CN111924899A - Method for preparing nickel-cobalt-iron-aluminum-magnesium five-element high-entropy material, product and application - Google Patents
Method for preparing nickel-cobalt-iron-aluminum-magnesium five-element high-entropy material, product and application Download PDFInfo
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Abstract
The invention discloses a method for preparing a nickel-cobalt-iron-aluminum-magnesium five-element high-entropy material, a product and application, wherein the method comprises the following steps: (1) sequentially adding soluble nickel salt, soluble cobalt salt and soluble magnesium salt into a container a, and adding water to dissolve the soluble nickel salt, the soluble cobalt salt and the soluble magnesium salt into a transparent solution; (2) sequentially adding soluble aluminum salt and soluble ferric salt into the container b, adding water to dissolve the soluble aluminum salt and the soluble ferric salt into a transparent solution, adding a certain amount of composite complexing agent, fully stirring, and standing; (3) adding four materials of the container a, the container b, ammonia water and alkali liquor into a reaction container in a parallel flow manner, stirring, controlling the reaction pH, generating slurry at a certain reaction temperature, filtering, washing, drying and crushing to obtain powder C; (4) and (3) obtaining the high-entropy material from the powder C at a certain roasting temperature. After the high-entropy material is added with lithium, the battery has good cycling stability, greatly improved safety and higher discharge capacity.
Description
Technical Field
The invention belongs to the field of high-entropy battery materials, and particularly relates to a method for preparing a nickel-cobalt-iron-aluminum-magnesium quinary high-entropy material, a product and application.
Background
The high-entropy material is a novel multi-principal-element material consisting of multiple elements in an equimolar ratio or a nearly equimolar ratio, and breaks through the traditional material design concept. High entropy materials exhibit many structural and performance characteristics that are different from conventional materials due to their unique crystal structure characteristics.
In 2019, the nanometer technical expert, the hoster-Hahn (Horst Hahn) team of karsleu technical institute (KIT), germany, found: high Entropy Oxide (HEO) materials can significantly improve the storage capacity and cycling stability of batteries. The material has high stability due to the disordered distribution of atoms. The special property of HEO is a result of entropy stabilization, which is a composite oxide containing 5 or more different metal ions in different amounts and having a single-phase crystal structure. Although the typical crystal structures of these elements are very different, they form a kind of united lattice and there is no obvious order in the positions in the crystal. This disorder, also called high entropy, is probably because it hinders the migration of defects in the crystal lattice and therefore enables a high stability of the material to be maintained.
The existing method for preparing the high-entropy oxide is generally a solid-phase sintering method, the application of a chemical precipitation method is few, and the high-entropy powder prepared by the chemical precipitation method is fine in particle size, uniform in particle size distribution, good in activity and uniform in distribution of elements compared with a solid-phase method.
The prior chemical precipitation method for preparing the high-entropy oxide has some defects. For example, application publication No. CN110845237A La (NO)3)3、Co(NO3)2、Cr(NO3)3、Fe(NO3)3、Mn(NO3)2And Ni (NO)3)2The mixed solution is mixed with ammonia water for coprecipitation reaction, high-entropy ceramic precursor powder is obtained after solid-liquid separation, the pH value of the coprecipitation reaction is 9-10, and obviously the pH value of iron ion precipitation is much different from that of other cation precipitation, so that the coprecipitation effect is difficult to achieve; NiSO for application publication No. CN111302781A4·6H2O，CoSO4·7H2O，TiOSO4Solution of MnSO4·H2O，FeSO4Citric acid or oxalic acid is used as a raw material as a complexing agent to prepare the high-entropy oxide, but five salt solutions are added together (an alkaline solution, the complexing agent and a Fe-Ti-Ni-Co-Mn transparent solution are added into a reactor to be stirred and mixed for reaction, the pH value of the solution is controlled, and a five-membered coprecipitate is generated), and the citric acid or oxalic acid has no selectivity on the complexation of nickel, cobalt, titanium, manganese and iron elements, so that the iron and titanium precipitation speed is high, and the coprecipitation effect is difficult to achieve. The document "Nanocrystalline multicomponent elementary transfer metal oxides" is to continuously add ammonia water dropwise to a mixed nitrate solution to maintain the solution pH at about 10, to cause the solution to precipitate, then to dry at 120 ℃ for 4 hours, and to calcine at 1000 ℃ for 1 hour to obtain a high-entropy oxide (Co)0.2Cu0.2Mg0.2Ni0.2Zn0.2) O ceramic powder. The pH value of the precipitation reaction in the elements of the high-entropy oxide is relatively close, but the precipitation reaction is not suitable for the coprecipitation containing Fe element.
In addition, the high-entropy oxide can be obtained in a gel manner. For example, CN110600703A uses equimolar metal nitrate, then adds glycine, ethylene diamine tetraacetic acid, hexamethylene tetramine, hexamethylene diisocyanate, citric acid or oxalic acid, and keeps the temperature at high temperature to obtain the pentabasic spinel type oxide high-entropy material with the chemical formula of (Cr)0.2Fe0.2Mn0.2Zn0.2M0.2)3O4Wherein M is a divalent metal cation Co2+Or Ni2+. The publication No. CN110818430A A uniform high-entropy oxide ceramic nano-powder and its preparation method, the CoCl with equal molar ratio2、CuCl2、MgCl2、NiCl2And ZnCl2Blending in absolute ethyl alcohol until the mixture is completely dissolved to obtain a mixed solution, adding urea into the mixed solution, fully mixing to enable the metal chloride and the urea to generate a crosslinking reaction to form gel, and performing high-temperature pyrolysis treatment on the dried gel to obtain uniform high-entropy oxide (Co, Cu, Mg, Ni, Zn) O ceramic submicron spherical powder. It can be easily found that the performance of the high-entropy oxides disclosed in these patents is still to be improved when applied to lithium ion batteries.
Disclosure of Invention
1. Problems to be solved
Aiming at the problems, the invention provides a method for preparing a nickel-cobalt-iron-aluminum-magnesium five-element high-entropy material, which improves Ni0.2Co0.2Fe0.2Al0.2Mg0.2The performance of the O high-entropy material meets the use requirement.
The invention also provides Ni obtained by the method0.2Co0.2Fe0.2Al0.2Mg0.2O high entropy material.
The invention also provides an application of the high-entropy material in a lithium ion battery.
2. Technical scheme
In order to solve the problems, the technical scheme adopted by the invention is as follows:
the method for preparing the nickel-cobalt-iron-aluminum-magnesium quinary high-entropy material comprises the following steps of:
(1) sequentially adding a battery-grade soluble nickel salt, a soluble cobalt salt and a soluble magnesium salt into a container a, and adding water to dissolve the materials into a transparent solution;
(2) sequentially adding battery-grade soluble aluminum salt and soluble ferric salt into the container b, adding water to dissolve the materials into a transparent solution, adding a certain amount of composite complexing agent, fully stirring and standing;
(3) adding four materials of the container a, the container b, ammonia water and alkali liquor into a reaction container in a parallel flow manner, stirring to control the reaction pH, generating slurry at a certain reaction temperature, filtering, washing, drying and crushing to obtain powder C;
(4) the powder C is roasted at a certain temperature to obtain Ni0.2Co0.2Fe0.2Al0.2Mg0.2O high entropy material.
In one possible embodiment of the present invention, the soluble nickel salt in step (1) is nickel sulfate or nickel nitrate, the soluble cobalt salt is cobalt sulfate or cobalt nitrate, and the soluble magnesium salt is magnesium sulfate or magnesium nitrate; the concentration of the soluble nickel salt, the soluble cobalt salt and the soluble magnesium salt is 0.4-6 mol/L, preferably 2-4 mol/L.
In one possible embodiment of the present invention, the molar ratio of the soluble nickel salt, the soluble cobalt salt, the soluble magnesium salt, the soluble aluminum salt and the soluble iron salt in step (1) and step (2) is 1: 1: 1: 1: 1.
in one possible embodiment of the invention, the concentration of the aluminum salt and the iron salt in the step (2) is 0.4-6 mol/L, preferably 2-4 mol/L; the soluble aluminum salt and the soluble ferric salt are sodium metaaluminate, aluminum sulfate and ferric sulfate or aluminum nitrate and ferric nitrate;
the composite complexing agent is obtained by dissolving citric acid, ethylene diamine tetraacetic acid and ethylene glycol in pure water, wherein the molar ratio of the citric acid to the ethylene diamine tetraacetic acid to the ethylene glycol is 0.75-0.85: 0.1-0.2: 0.02 to 0.08;
the concentration of citric acid in the composite complexing agent is 0.3-5 mol/L, preferably 0.5-2 mol/L;
the molar weight of the composite complexing agent is 0.5-1.5 times, preferably 0.5-1 time of the sum of the molar weights of the soluble aluminum salt and the soluble ferric salt.
In one possible embodiment of the invention, the adding amount of the ammonia water in the step (3) is 3-10 times of the molar amount of the composite complexing agent, and the concentration is 1.0-10.0 mol/L;
the adding speed of the ammonia water is that the amount of the added ammonia water in unit time is 1-5 times, preferably 2-3 times of the molar weight of the composite complexing agent;
the molar concentrations of the soluble nickel salt, the soluble cobalt salt, the soluble magnesium salt, the soluble aluminum salt and the soluble iron salt which are added into the reactor in unit time are the same when the container a and the container b are added into the reactor;
the alkali liquor is at least one of liquid alkali, sodium carbonate and sodium bicarbonate, and the molar concentration is 1.5-10.0 mol/L, preferably 4-8 mol/L; the rate of addition of the lye is determined by the pH of the system.
The pH is 10.0-11.5, preferably 10.5-11.0; the reaction temperature is 40-95 ℃, preferably 50-75 ℃.
In one possible embodiment of the invention, the roasting temperature in the step (4) is 600-1200 ℃, preferably 700-1000 ℃;
in one possible embodiment of the present invention, the Ni in the step (4)0.2Co0.2Fe0.2Al0.2Mg0.2Ni in O: co: fe: al: mg molar ratio of 1 +/-0.1: 1 ± 0.1: 1 ± 0.1: 1 ± 0.1: 1 + -0.1.
3. Advantageous effects
Compared with the prior art, the invention has the beneficial effects that:
(1) the method adopts a chemical precipitation method and a composite complexing agent to prepare the high-entropy oxide battery material, dissolves nickel salt, cobalt salt and magnesium salt with high and similar precipitation pH value together, dissolves ferric salt and aluminum salt with low precipitation pH value together and adds the composite complexing agent for complexing, and five-element coprecipitation of the nickel salt, the cobalt salt, the magnesium salt, the ferric salt and the aluminum salt can be realized by controlling the proportion of citric acid, ethylene diamine tetraacetic acid and ethylene glycol in the composite complexing agent and the adding speed of ammonia water, so that the obtained high-entropy material has small granularity, high activity and uniform granularity distribution, as can be seen in figures 1 to 3, the high-entropy oxide battery material prepared by reaction examples 1 to 3 has small granularity and uniform size;
(2) the high-entropy oxide battery material Ni0.2Co0.2Fe0.2Al0.2Mg0.2After the O lithium is added, the battery has good cycling stability, greatly improved safety and higher discharge gram capacity; the technical scheme uses most metal elements with low price, and is convenient for industrial production.
Drawings
The invention is further described below with reference to the accompanying drawings.
FIG. 1 is an SEM image of a quinary high-entropy oxide cell material in example 1 of the present invention;
FIG. 2 is an SEM image of a quinary high-entropy oxide cell material in example 2 of the invention;
FIG. 3 is an SEM image of a quinary high-entropy oxide cell material in example 3 of the invention.
Detailed Description
Exemplary embodiments of the present invention are described in detail below. Although these exemplary embodiments are described in sufficient detail to enable those skilled in the art to practice the invention, it should be understood that other embodiments may be realized and that various changes to the invention may be made without departing from the spirit and scope of the present invention. The following more detailed description of the embodiments of the invention is not intended to limit the scope of the invention, as claimed, but is presented for purposes of illustration only and not limitation to describe the features and characteristics of the invention, to set forth the best mode of carrying out the invention, and to sufficiently enable one skilled in the art to practice the invention. Accordingly, the scope of the invention is to be limited only by the following claims.
The experimental procedures used in the following examples are conventional unless otherwise specified.
Materials, reagents and the like used in the following examples are commercially available unless otherwise specified.
The method for preparing the nickel-cobalt-iron-aluminum-magnesium quinary high-entropy material comprises the following steps of:
(1) sequentially adding a battery-grade soluble nickel salt, a soluble cobalt salt and a soluble magnesium salt into a container a, wherein the container a can be selected from test equipment such as a beaker, and adding water to dissolve the materials into a transparent solution;
the soluble nickel salt is nickel sulfate or nickel nitrate, the soluble cobalt salt is cobalt sulfate or cobalt nitrate, and the soluble magnesium salt is magnesium sulfate or magnesium nitrate; the concentration of the soluble nickel salt, the soluble cobalt salt and the soluble magnesium salt is 0.4-6 mol/L, preferably 2-4 mol/L.
(2) Sequentially adding battery-grade soluble aluminum salt and soluble ferric salt into a container b, wherein the container b can be selected from test equipment such as a beaker and the like, adding water to dissolve the materials into a transparent solution, adding a certain amount of composite complexing agent, fully stirring and standing;
the concentration of the aluminum salt and the ferric salt is 0.4-6 mol/L, preferably 2-4 mol/L; the soluble aluminum salt and the soluble ferric salt are sodium metaaluminate, aluminum sulfate and ferric sulfate or aluminum nitrate and ferric nitrate; the composite complexing agent is obtained by dissolving citric acid, ethylene diamine tetraacetic acid and ethylene glycol in pure water, wherein the molar ratio of the citric acid to the ethylene diamine tetraacetic acid to the ethylene glycol is 0.75-0.85: 0.1-0.2: 0.02 to 0.08; the concentration of citric acid in the composite complexing agent is 0.3-5 mol/L, preferably 0.5-2 mol/L; the molar weight of the composite complexing agent is 0.5-1.5 times, preferably 0.5-1 time of the sum of the molar weights of the soluble aluminum salt and the soluble ferric salt.
The mol ratio of the soluble nickel salt to the soluble cobalt salt to the soluble magnesium salt to the soluble aluminum salt to the soluble iron salt is 1: 1: 1: 1: 1.
(3) adding four materials of the container a, the container b, ammonia water and alkali liquor into a reaction container in a parallel flow manner, wherein the reaction container can select sample equipment such as a reaction kettle and the like, stirring to control the reaction pH, generating slurry at a certain reaction temperature, filtering, washing, drying and crushing to obtain powder C;
the adding amount of the ammonia water is 3-10 times of the molar amount of the composite complexing agent, and the concentration of the ammonia water is 1.0-10.0 mol/L; the adding speed of the ammonia water is that the amount of the added ammonia water in unit time is 1-5 times, preferably 2-3 times of the molar weight of the composite complexing agent; the molar concentrations of the soluble nickel salt, the soluble cobalt salt, the soluble magnesium salt, the soluble aluminum salt and the soluble iron salt which are added into the reactor in unit time are the same when the container a and the container b are added into the reactor; the alkali liquor is at least one of liquid alkali, sodium carbonate and sodium bicarbonate, and the molar concentration is 1.5-10.0 mol/L, preferably 4-8 mol/L; the rate of addition of the lye is determined by the pH of the system. The pH is 10.0-11.5, preferably 10.5-11.0; the reaction temperature is 40-95 ℃, preferably 50-75 ℃.
(4) The powder C is roasted at a certain temperature to obtain Ni0.2Co0.2Fe0.2Al0.2Mg0.2O high entropy materialAnd (5) feeding. The roasting temperature is 600-1200 ℃, and preferably 700-1000 ℃; the Ni0.2Co0.2Fe0.2Al0.2Mg0.2Ni in O: co: fe: al: mg molar ratio of 1 +/-0.1: 1 ± 0.1: 1 ± 0.1: 1 ± 0.1: 1 + -0.1.
Example 1
(1) Weighing a certain amount of battery-grade nickel sulfate, cobalt sulfate and magnesium sulfate, adding into a beaker a, and dissolving in pure water, wherein the molar concentrations of nickel, cobalt and magnesium are all 6mol/L, and the total volume is 500 mL;
(2) weighing a certain amount of battery-grade aluminum sulfate and ferric sulfate, adding the battery-grade aluminum sulfate and ferric sulfate into a beaker b, dissolving the beaker b in pure water, adding 4.8mol of citric acid, 0.9mol of ethylene diamine tetraacetic acid and 0.3mol of ethylene glycol, stirring and dissolving, wherein the molar concentrations of aluminum and iron are both 3mol/L, and the total volume is 1000 mL;
(3) adding 2L and 8L sodium hydroxide solution of beaker a, beaker b and 9mol/L ammonia water into a reaction kettle (with heating and stirring) in a concurrent flow manner, wherein the adding speeds of beaker a, beaker b and ammonia water are respectively 5ml/min, 10ml/min and 20 ml/min; the reaction temperature is 40 ℃, the reaction pH is controlled at 10, and after the reaction is finished, the powder C is obtained by filtering, washing, drying and crushing at 100 ℃;
(4) the powder C is roasted at 1200 ℃ in a rotary kiln to obtain Ni0.2Co0.2Fe0.2Al0.2Mg0.2O high entropy material.
The high-entropy material has small particle size and uniform particle size distribution (as shown in figure 1).
Example 2
(1) Weighing a certain amount of battery-grade nickel nitrate, cobalt nitrate and magnesium nitrate, adding the nickel nitrate, the cobalt nitrate and the magnesium nitrate into a beaker a, dissolving the mixture in pure water, wherein the molar concentrations of the nickel, the cobalt and the magnesium are all 3mol/L, and the total volume is 1000 mL;
(2) weighing a certain amount of battery-grade aluminum nitrate and ferric nitrate, adding the battery-grade aluminum nitrate and ferric nitrate into a beaker b, dissolving the beaker b in pure water, adding 2.25mol of citric acid, 0.6mol of ethylene diamine tetraacetic acid and 0.15mol of ethylene glycol, stirring and dissolving, wherein the molar concentrations of aluminum and iron are both 3mol/L, and the total volume is 1000 mL;
(3) adding 2L of 6mol/L sodium hydroxide solution into a reaction kettle in parallel in a beaker a, a beaker b and 6mol/L ammonia water, wherein the adding speeds of the beaker a, the beaker b and the ammonia water are respectively 10ml/min, 10ml/min and 20 ml/min; the reaction temperature is 60 ℃, the reaction pH is controlled at 10.8, and after the reaction is finished, the powder C is obtained by filtering, washing, drying and crushing at 100 ℃;
(4) the powder C is roasted in a rotary kiln at the temperature of 900 ℃ to obtain Ni0.2Co0.2Fe0.2Al0.2Mg0.2O high entropy material.
The high-entropy material has small particle size and uniform particle size distribution (as shown in figure 2).
Example 3
(1) Weighing a certain amount of battery-grade nickel sulfate, cobalt sulfate and magnesium sulfate, adding into a beaker a, and dissolving in pure water, wherein the molar concentrations of nickel, cobalt and magnesium are all 1mol/L, and the total volume is 3L;
(2) weighing a certain amount of battery-grade aluminum sulfate and ferric sulfate, adding the battery-grade aluminum sulfate and ferric sulfate into a beaker b, dissolving the beaker b in pure water, adding 7.65mol of citric acid, 0.9mol of ethylene diamine tetraacetic acid and 0.45mol of ethylene glycol, stirring and dissolving, wherein the molar concentrations of aluminum and iron are both 1mol/L, and the total volume is 3L;
(3) adding 3L and 2L sodium hydroxide solution of beaker a, beaker b and 9mol/L ammonia water into the reaction kettle in a concurrent flow manner, wherein the adding speeds of beaker a, beaker b and ammonia water are respectively 30ml/min, 30ml/min and 30 ml/min; the reaction temperature is 90 ℃, the reaction pH is controlled to be 11.2, and after the reaction is finished, the powder C is obtained by filtering, washing, drying and crushing at 100 ℃;
(4) the powder C is roasted at 600 ℃ in a rotary kiln to obtain Ni0.2Co0.2Fe0.2Al0.2Mg0.2O high entropy material.
The high-entropy material has small particle size and uniform particle size distribution (as shown in figure 3).
Comparative example 1
A certain amount of battery-grade aluminum sulfate and ferric sulfate are weighed and added into a beaker b to be dissolved in pure water, 4.8mol of citric acid and 0.3mol of ethylene glycol are added, and after the mixture is stirred and dissolved, the molar concentrations of aluminum and iron are both 3mol/L, and the total volume is 1000 mL; others remain unchanged.
Comparative example 2
Weighing a certain amount of battery-grade aluminum nitrate and ferric nitrate, adding the battery-grade aluminum nitrate and ferric nitrate into a beaker b, dissolving the beaker b in pure water, adding 0.6mol of ethylene diamine tetraacetic acid and 0.15mol of ethylene glycol, stirring and dissolving, wherein the molar concentrations of aluminum and iron are both 3mol/L, and the total volume is 1000 mL; others remain unchanged.
Comparative example 3
Changing the step (3) of the embodiment 2 into a beaker a, a beaker b and 6mol/L sodium hydroxide solution, and adding the mixture into the reactor in a concurrent flow manner, wherein the adding speeds of the beaker a and the beaker b are respectively 10ml/min and 10 ml/min; the reaction temperature is 60 ℃, the reaction pH is controlled at 10.8, and after the reaction is finished, the powder C is obtained by filtering, washing, drying and crushing at 100 ℃.
Comparative example 4
The citric acid, the ethylene diamine tetraacetic acid and the ethylene glycol in the step (2) of the example 2 are not added, and other conditions are not changed.
The gram discharge capacity after addition of lithium carbonate for the examples and comparative examples is shown in Table 1 below.
TABLE 1 gram Capacity after lithium carbonate discharge
As can be seen from the data in Table 1, Ni prepared using the complex complexing agent0.2Co0.2Fe0.2Al0.2Mg0.2The electrical property of the O high-entropy quinary cell material added with lithium is obviously higher.
It should be noted that: ni of the invention0.2Co0.2Fe0.2Al0.2Mg0.2The preparation method of O high-entropy material includes mixing soluble nickel salt, soluble cobalt salt and soluble magnesium salt into transparent solution, forming soluble aluminum salt and soluble iron salt into complex, mixing the transparent solution with the complex, ammonia water and alkali liquor, wherein citric acid in the complex complexing agent can complex iron and aluminum, ethylenediaminetetraacetic acid can chelate iron and aluminum, both of which have complexing action, but the complexing ability of ethylenediaminetetraacetic acid is stronger, and the two combinations can better control the decomplexing speedTo prevent the iron and aluminum from precipitating too quickly; the ethylene glycol reacts with citric acid and ethylene diamine tetraacetic acid to generate corresponding ester, so that the ability of the composite complexing agent for complexing iron and aluminum is reduced, the corresponding ester is hydrolyzed when the ethylene glycol is added into a reactor for reaction, the complexing ability of the composite complexing agent can be improved, the precipitation speed is convenient to control, and the ethylene glycol has the effect of refining grains. The invention can realize the coprecipitation of five metal ions by controlling the proportion of citric acid, ethylene diamine tetraacetic acid and glycol and the dropping rate of ammonia water. In addition, the ammonia water is added to generate ammonium citrate and ethylenediamine tetraacetic acid diamine with citric acid and ethylenediamine tetraacetic acid during reaction, so that the decomplexing rate of aluminum and iron can be adjusted, and the metal elements are completely and easily precipitated; the alkali liquor mainly adjusts the pH value of the system.
Under the combined action of the factors, the Ni prepared by the invention0.2Co0.2Fe0.2Al0.2Mg0.2The O high-entropy material has good cycling stability of the battery after lithium is added, the safety is greatly improved, the gram discharge capacity is higher, and the O high-entropy material has greater progress compared with the high-entropy material in the prior art.
Finally, it should be noted that the above embodiments are only used for illustrating the technical solutions of the present invention and not for limiting the technical solutions, and it should be noted that, for those skilled in the art, several modifications or equivalent substitutions can be made without departing from the principle of the present invention, and the spirit and scope of the technical solutions should be covered by the claims of the present invention.
Claims (10)
1. A method for preparing a nickel-cobalt-iron-aluminum-magnesium five-element high-entropy material is characterized by comprising the following steps of:
(1) sequentially adding soluble nickel salt, soluble cobalt salt and soluble magnesium salt into a container a, and adding water to dissolve the soluble nickel salt, the soluble cobalt salt and the soluble magnesium salt into a transparent solution;
(2) sequentially adding soluble aluminum salt and soluble ferric salt into the container b, adding water to dissolve the soluble aluminum salt and the soluble ferric salt into a transparent solution, adding a certain amount of composite complexing agent, fully stirring, and standing;
(3) adding four materials of the container a, the container b, ammonia water and alkali liquor into a reaction container in a parallel flow manner, stirring to control the reaction pH, generating slurry at a certain reaction temperature, filtering, washing, drying and crushing to obtain powder C;
(4) the powder C is roasted at a certain temperature to obtain Ni0.2Co0.2Fe0.2Al0.2Mg0.2O high entropy material.
2. The method for preparing the five-element high-entropy material of nickel, cobalt, iron, aluminum and magnesium, according to claim 1, wherein the soluble nickel salt in the step (1) is nickel sulfate or nickel nitrate, the soluble cobalt salt is cobalt sulfate or cobalt nitrate, and the soluble magnesium salt is magnesium sulfate or magnesium nitrate; the concentration of the soluble nickel salt, the soluble cobalt salt and the soluble magnesium salt is 0.4-6 mol/L, preferably 2-4 mol/L.
3. The method for preparing the five-element high-entropy material of nickel-cobalt-iron-aluminum-magnesium as claimed in claim 1, wherein the soluble aluminum salt in the step (2) is sodium metaaluminate, aluminum sulfate or aluminum nitrate, and the soluble iron salt is ferric sulfate or ferric nitrate; the concentration of the soluble aluminum salt and the soluble ferric salt is 0.4-6 mol/L, preferably 2-4 mol/L.
4. The method for preparing the quinary high-entropy nickel-cobalt-iron-aluminum-magnesium material as claimed in claim 1, wherein the complex complexing agent is obtained by dissolving citric acid, ethylene diamine tetraacetic acid and ethylene glycol with pure water, and the molar ratio of the citric acid to the ethylene diamine tetraacetic acid to the ethylene glycol is 0.75-0.85: 0.1-0.2: 0.02 to 0.08; the concentration of citric acid in the composite complexing agent is 0.3-5 mol/L, and preferably 0.5-2 mol/L.
5. The method for preparing the five-element high-entropy nickel-cobalt-iron-aluminum-magnesium material according to claim 1, wherein the molar weight of the composite complexing agent is 0.5 to 1.5 times, preferably 0.5 to 1 time of the sum of the molar weights of the soluble aluminum salt and the soluble iron salt.
6. The method for preparing the nickel-cobalt-iron-aluminum-magnesium quinary high-entropy material as claimed in claim 1, wherein the ammonia water in the step (3) is added in an amount which is 3-10 times of the molar amount of the composite complexing agent, and the concentration is 1.0-10.0 mol/L;
the adding speed of the ammonia water is that the amount of the added ammonia water in unit time is 1-5 times, preferably 2-3 times of the molar weight of the composite complexing agent;
the molar concentrations of the soluble nickel salt, the soluble cobalt salt, the soluble magnesium salt, the soluble aluminum salt and the soluble iron salt which are added into the reactor in unit time are the same when the container a and the container b are added into the reactor.
7. The method for preparing the nickel-cobalt-iron-aluminum-magnesium quinary high-entropy material according to claim 1, wherein the alkali liquor is at least one of liquid alkali, sodium carbonate and sodium bicarbonate, and the molar concentration is 1.5-10.0 mol/L, preferably 4-8 mol/L; the pH is 10.0-11.5, preferably 10.5-11.0; the reaction temperature is 40-95 ℃, preferably 50-75 ℃.
8. The method for preparing the nickel-cobalt-iron-aluminum-magnesium quinary high-entropy material as claimed in claim 1, wherein the roasting temperature in the step (4) is 600-1200 ℃, preferably 700-1000 ℃.
9. A product obtained by the method for preparing a nickel-cobalt-iron-aluminum-magnesium pentabasic high-entropy material according to any one of claims 1 to 8.
10. The Ni of claim 90.2Co0.2Fe0.2Al0.2Mg0.2The application of the O high-entropy material in the lithium ion battery.
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