WO2019152738A1 - Alliage d'électrode d'aluminium résistant à la corrosion - Google Patents

Alliage d'électrode d'aluminium résistant à la corrosion Download PDF

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Publication number
WO2019152738A1
WO2019152738A1 PCT/US2019/016184 US2019016184W WO2019152738A1 WO 2019152738 A1 WO2019152738 A1 WO 2019152738A1 US 2019016184 W US2019016184 W US 2019016184W WO 2019152738 A1 WO2019152738 A1 WO 2019152738A1
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ppm
corrosion resistant
aluminum
aluminum alloy
alloy composition
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PCT/US2019/016184
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English (en)
Inventor
Hasso Weiland
Elizabeth L. RALPH
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Arconic Inc.
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Publication of WO2019152738A1 publication Critical patent/WO2019152738A1/fr
Priority to US16/923,886 priority Critical patent/US20200332395A1/en

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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C21/00—Alloys based on aluminium
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/02—Making non-ferrous alloys by melting
    • C22C1/026—Alloys based on aluminium
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C21/00—Alloys based on aluminium
    • C22C21/06—Alloys based on aluminium with magnesium as the next major constituent
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/055—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material
    • C25B11/057—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material consisting of a single element or compound
    • C25B11/061—Metal or alloy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/46—Alloys based on magnesium or aluminium
    • H01M4/463—Aluminium based
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present disclosure is directed towards aluminum electrode alloys with improved corrosion resistance.
  • Utilizing aluminum alloy compositions as an aluminum electrode (e.g., anode) alloy product in an electrochemical cell can be evaluated by quantifying and/or qualifying two phenomena: (1) the anodic reaction and (2) the corrosion reaction of the aluminum electrode alloy composition.
  • aluminum reacts with hydroxyl ions which results in the release of electrons, the primary and desirable product of an electrochemical cell.
  • the aluminum in the aluminum electrode (e.g., anode) alloy product material is oxidized in the presence of water and as the oxygen in the water reacts with the aluminum, aluminum oxide is formed, generating hydrogen gas (e.g. a byproduct of the corrosion reaction of the aluminum anode alloy composition).
  • the extent of corrosion reaction i.e. the amount of hydrogen generated for an aluminum electrode alloy product used as an anode, is a function of electrolyte temperatures and current densities in the electrochemical cell. As operating temperatures and applied current vary for the operation of the cell, so too does the aluminum electrode alloy composition experience varying instances of high anodic reaction and high corrosion reaction windows within the operating parameters/ranges of the electrolytic cell.
  • the present disclosure is directed towards aluminum alloys with improved corrosion resistance when employed as an aluminum electrode alloy product in an electrochemical cell. More specifically, the present disclosure is directed towards aluminum electrode alloys having compositions including from 20 to 600 ppm Fe (i.e., from 0.002 to 0.06 wt.
  • One or more embodiments of the present disclosure are directed towards aluminum electrode alloy compositions configured with corrosion resistant additives present in an effective amount to reduce the hydrogen generation in an electrochemical cell thereby controlling (i.e. reducing and/or eliminating) the corrosion reaction.
  • the phrase “the aluminum alloy” means an alloy with aluminum as the predominant alloying element.
  • the aluminum alloy body may be selected from the group consisting of series of aluminum alloys registered with the Aluminum Association and unregistered variants of the same, as defined by the Aluminum Association document “International Alloy Designations and Chemical Composition Limits for Wrought Aluminum and Wrought Aluminum Alloys” (2009).
  • the aluminum alloy is a lxxx series aluminum alloy.
  • the aluminum alloy is a 2xxx series aluminum alloy.
  • the aluminum alloy is a 3xxx series aluminum alloy.
  • the aluminum alloy is a 4xxx series aluminum alloy.
  • the aluminum alloy is a 5xxx series aluminum alloy. In some embodiments, the aluminum alloy is a 6xxx series aluminum alloy. In some embodiments, the aluminum alloy is a 7xxx series aluminum alloy. In some embodiments, the aluminum alloy is an 8xxx series aluminum alloy. In some embodiments, the aluminum alloy is selected from the group consisting of a lxxx series aluminum alloy, a 2xxx series aluminum alloy, a 3xxx series aluminum alloy, a 4xxx series aluminum alloy, a 5xxx series aluminum alloy, a 6xxx series aluminum alloy, a 7xxx series aluminum alloy, and an 8xxx series aluminum alloy.
  • unavoidable impurities in this embodiment means the presence of an undesirable component.
  • an unavoidable impurity is present in a quantity or amount that is low enough to not change a desired property and/or characteristic (i.e. below a threshold to modify the corrosion resistance of the corrosion resistant aluminum alloy composition and/or reduce the corrosion resistance above a certain margin of improvement when compared to the reference aluminum alloy composition material evaluated in an electrochemical cell test).
  • Mn as the corrosion resistant additives in an iron-containing lxxx, 2xxx, 3xxx, 4xxx, 5xxx, 6xxx, 7xxx, or 8xxx series aluminum electrode alloy composition will provide improved corrosion resistance (e.g. reduced corrosion) as compared to an iron-containing aluminum alloy composition (of the same series) that does not have these Mn additions (e.g. as an alloying element).
  • additions of Mn in the aluminum electrode alloy composition will improve corrosion resistance of the resulting aluminum anode alloy product in the electrochemical cell during a wide range of electrochemical cell operating conditions (e.g. temperature and current efficiency) as compared to an iron- containing aluminum alloy without such Mn additions.
  • electrochemical cell operating conditions e.g. temperature and current efficiency
  • the additions of Mn will provide significant improvement to corrosion resistance at electrochemical cell operating conditions of high corrosion (e.g. low current densities and/or low temperatures) for conventional aluminum alloy compositions without such additions.
  • an aluminum alloy composition comprising: an effective amount of a corrosion resistant additive.
  • an“effective amount” in this embodiment is a large enough quantity to provide an improved corrosion resistance in the aluminum electrode alloy composition (e.g. measurable, observable, and/or quantifiable).
  • improved corrosion resistance is evaluated in an electrochemical cell test.
  • the aluminum electrode alloy composition is an iron-containing lxxx, 2xxx, 3xxx, 4xxx, 5xxx, 6xxx, 7xxx, or 8xxx series aluminum electrode alloy composition.
  • corrosion resistant additive in this embodiment refers to an addition of a component to an aluminum alloy composition (e.g. lxxx, 2xxx, 3xxx, 4xxx, 5xxx, 6xxx, 7xxx, or 8xxx series aluminum alloys) in order to impart corrosion resistance (e.g. reduce corrosion when evaluated as an aluminum electrode alloy product in an electrochemical cell) as compared to the alloy’s corrosion without such additions.
  • an aluminum alloy composition e.g. lxxx, 2xxx, 3xxx, 4xxx, 5xxx, 6xxx, 7xxx, or 8xxx series aluminum alloys
  • the corrosion resistant additive may include Mn.
  • aluminum is the predominant alloying element of the aluminum alloy composition.
  • the aluminum alloy composition includes at least 90 wt. % Al.
  • the corrosion resistant aluminum alloy composition may have: an effective amount of a corrosion resistant additive; from 20 to 600 ppm Fe; from 10 - 800 ppm Mn; and the balance being aluminum (e.g., and unavoidable impurities).
  • the corrosion resistant aluminum alloy composition may have at least 1 ppm, or at least 5 ppm, or at least 10 ppm, or at least 20 ppm, or at least 30 ppm, or at least 40 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm Fe.
  • the corrosion resistant aluminum alloy composition may have not greater than 1 ppm, or not greater than 5 ppm, or not greater than 10 ppm, or not greater than 20 ppm, or not greater than 30 ppm, or not greater than 40 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm, or not greater than 550 ppm, or not greater than 600 ppm Fe.
  • the corrosion resistant aluminum alloy composition may have at least 1 ppm, at least 5 ppm, or at least 10 ppm, or at least 15 ppm, or at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm, or at least 650 ppm, or at least 700 ppm, or at least 750 ppm, or at least 800 ppm Mn, where at least some (an effective amount of) Mn is present, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum alloy composition may have from 10 to 800 ppm, or from 80 to 800 ppm, or from 70 to 800 ppm, or from 60 to 800 ppm, or from 50 to 800 ppm, or from 40 to 800 ppm, or from 30 to 600 ppm, or from 28 to 560 ppm, or from 26 to 520 ppm, or from 24 to 480 ppm, or from 22 to 440 ppm, or from 20 to 400 ppm, or from 18 to 360 ppm, or from 16 to 320 ppm, or from 14 to 280 ppm, or or from 12 to 240 ppm, or from 10 to 200 ppm, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum alloy composition may have about 10 ppm, or about 15 ppm, or about 20 ppm, or about 50 ppm, or about 60 ppm, or about 70 ppm, or about 80 ppm, or about 100 ppm, or about 150 ppm, or about 200 ppm, or about 250 ppm, or about 300 ppm, or about 350 ppm, or about 400 ppm, or about 450 ppm, or about 500 ppm, or about 550 ppm, or about 600 ppm, or about 650 ppm, or about 700 ppm, or about 750 ppm, or about 800 ppm, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum alloy composition may have 10 ppm, or 15 ppm, or 20 ppm, or 50 ppm, or 60 ppm, or 70 ppm, or 80 ppm, or 100 ppm, or 150 ppm, or 200 ppm, or 250 ppm, or 300 ppm, or 350 ppm, or 400 ppm, or 450 ppm, or 500 ppm, or 550 ppm, or 600 ppm, or 650 ppm, or 700 ppm, or 750 ppm, or 800 ppm, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum alloy composition may contain an effective amount of the corrosion resistant additive, Mn.
  • the effective amount of the corrosion resistant additive, Mn may include any of the manganese amounts described above, e.g. from 10 to 800 ppm Mn.
  • the corrosion resistant aluminum alloy composition may contain, as a purposefully added alloying element, Mn in any of the amounts described above, e.g. from 10 to 800 ppm Mn, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum alloy composition may be any suitable aluminum alloy, such as any of the lxxx series, 2xxx series, 3xxx series, 4xxx series, 5xxx series, 6xxx series, 7xxx series, or 8xxx series aluminum alloy compositions described above, and the corrosions resistant aluminum alloy composition may include any of the manganese amounts described above, e.g. an effective amount of Mn as corrosion resistant additive; from 20 to 600 ppm Fe; from 10 - 800 ppm Mn; and the balance being aluminum (e.g., and unavoidable impurities).
  • the corrosion resistant aluminum alloy composition may include at least 0.005 vol. % of Fe-Mn-bearing intermetallic particles, where a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy is from 0.25: 1 to 7: 1.
  • a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum alloy composition may be from about 0.25: 1 to about 7: 1. In one embodiment, a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum alloy composition may be 1.0. In another embodiment, a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum alloy composition may be about 1.0.
  • a ratio of Fe (ppm)- to-Mn (ppm) in the corrosion resistant aluminum alloy composition may be at least 0.25, or at least 0.35, or at least 0.45, or least 0.5, or at least 0.6, or at least 0.7, or at least 0.8, or at least 0.9, or at least 1.0.
  • a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum alloy composition may be not greater than 7.0, or not greater than 6.5, or not greater than 6.0, or not greater than 5.5, or not greater than 5.0, or not greater than 4.5, or not greater than 4.0, or not greater than 3.5, or not greater than 3.0, or not greater than 2.5, or not greater than 2.0, or not greater than 1.5, or not greater than 1.0.
  • the corrosion resistant aluminum alloy composition may include not greater than 0.04 vol. % of Fe-Mn-bearing intermetallic particles.
  • Optional corrosion resistant additives may include, for instance, zinc and/or gallium.
  • zinc and/or gallium as corrosion resistant additives are defined and described in commonly-owned International Patent Application No. PCT/US2017/066053, entitled, “Corrosion Resistant Aluminum Alloy,” filed December 13, 2017, published as WO2018/112018.
  • optional corrosion resistant additive refers to an optional addition of a component to an aluminum alloy composition in order to impart corrosion resistance as compared to the alloy’s corrosion without such additions.
  • the optional corrosion resistant additive may be added in addition to manganese.
  • Various embodiments relating to optional corrosion resistant additives are described herein.
  • an optional corrosion resistant additive may be Zn. In another embodiment, an optional corrosion resistant additive may be Ga. In yet another embodiment, optional corrosion resistant additives may be Zn and Ga. In another embodiment, optional corrosion resistant additives are selected from the group consisting of: Zn, Ga, and combinations thereof.
  • the effective amount of optional corrosion resistant additive may be at least 5 ppm, or at least 10 ppm, or at least 15 ppm, or at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm, or at least 650 ppm, or at least 700 ppm, or at least 750 ppm, or at least 800 ppm, or at least 850 ppm, or at least 900 ppm, or at least 950 ppm, or at least 1000 ppm, where at least some (an effective amount of) Zn and Ga are present, when both Zn and Ga are utilized as the optional corrosion resistant additives.
  • the effective amount of optional corrosion resistant additive may be not greater than 5 ppm, or not greater than 10 ppm, or not greater than 15 ppm, or not greater than 20 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm, or not greater than 550 ppm, or not greater than 600 ppm, or not greater than 650 ppm, or not greater than 700 ppm, or not greater than 750 ppm, or not greater than 800 ppm, or not greater than 850 ppm, or not greater than 900 ppm, or not greater than 950 ppm, or not greater than 1000 ppm, where not greater than some (an effective amount of) Zn and
  • the amount of Zn as an optional corrosion resistant additive as an individual addition may be not greater than 500 ppm of the corrosion resistant aluminum alloy composition.
  • the effective amount of optional corrosion resistant additive of Zn may be at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm.
  • the effective amount of optional corrosion resistant additive of Zn may be not greater than 20 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm.
  • an effective amount of the optional corrosion resistant additive of Zn may be at least 20 ppm to not greater than 500 ppm.
  • the amount of Ga as an optional corrosion resistant additive as an individual addition may be not greater than 600 ppm of the corrosion resistant aluminum alloy composition. In one or more of the aforementioned embodiments, the amount of Ga as an optional corrosion resistant additive as an individual addition may be not greater than 0.0 ppm of the corrosion resistant aluminum alloy composition.
  • the effective amount of an optional corrosion resistant additive of Ga may be at least 5 ppm, or at least 10 ppm, or at least 15 ppm, or at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm.
  • the effective amount of an optional corrosion resistant additive of Ga may be not greater than 5 ppm, or not greater than 10 ppm, or not greater than 15 ppm, or not greater than 20 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm, or not greater than 550 ppm, or not greater than 600 ppm. In some embodiments, the effective amount of an optional corrosion resistant additive of Ga may be at least 20 ppm to not greater than 500 ppm.
  • an effective amount of the optional corrosion resistant additive may be at least 5 ppm to not greater than 600 ppm, or at least 10 ppm to not greater than 300 ppm, or at least 5 ppm to not greater than 100 ppm, or at least 5 ppm to not greater than 50 ppm, or at least 20 ppm to not greater than 100 ppm, or at least 20 ppm to not greater than 50 ppm, or at least 20 ppm to not greater than 1000 ppm, or at least 50 ppm to not greater than 1000 ppm, or at least 50 ppm to not greater than 700 ppm, or at least 50 ppm to not greater than 500 ppm, or at least 50 ppm to not greater than 300 ppm, or at least 50 ppm to not greater than 200 ppm, or at least 50 ppm to not greater than 100 ppm, or at least 20 ppm to not greater than 500 ppm of each additive, where the total amount of the optional corrosion resistant
  • an effective amount of optional corrosion resistant additive may be not greater than 1000 ppm, or not greater than 500 ppm, or not greater than 250 ppm, or not greater than 100 ppm, or not greater than 50 ppm, or not greater than 20 ppm, where at least some optional corrosion resistant additive is present
  • the optional corrosion resistant additive may be Zn and Ga in equal amounts. In any of the foregoing embodiments, the optional corrosion resistant additive may be Zn and Ga, with a greater amount of Zn than Ga. In any of the foregoing embodiments, the optional corrosion resistant additive may be Zn and Ga, with a lesser amount of Zn than Ga.
  • the corrosion resistant aluminum alloy composition may be a 5xxx series alloy.
  • the corrosion resistant aluminum alloy composition may include at least 0.2 wt. % Mg, or at least 0.5 wt. %, or at least 1.0 wt. %, or at least 1.5 wt. %, or at least 2.0 wt. % Mg.
  • the corrosion resistant aluminum alloy composition may include not greater than 5.0 wt. %, or not greater than 4.0 wt. %, or not greater than 3.0 wt. %, or not greater than 2.0 wt. % Mg, or not greater than 1.5 wt. %, or not greater than 1.0 wt.
  • the corrosion resistant aluminum alloy composition may include from 0.2 to 5.0 wt. %, or from 0.5 to 5.0 wt. %, or from 1.0 to 5.0 wt. %, or from 1.5 to 5.0 wt. %, or from 2.0 to 5.0 wt. %, or from 3.0 to 5.0 wt. %, or from 4.0 to 5.0 wt. %, or from 0.01 to 4.0 wt. %, or from 0.2 to 3.0 wt. %, or from 0.2 to 2.0 wt. %, or from 0.2 to 1.5 wt. %, or from 0.2 to 1.0 wt. % Mg.
  • the corrosion resistant aluminum alloy composition has no Mg (i.e. includes Mg as an impurity only).
  • the corrosion resistant aluminum alloy composition may be a 5xxx series alloy and may include 0.2-5.0 wt. % Mg, 20-600 ppm Fe, 10-800 ppm Mn, where a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy is from 0.25: 1 to 7: 1.
  • the corrosion resistant 5xxx aluminum alloy may include 70-110 ppm Fe, 30-50 ppm Mn, where a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy is from 1.4: 1 to 3.6: 1, 90-110 ppm Zn, and 90-110 ppm Ga.
  • the corrosion resistant 5xxx aluminum alloy may include from 0.005 to 0.04 vol. % of Fe-Mn -bearing intermetallic particles.
  • “reference aluminum alloy composition” in this embodiment means an aluminum alloy composition having less than 3 ppm Mn.
  • reference aluminum electrode alloy product in this embodiment means an aluminum electrode (e.g., anode) alloy product formed from the reference aluminum alloy composition.
  • the iron-containing corrosion resistant aluminum alloy composition may be configured with the corrosion resistant additive(s) (e.g., Mn) in an effective amount such, when employed as an aluminum electrode (e.g., anode) alloy product, the aluminum alloy composition has a greater corrosion resistance as compared to an a reference aluminum electrode (e.g., anode) alloy product formed from an iron-containing reference (e.g., baseline/control) aluminum alloy composition without such Mn additives, when measured in accordance with an electrochemical cell test.
  • the corrosion resistant additive(s) e.g., Mn
  • Mn corrosion resistant additive
  • the reference aluminum alloy composition may contain a substantially equivalent amount of Fe as a sample (non-baseline/control) aluminum electrode alloy composition.
  • an aluminum electrode alloy comprising: an effective amount of a corrosion resistant additive.
  • an“effective amount” in this embodiment is a large enough quantity to provide an improved corrosion resistance in the aluminum electrode alloy composition (e.g. measurable, observable, and/or quantifiable).
  • improved corrosion resistance is evaluated in an electrochemical cell test.
  • the aluminum electrode alloy composition is an iron-containing lxxx, 2xxx, 3xxx, 4xxx, 5xxx, 6xxx, 7xxx, or 8xxx series aluminum electrode alloy composition.
  • corrosion resistant additive in this embodiment refers to an addition of a component to an aluminum electrode alloy (e.g. lxxx, 2xxx, 3xxx, 4xxx, 5xxx, 6xxx, 7xxx, or 8xxx series aluminum alloys) in order to impart corrosion resistance (e.g. reduce corrosion when evaluated as an aluminum electrode alloy product in an electrochemical cell) as compared to the alloy’s corrosion without such additions.
  • an aluminum electrode alloy e.g. lxxx, 2xxx, 3xxx, 4xxx, 5xxx, 6xxx, 7xxx, or 8xxx series aluminum alloys
  • the corrosion resistant additive may include Mn.
  • aluminum is the predominant alloying element of the aluminum electrode alloy.
  • the aluminum electrode alloy includes at least 90 wt. % Al.
  • the corrosion resistant aluminum electrode alloy has: an effective amount of a corrosion resistant additive; from 20 to 600 ppm Fe; from 10 - 800 ppm Mn; and the balance being aluminum (e.g., and unavoidable impurities).
  • the corrosion resistant aluminum electrode alloy may have at least 1 ppm, or at least 5 ppm, or at least 10 ppm, or at least 20 ppm, or at least 30 ppm, or at least 40 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm Fe.
  • the corrosion resistant aluminum electrode alloy may have not greater than 1 ppm, or not greater than 5 ppm, or not greater than 10 ppm, or not greater than 20 ppm, or not greater than 30 ppm, or not greater than 40 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm, or not greater than 550 ppm, or not greater than 600 ppm Fe.
  • the corrosion resistant aluminum electrode alloy may have at least 1 ppm, at least 5 ppm, or at least 10 ppm, or at least 15 ppm, or at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm, or at least 650 ppm, or at least 700 ppm, or at least 750 ppm, or at least 800 ppm Mn, where at least some (an effective amount of) Mn is present, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum electrode alloy may have not greater than 1 ppm, or not greater than 5 ppm, or not greater than 10 ppm, or not greater than 15 ppm, or not greater than 20 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm, or not greater than 550 ppm, or not greater than 600 ppm, or not greater than 650 ppm, or not greater than 700 ppm, or not greater than 750 ppm, or not greater than 800 ppm Mn, where not greater than some (an effective amount of) Mn is present, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum electrode alloy may have from 10 to 800 ppm, or from 80 to 800 ppm, or from 70 to 800 ppm, or from 60 to 800 ppm, or from 50 to 800 ppm, or from 40 to 800 ppm, or from 30 to 600 ppm, or from 28 to 560 ppm, or from 26 to 520 ppm, or from 24 to 480 ppm, or from 22 to 440 ppm, or from 20 to 400 ppm, or from 18 to 360 ppm, or from 16 to 320 ppm, or from 14 to 280 ppm, or from 12 to 240 ppm, or from 10 to 200 ppm, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum electrode alloy may have about 10 ppm, or about 15 ppm, or about 20 ppm, or about 50 ppm, or about 60 ppm, or about 70 ppm, or about 80 ppm, or about 100 ppm, or about 150 ppm, or about 200 ppm, or about 250 ppm, or about 300 ppm, or about 350 ppm, or about 400 ppm, or about 450 ppm, or about 500 ppm, or about 550 ppm, or about 600 ppm, or about 650 ppm, or about 700 ppm, or about 750 ppm, or about 800 ppm, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum electrode alloy may have 10 ppm, or 15 ppm, or 20 ppm, or 50 ppm, or 60 ppm, or 70 ppm, or 80 ppm, or 100 ppm, or 150 ppm, or 200 ppm, or 250 ppm, or 300 ppm, or 350 ppm, or 400 ppm, or 450 ppm, or 500 ppm, or 550 ppm, or 600 ppm, or 650 ppm, or 700 ppm, or 750 ppm, or 800 ppm, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum electrode alloy may contain an effective amount of the corrosion resistant additive, Mn.
  • the effective amount of the corrosion resistant additive, Mn may include any of the manganese amounts described above, e.g. from 10 to 800 ppm Mn.
  • the corrosion resistant aluminum electrode alloy may contain, as a purposefully added alloying element, Mn in any of the amounts described above, e.g. from 10 to 800 ppm Mn, when Mn is utilized as the corrosion resistant additive.
  • the corrosion resistant aluminum electrode alloy may be any suitable aluminum alloy, such as any of the lxxx series, 2xxx series, 3xxx series, 4xxx series, 5xxx series, 6xxx series, 7xxx series, or 8xxx series aluminum alloy compositions described above, and the corrosion resistant aluminum electrode alloy may include any of the Mn amounts described above, e.g. an effective amount of Mn as a corrosion resistant additive; from 20 to 600 ppm Fe; from 10 - 800 ppm Mn; and the balance being aluminum (e.g., and unavoidable impurities).
  • the corrosion resistant aluminum electrode alloy may include at least 0.005 vol. % of Fe-Mn-bearing intermetallic particles, where a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy is from 0.25: 1 to 7: 1.
  • a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy may be from about 0.25: 1 to about 7: 1. In one embodiment, a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy may be 1.0. In another embodiment, a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy may be about 1.0.
  • a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum electrode alloy may be at least 0.25, or at least 0.35, or at least 0.45, or at least 0.5, or at least 0.6, or at least 0.7, or at least 0.8, or at least 0.9, or at least 1.0.
  • a ratio of Fe (ppm)-to-Mn (ppm) in the corrosion resistant aluminum alloy composition may be: not greater than 7.0, or not greater than 6.5, or not greater than 6.0, or not greater than 5.5, or not greater than 5.0, or not greater than 4.5, or not greater than 4.0, or not greater than 3.5, or not greater than 3.0, or not greater than 2.5, or not greater than 2.0, or not greater than 1.5, or not greater than 1.0.
  • the corrosion resistant aluminum electrode alloy may include not greater than 0.04 vol. % of Fe-Mn-bearing intermetallic particles.
  • “reference aluminum electrode alloy” in this embodiment means an aluminum alloy having less than 3 ppm Mn.
  • Optional corrosion resistant additives may include, for instance, zinc and/or gallium.
  • zinc and/or gallium as corrosion resistant additives are defined and described in commonly-owned International Patent Application No. PCT/US2017/066053, entitled, “Corrosion Resistant Aluminum Alloy,” filed December 13, 2017, published as WO2018/112018.
  • optional corrosion resistant additive refers to an optional addition of a component to an aluminum electrode alloy in order to impart corrosion resistance as compared to the alloy’s corrosion without such additions.
  • the optional corrosion resistant additive may be added in addition to manganese.
  • Various embodiments relating to optional corrosion resistant additives are described herein.
  • an optional corrosion resistant additive may be Zn. In another embodiment, an optional corrosion resistant additive may be Ga. In yet another embodiment, optional corrosion resistant additives may be Zn and Ga. In another embodiment, optional corrosion resistant additives are selected from the group consisting of: Zn, Ga, and combinations thereof.
  • the effective amount of optional corrosion resistant additive may be at least 5 ppm, or at least 10 ppm, or at least 15 ppm, or at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm, or at least 650 ppm, or at least 700 ppm, or at least 750 ppm, or at least 800 ppm, or at least 850 ppm, or at least 900 ppm, or at least 950 ppm, or at least 1000 ppm, where at least some (an effective amount of) Zn and Ga are present, when both Zn and Ga are utilized as the optional corrosion resistant additives.
  • the effective amount of optional corrosion resistant additive may be not greater than 5 ppm, or not greater than 10 ppm, or not greater than 15 ppm, or not greater than 20 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm, or not greater than 550 ppm, or not greater than 600 ppm, or not greater than 650 ppm, or not greater than 700 ppm, or not greater than 750 ppm, or not greater than 800 ppm, or not greater than 850 ppm, or not greater than 900 ppm, or not greater than 950 ppm, or not greater than 1000 ppm, where not greater than some (an effective amount of) Zn and
  • the amount of Zn as an optional corrosion resistant additive as an individual addition may be not greater than 500 ppm of the corrosion resistant aluminum electrode alloy.
  • the effective amount of optional corrosion resistant additive of Zn may be at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm.
  • the effective amount of optional corrosion resistant additive of Zn may be not greater than 20 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm.
  • an effective amount of the optional corrosion resistant additive of Zn may be at least 20 ppm to not greater than 500 ppm.
  • the amount of Ga as an optional corrosion resistant additive as an individual addition may be: not greater than 600 ppm of the corrosion resistant aluminum electrode alloy. In one or more of the aforementioned embodiments, the amount of Ga as an optional corrosion resistant additive as an individual addition may be not greater than 0.0 ppm of the corrosion resistant aluminum electrode alloy.
  • the effective amount of an optional corrosion resistant additive of Ga may be at least 5 ppm, or at least 10 ppm, or at least 15 ppm, or at least 20 ppm, or at least 50 ppm, or at least 100 ppm, or at least 150 ppm, or at least 200 ppm, or at least 250 ppm, or at least 300 ppm, or at least 350 ppm, or at least 400 ppm, or at least 450 ppm, or at least 500 ppm, or at least 550 ppm, or at least 600 ppm.
  • the effective amount of an optional corrosion resistant additive of Ga may be not greater than 5 ppm, or not greater than 10 ppm, or not greater than 15 ppm, or not greater than 20 ppm, or not greater than 50 ppm, or not greater than 100 ppm, or not greater than 150 ppm, or not greater than 200 ppm, or not greater than 250 ppm, or not greater than 300 ppm, or not greater than 350 ppm, or not greater than 400 ppm, or not greater than 450 ppm, or not greater than 500 ppm, or not greater than 550 ppm, or not greater than 600 ppm. In some embodiments, the effective amount of an optional corrosion resistant additive of Ga may be at least 20 ppm to not greater than 500 ppm.
  • an effective amount of the optional corrosion resistant additive may be at least 5 ppm to not greater than 600 ppm, or at least 10 ppm to not greater than 300 ppm, or at least 5 ppm to not greater than 100 ppm, or at least 5 ppm to not greater than 50 ppm, or at least 20 ppm to not greater than 100 ppm, or at least 20 ppm to not greater than 50 ppm, or at least 20 ppm to not greater than 1000 ppm, or at least 50 ppm to not greater than 1000 ppm, or at least 50 ppm to not greater than 700 ppm, or at least 50 ppm to not greater than 500 ppm, or at least 50 ppm to not greater than 300 ppm, or at least 50 ppm to not greater than 200 ppm, or at least 50 ppm to not greater than 100 ppm, or at least 20 ppm to not greater than 500 ppm of each additive, where the total amount of the optional corrosion resistant
  • an effective amount of optional corrosion resistant additive may be not greater than 1000 ppm, or not greater than 500 ppm, or not greater than 250 ppm, or not greater than 100 ppm, not greater than 50 ppm, or not greater than 20 ppm, where at least some optional corrosion resistant additive is present.
  • the optional corrosion resistant additive may be Zn and Ga in equal amounts. In any of the foregoing embodiments, the optional corrosion resistant additive may be Zn and Ga, with a greater amount of Zn than Ga. In any of the foregoing embodiments, the optional corrosion resistant additive may be Zn and Ga, with a lesser amount of Zn than Ga.
  • the corrosion resistant aluminum electrode alloy may be a 5xxx series alloy.
  • the corrosion resistant aluminum alloy composition may include at least 0.2 wt. % Mg, or at least 0.5 wt. %, or at least 1.0 wt. %, or at least 1.5 wt. %, or at least 2.0 wt. % Mg.
  • the corrosion resistant aluminum electrode alloy may include not greater than 5.0 wt. %, or not greater than 4.0 wt. %, or not greater than 3.0 wt. %, or not greater than 2.0 wt. % Mg, or not greater than 1.5 wt. %, or not greater than 1.0 wt.
  • the corrosion resistant aluminum electrode alloy may include from 0.2 to 5.0 wt. %, or from 0.5 to 5.0 wt. %, or from 1.0 to 5.0 wt. %, or from 1.5 to 5.0 wt. %, or from 2.0 to 5.0 wt. %, or from 3.0 to 5.0 wt. %, or from 4.0 to 5.0 wt. %, or from 0.2 to 4.0 wt. %, or from 0.2 to 3.0 wt. %, or from 0.2 to 2.0 wt. %, or from 0.2 to 1.5 wt. %, or from 0.2 to 1.0 wt. % Mg.
  • the corrosion resistant aluminum electrode alloy has no Mg (i.e. includes Mg as an impurity only).
  • reference aluminum electrode alloy product in this embodiment means an aluminum electrode (e.g., anode) alloy product formed from the reference aluminum electrode alloy.
  • the iron-containing corrosion resistant aluminum electrode alloy may be configured with the corrosion resistant additive(s) (e.g., Mn) in an effective amount such, when employed as an aluminum electrode (e.g., anode) alloy product, the aluminum electrode alloy may have a greater corrosion resistance as compared to an a reference aluminum electrode (e.g., anode) alloy product formed from an iron-containing reference (e.g., baseline/control) aluminum electrode alloy without such Mn additives, when measured in accordance with an electrochemical cell test.
  • the corrosion resistant additive(s) e.g., Mn
  • Mn corrosion resistant additive
  • the reference aluminum electrode alloy may contain a substantially equivalent amount of Fe as a sample (non-baseline/control) aluminum electrode alloy.
  • a method for producing an aluminum electrode alloy product may comprise the steps of: a) forming a melt of an aluminum alloy, and (b) depositing the melt to form an aluminum electrode alloy product.
  • the forming step a) may comprise (i) using 20 - 600 ppm Fe in the melt, and (ii) using 10 - 800 ppm Mn in the melt, where a ratio of Fe (ppm)-to-Mn (ppm) in the melt is from 0.5: 1 to 4: 1, and where aluminum is the predominant alloying element of the aluminum alloy product.
  • the depositing step b) may comprise (i) casting the melt into the aluminum electrode alloy product, and (ii) producing at least 0.005 vol. % of Fe-Mn-bearing intermetallic particles, where the aluminum electrode alloy product includes at least 0.005 vol. % of the Fe-Mn- bearing intermetallic particles.
  • Figure 1 is a schematic view of an example of an electrochemical cell that is configured for use in evaluating the corrosion of electrodes in an electrolyte in accordance with Example 2.
  • Figure 2 is a graph showing hydrogen gas generation for different aluminum electrode alloy compositions in accordance with Examples 1 and 2.
  • Aluminum electrode alloys having the compositions shown in Table 2, below, were cast as ingots.
  • the target magnesium content for all alloys was 2.5 wt. %.
  • the target iron content for all alloys was 90 ppm.
  • the A-alloys had varying amounts of manganese, but contained no gallium or zinc.
  • the B-alloys had varying amounts of manganese and also contained gallium and zinc.
  • the ingots were then rolled to the desired thickness, and machined into disks having a desired thickness and a diameter, with a sufficient cross-sectional surface area to provide a viable testing surface for immersion into an electrochemical cell (schematically depicted in Figure 1) for the evaluation and assessment of corrosion within the range of operating conditions of the cell (e.g. time, temperatures, current efficiency, etc.).
  • the electrochemical cell consists of a counter electrode and an aluminum electrode (anode) alloy product submerged in an aqueous electrolyte.
  • the electrochemical cell is equipped with a mass-flow meter for measuring hydrogen gas evolved from the aluminum anode alloy product. Current is applied on the aluminum anode alloy product, through the electrolyte, into the counter electrode.
  • the alloys were tested according to the following procedure.
  • a predefined temperature-and-current step control program was applied to the cell so that the hydrogen evolution rate was measured over a set range of operating temperatures, i.e. between room temperature and l00°C and over a set of current densities, ranging from 0 to 300 mA/cm 2 .
  • Figure 2 shows the hydrogen generation results for all alloys.
  • the results of the A-alloys show the effects of adding manganese to the alloy.
  • Alloy l-A contains no manganese to serve as a control.
  • Alloys 3 -A, 4 -A, and 5- A generated less hydrogen than alloy l-A, demonstrating a beneficial effect of manganese on corrosion resistance at some amounts.
  • Both alloys 2- A and 6- A generated more hydrogen than alloy l-A, indicating there may be a beneficial range of manganese addition.
  • all of the B Alloys contained the same amount of gallium and zinc, and the manganese content was varied in a similar manner to the A-alloys.
  • alloys 2-B, 3-B and 4-B all generated less hydrogen than the corresponding A-alloys. Additionally, these three B-alloys all generated less hydrogen than both alloys l-A and l-B, indicating the beneficial effect of manganese, gallium and zinc on hydrogen generation. Alloy 5-B generated more hydrogen than alloy 5 -A, and alloy 6-B generated the most hydrogen of all samples, indicating that there may be a beneficial range of concentrations of manganese, gallium and zinc for hydrogen generation.
  • iron-containing aluminum electrode e.g., anode
  • alloy products e.g., having 70 ppm Fe
  • the hydrogen gas generation observed in the electrochemical cell test occurs primarily at Fe- bearing phases and/or particles present in the material.
  • aluminum electrode anode products containing iron e.g., having greater than about 60 ppm Fe
  • manganese e.g., alloys l-A and l-B
  • the corrosion reaction in the electrochemical cell test proceeds at a faster rate as compared to, for instance, alloys 3 -A and 3-B, due to a comparatively higher electrochemical difference between Fe- bearing phases and the aluminum alloy matrix.
  • alloys l-A and l-B were prone to greater material degradation and a lower electrical energy generation performance as compared other samples that contained manganese.
  • the Mn additives to the aluminum anode alloy products facilitate sequestration of at least a portion of the iron, thereby forming Fe-Mn -bearing interm etallic particles, and so reducing the electrochemical difference between the Fe-bearing phases and the aluminum alloy matrix.
  • An aluminum alloy composition comprising:
  • a ratio of Fe (ppm)-to-Mn (ppm) in the aluminum composition alloy is from 0.25: 1 to 7: 1.
  • the aluminum alloy composition comprises an optional corrosion resistant additive, wherein the optional corrosion resistant additive is selected from the group consisting of Zn, Ga, and combinations thereof.
  • a method comprising:
  • a melt of an aluminum alloy composition comprising:
  • a ratio of Fe (ppm)-to-Mn (ppm) in the melt is from 0.25: 1 to 7: 1; and b) depositing the melt to form an aluminum electrode alloy product, wherein the depositing comprises:
  • a 5xxx aluminum alloy composition comprising:

Abstract

L'invention concerne une composition d'alliage d'aluminium. La composition d'alliage d'aluminium peut comprendre de 20 à 600 ppm de Fe et de 10 à 800 ppm de Mn. Un rapport de Fe (ppm) à Mn (ppm) dans la composition d'alliage d'aluminium peut être situé dans la plage allant de 0,25:1 à 7:1.
PCT/US2019/016184 2018-01-31 2019-01-31 Alliage d'électrode d'aluminium résistant à la corrosion WO2019152738A1 (fr)

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JPH07116542B2 (ja) * 1990-10-15 1995-12-13 住友軽金属工業株式会社 自己耐食性および犠牲陽極効果にすぐれた熱交換器用アルミニウム合金フィン材
US20050199318A1 (en) * 2003-06-24 2005-09-15 Doty Herbert W. Castable aluminum alloy
CN104962792A (zh) * 2015-07-10 2015-10-07 湖南朗圣实验室技术发展有限公司 耐腐蚀硬质铝合金型材及其制备工艺
US20160153073A1 (en) * 2012-04-27 2016-06-02 Rio Tinto Alcan International Limited Aluminum alloy having an excellent combination of strength, extrudability and corrosion resistance
JP2016180175A (ja) * 2015-03-23 2016-10-13 株式会社神戸製鋼所 製缶後の光沢性に優れた樹脂被覆絞りしごき缶用アルミニウム合金板および絞りしごき缶用樹脂被覆アルミニウム合金板

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Publication number Priority date Publication date Assignee Title
JPH07116542B2 (ja) * 1990-10-15 1995-12-13 住友軽金属工業株式会社 自己耐食性および犠牲陽極効果にすぐれた熱交換器用アルミニウム合金フィン材
US20050199318A1 (en) * 2003-06-24 2005-09-15 Doty Herbert W. Castable aluminum alloy
US20160153073A1 (en) * 2012-04-27 2016-06-02 Rio Tinto Alcan International Limited Aluminum alloy having an excellent combination of strength, extrudability and corrosion resistance
JP2016180175A (ja) * 2015-03-23 2016-10-13 株式会社神戸製鋼所 製缶後の光沢性に優れた樹脂被覆絞りしごき缶用アルミニウム合金板および絞りしごき缶用樹脂被覆アルミニウム合金板
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