US20220195564A1 - A casting magnesium alloy for providing improved thermal conductivity - Google Patents
A casting magnesium alloy for providing improved thermal conductivity Download PDFInfo
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- 229910000861 Mg alloy Inorganic materials 0.000 title claims abstract description 42
- 238000005266 casting Methods 0.000 title abstract description 29
- 239000011777 magnesium Substances 0.000 claims abstract description 32
- 229910052749 magnesium Inorganic materials 0.000 claims abstract description 22
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims abstract description 21
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 16
- 229910052727 yttrium Inorganic materials 0.000 claims abstract description 16
- 229910052684 Cerium Inorganic materials 0.000 claims abstract description 15
- 239000011701 zinc Substances 0.000 claims abstract description 15
- 229910052725 zinc Inorganic materials 0.000 claims abstract description 13
- 229910052688 Gadolinium Inorganic materials 0.000 claims abstract description 11
- 229910052779 Neodymium Inorganic materials 0.000 claims abstract description 11
- 239000004411 aluminium Substances 0.000 claims abstract description 11
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 11
- 239000012535 impurity Substances 0.000 claims abstract description 11
- 229910052746 lanthanum Inorganic materials 0.000 claims abstract description 10
- 229910052777 Praseodymium Inorganic materials 0.000 claims abstract description 8
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052790 beryllium Inorganic materials 0.000 claims abstract description 8
- ATBAMAFKBVZNFJ-UHFFFAOYSA-N beryllium atom Chemical compound [Be] ATBAMAFKBVZNFJ-UHFFFAOYSA-N 0.000 claims abstract description 8
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims abstract description 7
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims abstract description 6
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 claims abstract description 6
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 claims abstract description 5
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims abstract description 4
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 claims abstract description 4
- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 0.000 claims abstract description 4
- 239000011572 manganese Substances 0.000 claims description 16
- 229910052748 manganese Inorganic materials 0.000 claims description 10
- 239000000956 alloy Substances 0.000 description 64
- 229910045601 alloy Inorganic materials 0.000 description 63
- 238000004512 die casting Methods 0.000 description 21
- 239000000203 mixture Substances 0.000 description 11
- 238000000034 method Methods 0.000 description 10
- 229910052761 rare earth metal Inorganic materials 0.000 description 9
- 229910000838 Al alloy Inorganic materials 0.000 description 8
- 238000005275 alloying Methods 0.000 description 8
- 239000011575 calcium Substances 0.000 description 6
- 239000000463 material Substances 0.000 description 6
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 5
- 238000004458 analytical method Methods 0.000 description 4
- 229910052791 calcium Inorganic materials 0.000 description 4
- 230000005496 eutectics Effects 0.000 description 4
- 229910052747 lanthanoid Inorganic materials 0.000 description 4
- 150000002602 lanthanoids Chemical class 0.000 description 4
- 239000000047 product Substances 0.000 description 4
- 229910052726 zirconium Inorganic materials 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000011159 matrix material Substances 0.000 description 3
- 238000007711 solidification Methods 0.000 description 3
- 230000008023 solidification Effects 0.000 description 3
- 238000005728 strengthening Methods 0.000 description 3
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 2
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 230000001419 dependent effect Effects 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- 230000005484 gravity Effects 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal 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
- 230000008569 process Effects 0.000 description 2
- 150000002910 rare earth metals Chemical class 0.000 description 2
- 238000007528 sand casting Methods 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000010959 steel Substances 0.000 description 2
- 229910052712 strontium Inorganic materials 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 229910052718 tin Inorganic materials 0.000 description 2
- 229910052719 titanium Inorganic materials 0.000 description 2
- FRWYFWZENXDZMU-UHFFFAOYSA-N 2-iodoquinoline Chemical compound C1=CC=CC2=NC(I)=CC=C21 FRWYFWZENXDZMU-UHFFFAOYSA-N 0.000 description 1
- 235000001674 Agaricus brunnescens Nutrition 0.000 description 1
- 229910003023 Mg-Al Inorganic materials 0.000 description 1
- 229910006776 Si—Zn Inorganic materials 0.000 description 1
- 229910052776 Thorium Inorganic materials 0.000 description 1
- 229910052769 Ytterbium Inorganic materials 0.000 description 1
- 229910001297 Zn alloy Inorganic materials 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- LTPBRCUWZOMYOC-UHFFFAOYSA-N beryllium oxide Inorganic materials O=[Be] LTPBRCUWZOMYOC-UHFFFAOYSA-N 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000002860 competitive effect Effects 0.000 description 1
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- 229910000765 intermetallic Inorganic materials 0.000 description 1
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Images
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22D—CASTING OF METALS; CASTING OF OTHER SUBSTANCES BY THE SAME PROCESSES OR DEVICES
- B22D21/00—Casting non-ferrous metals or metallic compounds so far as their metallurgical properties are of importance for the casting procedure; Selection of compositions therefor
- B22D21/02—Casting exceedingly oxidisable non-ferrous metals, e.g. in inert atmosphere
- B22D21/04—Casting aluminium or magnesium
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C23/00—Alloys based on magnesium
- C22C23/06—Alloys based on magnesium with a rare earth metal as the next major constituent
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22D—CASTING OF METALS; CASTING OF OTHER SUBSTANCES BY THE SAME PROCESSES OR DEVICES
- B22D21/00—Casting non-ferrous metals or metallic compounds so far as their metallurgical properties are of importance for the casting procedure; Selection of compositions therefor
- B22D21/002—Castings of light metals
- B22D21/007—Castings of light metals with low melting point, e.g. Al 659 degrees C, Mg 650 degrees C
Definitions
- the invention relates to a casting magnesium alloy, in particular the die-casting magnesium alloy that can provide the significantly improved thermal conductivity in comparison with the commonly used AZ91D (Mg-9wt.%Al-1wt.%Zn) die-casting magnesium alloy.
- the typical thermal conductivity of the die-casting magnesium alloys of the present invention is at a level of more than110 W/m.K (that is, Watts per metre-Kelvin) under as-cast condition and room temperature (about 20° C.), which is close to the thermal conductivity of the commonly used A380 (Al-9wt.%Si-3wt.%Cu) die-casting aluminium alloy.
- magnesium alloys In competing with aluminium alloys as structural materials, magnesium alloys have advantages of low density, high strength ratio, and better electromagnetic shielding properties and castability. These result in the preferential applications of magnesium alloys in the components where the lightweight and electromagnetic shielding is critical.
- the currently used magnesium alloys have inferior thermal conductivity in comparison with its competitive materials of aluminium alloys.
- the thermal conductivity of pure magnesium is 156 W/m ⁇ K at 25° C., but that of pure aluminium is 205
- the most commonly used die-casting alloys show significant differences in the thermal conductivity.
- the commonly used AZ91D die-casting magnesium alloy has the thermal conductivity of 51 W/m ⁇ K at 20° C.
- the commonly used A380 die-casting aluminium alloy has the thermal conductivity of 108 W/m ⁇ K at 20° C. Therefore, the ratio of thermal conductivity is 0.76 between pure Mg and Al but is 0.47 between AZ91D and
- the thermal conductivity of a component having the same weight is similar for aluminium and magnesium, the thermal conductivity for AZ91D magnesium components is about half that of comparable A380 aluminium components. Therefore, it is desirable to produce magnesium alloys having improved thermal conductivity.
- High thermal conductivity is desirable for increasing the capacity of heat exchange and heat sink of engineering components. Improved thermal conductivity can reduce the working temperatures of final products and therefore increase the energy efficiency and product life.
- the technical routes of the prior arts can be described as (1) using the currently available magnesium alloys as thermal conductive alloys, which include Mg-Si-Zn based alloys; (2) modifying the existing magnesium alloys with special elements at low levels, which include alkaline earth metals and rare earth (Re) elements; (3) developing new alloys, such Mg-Sn- Zn-Zr based alloys.
- the existing research in the field of high thermal conductive casting magnesium alloys has the following problems: (1) in casting alloys, the magnesium alloys contain high solute contents cannot provide sufficient thermal conductivity such as the commonly used AZ91D alloy, more particularly, are not capable of competing with its aluminium alloy counterparts; (2) in wrought alloys, low level solutes are used. Therefore, the alloy can provide better thermal conductivity than casting alloys.
- the current market share of wrought magnesium alloys is less than 5%; (3) the contradiction between the thermal conductivity and castability of the alloy is a serious problem for the development of thermal conductive magnesium alloys. The castability is often not sufficiently good for the new magnesium alloys that have better thermal conductivity in comparison with the popular
- U.S. Ser. No. 2010/0310409 A1 discloses a magnesium based alloy consisting of, by weight: 2-5% rare earth elements, wherein the alloy contains lanthanum and cerium as rare earth elements and the lanthanum content is greater than the cerium content; 0.2-0.8% zinc;
- US 2009/0136380 A1 discloses a magnesium-based alloy consists of 1.5-4.0% by weight rare earth element(s), 0.3-0.8% by weight zinc, 0.02-0.1% by weight aluminium, and 4-25 ppm beryllium.
- the alloy optionally contains up to 0.2% by weight zirconium, 0.3% by weight manganese, 0.5% by weight yttrium and 0.1% by weight calcium. The remainder of the alloy is magnesium except for incidental impurities.
- US 2008/0193322 Al discloses a magnesium-rare earth-yttrium-zinc alloy consists of 0.2-1.5% by weight zinc and rare earth(s) (RE) and yttrium in amounts which fall within a quadrangle defined by lines AB, BC, CD and DA wherein: A is 1.8% RE-0.05% Y, B is 1.0% RE-0.05% Y, C is 0.2% RE-0.8% Y, and D is 1.8% RE-0.8% Y.
- a magnesium alloy including:
- the present invention intends to provide a casting magnesium alloy for significantly improved thermal conductivity in comparison with the commonly used commercial AZ91D alloy.
- the claimed alloy can provide the thermal conductivity at a level that A380 Aluminium alloy can.
- the claimed alloy provides good castability and works well under as-cast condition with excellent mechanical properties.
- a magnesium alloy for providing improved thermal conductivity more than 110 W/m.K including:
- a first lanthanide preferably lanthanum
- a second lanthanide preferably cerium
- the magnesium alloy contains:
- a casting magnesium alloy material for providing significantly improved thermal conductivity under as-cast condition comprising at least two elements from rare earth elements, each is at a level of more than lwt.% and less than 5wt.%, one of which is used to provide the improvement of castability and the other one is used to provide strengthening of the alloy.
- the alloy is capable of providing a thermal conductivity at a level of more than 110W/ m ⁇ K under as-cast condition and room temperature (20° C.).
- the rare earth elements can be any in the Lanthanoids, it is preferred to have La and Ce or any other low-cost rare-earth elements. Therefore, the elements such as Nd and Gd should be added in a controlled amount in the alloy. More importantly, La or Ce can be obtained from recycled materials, which is an effective way to reduce the alloy cost.
- the elements used in the present invention can be replaced by other elements that promote the formation of intermetallic phases easier than Mg-Al phase in the Mg matrix.
- Another element in the alloy is preferably required to have a high solubility in the primary ⁇ -Mg phase at elevated temperatures close to its eutectic solidification but has very low solubility at ambient temperature.
- the element can improve the castability and mechanical properties of the magnesium alloy, and it promotes the formation of precipitates in the primary ⁇ -Mg phase after solidification, which can provide effective strengthening in the alloy and reduce the solute concentration in the primary ⁇ -Mg phase. More importantly, this can reduce the solute content in the primary ⁇ -Mg phase to improve the thermal conductivity.
- the elements including Ca, Ce, Cu, La, Nd, Sr, Th, Zr, Sn, Yb, Bi, Ca, Ti and Au can be the candidates.
- the rare earth elements are one of the preferred options because of their low solubility in primary magnesium phase and the multiple functions to promote the formation of eutectic phase.
- the other elements including Ca, Cu,
- Manganese (Mn) is an important alloying element for all embodiments of the casting magnesium alloy according to the present invention.
- the role of Mn includes the neutralisation of Fe to form compact Fe-rich intermetallics, and to promote die releasing during die-casting, which allows the alloy to be die-castable for massive production. For these reasons, Mn content is lower in the castings made by sand casting and other method without using a metallic mould, but higher in the casting methods using metallic mould.
- the Mn level is in the range of 0.1 to 0.8 wt.%. A more preferred Mn level is in the range of 0.1 to 0.3%.
- Beryllium (Be) is commonly added to casting magnesium alloys to prevent oxidation of the magnesium alloy. As little as up to 20ppm causes a protective beryllium oxide film to form on the surface. Preferably, as usual, the Be level is controlled to be about 20ppm.
- the present invention also includes products made from the casting magnesium alloys set out a variety of casting operations, which including the common casting methods including but not limited to sand casting, investment casting, lost foam casting, gravity and permanent mould die casting, low pressure die casting, high pressure die casting, and squeeze casting.
- the alloying elements are selected to promote the alloy not only having improved thermal conductivity, but also having good castability. Therefore, it is suitable for common castings methods, in particular in die-casting operations without soldering problems. This is a huge advantage because die-casting is dominant process for magnesium alloys. In the meantime, die-casting can make thin wall components. Therefore, the alloy is particularly suited for manufacturing products having requirements where the high conductivity and light-weighting are desirable.
- the following levels for the alloying element are selected (all composition percentages are by weight): La 1.0-5.0 wt.%, Ce 1.0-5.0 wt.%, Nd 0.5-2wt.%, Gd 0.5-1.5wt.%, Y 0-0.2wt.%, Pr ⁇ 0.6wt.%, Mn 0.1-0.4 wt.%, and Al ⁇ 1.0wt.%, Zn ⁇ 0.8wt.%, with Be 20ppm and the balanced magnesium and inevitable impurities.
- the preferred levels of the alloying element are selected: La 1.0-3.0 wt.%, Ce 1.0-3.0 wt.%, Nd 0.5-1.5wt.%, Gd 0.5-1.5wt.%, Y 0-0.15wt.%, Pr ⁇ 0.5wt.%, Mn 0.1-0.3 wt.%, and Al ⁇ 0.6wt.%, Zn ⁇ 0.5wt.%, with Be12ppm and the balanced magnesium and inevitable impurities.
- FIG. 1 is a graph showing the thermal conductivity as a function of temperature for an alloy in accordance with the invention
- FIG. 2 is a series of photographs of samples of prior art alloys and an alloy in accordance with the invention illustrating high pressure die casting capability
- FIG. 3 is a graph showing the strain as a function of time for a prior art alloy and an alloy in accordance with the invention.
- the composition was analysed using an optical mass spectroscopy, in which at least five spark analyses were carried out and the average value was taken as the chemical composition of the alloy.
- the actual composition of the alloy was Mg-5.5(La, Ce, Nd, Gd, Y)-0.5Al-0.3Zn-0.3Mn (wt.%), with Be also being present at about 20ppm with balanced Mg.
- the casting samples were made by a 4500 kN cold chamber HPDC machine, in which all casting parameters were fully monitored and recorded.
- the pouring temperature was controlled at 700° C., which was measured by a K-type thermocouple.
- the die to make standard samples for mechanical properties and thermal conductivity were made under the corresponding optimised condition.
- the dies were heated by the circulation of mineral oil at 250° C.
- the samples for thermal conductivity were ⁇ 12 ⁇ 20 mm round bars.
- the mechanical properties and thermal conductivity were measured following a standard method defined by ASTM.
- Example 1 A number of other samples were made in accordance with the method of Example 1 using high pressure die casting and gravity and permanent mould die casting.
- the thermal conductivity was tested under as-cast condition and various temperatures.
- the thermal conductivity at room temperature is shown in Table 2.
- the castability was assessed to the commercial A380 and AZ91D alloy and the value in the following Table 2 is a ratio between the filling lengths in permanent mould casting.
- the thermal conductivity at various elevated temperatures is shown in FIG. 1 .
- magnesium alloy samples which are not in accordance with the invention have a lower thermal conductivity than the reference aluminium alloy (Sample 1).
- the magnesium alloy samples which are in accordance with the invention have a comparable thermal conductivity to Sample 1.
- FIG. 2 as follows:
- FIG. 3 shows high temperature creep properties of AZ91D (a typical prior art alloy) and a magnesium alloy in accordance with the invention (Mg-1.4La-2.1Ce-0.6Nd-1.2Gd-0.1Y-0.3Zn-0.8Al-0.3Mn).
- the short dot curve shows the typical creep properties of the AZ91D alloy at 150° C. and 90 MPa (labelled “reference”).
- the solid curve shows the typical creep properties of the alloy of the present invention (labelled “present”) at 200 ° C. and 100 MPa.
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Abstract
A casting magnesium alloy for providing improved thermal conductivity A magnesium alloy for providing improved thermal conductivity includes from 1 wt.% to 5 wt.% of lanthanum, from 1 wt.% to 5 wt.% of cerium or a combination thereof, and from 0.5 wt.% to 3 wt.% of neodymium, from 0.5 wt.% to 3 wt.% of gadolinium or a combination thereof, and from 0.0 wt.% to 0.2 wt.% of yttrium, and up to 0.8 wt.% of praseodymium, and up to 0.8 wt.% manganese, and up to 1.0 wt.% aluminium, and up to 0.8 wt.% zinc, and up to 20ppm beryllium, and with balanced magnesium and inevitable impurities.
Description
- The invention relates to a casting magnesium alloy, in particular the die-casting magnesium alloy that can provide the significantly improved thermal conductivity in comparison with the commonly used AZ91D (Mg-9wt.%Al-1wt.%Zn) die-casting magnesium alloy. The typical thermal conductivity of the die-casting magnesium alloys of the present invention is at a level of more than110 W/m.K (that is, Watts per metre-Kelvin) under as-cast condition and room temperature (about 20° C.), which is close to the thermal conductivity of the commonly used A380 (Al-9wt.%Si-3wt.%Cu) die-casting aluminium alloy.
- In competing with aluminium alloys as structural materials, magnesium alloys have advantages of low density, high strength ratio, and better electromagnetic shielding properties and castability. These result in the preferential applications of magnesium alloys in the components where the lightweight and electromagnetic shielding is critical.
- However, the currently used magnesium alloys have inferior thermal conductivity in comparison with its competitive materials of aluminium alloys. For examples, the thermal conductivity of pure magnesium is 156 W/m·K at 25° C., but that of pure aluminium is 205
- W/m·K at 25° C. Similarly, the most commonly used die-casting alloys show significant differences in the thermal conductivity. The commonly used AZ91D die-casting magnesium alloy has the thermal conductivity of 51 W/m·K at 20° C., and the commonly used A380 die-casting aluminium alloy has the thermal conductivity of 108 W/m·K at 20° C. Therefore, the ratio of thermal conductivity is 0.76 between pure Mg and Al but is 0.47 between AZ91D and
- A380.
- Although the thermal conductivity of a component having the same weight is similar for aluminium and magnesium, the thermal conductivity for AZ91D magnesium components is about half that of comparable A380 aluminium components. Therefore, it is desirable to produce magnesium alloys having improved thermal conductivity.
- High thermal conductivity is desirable for increasing the capacity of heat exchange and heat sink of engineering components. Improved thermal conductivity can reduce the working temperatures of final products and therefore increase the energy efficiency and product life.
- This is particularly important when combined with the advantages of magnesium alloys, namely their low density, electromagnetic shielding properties and castability.
- In general, the addition of solute elements into pure magnesium reduces the thermal conductivity, although alloying is in many instances essential in order that the pure metals can be useful in engineering. Therefore, it is a favoured method to use alloying elements to improve the thermal conductivity of magnesium alloys. Prior attempts to provide improved thermal conductivity of magnesium alloys using different alloying elements at different levels have been disclosed and a number of these disclosures are set out in Table 1 below, in which the alloys include casting alloys and wrought alloys.
- The technical routes of the prior arts can be described as (1) using the currently available magnesium alloys as thermal conductive alloys, which include Mg-Si-Zn based alloys; (2) modifying the existing magnesium alloys with special elements at low levels, which include alkaline earth metals and rare earth (Re) elements; (3) developing new alloys, such Mg-Sn- Zn-Zr based alloys.
- However, the existing research in the field of high thermal conductive casting magnesium alloys has the following problems: (1) in casting alloys, the magnesium alloys contain high solute contents cannot provide sufficient thermal conductivity such as the commonly used AZ91D alloy, more particularly, are not capable of competing with its aluminium alloy counterparts; (2) in wrought alloys, low level solutes are used. Therefore, the alloy can provide better thermal conductivity than casting alloys. However, the current market share of wrought magnesium alloys is less than 5%; (3) the contradiction between the thermal conductivity and castability of the alloy is a serious problem for the development of thermal conductive magnesium alloys. The castability is often not sufficiently good for the new magnesium alloys that have better thermal conductivity in comparison with the popular
- AZ91D alloy; (4) precious metals such as Ag are used, thus increasing the materials cost, limiting the material source and making the alloys difficult to popularize and put into civil use; (5) heat treatment of the alloy is usually employed, which increases the energy consumption during manufacturing.
- In addition, it has been discovered that many of the prior art alloys shown in Table 1 have at least some of the following disadvantages:
- ⊇ they are not suitable for high pressure diecasting (HPDC) because the alloy is more likely to stick to the mould
- ⊇ also HPDC results in defects in the alloy
- ⊇ they are unlikely to have a good thermal conductivity at higher temperatures that ambient (for example over 150° C.)
- U.S. Ser. No. 2010/0310409 A1 (Gibson et al.) discloses a magnesium based alloy consisting of, by weight: 2-5% rare earth elements, wherein the alloy contains lanthanum and cerium as rare earth elements and the lanthanum content is greater than the cerium content; 0.2-0.8% zinc;
- 0-0.15% aluminium; 0-0.5% yttrium or gadolinium; 0-0.2% zirconium, 0-0.3% manganese;
- 0-0.1% calcium; 0-25 ppm beryllium; and the remainder being magnesium except for incidental impurities.
- US 2009/0136380 A1 (Gibson et al.) discloses a magnesium-based alloy consists of 1.5-4.0% by weight rare earth element(s), 0.3-0.8% by weight zinc, 0.02-0.1% by weight aluminium, and 4-25 ppm beryllium. The alloy optionally contains up to 0.2% by weight zirconium, 0.3% by weight manganese, 0.5% by weight yttrium and 0.1% by weight calcium. The remainder of the alloy is magnesium except for incidental impurities.
- US 2008/0193322 Al (Gibson et al.) discloses a magnesium-rare earth-yttrium-zinc alloy consists of 0.2-1.5% by weight zinc and rare earth(s) (RE) and yttrium in amounts which fall within a quadrangle defined by lines AB, BC, CD and DA wherein: A is 1.8% RE-0.05% Y, B is 1.0% RE-0.05% Y, C is 0.2% RE-0.8% Y, and D is 1.8% RE-0.8% Y.
- In accordance with a first aspect of the invention, there is provided a magnesium alloy including:
-
- a. from 1 wt.% to 5 wt.% of lanthanum, from 1 wt.% to 5 wt.% of cerium or a combination thereof, and
- b. from 0.5 wt.% to 3 wt.% of Neodymium (preferably from 0.5 wt.% to 2 wt.%), from 0.5 wt.% to 3 wt.% (preferably 0.5 wt.% to 1.5 wt.%) of Gadolinium or a combination thereof, and
- c. up to 0.2 wt.% of Yttrium, and
- d. up to 0.8 wt.% of Praseodymium, and
- e. up to 0.8 wt.% Manganese, and
- f. up to 1.0 wt.% (preferably up to 0.5 wt%) Aluminium, and
- g. up to 0.8 wt.% Zinc, and
- h. up to 20ppm beryllium, and
- i. with the balance being magnesium and inevitable impurities.
- By “a combination thereof” is meant both of the previously listed elements in the amounts listed.
- The present invention intends to provide a casting magnesium alloy for significantly improved thermal conductivity in comparison with the commonly used commercial AZ91D alloy. In particular, the claimed alloy can provide the thermal conductivity at a level that A380 Aluminium alloy can. Moreover, the claimed alloy provides good castability and works well under as-cast condition with excellent mechanical properties. In a preferred embodiment of the present invention, there is provided a magnesium alloy for providing improved thermal conductivity more than 110 W/m.K including:
- a. from 1 wt.% to 5 wt.% of a first lanthanide (preferably lanthanum), from 1 wt.% to 5 wt.% of a second lanthanide (preferably cerium) or a combination thereof, wherein the first and second lanthanide is the same of different, and
- b. from 0.5 wt.% to 3 wt.% of Neodymium, from 0.5 wt.% to 3 wt.% of Gadolinium or a combination thereof, and
- c. up to 0.2 wt.% of Yttrium, and
- d. up to 0.8 wt.% of Praseodymium, and
- e. up to 0.8 wt.% Manganese (with the amount of manganese being non-zero), and
- f. up to 1.0 wt.% Aluminium (with the amount of aluminium being non-zero), and
- g. up to 0.8 wt.% Zinc (with the amount of zinc being non-zero), and
- h. up to 20ppm beryllium, and
- i. with the balance being magnesium and inevitable impurities.
- Preferably, the magnesium alloy contains:
- ⋅ one or more elements that is more reactive with aluminium than magnesium in the alloy melt during solidification and therefore forming eutectic phase without destroy the continuity of α-Mg phase in the matrix to reduce the solute concentration in the primary α-Mg phase
- ⋅ an appropriate amount of manganese to neutralise impurities and improve die releasing capability
- ⋅ and a small amount of beryllium and/or other elements to protect the oxidation during casting operation
- In a preferred embodiment, there is provided a casting magnesium alloy material for providing significantly improved thermal conductivity under as-cast condition comprising at least two elements from rare earth elements, each is at a level of more than lwt.% and less than 5wt.%, one of which is used to provide the improvement of castability and the other one is used to provide strengthening of the alloy. The alloy is capable of providing a thermal conductivity at a level of more than 110W/ m·K under as-cast condition and room temperature (20° C.). Without wishing to be constrained by theory, it is believed that the improved thermal conductivity available with the invention, particularly in combination with good casting characteristics results from the combination of Mg with Re within the given ranges because Re in the alloy can reduce the liquidus temperature and improve the castability. Accordingly, the method used in this patent is that to use Re solute elements to improve the castability. In the meantime, some of the Re elements have high solubility in Mg matrix and capable of providing materials strengthening.
- Although the rare earth elements can be any in the Lanthanoids, it is preferred to have La and Ce or any other low-cost rare-earth elements. Therefore, the elements such as Nd and Gd should be added in a controlled amount in the alloy. More importantly, La or Ce can be obtained from recycled materials, which is an effective way to reduce the alloy cost. The elements used in the present invention can be replaced by other elements that promote the formation of intermetallic phases easier than Mg-Al phase in the Mg matrix.
- Another element in the alloy is preferably required to have a high solubility in the primary α-Mg phase at elevated temperatures close to its eutectic solidification but has very low solubility at ambient temperature. The element can improve the castability and mechanical properties of the magnesium alloy, and it promotes the formation of precipitates in the primary α-Mg phase after solidification, which can provide effective strengthening in the alloy and reduce the solute concentration in the primary α-Mg phase. More importantly, this can reduce the solute content in the primary α-Mg phase to improve the thermal conductivity.
- The maximum solid solubility for alloying elements in magnesium have been reported (at.%) as Ag (3.8), A1(11.6), Ca(0.8), Ce (0.1), Cu (0.15), Gd (4.5), In (19.4), La (0.1), Li (18), Mn (1.0), Nd (0.1), Si (0.003), Sn(3.35), Sr (0), Tb (4.6), Th (0.52), Y (3.35), Zn (2.4), Zr (1.0), Zn(2.4), Tm (6.3), Sc (15), Pb(7.75), Sn (0.35), Yb (1.2), Bi (1.1), Ca (0.82), Ti (0.1) and Au (0.1). Therefore, the options are apparent for the element that has very low solubility at ambient temperature. The elements including Ca, Ce, Cu, La, Nd, Sr, Th, Zr, Sn, Yb, Bi, Ca, Ti and Au can be the candidates. Clearly, the rare earth elements are one of the preferred options because of their low solubility in primary magnesium phase and the multiple functions to promote the formation of eutectic phase. The other elements including Ca, Cu,
- Sr, Zr, Sn, Bi, Ti and Au are good options for the alloy. All these elements should be controlled within the maximum solubility at the eutectic reaction temperature.
- Manganese (Mn) is an important alloying element for all embodiments of the casting magnesium alloy according to the present invention. The role of Mn includes the neutralisation of Fe to form compact Fe-rich intermetallics, and to promote die releasing during die-casting, which allows the alloy to be die-castable for massive production. For these reasons, Mn content is lower in the castings made by sand casting and other method without using a metallic mould, but higher in the casting methods using metallic mould. The Mn level is in the range of 0.1 to 0.8 wt.%. A more preferred Mn level is in the range of 0.1 to 0.3%.
- Beryllium (Be) is commonly added to casting magnesium alloys to prevent oxidation of the magnesium alloy. As little as up to 20ppm causes a protective beryllium oxide film to form on the surface. Preferably, as usual, the Be level is controlled to be about 20ppm.
- The present invention also includes products made from the casting magnesium alloys set out a variety of casting operations, which including the common casting methods including but not limited to sand casting, investment casting, lost foam casting, gravity and permanent mould die casting, low pressure die casting, high pressure die casting, and squeeze casting. By the present invention, the alloying elements are selected to promote the alloy not only having improved thermal conductivity, but also having good castability. Therefore, it is suitable for common castings methods, in particular in die-casting operations without soldering problems. This is a huge advantage because die-casting is dominant process for magnesium alloys. In the meantime, die-casting can make thin wall components. Therefore, the alloy is particularly suited for manufacturing products having requirements where the high conductivity and light-weighting are desirable.
- In an embodiment of the casting magnesium alloy according to the invention the following levels for the alloying element are selected (all composition percentages are by weight): La 1.0-5.0 wt.%, Ce 1.0-5.0 wt.%, Nd 0.5-2wt.%, Gd 0.5-1.5wt.%, Y 0-0.2wt.%, Pr <0.6wt.%, Mn 0.1-0.4 wt.%, and Al<1.0wt.%, Zn<0.8wt.%, with Be 20ppm and the balanced magnesium and inevitable impurities.
- In another embodiment of the casting aluminium alloy according to the present invention of the preferred levels of the alloying element are selected: La 1.0-3.0 wt.%, Ce 1.0-3.0 wt.%, Nd 0.5-1.5wt.%, Gd 0.5-1.5wt.%, Y 0-0.15wt.%, Pr<0.5wt.%, Mn 0.1-0.3 wt.%, and Al<0.6wt.%, Zn<0.5wt.%, with Be12ppm and the balanced magnesium and inevitable impurities.
- A number of preferred embodiments of the invention will now be described with reference to the drawings, in which:
-
FIG. 1 is a graph showing the thermal conductivity as a function of temperature for an alloy in accordance with the invention; -
FIG. 2 is a series of photographs of samples of prior art alloys and an alloy in accordance with the invention illustrating high pressure die casting capability; and -
FIG. 3 is a graph showing the strain as a function of time for a prior art alloy and an alloy in accordance with the invention. - EXAMPLE 1
- Pure magnesium ingots, Mg-5wt.%Mn master alloys and a master alloy containing the mixture of La and Ce in magnesium were used as starting materials. Each element was weighted at a special ratio with an extra amount for burning loss during melting. During alloy making, a top loaded electrical resistant furnace was used to melt the metal in a steel crucible under protection of N2+(0.05−0.1)vol.% SF6. A batch of 10 kg alloy was melted at a temperature of 730° C. each time. After the melt was homogenised in the crucible, a mushroom sample with ϕ60×10 mm testing part for composition analysis was made by casting melt directly into a steel mould. The casting was cut off 3mm from the bottom before performing composition analysis. The composition was analysed using an optical mass spectroscopy, in which at least five spark analyses were carried out and the average value was taken as the chemical composition of the alloy. The actual composition of the alloy was Mg-5.5(La, Ce, Nd, Gd, Y)-0.5Al-0.3Zn-0.3Mn (wt.%), with Be also being present at about 20ppm with balanced Mg.
- After composition analysis, the casting samples were made by a 4500 kN cold chamber HPDC machine, in which all casting parameters were fully monitored and recorded. The pouring temperature was controlled at 700° C., which was measured by a K-type thermocouple. The die to make standard samples for mechanical properties and thermal conductivity were made under the corresponding optimised condition. The dies were heated by the circulation of mineral oil at 250° C. The samples for thermal conductivity were ϕ12×20 mm round bars. The mechanical properties and thermal conductivity were measured following a standard method defined by ASTM.
- A number of other samples were made in accordance with the method of Example 1 using high pressure die casting and gravity and permanent mould die casting. The thermal conductivity was tested under as-cast condition and various temperatures. The thermal conductivity at room temperature is shown in Table 2. The castability was assessed to the commercial A380 and AZ91D alloy and the value in the following Table 2 is a ratio between the filling lengths in permanent mould casting. The thermal conductivity at various elevated temperatures is shown in
FIG. 1 . - It can be seen that the magnesium alloy samples which are not in accordance with the invention (Samples 2-4) have a lower thermal conductivity than the reference aluminium alloy (Sample 1). However, the magnesium alloy samples which are in accordance with the invention (Samples 5-8) have a comparable thermal conductivity to Sample 1.
-
TABLE 2 Thermal conductivity Castability (20° C., (ratio Sample Alloy composition (wt. %)* W/m · K) value) 1 Al—9Si—3Cu—1Fe (A380**) 110 100 2 Mg—9Al—1Zn—0.2Mn (AZ91D**) 50 95 3 Mg—4Al—3.5Re—0.25Mn—0.2Zn (AE44**) 82 80 4 Mg—3.5Al—4Re—0.3Mn—0.2Zn (AE44**) 85 85 5 Mg—1.5La—1.1Ce—0.9Nd—1.6Gd—0.1Y—0.2Zn—0.5Al—0.3 Mn 110 95 6 Mg—1.1La—1.8Ce—1.2Nd—1.5Gd—0.1Y—0.3Zn—0.6Al—0.2Mn 107 90 7 Mg—1.6La—1.2Ce—1.0Nd—1.0Gd—0.1Y—0.2Zn—0.4Al—0.1Mn 105 90 8 Mg—2.1La—1.3Ce—0.8Nd—1.2Gd—0.1Y—0.2Zn—0.5Al—0.3Mn 108 90 *Be also present in amounts of up to 20 ppm **Commercially available alloys - Turning to
FIG. 2 , the inventors have tried to test the castability of different alloys with the typical composition disclosed in the art. This is not quantitative method as only relative methods are used in industry. Experiments were carried out to show that the references in Table 1 were not suitable for high pressure die casting and designed for low temperature (<=150° C.) application only, while the alloys of the present invention are suitable for high pressure die casting and could be worked at high temperature (>=200° C.). - The alloys that were tested were those listed in Table 1 above, and these are identified in
-
FIG. 2 as follows: - (a) CN101113502A, (b) CN101113504A, (c) CN101113503A, (d) CN104046867A, (e) CN102251161A, (f) CN101709418A, (g) CN104152769A, (h) CN102719716A, (i) US20090068053, (j) JP2012197490, (k) CN102560210A, (1) US3094413, (m) the present claimed magnesium alloy with the composition of Mg-1.4La-2.1Ce-0.6Nd-1.2Gd-0.1Y-0.3Zn-0.8Al-0.3Mn.
- From
FIG. 2 , it is clear that many of existing alloys are not able to make sound castings using high pressure die casting process. However, the casting of the alloy (m) in accordance with the invention is sound, which means the castability of the alloy is very good. - Turning to
FIG. 3 , this shows high temperature creep properties of AZ91D (a typical prior art alloy) and a magnesium alloy in accordance with the invention (Mg-1.4La-2.1Ce-0.6Nd-1.2Gd-0.1Y-0.3Zn-0.8Al-0.3Mn). The short dot curve shows the typical creep properties of the AZ91D alloy at 150° C. and 90 MPa (labelled “reference”). The solid curve shows the typical creep properties of the alloy of the present invention (labelled “present”) at 200 ° C. and 100 MPa. - All optional and preferred features and modifications of the described embodiments and dependent claims are usable in all aspects of the invention taught herein. Furthermore, the individual features of the dependent claims, as well as all optional and preferred features and modifications of the described embodiments are combinable and interchangeable with one another.
- The disclosures in UK patent application number 1905971.6, from which this application claims priority, and in the abstract accompanying this application are incorporated herein by reference. Claims
Claims (3)
1. A magnesium alloy including:
a. from 1 wt.% to 5 wt.% of lanthanum, from 1 wt.% to 5 wt.% of cerium or a combination thereof, and
b. from 0.5 wt.% to 3 wt.% of Neodymium, from 0.5 wt.% to 3 wt.% of Gadolinium or a combination thereof, and
c. up to 0.2 wt.% of Yttrium, and
d. up to 0.8 wt.% of Praseodymium, and
e. up to 0.8 wt.% Manganese, and
f. up to 1.0 wt.% Aluminium, and
g. up to 0.8 wt.% Zinc, and
h. up to 20ppm beryllium, and
i. with the balance being magnesium and inevitable impurities.
2. A magnesium alloy as claimed in claim 1 including: La 1.0-5.0 wt.%, Ce 1.0-5.0 wt.%, Nd 0.5-2wt.%, Gd 0.5-1.5wt.%, Y up to 0.2wt.%, Pr up to 0.6wt.%, Mn 0.1-0.4 wt.%, and Al up to 0.8wt.%, Zn up to 0.8wt.%, with Be 20ppm with the balance being magnesium and inevitable impurities.
3. A magnesium alloy for providing improved thermal conductivity as claimed in claim 1 or 2 including: La 1.0-3.0 wt.%, Ce 1.0-3.0 wt.%, Nd 0.5-1.5wt.%, Gd 0.5-1.5wt.%, Y up to 0.15wt.%, Pr up to 0.5wt.%, Mn 0.1-0.3 wt.%, and Al up to 0.6wt.%, Zn up to 0.5wt.%, with Be 20ppm with the balance being magnesium and inevitable impurities.
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PCT/EP2020/061769 WO2020221752A1 (en) | 2019-04-29 | 2020-04-28 | A casting magnesium alloy for providing improved thermal conductivity |
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US20100310409A1 (en) * | 2008-01-09 | 2010-12-09 | Cast Crc Limited | Magnesium based alloy |
US11926887B2 (en) * | 2019-02-20 | 2024-03-12 | Husqvarna Ab | Magnesium alloy, a piston manufactured by said magnesium alloy and a method for manufacturing said piston |
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US3094413A (en) | 1960-09-14 | 1963-06-18 | Magnesium Elektron Ltd | Magnesium base alloys |
GB0323855D0 (en) * | 2003-10-10 | 2003-11-12 | Magnesium Elektron Ltd | Castable magnesium alloys |
CN100338250C (en) | 2004-05-19 | 2007-09-19 | 中国科学院金属研究所 | High strength and high toughness cast magnesium alloy and preparing process thereof |
JP2008536008A (en) * | 2005-04-04 | 2008-09-04 | カースト センター ピーティーワイ リミテッド | Magnesium alloy |
CN101228286A (en) * | 2005-05-26 | 2008-07-23 | 铸造中心有限公司 | Hpdc magnesium alloy |
CN100513606C (en) | 2007-09-06 | 2009-07-15 | 北京有色金属研究总院 | Heat conductive magnesium alloy and method for preparing the same |
CN100575522C (en) | 2007-09-06 | 2009-12-30 | 北京有色金属研究总院 | Heat conductive magnesium alloy and preparation method thereof |
CN100513607C (en) | 2007-09-06 | 2009-07-15 | 北京有色金属研究总院 | Heat conductive magnesium alloy and method for preparing the same |
CN101158002B (en) * | 2007-11-06 | 2011-01-12 | 中国科学院长春应用化学研究所 | AE series thermo-stable die-casting magnesium alloy containing cerium and lanthanide |
CN101709418B (en) | 2009-11-23 | 2013-01-30 | 北京有色金属研究总院 | Thermally conductive magnesium alloy and preparation method thereof |
CN102061415B (en) * | 2011-01-19 | 2012-05-09 | 创金美科技(深圳)有限公司 | Die cast magnesium alloy with heat cracking resistance and high fluidity |
JP5590413B2 (en) | 2011-03-22 | 2014-09-17 | 株式会社豊田自動織機 | High thermal conductivity magnesium alloy |
CN102251161A (en) | 2011-07-14 | 2011-11-23 | 四川大学 | Heat conductive magnesium alloy |
CN102560210A (en) | 2012-03-28 | 2012-07-11 | 四川大学 | Mg-Sn-Ca heat-conductive cast magnesium alloy |
CN102719716B (en) | 2012-05-28 | 2014-10-15 | 哈尔滨工业大学 | Preparation method of heat conduction magnesium alloy |
CN104046867B (en) | 2014-06-26 | 2017-01-25 | 宝山钢铁股份有限公司 | High-plasticity heat-conducting magnesium alloy and preparation method thereof |
CN104152769B (en) | 2014-08-21 | 2016-05-04 | 重庆大学 | A kind of heat conductive magnesium alloy and preparation method thereof |
CN105401032B (en) * | 2015-12-14 | 2017-08-25 | 宝山钢铁股份有限公司 | A kind of inexpensive high heat conduction diecast magnesium alloy and its manufacture method |
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