CN108893690B - Fine crystal strengthening method for silver-magnesium-nickel alloy - Google Patents

Fine crystal strengthening method for silver-magnesium-nickel alloy Download PDF

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CN108893690B
CN108893690B CN201810604878.4A CN201810604878A CN108893690B CN 108893690 B CN108893690 B CN 108893690B CN 201810604878 A CN201810604878 A CN 201810604878A CN 108893690 B CN108893690 B CN 108893690B
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magnesium
silver
nickel alloy
sheet
temperature
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CN108893690A (en
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王玉天
傅强
陈清明
胡劲
王开军
张维钧
段云彪
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Kunming University of Science and Technology
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    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22FCHANGING THE PHYSICAL STRUCTURE OF NON-FERROUS METALS AND NON-FERROUS ALLOYS
    • C22F1/00Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working
    • C22F1/14Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working of noble metals or alloys based thereon
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22FCHANGING THE PHYSICAL STRUCTURE OF NON-FERROUS METALS AND NON-FERROUS ALLOYS
    • C22F1/00Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working
    • C22F1/02Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working in inert or controlled atmosphere or vacuum
    • CCHEMISTRY; METALLURGY
    • C23COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23CCOATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C8/00Solid state diffusion of only non-metal elements into metallic material surfaces; Chemical surface treatment of metallic material by reaction of the surface with a reactive gas, leaving reaction products of surface material in the coating, e.g. conversion coatings, passivation of metals
    • C23C8/06Solid state diffusion of only non-metal elements into metallic material surfaces; Chemical surface treatment of metallic material by reaction of the surface with a reactive gas, leaving reaction products of surface material in the coating, e.g. conversion coatings, passivation of metals using gases
    • C23C8/08Solid state diffusion of only non-metal elements into metallic material surfaces; Chemical surface treatment of metallic material by reaction of the surface with a reactive gas, leaving reaction products of surface material in the coating, e.g. conversion coatings, passivation of metals using gases only one element being applied
    • C23C8/10Oxidising
    • C23C8/12Oxidising using elemental oxygen or ozone
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25DPROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D11/00Electrolytic coating by surface reaction, i.e. forming conversion layers

Abstract

The invention discloses a method for strengthening fine grains of a silver-magnesium-nickel alloy, and belongs to the technical field of electric contact materials. The method comprises the steps of putting raw materials into a vacuum induction furnace according to a ratio, smelting to obtain a silver-magnesium-nickel alloy billet, and cold-rolling the billet into a sheet. Taking a silver-magnesium-nickel alloy sheet as a cathode, taking a metal platinum sheet as an anode, taking a hydrogenated electrolyte as an acid system, adding a hydrogenation inhibitor into the solution, after carrying out direct-current electrolytic hydrogenation for a period of time, taking the silver-magnesium-nickel alloy sheet out, cleaning, drying, taking out, finishing rolling, correcting shape, placing in an atmosphere sintering furnace, firstly preserving the temperature at a low temperature in vacuum for a period of time, then introducing oxygen to raise the temperature, carrying out thermal internal oxidation at a high temperature, and cooling along with the furnace. The material prepared by the method has the advantages of high strength, high hardness, good plasticity, good elasticity, excellent conductivity and good arc resistance.

Description

Fine crystal strengthening method for silver-magnesium-nickel alloy
Technical Field
The invention relates to a method for strengthening fine grains of a silver-magnesium-nickel alloy, belonging to the technical field of electric contact materials.
Background
The silver-magnesium-nickel alloy is characterized by that it uses silver as base body, contains small quantity of magnesium and nickel, and after internal oxidation said alloy possesses excellent elasticity and mechanical fatigue resistance, good electric conductivity and thermal conductivity and unchangeable elasticity at high temperature, and possesses excellent electroerosion-resisting property and reliable electric contact property, and has small creep speed, and its creep speed is only one tenth of that of pure silver, and its hardness is not affected by temperature. The material is commonly used as an elastic electric contact material and widely applied to the fields of high technologies such as aviation, aerospace, navigation and the like, national defense and spring contact elements of various alternating current and direct current contactors, circuit breakers, relays and micro relays in transfer switches in the civil industry; in particular to a shunt contact element in a large switch which bears stress, a spring of a meter and a relay which work at high temperature, and the like.
Magnesium in the silver-magnesium-nickel alloy is dissolved in a silver matrix to form a substitutional solid solution, and a part of the substitutional solid solution forms second-phase Mg54Ag17Dispersed in a silver matrix, presents a coherent or semi-coherent relationship, and magnesium is easy to be deviated and gathered at the position of the solid solution screw dislocation,because the radius of magnesium atoms is larger than that of silver atoms, the crystal lattice distortion can be generated after magnesium is dissolved into a silver matrix. The element nickel can not be dissolved in the silver matrix in a solid solution mode, is dispersed in the silver-magnesium solid solution in a particle mode to serve as a second phase, and has limited effects of grain refinement and dispersion strengthening on the silver matrix due to low strength of the element nickel. MgNi formed by partial nickel and magnesium2The silver, magnesium and nickel alloy is partially aggregated in a grain boundary, the resistance of the expansion of the grain boundary is increased, and although grains can be refined, larger internal stress at the grain boundary is also caused, which is an important factor influencing the plasticity and the conductivity of the silver, magnesium and nickel alloy.
In recent years, silver-magnesium-nickel alloy materials are widely concerned at home and abroad, and the influence of a heat treatment process, internal oxidation on the structure performance of the alloy and the influence of modified elements on the structure performance of the alloy are deeply researched. However, the existing processing technology is difficult to solve the problems of higher internal oxidation temperature, larger oxide particles and larger grain size, which causes the increase of the internal stress of the silver-magnesium-nickel alloy, the reduction of plasticity, the increase of brittleness and the obvious reduction of conductivity. Although the addition of the rare earth elements can refine grains, the difficulty of the preparation process is increased, and the manufacturing cost of the silver-magnesium-nickel alloy material is increased.
Disclosure of Invention
The invention aims to provide a silver-magnesium-nickel alloy fine crystal strengthening method, which specifically comprises the following steps:
(1) putting the raw materials into a vacuum induction furnace according to the proportion, smelting to obtain a silver-magnesium-nickel alloy billet, and cold-rolling the ingot into a sheet with the thickness of 0.1-2 mm;
(2) putting the slices obtained in the step (1) into an ethanol and acetone solution for ultrasonic cleaning, taking out, washing with pure water, and airing for later use;
(3) taking a metal platinum sheet as an anode, a silver-magnesium-nickel alloy sheet as a cathode, a hydrogenated electrolyte as an acid system, adding a hydrogenation inhibitor into the solution, and carrying out direct-current electrolytic hydrogenation;
(4) and (4) cleaning and drying the silver-magnesium-nickel alloy sheet obtained in the step (3), then performing finish rolling and shape correction, placing the silver-magnesium-nickel alloy sheet in an atmosphere sintering furnace, performing vacuum low-temperature calcination, then introducing oxygen, heating, performing thermal internal oxidation at high temperature, and cooling along with the furnace to obtain the silver-magnesium-nickel alloy.
Preferably, the hydrogenated electrolyte in step (3) of the present invention is HCl or H2SO4、HNO3Or CH3COOH in a concentration of 0.5 to 3 mol/L.
Preferably, the hydrogenation inhibitor in step (3) of the present invention is As2O3、Al2O3、Na2HAsO4、SnCl4Or PdCl2The addition amount is 0.01-1 g/L.
Preferably, the conditions of the direct current electrolytic hydrogenation in the step (3) of the present invention are as follows: charging Ag-Mg-Ni alloy sheet into electrolytic bath at 0.3-4V and current density of 0.05-0.3A.cm2The electrolysis time is 1-48 hours.
Preferably, the deformation amount of the finish rolling shape correction of the present invention is 1 to 5%.
Preferably, the conditions of the vacuum low-temperature calcination of the invention are as follows: the vacuum degree is 0.001-0.008Pa, the temperature is raised to 300-500 ℃ at 1-5 ℃/min, and the temperature is kept for 1-4 hours.
Preferably, the conditions of the thermal internal oxidation at high temperature of the invention are as follows: introducing oxygen with the purity of more than 99 percent, wherein the flow rate is 0.1-1 liter/second, the vacuum degree is 10-50Pa, the temperature is raised to 650 plus materials at 5-10 ℃/min, and the temperature is kept for 10-40 hours.
The principle of the invention is as follows:
in the electrolytic hydrogenation stage of the silver-magnesium-nickel alloy, the generated atomic hydrogen is enriched on the surface of the silver-magnesium-nickel alloy, the hydrogen atomic radius is small, the diffusion capacity is strong, the atomic hydrogen enters the alloy along the grain boundary of the silver-magnesium-nickel alloy and reacts with magnesium element in a hydrogenation mode to generate MgH2:
MgH2The alloy is an ionic hydride and has a rutile-like structure, the hardness is high, large lattice distortion can be caused after the alloy is formed in a silver-magnesium-nickel solid solution, and large grains in the original silver-magnesium-nickel alloy are cracked into small grains under the action of internal and external stress in the subsequent finish rolling orthopedic process.
Under vacuum heating condition, MgH2The decomposition releases hydrogen atoms which escape through the grain boundaries. Then under the subsequent heating and pressurizing pure oxygen atmosphere, MgH2Part of the decomposed magnesium atoms enter into a silver-magnesium-nickel solid solution in a solid solution mode, and part of the decomposed magnesium atoms react as follows:
the generated magnesium oxide nano particles are used as strengthening second phase particles to be dispersed in the silver-magnesium-nickel alloy.
The invention has the beneficial effects that:
(1) in the electrolytic hydrogenation stage, the hydrogen atom has strong diffusion capacity, and is easy to be in solid solution screw dislocation with magnesium atoms in the silver-magnesium-nickel alloy and a second phase MgNi at the grain boundary2And a second phase Mg dispersed in the silver matrix54Ag17Hydrogenation reaction is carried out to generate MgH2At the same time, the hydrogenation reaction can also occur with the displaced magnesium atoms at each bit of the silver unit cell due to MgH2The generation further increases the lattice distortion in the solid solution, the internal stress is increased, and the distribution in the silver matrix is more uniform.
(2) In subsequent finish rolling and shaping, large grains are crushed under the action of internal and external stress and are cracked into small grains. In the vacuum heating process, MgH2Decomposing to release hydrogen atoms, dissolving magnesium atoms partially into silver matrix, leaving a part as simple substance in situ, but not forming a second phase Mg54Ag17And a second phase of MgNi2In the subsequent internal oxidation process, MgH2The magnesium atoms left after decomposition have larger chemical activity, can react with oxygen rapidly to generate magnesium oxide fine particles with the particle size of 1-10nm, have good interface compatibility with a silver matrix, and well hinder the growth of small crystal grains. Meanwhile, partial nickel which is partially gathered at the grain boundary can also react with oxygen to generate fine nickel oxide particles, so that the movement of the grain boundary is hindered, and the grains are further refined.
In conclusion, the silver-magnesium-nickel alloy prepared by the method has fine crystal grains, the second-phase magnesium oxide particles are uniformly dispersed in a nanoscale range, and the alloy material has the advantages of high strength, high hardness, good plasticity, good elasticity, excellent conductivity and good arc resistance.
Detailed Description
The present invention will be described in further detail with reference to specific examples, but the scope of the present invention is not limited to the examples.
Example 1
A silver-magnesium-nickel alloy fine crystal strengthening method specifically comprises the following steps:
(1) putting the raw materials into a vacuum induction furnace according to the proportion to be smelted to obtain AgMg0.24Ni0.29The alloy ingot is cold-rolled into a sheet, and the thickness of the sheet is 0.1 mm.
(2) AgMg obtained in the step (1)0.24Ni0.29And (3) putting the slices into an ethanol solution, ultrasonically cleaning for 1 minute, taking out, washing with pure water, and airing for later use.
(3) Using a platinum sheet as an anode, AgMg0.24Ni0.29Using the slice As cathode, adding hydrogenation inhibitor into the solution to perform direct current electrolytic hydrogenation, adding 0.01 g/L hydrogenation inhibitor As into 0.5 mol/L mol/HCl solution2O3Stirring for 10 minutes, taking a metal platinum sheet as an anode, and AgMg0.24Ni0.29The sheet is used as cathode to be charged into a slot, the voltage of the slot is 0.3V, and the current density is 0.05A.cm2The electrolysis time was 48 hours.
(4) Hydrogenation AgMg0.24Ni0.29Taking out the slice from the electrolytic tank, washing with pure water until the washing liquid is neutral, drying, finish rolling and reshaping by 5% deformation on a four-roller mill, placing in an atmosphere sintering furnace, vacuumizing until the vacuum degree is 0.001Pa, heating to 300 ℃ at the speed of 5 ℃/min, and keeping the temperature for 1 hour. Then introducing oxygen with the purity of 99.9 percent, the flow rate is 0.1 liter/second, the vacuum degree is 10Pa, heating to 650 ℃ at the speed of 5 ℃/minute, preserving the temperature for 10 hours, stopping introducing the oxygen, stopping heating, cooling to the room temperature along with the furnace, and then adding AgMg0.24Ni0.29And taking out the thin sheet.
AgMg prepared in this example0.24Ni0.29The average grain size was 5.7 μm, the average grain size of the dispersed magnesium oxide particles was 8nm, and the hardness was 188kgf/mm2The tensile strength was 512MPa, the elongation was 14%, and the resistivity was 2.43. mu. omega. cm.
Example 2
A silver-magnesium-nickel alloy fine crystal strengthening method specifically comprises the following steps:
(1) putting the raw materials into a vacuum induction furnace according to the proportion to be smelted to obtain AgMg0.17Ni0.15The alloy ingot was cold-rolled into a sheet having a thickness of 2 mm.
(2) AgMg obtained in the step (1)0.17Ni0.15And (3) putting the slices into a pure acetone solution, ultrasonically cleaning for 5 minutes, taking out, washing with pure water, and airing for later use.
(3) Taking a metal platinum sheet as an anode, a silver-magnesium-nickel alloy sheet as a cathode, a hydrogenated electrolyte as an acid system, adding a hydrogenation inhibitor into the solution, and carrying out direct-current electrolytic hydrogenation, wherein the electrolyte is HNO with the concentration of 3 mol/L31 g/L hydrogenation inhibitor Na is added2HAsO4Stirring for 10 minutes, taking a metal platinum sheet as an anode, and AgMg0.17Ni0.15The slice is taken as a cathode to be charged into a slot, the voltage of the slot is 4V, and the current density is 3A.cm2The electrolysis time was 24 hours.
(4) Hydrogenation AgMg0.17Ni0.15Taking out the charged sheet from the electrolytic bath, washing with pure water until the washing liquid is neutral, drying, finish-rolling and reshaping by 1% deformation on a four-roller mill, placing in an atmosphere sintering furnace, vacuumizing to 0.008Pa, heating to 500 ℃ at 1 ℃/min, and keeping the temperature for 4 hours. Introducing oxygen with the purity of 99.9 percent at the flow rate of 1 liter/second until the vacuum degree is 50Pa, stopping vacuumizing, heating to 800 ℃ at the speed of 10 ℃/min, preserving the temperature for 40 hours, stopping introducing the oxygen, stopping heating, cooling to room temperature along with the furnace, and then adding AgMg0.17Ni0.15And taking out the thin sheet.
AgMg prepared in this example0.17Ni0.15The average grain size was 8.2 μm, the average grain size of the dispersed magnesium oxide particles was 9nm, and the hardness was 162kgf/mm2The tensile strength was 483MPa, the elongation was 21% and the resistivity was 2.21. mu.Ω.cm。
Example 3
A silver-magnesium-nickel alloy fine crystal strengthening method specifically comprises the following steps:
(1) putting the raw materials into a vacuum induction furnace according to the proportion to be smelted to obtain AgMg0.21Ni0.19The alloy ingot was cold-rolled into a sheet having a thickness of 0.5 mm.
(2) And (2) placing the slices obtained in the step (1) into an ethanol solution for ultrasonic cleaning for 3 minutes, taking out, washing with pure water, and airing for later use.
(3) Taking a metal platinum sheet as an anode, a silver-magnesium-nickel alloy sheet as a cathode, a hydrogenated electrolyte as an acid system, adding a hydrogenation inhibitor into the solution, and carrying out direct-current electrolytic hydrogenation, wherein the electrolyte is 2 mol/L CH3COOH, 0.2 g/L hydrogenation inhibitor Al2O3Stirring for 10 minutes, taking a metal platinum sheet as an anode, and AgMg0.21Ni0.19The slice is taken as a cathode to be charged into a slot, the voltage of the slot is 2,3V, and the current density is 0.2A.cm2The electrolysis time was 36 hours.
(4) Hydrogenation AgMg0.21Ni0.19Taking out the charged sheet from the electrolytic bath, washing with pure water until the washing solution is neutral, drying, performing finish rolling on the sheet on a four-roller mill by 5% of deformation for shape correction, placing the sheet in an atmosphere sintering furnace, vacuumizing to 0.008Pa of vacuum degree, heating to 480 ℃ at the speed of 5 ℃/min, and preserving heat for 2 hours; then introducing oxygen with the purity of 99.9 percent, the flow rate is 0.8 liter/second, the vacuum degree is 30Pa, heating to 700 ℃ at the speed of 5 ℃/minute, preserving the temperature for 10 hours, stopping introducing the oxygen, stopping heating, cooling to the room temperature along with the furnace, and then adding AgMg0.21Ni0.19And taking out the thin sheet.
AgMg prepared in this example0.21Ni0.19The average grain size was 4.2 μm, the average grain size of the dispersed magnesium oxide particles was 4nm, and the hardness was 172kgf/mm2The tensile strength was 498MPa, the elongation 13%, and the resistivity 2.57. mu. omega. cm.
Example 4
A silver-magnesium-nickel alloy fine crystal strengthening method specifically comprises the following steps:
(1) will be originalThe materials are put into a vacuum induction furnace according to the proportion to be smelted to obtain AgMg0.21Ni0.19The alloy ingot was cold-rolled into a sheet having a thickness of 1 mm.
(2) And (2) placing the slices obtained in the step (1) into an ethanol solution for ultrasonic cleaning for 3 minutes, taking out, washing with pure water, and airing for later use.
(3) Taking a metal platinum sheet as an anode, a silver-magnesium-nickel alloy sheet as a cathode, a hydrogenated electrolyte as an acid system, adding a hydrogenation inhibitor into the solution, and carrying out direct-current electrolytic hydrogenation, wherein the electrolyte is H with the concentration of 1 mol/L2SO4Adding 0.1 g/L hydrogenation inhibitor SnCl4Stirring for 10 minutes, taking a metal platinum sheet as an anode, and AgMg0.21Ni0.19The slice is taken as a cathode to be charged into a slot, the voltage of the slot is 1.2V, and the current density is 0.15A.cm2The electrolysis time was 36 hours.
(4) Hydrogenation AgMg0.21Ni0.19Taking out the charged sheet from the electrolytic bath, washing with pure water until the washing solution is neutral, drying, performing finish rolling on the sheet on a four-roller mill by 3% of deformation amount to shape, placing the sheet in an atmosphere sintering furnace, vacuumizing to the vacuum degree of 0.005Pa, heating to 450 ℃ at the speed of 2 ℃/min, and preserving heat for 2 hours; introducing oxygen with the purity of 99.9 percent at the flow rate of 0.5 liter/second until the vacuum degree is 20Pa, stopping vacuumizing, heating to 750 ℃ at the temperature of 5 ℃/min, preserving the temperature for 30 hours, stopping introducing the oxygen, stopping heating, cooling to room temperature along with the furnace, and then adding AgMg0.21Ni0.19And taking out the thin sheet.
AgMg prepared in this example0.21Ni0.19The average grain size was 6.3 μm, the average grain size of the dispersed magnesium oxide particles was 6nm, and the hardness was 177kgf/mm2The tensile strength was 502MPa, the elongation was 13%, and the resistivity was 2.33. mu. omega. cm.

Claims (4)

1. The fine crystal strengthening method of the silver-magnesium-nickel alloy is characterized by comprising the following steps:
(1) putting the raw materials into a vacuum induction furnace according to the proportion, smelting to obtain a silver-magnesium-nickel alloy billet, and cold-rolling the ingot into a sheet with the thickness of 0.1-2 mm;
(2) putting the slices obtained in the step (1) into an ethanol or acetone solution for ultrasonic cleaning, taking out, washing with pure water, and airing for later use;
(3) taking a metal platinum sheet as an anode, a silver-magnesium-nickel alloy sheet as a cathode, a hydrogenated electrolyte as an acid system, adding a hydrogenation inhibitor into the solution, and carrying out direct-current electrolytic hydrogenation;
(4) cleaning and drying the silver-magnesium-nickel alloy sheet obtained in the step (3), then performing finish rolling and shape correction, placing the silver-magnesium-nickel alloy sheet in an atmosphere sintering furnace, performing vacuum low-temperature calcination, introducing oxygen, heating, performing thermal internal oxidation at high temperature, and cooling along with the furnace to obtain silver-magnesium-nickel alloy;
the conditions of the direct current electrolytic hydrogenation in the step (3) are as follows: charging Ag-Mg-Ni alloy sheet into electrolytic bath at 0.3-4V and current density of 0.05-0.3A.cm2The electrolysis time is 1-48 hours;
the conditions of the vacuum low-temperature calcination are as follows: the vacuum degree is 0.001-0.008Pa, the temperature is raised to 300-500 ℃ at the speed of 1-5 ℃/min, and the temperature is kept for 1-4 hours;
the conditions of thermal internal oxidation at high temperature are as follows: introducing oxygen with the purity of more than 99 percent, wherein the flow rate is 0.1-1 liter/second, the vacuum degree is 10-50Pa, heating to 650 plus materials 800 ℃ at the speed of 5-10 ℃/min, and preserving the heat for 10-40 hours.
2. The fine crystal strengthening method of silver-magnesium-nickel alloy according to claim 1, characterized in that: the hydrogenated electrolyte in the step (3) is HCl and H2SO4、HNO3Or CH3COOH in a concentration of 0.5 to 3 mol/L.
3. The fine crystal strengthening method of silver-magnesium-nickel alloy according to claim 1, characterized in that: the hydrogenation inhibitor in the step (3) is As2O3、Al2O3、Na2HAsO4、SnCl4Or PdCl2The addition amount is 0.01-1 g/L.
4. The fine crystal strengthening method of silver-magnesium-nickel alloy according to claim 1, characterized in that: the deformation amount of finish rolling and shape correction is 1-5%.
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CN101914697B (en) * 2010-07-29 2011-11-16 贵研铂业股份有限公司 Method for preparing silver-magnesium-nickel alloy billets
CN101982557B (en) * 2010-09-29 2013-01-30 北京航空航天大学 Method for increasing room-temperature magnetic entropy change of amorphous soft magnetic alloy
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FR2349941A2 (en) * 1976-04-26 1977-11-25 Anvar Electrical contact elements for systems subject to friction - have oxide particles embodied in surface layer deposited electrolytically

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