US3627517A - Ternary fusible alloy - Google Patents
Ternary fusible alloy Download PDFInfo
- Publication number
- US3627517A US3627517A US783764A US3627517DA US3627517A US 3627517 A US3627517 A US 3627517A US 783764 A US783764 A US 783764A US 3627517D A US3627517D A US 3627517DA US 3627517 A US3627517 A US 3627517A
- Authority
- US
- United States
- Prior art keywords
- alloy
- ternary
- fusible
- eutectic
- melting
- 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.)
- Expired - Lifetime
Links
- 229910000743 fusible alloy Inorganic materials 0.000 title description 8
- 230000008018 melting Effects 0.000 abstract description 18
- 238000002844 melting Methods 0.000 abstract description 18
- 230000005496 eutectics Effects 0.000 abstract description 12
- 229910052709 silver Inorganic materials 0.000 abstract description 7
- 239000004332 silver Substances 0.000 abstract description 6
- 229910002058 ternary alloy Inorganic materials 0.000 abstract description 6
- 229910052738 indium Inorganic materials 0.000 abstract description 5
- 229910052718 tin Inorganic materials 0.000 abstract description 5
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 abstract description 4
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 abstract description 4
- 229910045601 alloy Inorganic materials 0.000 description 17
- 239000000956 alloy Substances 0.000 description 17
- 239000000203 mixture Substances 0.000 description 10
- 239000012071 phase Substances 0.000 description 8
- 230000007704 transition Effects 0.000 description 8
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 229910052802 copper Inorganic materials 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000000155 melt Substances 0.000 description 3
- 230000001681 protective effect Effects 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 229910020836 Sn-Ag Inorganic materials 0.000 description 2
- 229910020988 Sn—Ag Inorganic materials 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 229910002056 binary alloy Inorganic materials 0.000 description 2
- 238000002425 crystallisation Methods 0.000 description 2
- 230000008025 crystallization Effects 0.000 description 2
- 230000006870 function Effects 0.000 description 2
- 230000004927 fusion Effects 0.000 description 2
- 238000011835 investigation Methods 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 238000007792 addition Methods 0.000 description 1
- 230000003466 anti-cipated effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 230000002860 competitive effect Effects 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000008014 freezing Effects 0.000 description 1
- 238000007710 freezing Methods 0.000 description 1
- 238000003780 insertion Methods 0.000 description 1
- 230000037431 insertion Effects 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000012768 molten material Substances 0.000 description 1
- 230000002028 premature Effects 0.000 description 1
- 230000009993 protective function Effects 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 238000005204 segregation Methods 0.000 description 1
- 238000005382 thermal cycling Methods 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01H—ELECTRIC SWITCHES; RELAYS; SELECTORS; EMERGENCY PROTECTIVE DEVICES
- H01H85/00—Protective devices in which the current flows through a part of fusible material and this current is interrupted by displacement of the fusible material when this current becomes excessive
- H01H85/02—Details
- H01H85/04—Fuses, i.e. expendable parts of the protective device, e.g. cartridges
- H01H85/05—Component parts thereof
- H01H85/055—Fusible members
- H01H85/06—Fusible members characterised by the fusible material
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C13/00—Alloys based on tin
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C28/00—Alloys based on a metal not provided for in groups C22C5/00 - C22C27/00
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01H—ELECTRIC SWITCHES; RELAYS; SELECTORS; EMERGENCY PROTECTIVE DEVICES
- H01H37/00—Thermally-actuated switches
- H01H37/74—Switches in which only the opening movement or only the closing movement of a contact is effected by heating or cooling
- H01H37/76—Contact member actuated by melting of fusible material, actuated due to burning of combustible material or due to explosion of explosive material
- H01H2037/768—Contact member actuated by melting of fusible material, actuated due to burning of combustible material or due to explosion of explosive material characterised by the composition of the fusible material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01H—ELECTRIC SWITCHES; RELAYS; SELECTORS; EMERGENCY PROTECTIVE DEVICES
- H01H37/00—Thermally-actuated switches
- H01H37/74—Switches in which only the opening movement or only the closing movement of a contact is effected by heating or cooling
- H01H37/76—Contact member actuated by melting of fusible material, actuated due to burning of combustible material or due to explosion of explosive material
- H01H37/761—Contact member actuated by melting of fusible material, actuated due to burning of combustible material or due to explosion of explosive material with a fusible element forming part of the switched circuit
Definitions
- This invention relates to fusible or low melting point alloys and, more particularly, to a ternary alloy suitable for use in the manufacture of thermal protective devices for electrical circuitry.
- fusible link comprising a length of a suitable low-melting alloy.
- Such links are subject to stringent temperature-time standards or, in other words, must be capable of melting rapidly at a specified temperature in order to drop out of and disrupt a circuit when critical conditions arise.
- a fusible link or the alloy from which it is made, to be suitable in every respect, must be characterized by rapid and substantially isothermal phase transition from solid to liquid.
- the alloy must possess satisfactory mechanical strength and good resistance to the formation of surface films (occurring primarily through the agency of oxidation), such that the desired response to critical temperature changes remains unimpaired.
- an alloy in order to be satisfactory in use as a fusible link, must remain substantially solid with limited expansion or contraction until the temperature in its operative environment reaches a predetermined point. At that time, the alloy must transform rapidly and substantially isothermally to the liquid phase, dropping out of circuit and thus disrupting the latter.
- the temperature range over which an alloy melts may be termed a function of the variation as between the crystallization rates of the components elements, while the phase transition time may be stated as a function of the various crystallization rates considered together with the latent heat of fusion of the particular composition.
- the melting point of an alloy bears no apparent relationship to the individual melting points of its components and, similarly, it is extremely difiicult to predict, with any accuracy, the numerical value of latent heat of fusion of an alloy merely by reference to the characteristics of the individual elements involved.
- Copper was found to provide a definite decrease in melting point while silver has an even more desirable effect.
- metallographic examination of a sample of the new alloy revealed a substantially homogenous structure over the entire cross-section, indicative of a eutectic or near-eutectic composition.
- the true eutectic is the most preferred composition when one considers the desirability of a pure isothermal transition, but observation has established that for the purpose in question, the alloy may be comprised within the approximate composition given and still melt at a temperature in the prescribed area.
- a fusible link manufactured from the novel material proved to have satisfactory mechanical strength for its purpose and exhibited good resistance to surface film formation (oxidation).
- the new ternary alloy of In- Sn-Ag is eminently suitable for use in the manufacture of fusible links while additions of about 0.17% copper to the In-Sn eutectic result in an alloy suitable for use under present regulations, having an M.P. of 1l7.6 C. :1" C.
- the ternary fusible alloy according to the present invention can be processed to any desired configuration for use as a fusible link.
- any desired configuration for use as a fusible link.
- such use is not intended as being exhaustive of the overall utility of the alloy.
- Pat. No. 3,354,282 reveals a thermal fuse with capillary action in which the molten fusible link will separate reliably and completely under any practical service conditions, in any position, and after long, useful life.
- a tubular sleeve Enclosed within a tubular sleeve is a fusible link and a means attached to each end of the fusible link for providing capillary action on the molten fuse link so that when the fusible link melts upon increase of the environmental temperature beyond its melting point, the molten material is withdrawn into the capillary means thus en suring that the current flow in the electrical lead is entirely interrupted.
- a ternary fusible alloy comprising a substantially eutectic composition of ln-Sn with the balance made up of silver.
- a ternary fusible alloy having a composition of about 51.4% In, 47.3% Sn, and 1.3% Ag, characterized by a melting point of 113.811 C.
- a ternary fusible alloy as recited in claim 1, wherein the composition is chosen to have the lowest possible melting point, which is approximately 114 C.
- a ternary fusible alloy as recited in claim 1, wherein a sufiicient amount of silver is added to the ln-Sn to lower its melting point below the 117 C. minimum melting point of an In-Sn eutectic.
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Fuses (AREA)
Abstract
A LOW TEMPERATURE MELTING TERNARY ALLOY SUITABLE FOR THERMAL FUSES IN BALLASTS CONTAINING EUTECTIC OF INDIUM, TIN, AND THE BALANCE SILVER OR COPPER.
Description
United States Patent Oce 3,627,517 Patented Dec. 14, 1971 Int. Cl. C22c 31/00 US. Cl. 75-134 T 4 Claims ABSTRACT OF THE DISCLOSURE A low temperature melting ternary alloy suitable for thermal fuses in ballasts containing eutectic of indium, tin, and the balance silver or copper.
BACKGROUND OF THE INVENTION This invention relates to fusible or low melting point alloys and, more particularly, to a ternary alloy suitable for use in the manufacture of thermal protective devices for electrical circuitry.
In most industrial countries, authorities such as CSA in Canada, and Underwriters Laboratory in the United States, are set up and maintained for the specific purpose of establishing safety standards in respect of manufactured products, technical installation procedures and the like.
Insofar as electrical circuitry is concerned, regulations have been laid down in the interests of public safety requiring insertion of protective devices which will disrupt associated circuits should any potentially dangerous condition occur.
One type of protective device, widely used, for example, in ballasts or fluorescent lights, is the fusible link comprising a length of a suitable low-melting alloy. Such links are subject to stringent temperature-time standards or, in other words, must be capable of melting rapidly at a specified temperature in order to drop out of and disrupt a circuit when critical conditions arise.
However, while the safety standards set by the authorities must be met, a fusible link, in order to command a competitive position in the market, must be capable of maintaining its associated circuit in operation up to the maximum temperature permitted.
In short, a fusible link, or the alloy from which it is made, to be suitable in every respect, must be characterized by rapid and substantially isothermal phase transition from solid to liquid.
Additionally, the alloy must possess satisfactory mechanical strength and good resistance to the formation of surface films (occurring primarily through the agency of oxidation), such that the desired response to critical temperature changes remains unimpaired.
Put in another way, an alloy, in order to be satisfactory in use as a fusible link, must remain substantially solid with limited expansion or contraction until the temperature in its operative environment reaches a predetermined point. At that time, the alloy must transform rapidly and substantially isothermally to the liquid phase, dropping out of circuit and thus disrupting the latter.
Obviously, the formation of surface films could well alter the melting characteristics of a fusible link. Further, to avoid premature circuit discontinuity arising from permissible temperature fluctuations below the critical point, and to negate excursions slightly beyond that same point, the alloy must change phase in a sharply defined manner so that the link maintains its integrity substantially up to the melting point but not beyond it.
The requirements for a fusible link alloy thus call for the use of a eutectic or near-eutectic composition wherein, as is well known, the phase transition from solid to liquid occurs in an isothermal or near-isothermal manner.
In non-eutectic compositions, repeated thermal cycling through the melt point can cause segregation of elements and gradual variation of the melting and freezing characteristics. However, in the field with which the present invention is concerned, such cycling and its inherent problems are of no consequence since a fusible link is naturally discarded after a single cycle.
The temperature range over which an alloy melts may be termed a function of the variation as between the crystallization rates of the components elements, while the phase transition time may be stated as a function of the various crystallization rates considered together with the latent heat of fusion of the particular composition.
However, the melting point of an alloy bears no apparent relationship to the individual melting points of its components and, similarly, it is extremely difiicult to predict, with any accuracy, the numerical value of latent heat of fusion of an alloy merely by reference to the characteristics of the individual elements involved.
From the foregoing it will be readily appreciated that no logical steps can be followed in establishing a eutectic or near-eutectic composition to meet a very restricted and precise temperature-time target. Even though one alloy may be ideal insofar as melting point is concerned it may not be acceptable from a phase transition time aspect. If melting is too sluggish, a fuse or fusible link will not necessarily fullfil its protective function, failing to drop out of the circuit in the desired manner.
OBJECT OF THE INVENTION It is therefore the object of the present invention to provide fusible alloys possessing all desirable properties and, of most importance, having desired melting-point temperatures together with suitably rapid and complete phase transition characteristics.
SUMMARY OF THE INVENTION The foregoing object is accomplished in accordance with this invention, in its most preferred form, by providing a ternary alloy of indium (In), tin (Sn) and silver The specific percentage content ranges are, of course, governed by the temperature-time limitations imposed for the particular use.
DESCRIPTION OF THE PREFERRED EMBODIMENT Initially, investigation began with a study of the binary system of indium and tin. It was then determined that while the eutectic of this binary system is characterized by a melting point and transition (phase) time suitable for present regulations, it would not be satisfactory to meet the more stringent requirements which are expected to be imposed in the United States in the near future.
As a result, investigations were continued by adding relatively small percentages of Group IB elements to the In-Sn eutectic. I
Copper was found to provide a definite decrease in melting point while silver has an even more desirable effect.
By carrying out appropriate tests it was found that the novel ternary alloy of ln-Sn-Ag melted at ll3.8il C. and completed the phase transition within the time limits set for fusible links by both U.S. and Canadian authorities. This alloy also meets the anticipated U.S. revised regulations.
Further, metallographic examination of a sample of the new alloy revealed a substantially homogenous structure over the entire cross-section, indicative of a eutectic or near-eutectic composition.
Naturally, the true eutectic is the most preferred composition when one considers the desirability of a pure isothermal transition, but observation has established that for the purpose in question, the alloy may be comprised within the approximate composition given and still melt at a temperature in the prescribed area.
A fusible link manufactured from the novel material proved to have satisfactory mechanical strength for its purpose and exhibited good resistance to surface film formation (oxidation).
In all respects therefore, the new ternary alloy of In- Sn-Ag is eminently suitable for use in the manufacture of fusible links while additions of about 0.17% copper to the In-Sn eutectic result in an alloy suitable for use under present regulations, having an M.P. of 1l7.6 C. :1" C.
It is not considered necessary to comment upon production of these new alloys since no peculiar problems exist in this respect. Naturally, however, purity of the components must be afforded consideration.
For the record, initial experimentation was carried out using component elements of 99.9999% purity, but later tests showed that 99.99% is acceptable. Purity considerations are not, of course, essential to the actual point of invention.
In practice, the ternary fusible alloy according to the present invention can be processed to any desired configuration for use as a fusible link. Of course, such use is not intended as being exhaustive of the overall utility of the alloy.
As regards mounting the link, one mode is suggested by reference to Pat. No. 3,354,282 issued to Norbert C. Batsch on Nov. 21, 1967, and assigned to the assignee of the present invention.
Pat. No. 3,354,282 reveals a thermal fuse with capillary action in which the molten fusible link will separate reliably and completely under any practical service conditions, in any position, and after long, useful life. Enclosed within a tubular sleeve is a fusible link and a means attached to each end of the fusible link for providing capillary action on the molten fuse link so that when the fusible link melts upon increase of the environmental temperature beyond its melting point, the molten material is withdrawn into the capillary means thus en suring that the current flow in the electrical lead is entirely interrupted.
While a particular embodiment of this invention has been described, it will be obvious to those skilled in the art that various changes and modifications may be made without departing from this invention in its broader aspects and, therefore, it is intended that the appended claims cover all such changes and modifications as fall within the true spirit and scope of this invention.
What I claim as new and desire to secure by Letters Patent of the United States is:
1. A ternary fusible alloy comprising a substantially eutectic composition of ln-Sn with the balance made up of silver.
2. A ternary fusible alloy having a composition of about 51.4% In, 47.3% Sn, and 1.3% Ag, characterized by a melting point of 113.811 C.
3. A ternary fusible alloy, as recited in claim 1, wherein the composition is chosen to have the lowest possible melting point, which is approximately 114 C.
4. A ternary fusible alloy, as recited in claim 1, wherein a sufiicient amount of silver is added to the ln-Sn to lower its melting point below the 117 C. minimum melting point of an In-Sn eutectic.
References Cited UNITED STATES PATENTS 11/1950 Zickrick -134 X 3/1955 Kozacka 75134 X U.S. Cl. X.R. 75-134 B
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CA7770 | 1967-12-16 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| US3627517A true US3627517A (en) | 1971-12-14 |
Family
ID=4083945
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| US783764A Expired - Lifetime US3627517A (en) | 1967-12-16 | 1968-12-13 | Ternary fusible alloy |
Country Status (6)
| Country | Link |
|---|---|
| US (1) | US3627517A (en) |
| CA (1) | CA868830A (en) |
| DE (1) | DE1814107A1 (en) |
| FR (1) | FR1594275A (en) |
| GB (1) | GB1244186A (en) |
| NO (1) | NO120655B (en) |
Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3833362A (en) * | 1970-09-18 | 1974-09-03 | Ppg Industries Inc | Electroconductive solder |
| US5120498A (en) * | 1991-05-15 | 1992-06-09 | C-Innovations, Inc. | Solders having exceptional adhesion to glass |
| US5242658A (en) * | 1992-07-07 | 1993-09-07 | The Indium Corporation Of America | Lead-free alloy containing tin, zinc and indium |
| US5256370A (en) * | 1992-05-04 | 1993-10-26 | The Indium Corporation Of America | Lead-free alloy containing tin, silver and indium |
| EP1189252A1 (en) * | 2000-09-13 | 2002-03-20 | Siemens Aktiengesellschaft | Fuse link, method of manufacturing the same and solder material |
| EP1383149A3 (en) * | 2002-07-16 | 2004-01-28 | Uchihashi Estec Co., Ltd. | Alloy type thermal fuse and wire member for a thermal fuse element |
| WO2005045870A1 (en) * | 2003-11-06 | 2005-05-19 | Pratt & Whitney Canada Corp. | Electro-magnetically enhanced current interrupter |
| US20050128044A1 (en) * | 2003-12-15 | 2005-06-16 | Uchihashi Estec Co., Ltd. | Alloy type thermal fuse and wire member for a thermal fuse element |
| US20140138155A1 (en) * | 2011-05-03 | 2014-05-22 | Pilkington Group Limited | Glazing with a soldered connector |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE2121120C3 (en) * | 1971-04-29 | 1973-11-22 | Robert Bosch Gmbh, 7000 Stuttgart | Overtemperature protection for an electrical winding |
-
1967
- 1967-12-16 CA CA868830A patent/CA868830A/en not_active Expired
-
1968
- 1968-12-10 FR FR1594275D patent/FR1594275A/fr not_active Expired
- 1968-12-12 DE DE19681814107 patent/DE1814107A1/en active Pending
- 1968-12-13 NO NO4993/68A patent/NO120655B/no unknown
- 1968-12-13 US US783764A patent/US3627517A/en not_active Expired - Lifetime
- 1968-12-16 GB GB59666/68A patent/GB1244186A/en not_active Expired
Cited By (18)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3833362A (en) * | 1970-09-18 | 1974-09-03 | Ppg Industries Inc | Electroconductive solder |
| US5120498A (en) * | 1991-05-15 | 1992-06-09 | C-Innovations, Inc. | Solders having exceptional adhesion to glass |
| US5256370A (en) * | 1992-05-04 | 1993-10-26 | The Indium Corporation Of America | Lead-free alloy containing tin, silver and indium |
| US5580520A (en) * | 1992-05-04 | 1996-12-03 | The Indium Corporation Of America | Lead-free alloy containing tin, silver and indium |
| US5242658A (en) * | 1992-07-07 | 1993-09-07 | The Indium Corporation Of America | Lead-free alloy containing tin, zinc and indium |
| US20040027226A1 (en) * | 2000-09-13 | 2004-02-12 | Alexander Etschmaier | Fuse link, method for the production thereof and soldering substance |
| WO2002023575A1 (en) * | 2000-09-13 | 2002-03-21 | Siemens Aktiengesellschaft | Fuse link, method for the production thereof and soldering substance |
| EP1189252A1 (en) * | 2000-09-13 | 2002-03-20 | Siemens Aktiengesellschaft | Fuse link, method of manufacturing the same and solder material |
| US7109839B2 (en) | 2000-09-13 | 2006-09-19 | Siemens Aktiengesellschaft | Fuse link, method for the production thereof and soldering substance |
| CN100350539C (en) * | 2000-09-13 | 2007-11-21 | 西门子公司 | Fuse, its manufacturing method and solder |
| CZ299341B6 (en) * | 2000-09-13 | 2008-06-25 | Siemens Aktiengesellschaft | Fuse link, method for the production thereof and soldering material |
| EP1383149A3 (en) * | 2002-07-16 | 2004-01-28 | Uchihashi Estec Co., Ltd. | Alloy type thermal fuse and wire member for a thermal fuse element |
| WO2005045870A1 (en) * | 2003-11-06 | 2005-05-19 | Pratt & Whitney Canada Corp. | Electro-magnetically enhanced current interrupter |
| US20050128044A1 (en) * | 2003-12-15 | 2005-06-16 | Uchihashi Estec Co., Ltd. | Alloy type thermal fuse and wire member for a thermal fuse element |
| EP1544883A1 (en) * | 2003-12-15 | 2005-06-22 | Uchihashi Estec Co., Ltd. | Alloy type thermal fuse and wire member for a thermal fuse element |
| CN100508095C (en) * | 2003-12-15 | 2009-07-01 | 内桥艾斯泰克股份有限公司 | Alloy type temperature fuse and wire for temperature fuse |
| US20140138155A1 (en) * | 2011-05-03 | 2014-05-22 | Pilkington Group Limited | Glazing with a soldered connector |
| US9595768B2 (en) * | 2011-05-03 | 2017-03-14 | Pilkington Group Limited | Glazing with a soldered connector |
Also Published As
| Publication number | Publication date |
|---|---|
| DE1814107A1 (en) | 1969-08-14 |
| FR1594275A (en) | 1970-06-01 |
| NO120655B (en) | 1970-11-16 |
| GB1244186A (en) | 1971-08-25 |
| CA868830A (en) | 1971-04-20 |
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