CN116750810B - Single-crystal type high-nickel ternary positive electrode material for high-voltage lithium ion battery and preparation method thereof - Google Patents

Single-crystal type high-nickel ternary positive electrode material for high-voltage lithium ion battery and preparation method thereof Download PDF

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CN116750810B
CN116750810B CN202310846574.XA CN202310846574A CN116750810B CN 116750810 B CN116750810 B CN 116750810B CN 202310846574 A CN202310846574 A CN 202310846574A CN 116750810 B CN116750810 B CN 116750810B
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lithium
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王英
刘泽瑞
曾黎明
唐仁衡
肖方明
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Institute of Resource Utilization and Rare Earth Development of Guangdong Academy of Sciences
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    • C01G53/50Complex oxides containing nickel and at least one other metal element containing alkali metals, e.g. LiNiO2 containing manganese of the type (MnO2)n-, e.g. Li(NixMn1-x)O2 or Li(MyNixMn1-x-y)O2
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Abstract

The invention discloses a preparation method of a monocrystal type high-nickel ternary anode material for a high-voltage lithium ion battery, which is characterized in that a binary fluxing agent is constructed by lithium hydroxide and lithium carbonate, the minimum eutectic temperature is about 418.2 ℃, and on one hand, the uniformity and the reaction rate of lithiation reaction are improved; on the other hand, the sintering temperature is reduced, and the specific capacity and the sintering morphology of the material are improved; meanwhile, the excessive lithium source obtained by selecting the two lithium salts as fluxing agents can inhibit unstable Ni 3+ from being reduced at high temperature, reduce the phenomenon of mixed discharge of lithium and nickel, and avoid environmental pollution caused by emission of toxic gases (SO 2、NO2, cl 2 and the like) caused by adopting the sintering process of lithium sulfate, lithium chloride and lithium nitrate, and the single crystal type high-nickel ternary positive electrode material prepared by the sectional high-temperature primary sintering, water washing and high-temperature secondary sintering has uniform particle size and good dispersibility and shows good comprehensive electrochemical performance in high-voltage electrolyte.

Description

Single-crystal type high-nickel ternary positive electrode material for high-voltage lithium ion battery and preparation method thereof
Technical field:
The invention relates to a monocrystal type high-nickel ternary positive electrode material for a high-voltage lithium ion battery and a preparation method thereof.
The background technology is as follows:
The lithium ion battery has the advantages of high energy density, high working voltage, small volume and the like, and is widely applied to the fields of mobile communication equipment, small electronic products, new energy automobiles and the like. With the continuous improvement of the demands of people, the consumer market has higher requirements on the comprehensive performances of the lithium ion battery, such as capacity, cycle life, safety and the like. Meanwhile, under the background of global carbon peak and carbon neutralization, the high requirements of new energy markets on the continuous voyage of electric automobiles force the lithium ion power battery anode material to develop to a high-energy density material, so that the single crystallization of the high-nickel anode material becomes the trend of the future lithium battery anode material development. The high-nickel ternary positive electrode material is made into a single crystal morphology, so that the positive electrode material has larger primary particles and lower specific surface area, lattice distortion generated in the high-voltage charge-discharge process of the material can be effectively inhibited, side reaction between the surface of the positive electrode material and electrolyte is reduced, and excellent electrochemical performance is realized.
The monocrystal type high-nickel ternary anode material has good thermal stability and structural stability. Mainly because the material particles have no grain boundary inside, the inter-crystal cracks generated by anisotropic shrinkage and expansion of the lithium intercalation and deintercalation active substance particles in the electrochemical process are radically eliminated, thereby inhibiting the structural collapse of the material and the side reaction inside the crystal grains in the charge and discharge process. Compared with the high-nickel polycrystalline material, single crystal particles of the single crystal high-nickel material have better structural integrity than loosely aggregated polycrystalline particles, and can reach higher tap density in the pressing process of the pole piece to realize higher volume energy density; the expansion/contraction of the lattice volume of the monocrystal material in the lithium intercalation and deintercalation process is isotropic, so that the risk of microcrack generation in the circulation process can be greatly reduced; the monocrystal particles have smaller specific surface area and good dispersibility, can be better contacted with the conductive agent, and are beneficial to the transmission of lithium ions.
The high-temperature solid phase method and the molten salt auxiliary method are the main methods for synthesizing the single crystal cathode material at present. The molten salt auxiliary method is used for reducing the calcination temperature, and auxiliary agents such as fluxing agent, pore-forming agent, crystal face modifier and the like are added into the precursor in the process of preparing the monocrystal to sinter and synthesize the monocrystal anode material. The fluxing agent is typically one or more low melting salts. The method mainly uses the cosolvent to convert the lithiated solid-solid reaction into the solid-liquid reaction, so that the reactants can realize the atomic/molecular scale mixing in the liquid phase, thereby accelerating the diffusion rate of ions, shortening the reaction time and reducing the reaction temperature.
CN110923801B discloses a preparation method and application of single crystal ternary material. The method comprises the steps of firstly preparing a monocrystal precursor, adding a fluxing agent in the process of preparing the precursor, and preparing a monocrystal ternary material after lithium matching. The traditional one-step synthesis method is disassembled into two steps of synthesis of a monocrystal precursor and lithium-matching roasting, compared with the one-step lithiation monocrystal process, the Li/Ni mixed discharge is reduced, and the capacity and the first effect of the monocrystal ternary material are improved. The fluxing agent is a two-phase composite fluxing agent B2O3+Bi2O3、ZrO2+B2O3、Al2O3+B2O3、LiF+AlF、KCl+MgCl2 or a three-phase composite fluxing agent LiF+NaF+KF, liF+AlF+CsF and KF+LiF+CsF.
CN115172719a discloses a preparation method of a high-voltage monocrystal ternary material. The grain boundary fusion energy is reduced by means of a low-melting-point fluxing agent, the directional microcrystal nucleus is obtained by presintering at low temperature, the directional microcrystal nucleus reacts with a structure stabilizer at high temperature to realize the directional growth of the crystal nucleus, the directional growth of the crystal grains is realized, meanwhile, the material has higher compaction density, and the capacity, the high-low temperature circulation and the multiplying power performance of the material are obviously superior to those of the traditional monocrystal ternary anode material. The selected fluxing agent is one or more of boron oxide, boric acid, boron chloride and boron fluoride.
CN114703545A discloses a method for preparing high-capacity monocrystal ternary cathode material by infiltration dispersion method, which effectively reduces the synthesis temperature of monocrystal ternary cathode material, and the prepared submicron-level material has the advantages of good morphology, good uniformity of particle size, etc. The molten salt is one or the combination of more than two of lithium oxide, lithium peroxide, lithium hydroxide, lithium acetate, lithium chloride, lithium nitrate and lithium sulfate.
The above patent applications all use molten salt assisted method to prepare single crystal ternary materials. The material particles obtained by selecting different molten salt systems still have a certain agglomeration phenomenon, so that the exerted technical effects have a certain difference.
The invention comprises the following steps:
The invention aims to provide a preparation method of a monocrystal type high-nickel ternary positive electrode material for a high-voltage lithium ion battery, which is characterized in that a binary fluxing agent is constructed by lithium hydroxide and lithium carbonate, the minimum eutectic temperature is about 418.2 ℃, and on one hand, the uniformity and the reaction rate of lithiation reaction are improved; on the other hand, the sintering temperature is reduced, and the specific capacity and the sintering morphology of the material are improved; meanwhile, the excessive lithium source obtained by selecting the two lithium salts as fluxing agents can inhibit unstable Ni 3+ from being reduced at high temperature, reduce the phenomenon of mixed discharge of lithium and nickel, and avoid environmental pollution caused by emission of toxic gases (SO 2、NO2, cl 2 and the like) caused by adopting the sintering process of lithium sulfate, lithium chloride and lithium nitrate, and the single crystal type high-nickel ternary positive electrode material prepared by the sectional high-temperature primary sintering, water washing and high-temperature secondary sintering has uniform particle size and good dispersibility and shows good comprehensive electrochemical performance in high-voltage electrolyte.
The invention is realized by the following technical scheme:
The preparation method of the monocrystal type high-nickel ternary positive electrode material for the high-voltage lithium ion battery comprises the following steps of:
1) Grinding the Ni 0.88Co0.09Mn0.03(OH)2 precursor and LiOH H 2O、Li2CO3 in a mortar, and uniformly mixing; the binary fluxing agent is formed by LiOH H 2 O and Li 2CO3, and the mole fraction of LiOH H 2 O in the cosolvent is as follows, wherein the total mole percentage of the fluxing agent is 100 percent: 74% -84%, and the balance of Li 2CO3; the molar ratio of Li to the sum of all metal atoms of the Ni 0.88Co0.09Mn0.03(OH)2 precursor in the fluxing agent (Li/Me, me=Ni+Co+Mn) is (1.15-2) 1; preferably (1.6-1.9): 1;
2) Placing the uniformly mixed material obtained in the step 1) in an oxygen atmosphere for sectional calcination, firstly heating to 400-600 ℃ at a heating rate of 3-5 ℃/min for 2-6 h, then heating to 750 ℃ for 5-15 h, continuously heating to 800-900 ℃ for 5-15 h, finally cooling to room temperature along with a furnace, crushing and grinding, and sieving with a 300-mesh sieve to obtain a ternary anode material;
3) Mixing the material obtained in the step 2) with deionized water, stirring for 20-40 min at a feed-liquid ratio of 1:20-1:30, standing until the solution is completely layered, pouring out the upper layer solution, adding deionized water, repeatedly washing for 3 times until the pH value is no longer reduced, carrying out suction filtration, putting the filter cake into a vacuum drying box, drying for 20-28 h at 70-90 ℃, putting the filter cake into a corundum crucible again, calcining for 4-8 h at 600-850 ℃ preferably 700-750 ℃ in an oxygen atmosphere, cooling to room temperature along with a furnace, grinding and screening, and obtaining the single crystal type high nickel ternary positive electrode material for the high voltage lithium ion battery.
The beneficial effects of the invention are as follows:
According to the invention, the binary fluxing agent is constructed by lithium hydroxide and lithium carbonate, the minimum eutectic temperature of the two is about 418.2 ℃, on one hand, precursor solutes are dissolved in molten salt, and the uniformity and the reaction rate of lithiation reaction are improved; on the other hand, the sintering temperature is reduced, and the specific capacity and the sintering morphology of the material are improved; meanwhile, the excessive lithium source obtained by selecting the two lithium salts as fluxing agents can inhibit unstable Ni 3+ from being reduced at high temperature, reduce the phenomenon of mixed discharge of lithium and nickel, and avoid environmental pollution caused by emission of toxic gases (SO 2、NO2, cl 2 and the like) caused by adopting the sintering process of lithium sulfate, lithium chloride and lithium nitrate, and the single crystal type high-nickel ternary positive electrode material prepared by the sectional high-temperature primary sintering, water washing and high-temperature secondary sintering has uniform particle size and good dispersibility and shows good comprehensive electrochemical performance in high-voltage electrolyte.
Description of the drawings:
Fig. 1 is an SEM image of a single-crystal type high-nickel ternary cathode material for a high-voltage lithium ion battery obtained in example 3.
Fig. 2 is an SEM image of the single-crystal type high-nickel ternary cathode material for a high-voltage lithium ion battery obtained in example 4.
Fig. 3 is an SEM image of the single-crystal type high-nickel ternary cathode material for a high-voltage lithium ion battery obtained in example 7.
Fig. 4 is an SEM image of the single-crystal high-nickel ternary cathode material for a high-voltage lithium ion battery obtained in example 8.
Fig. 5 is an SEM image of the single-crystal high-nickel ternary cathode material for a high-voltage lithium ion battery obtained in example 11.
Fig. 6 is an SEM image of a single-crystal type high-nickel ternary cathode material for a high-voltage lithium ion battery obtained in example 13.
Fig. 7 is an SEM image of the ternary cathode material obtained in comparative example 1.
Fig. 8 is an SEM image of the ternary cathode material obtained in comparative example 7.
Fig. 9 is a 1C cycle performance curve of the batteries assembled with the cathode materials of examples 12 to 15 and comparative example 7.
Fig. 10 is a graph showing the rate performance of the batteries assembled from the positive electrode materials of examples 12 to 15 and comparative example 7.
Fig. 11 is an SEM image of the electrode sheet of example 13 after 100 weeks of cycling.
Fig. 12 is an SEM image of the comparative example 7 electrode sheet after 100 weeks of cycling.
The specific embodiment is as follows:
the following is a further illustration of the invention and is not a limitation of the invention.
Example 1:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, and Li/Me=2:1 (i.e. n (Li) in flux: n (Ni+Co+Mn) =2:1 in precursor) were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. And repeatedly washing for 3 times, carrying out suction filtration without the pH value decreasing, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 600 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 2:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26 and Li/Me=2:1 were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 650 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 3:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26 and Li/Me=2:1 were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 700 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 4:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26 and Li/Me=2:1 were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 5:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26 and Li/Me=2:1 were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 800 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 6:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26 and Li/Me=2:1 were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 850 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 7:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26 and Li/Me=2:1 were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 8 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 8:
18.9912g of Ni 0.88Co0.09Mn0.03(OH)2 precursor, 10.2099g of LiOH H 2 O and 6.2829gLi 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26 and Li/Me=2:1 were weighed out separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 1h, standing the mixture until the solution is completely layered, pouring out the upper layer of solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 9:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.8707g LiOH H 2 O and 3.6127g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.15:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 10:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 6.3812g LiOH H 2 O and 3.9268g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.25:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 11:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 7.6574g LiOH H 2 O and 4.7122g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.5:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 12:
9.4956gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.0355g LiOH H 2 O and 1.6799g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =84:16, li/me=1.6:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 13:
9.4956gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.3502g LiOH H 2 O and 1.7849g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =84:16, li/me=1.7:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 14:
9.4956gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.6649g LiOH H 2 O and 1.8899g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =84:16, li/me=1.8:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Example 15:
9.4956gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.9796g LiOH H 2 O and 1.9949g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =84:16, li/me=1.9:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 single-crystal positive electrode material.
Comparative example 1:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.3602g LiOH H 2 O and 3.2985g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material, wherein the obtained LiNi 0.88Co0.09Mn0.03O2 positive electrode material is a polycrystalline material.
Comparative example 2:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.3602g LiOH H 2 O and 3.2985g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 10min, standing the mixture until the solution is completely layered, and carrying out suction filtration. The filter cake was dried in a vacuum oven at 80℃for 24h. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 anode material which is a polycrystalline material.
Comparative example 3:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.3602g LiOH H 2 O and 3.2985g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. And (5) filtering until the solution is completely layered. The filter cake was dried in a vacuum oven at 80℃for 24h. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 anode material which is a polycrystalline material.
Comparative example 4:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.3602g LiOH H 2 O and 3.2985g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 10min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 anode material which is a polycrystalline material.
Comparative example 5:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.3602g LiOH H 2 O and 3.2985g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 anode material which is a polycrystalline material.
Comparative example 6:
9.4956gNi 0.88Co0.09Mn0.03(OH)2 precursor, 3.3045g LiOH H 2 O and 1.1024g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =84:16, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 830 ℃ for 20 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 anode material which is a polycrystalline material.
Comparative example 7:
9.4956gNi 0.88Co0.09Mn0.03(OH)2 precursor, 3.3045g LiOH H 2 O and 1.1024g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =84:16, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 780 ℃ for 14 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 anode material which is a polycrystalline material.
Comparative example 8:
18.9912gNi 0.88Co0.09Mn0.03(OH)2 precursor, 5.3602g LiOH H 2 O and 3.2985g Li 2CO3,n(LiOH·H2O):n(Li2CO3) =74:26, li/me=1.05:1 were weighed separately. Grinding and mixing in a mortar, placing the powder in a crucible after the powder is uniformly mixed, transferring the crucible into an atmosphere furnace filled with oxygen for segmented calcination, heating to 500 ℃ at a heating rate of 5 ℃/min for 4 hours, heating to 750 ℃ for 5 hours, continuously heating to 850 ℃ for 15 hours, and finally cooling to room temperature along with the furnace. Crushing, grinding and sieving with a 300-mesh sieve to obtain the ternary positive electrode material. Weighing 4g of positive electrode material, placing the positive electrode material into a beaker, adding 100mL of deionized water, uniformly stirring the mixture at a feed-liquid ratio of 1:25, measuring the pH value, continuously stirring the mixture for 30min, standing the mixture until the solution is completely layered, pouring out the upper layer solution, adding 100mL of deionized water, uniformly stirring the mixture, and measuring the pH value again. Repeatedly washing for 3 times, performing suction filtration, and putting the filter cake into a vacuum drying oven to be dried for 24 hours at 80 ℃. Placing the mixture in a corundum crucible again, calcining the mixture for 4 hours at 750 ℃ in an oxygen atmosphere, and cooling the mixture to room temperature along with a furnace. And grinding and screening to obtain the LiNi 0.88Co0.09Mn0.03O2 anode material which is a polycrystalline material.
Comparative example 9:
Reference example 4 differs in that lithium sulfate was used instead of lithium carbonate.
The positive electrode materials prepared in examples 1 to 15 and comparative examples 1 to 8 were prepared into 2032-type button-type analog batteries, and their electrochemical properties were measured. The method comprises the following specific steps: (1) Respectively weighing active substances, conductive acetylene black and polyvinylidene fluoride (PVDF) according to the mass ratio of 80:10:10, firstly dissolving PVDF into a proper amount of N-methylpyrrolidone (NMP), then adding the uniformly mixed active substances and acetylene black powder into NMP, and uniformly stirring to prepare slurry; (2) Uniformly coating the slurry on an aluminum foil substrate, putting the wet electrode into a vacuum drying oven, and drying at 80 ℃ for 12 hours; (3) In a dry vacuum glove box, the simulated cells were assembled and the electrochemical performance test results are shown in table 1.
TABLE 1 electrochemical Properties of the cathode materials of examples 1 to 15 and comparative examples 1 to 8 (2.8 to 4.5V)
As can be seen from table 1, under the conditions of selecting Li/me=2:1 and n (lioh.h 2O):n(Li2CO3) =74:26, the single-crystal type high-nickel ternary cathode materials of examples 1 to 6 show the same rule in terms of the first-discharge specific capacity which tends to increase and decrease after the increase of the back firing temperature. Therefore, the calcination temperature is preferably 700 to 750 ℃. Wherein the capacity retention rate reached 89.1% after 100 weeks of cycling at 1C rate in example 3; the specific capacity for the first discharge was 182.0mAh/g in example 4. The positive electrode material particles have single crystal morphology, the primary particle size is mostly more than 3 mu m, and the dispersibility is good. As shown in fig. 1 and 2. In addition to the initial polycrystalline morphology, i.e., the primary particles agglomerated into secondary particles, comparative example 1, which had no subsequent water washing and calcination after water washing, had a morphology in which a small portion of the spheroidal secondary particles split into primary particles, as shown in fig. 6, with a Li/Me molar ratio of 1.05:1. The cycle stability of example 3 was better than that of comparative example 1, and that of comparative example 8, which had been back-burned with water, but lower than that of comparative example 5, which had not been back-burned with water. As can be seen from a comparison of example 4 and comparative example 8, the Li/Me molar ratio is 2:1, which is higher than 1.05:1 in terms of the first charge and discharge efficiency. As can be seen from comparison of example 10 and comparative example 5, the addition of the calcination step after washing with water allows for higher first charge and discharge efficiency. On the basis of example 4, the burn-back time was prolonged to 8 hours or the water washing time was increased to 1 hour, as shown in fig. 3 and 4, the primary particles were slightly agglomerated, but the first discharge capacity was improved, and the cycle stability of example 7 was improved. Comparative example 8, where n (lioh.h 2O):n(Li2CO3) =74:26/84:16, was a polycrystalline morphology and the combined electrochemical performance was better than comparative example 1 by water washing and backfire treatment. And the positive electrode material with Li/Me=1.15-1.9:1 is in a single crystal morphology, as shown in figures 5 and 6, and has better particle dispersibility. The first charge-discharge efficiency and cycling stability of the single crystalline materials of examples 12-15 are superior to comparative example 7, which is a distinct polycrystalline morphology with fusion between the agglomerate particles to form larger particle size agglomerate particles, see fig. 8. The initial discharge specific capacity of 0.2C of example 13 is 201.8mAh/g, the initial charge-discharge efficiency is 83.0%, and after 1C is cycled for 100 weeks, the discharge specific capacity can reach 162.3mAh/g, and the capacity retention rate is 86.7%, as shown in FIG. 9. As can be seen from fig. 10, the 159.9mAh/g capacity of example 13 was higher than 153.3mAh/g of comparative example 7 at 10C discharge, and the 150.1mAh/g capacity of example 12 was also closer to comparative example 7. When the 0.2C discharge was restored, the capacities of the materials of examples 12 to 14 were restored to 96.8%, 96.2%, 92.6% and 88.6% of their initial capacities, respectively, each higher than 86.8% of comparative example 7. The single-crystal type high nickel material has good multiplying power performance. Fig. 11 and 12 are SEM images of the electrode sheets of example 13 and comparative example 7, respectively, after 100 weeks of cycling. It can be seen that the particles with single crystal morphology remain intact through multiple charge and discharge cycles, the arrangement is relatively compact, and no obvious cracks exist in the particles with polycrystalline morphology. Therefore, the electrode structure using the single-crystal type high-nickel positive electrode material as an active material is stable, thereby exhibiting good cycle performance and reversibility of high-rate discharge cycle.
LiOH-Li 2CO3 mixed molten salt is selected as a fluxing agent, the lithium ratio (Li/Me) is important, and when the Li/Me exceeds 1.15, the single crystal type material can be obtained. But can obtain single crystal materials with good cycle stability and rate capability under proper process conditions; when Li/Me is 1.05, the polycrystalline material is obtained through one sintering. In addition, the secondary sintering condition and the water washing condition have a certain influence on the electrochemical performance of the single crystal material.

Claims (2)

1. The preparation method of the single-crystal high-nickel ternary positive electrode material for the high-voltage lithium ion battery is characterized by comprising the following steps of:
1) Grinding the Ni 0.88Co0.09Mn0.03(OH)2 precursor and LiOH H 2O、Li2CO3 in a mortar, and uniformly mixing; the binary fluxing agent is formed by LiOH H 2 O and Li 2CO3, and the mole fraction of LiOH H 2 O in the fluxing agent is as follows, wherein the total mole percentage of the fluxing agent is 100 percent: 74% -84%, and the balance of Li 2CO3; the molar ratio of Li to the sum of all metal atoms of the Ni 0.88Co0.09Mn0.03(OH)2 precursor in the fluxing agent is 1.6-1.9:1;
2) Placing the uniformly mixed material obtained in the step 1) in an oxygen atmosphere for sectional calcination, firstly heating to 400-600 ℃ at a heating rate of 3-5 ℃/min for 2-6 h, then heating to 750 ℃ for 5-15 h, continuously heating to 800-900 ℃ for 5-15 h, finally cooling to room temperature along with a furnace, crushing and grinding, and sieving with a 300-mesh sieve to obtain a ternary anode material;
3) Mixing the material obtained in the step 2) with deionized water, stirring for 20-40 min until the solution is completely layered, pouring out the upper layer solution, adding deionized water, repeatedly washing for 3 times until the pH value is no longer reduced, carrying out suction filtration, putting the filter cake into a vacuum drying box, drying for 20-28 h at 70-90 ℃, putting the filter cake into a corundum crucible again, calcining for 4-8 h at 600-850 ℃ in an oxygen atmosphere, cooling to room temperature along with a furnace, grinding and screening, and obtaining the single crystal type high nickel ternary positive electrode material for the high voltage lithium ion battery.
2. The process according to claim 1, wherein the calcination temperature in step 3) is 700 to 750 ℃ in an oxygen atmosphere.
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