys with improved hardness
WO2015173790A1 (en) * 2014-05-16 2015-11-19 Repl. Progold S.P.A. Use of gold powder alloys for manufacturing jewellery items by selective laser melting

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CH709207B1 (it) * 2012-12-03 2018-08-15 Argor Heraeus Sa Lega d'oro resistente alla decolorazione.

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH10245646A (ja) 1997-03-07 1998-09-14 Seiko Epson Corp 金合金、装飾部材、携帯時計及び装飾部材の製造方法
US5919320A (en) * 1997-11-17 1999-07-06 Leach & Garner Company Nickel-free white gold alloy with reversible hardness characteristics
GB2447620A (en) * 2007-03-21 2008-09-24 Sarah J Corbridge Alloys of gold which contain tin
JP2008308757A (ja) * 2007-05-15 2008-12-25 Raapisu:Kk 装飾用および歯科用金合金
EP2776597A1 (de) 2011-11-08 2014-09-17 The Swatch Group Research and Development Ltd. Golduhr oder schmuckstück
US20140305164A1 (en) * 2011-11-08 2014-10-16 The Swatch Group Research And Development Ltd. Timepiece or piece of jewellery made of gold
WO2015038636A1 (en) 2013-09-10 2015-03-19 Apple Inc. Crystalline gold alloys with improved hardness
WO2015173790A1 (en) * 2014-05-16 2015-11-19 Repl. Progold S.P.A. Use of gold powder alloys for manufacturing jewellery items by selective laser melting

Also Published As

Publication number Publication date
WO2019158481A1 (fr) 2019-08-22
EP3527678B1 (de) 2021-06-02

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