Method for simultaneously manufacturing nano and submicron spherical oxide fillers

Abstract

The present invention relates to the field of spherical oxide filler technology and provides a method for simultaneously manufacturing nano and submicron spherical oxide fillers. In the present invention, by combining an oxide raw material (raw material O) with a metal or non-metal raw material (raw material M), the reaction activity of the raw material is lowered, thereby reducing the uncontrollable risk of dust explosion and realizing safe production. Simultaneously, raw material O vaporizes under high-temperature conditions to form nano-level particles or is dispersed by shock waves generated by an explosion to become nano-level particles, while raw material M reacts with oxygen in an oxygen-rich state to form submicron-level particles through aggregation and cooling. The product particles obtained from the combustion reaction are cooled under oxygen-rich conditions to transform into spherical shapes, and through a precision separation process, submicron spherical oxide fillers and nano-spherical oxide fillers can be obtained simultaneously. Furthermore, the present invention reduces costs by minimizing gas when the temperature inside the reactor stabilizes, thereby stabilizing the temperature inside the reactor.

Description

Technology Field

[0001] The present application was filed with the Chinese Intellectual Property Office on October 18, 2022, and claims priority to a Chinese patent application with application number CN202211271930.1 and title of invention "Method for simultaneously manufacturing nano and submicron spherical oxide fillers," the full contents of which are incorporated into the present application by reference.

[0002] The present invention relates to the field of spherical oxide filler technology, and in particular to a method for simultaneously manufacturing nano and submicron spherical oxide fillers. Background Technology

[0003] Electronic packaging devices improve the performance of the system, such as the coefficient of thermal expansion, dielectric properties, moisture resistance, and stress, by adding fillers. As electronic devices are recently evolving to become thinner, lighter, and smaller, smaller particle sizes of the filler are desirable, and thus miniaturization of the filler particle size is essential.

[0004] Currently, the primary methods for producing nano and submicron fillers include liquid-phase synthesis, plasma, vaporization, and flame methods. Among these, the liquid-phase synthesis method is difficult to implement in large quantities due to the use of environmentally unfriendly organic solvents, high costs, and long production cycles. The plasma method is a physical process that involves high operating costs and low production capacity, making large-scale production difficult. The vaporization method utilizes light sources, such as lasers, to concentrate high heat to obtain submicron-level products; however, as this method is currently in the development stage, the stability of the produced products is poor. The flame method is currently one of the major manufacturing methods for spherical oxide fillers; in this process, the filler is introduced into a high-temperature environment formed by flammable gases and oxygen to melt it at high temperatures, followed by cooling. The action of surface tension causes the material to become spherical, ultimately forming spherical oxide fillers.

[0005] A 1990 U.S. patent (Patent No.: US4923520) described a method of forming a high-temperature flame using propane, a flammable gas, and oxygen, an auxiliary gas, to spheroidize angular silicon dioxide fine powder, but this method could only produce products with an average particle size of 10 μm to 50 μm. Subsequently, through continuous improvements, it became possible to obtain products with an average particle size of about 3 μm in the actual production process, but products smaller than 3 μm cannot be achieved with this method.

[0006] In Patent Publication No. 2009-263154 disclosed by Admatechs Co., Ltd., silicon is used as a raw material and the principle of dust explosion is utilized to produce an average particle size of 0.5 μm and a specific surface area of ​​6.0 m² 2 Spherical silicon dioxide powder with an average particle size of 0.1 to 10 μm was manufactured. In Shin-Echi Chemical’s patent JP Hei 4-132610, silicon powder was combusted in an oxygen-containing air stream to obtain fine spherical silicon dioxide powder with an average particle size of 0.1 to 10 μm. All of the above patents use silicon as a raw material, but metals are prone to dust explosions under high temperature and oxygen-rich conditions, resulting in poor safety for factory design, equipment, and personnel; therefore, this process is rarely used in China to produce sub-micrometer silicon dioxide products.

[0007] Therefore, there is an urgent need in this field for a method capable of simultaneously manufacturing nano and submicron spherical oxide fillers with excellent safety. The problem to be solved

[0008] In light of these circumstances, the present invention provides a method for simultaneously manufacturing nano and submicron spherical oxide fillers. The method provided by the present invention can simultaneously manufacture nano and submicron spherical oxide fillers and offers excellent safety. means of solving the problem

[0009] To achieve the objective of the above invention, the present invention provides the following technical solution.

[0010] A method for simultaneously manufacturing nano and submicron spherical oxide fillers comprises the following steps.

[0011] A first raw material and a second raw material are subjected to a combustion reaction under conditions in which gas and an auxiliary gas are present to obtain a combustion product, wherein the first raw material is a metal element powder, a non-metal element powder, or an alloy powder, and the second raw material is an oxide or a complex oxide corresponding to the first raw material, wherein the particle size of the first raw material is 3 to 300 μm, the particle size of the second raw material is 30 nm to 10 μm, and the mass of the second raw material is 30% or less of the total mass of the first raw material and the second raw material.

[0012] After cooling the above combustion product, a precise separation process is performed to obtain submicron spherical oxide fillers and nano-spherical oxide fillers.

[0013] Preferably, during the combustion reaction, the method of introducing the first raw material and the second raw material is to introduce them after mixing the first raw material and the second raw material, and the method of mixing the first raw material and the second raw material is dry mixing or liquid mixing.

[0014] Preferably, the liquid mixture is obtained by mixing the first raw material, the second raw material, and the solvent, and then drying to obtain a mixed powder.

[0015] Preferably, the solvent is one or more of water, methanol, ethanol, acetone, and butanone, the drying temperature is within the range of 100 to 200°C, and the drying time is 2 to 30 hours.

[0016] Preferably, the equipment used for the dry mixing includes a V-type mixer, a double cone mixer, a pneumatic mixer, a cone mixer, a high-speed mixer, or an air flow mixer.

[0017] Preferably, when the first and second raw materials are mixed and then added, the addition speed is 1.7g / min to 1020g / min.

[0018] Preferably, when the first raw material and the second raw material are each introduced during the combustion reaction, the introduction rate of the first raw material is 1.7 g / min to 700 g / min, and the introduction rate of the second raw material is 250 g / min or less.

[0019] Preferably, during the combustion reaction, the gas inflow rate is reduced to 2% to 10% of the initial inflow rate after the temperature inside the reactor has stabilized, and the temperature is considered stable when the upper and lower fluctuations of the temperature inside the reactor do not exceed 10℃.

[0020] Preferably, the initial inflow velocity of the gas is 50 m 3 The rate is / h, and after the temperature inside the reactor stabilizes, the gas inflow velocity is 2m 3 It decreases to / h.

[0021] Preferably, the metal element powder comprises one or more of aluminum, magnesium, iron, copper, titanium, zirconium, and zinc, the non-metal element powder is silicon, and the alloy powder comprises one or more of aluminum-iron alloy, aluminum-silicon alloy, aluminum-magnesium alloy, magnesium alloy, and silicon-iron alloy powder.

[0022] Preferably, the method of fine separation comprises one or more of cyclone classification, airflow classification, overflow classification, and sieve classification.

[0023] Preferably, D of the submicron spherical oxide filler 50 The particle size is 0.1 to 1.5 μm, and D of the nano-spherical oxide filler 50 The particle size is 10 to 100 nm.

[0024] Preferably, the gas comprises one or more of hydrogen, liquefied natural gas, liquefied petroleum gas, acetylene, and propane, and the auxiliary gas comprises one or two of oxygen and air. Effects of the invention

[0025] The present invention provides a method for simultaneously manufacturing nano and submicron spherical oxide fillers, comprising the following steps: a first raw material and a second raw material are subjected to a combustion reaction under conditions in which a gas and an auxiliary gas are present to obtain a combustion product, wherein the first raw material is a metal element powder, a non-metal element powder, or an alloy powder, and the second raw material is an oxide or a composite oxide corresponding to the first raw material; and after cooling the combustion product, a precise separation process is performed to obtain submicron spherical oxide fillers and nano spherical oxide fillers. In the present invention, by combining an oxide raw material (second raw material, denoted as raw material O) and a metal or non-metal raw material (first raw material, denoted as raw material M), the reaction activity of the obtained mixed raw material (inscribed as raw material MO) is lowered, thereby reducing the uncontrollable risk of dust explosion and realizing safe production. At the same time, raw material O vaporizes under high temperature conditions to form nano-level particles or is dispersed by shock waves generated by an explosion to form nano-level particles, and raw material M reacts with oxygen in an oxygen-rich state to form submicron-level particles through aggregation and cooling. The product particles obtained from the combustion reaction are cooled under high temperature and oxygen-rich conditions and change into a spherical shape due to the action of surface tension, thereby forming submicron-level particles and nano-level particles, respectively, and by subjecting the mixed particles to a precision separation process, submicron-spherical oxide filler and nano-spherical oxide filler can be obtained simultaneously.

[0026] In addition, raw material M releases a large amount of heat during the reaction with oxygen, and since the subsequent reaction can be maintained with this heat, the present invention reduces costs while stabilizing the temperature inside the reactor by minimizing gas when the temperature inside the reactor is stabilized. Specific details for implementing the invention

[0027] The present invention provides a method for simultaneously manufacturing nano and submicron spherical oxide fillers, comprising the following steps.

[0028] A first raw material and a second raw material are subjected to a combustion reaction under conditions in which gas and an auxiliary gas are present to obtain a combustion product, wherein the first raw material is a metal element powder, a non-metal element powder, or an alloy powder, and the second raw material is an oxide or a complex oxide corresponding to the first raw material, wherein the particle size of the first raw material is 3 to 300 μm, the particle size of the second raw material is 30 nm to 10 μm, and the mass of the second raw material is 30% or less of the total mass of the first raw material and the second raw material.

[0029] After cooling the above combustion product, a precise separation process is performed to obtain submicron spherical oxide fillers and nano-spherical oxide fillers.

[0030] The present invention obtains a combustion product by combusting a first raw material and a second raw material under conditions in which gas and an auxiliary gas are present. In the present invention, the first raw material is a metal element powder, a non-metal element powder, or an alloy powder; the metal element powder preferably comprises one or more of aluminum, magnesium, iron, copper, titanium, zirconium, and zinc, and the non-metal element powder preferably comprises silicon; and the second raw material comprises one or more of an aluminum-iron alloy, an aluminum-silicon alloy, an aluminum-magnesium alloy, a magnesium alloy, and a silicon-iron alloy powder, and the second raw material is an oxide corresponding to the first raw material, for example, when the first raw material is aluminum powder (Al), the second raw material is alumina powder (Al2O3); when the first raw material is silicon powder (Si), the second raw material is silicon dioxide powder (SiO2); and when the first raw material is an aluminum-silicon alloy, the second raw material is a mixture of alumina powder and silicon dioxide powder (i.e., a composite oxide). In the present invention, the first raw material is denoted as raw material M, the second raw material as raw material O, and the mixture of the first and second raw materials as raw material MO.

[0031] In the present invention, the average particle size of raw material M is 3 to 300 μm, specifically 3 μm, 5 μm, 15 μm, 35 μm, 50 μm, 100 μm, 200 μm, or 300 μm, and the average particle size of raw material O is 30 nm to 10 μm, specifically 30 nm, 100 nm, 1 μm, 3 μm, 5 μm, or 10 μm.

[0032] In the present invention, the mass of the raw material O is 30% or less of the total mass of the raw material M and the raw material O, specifically greater than 0 and 30% or less, preferably 5% to 25%, and more preferably 10% to 20%.

[0033] In the present invention, during the combustion reaction, the method of supplying the first raw material and the second raw material is preferably to mix raw material M and raw material O and then supply them, or to supply raw material M and raw material O separately. When adopting a method of supplying after mixing, the method of mixing raw material M and raw material O is preferably dry mixing or liquid mixing, and the device used for the dry mixing preferably includes a V-type mixer, a double cone mixer, a pneumatic mixer, a cone mixer, a high-speed mixer, or an air flow mixer, and the liquid mixing preferably involves mixing raw material M, raw material O, and a solvent and then drying to obtain a mixed powder (i.e., raw material MO), and the solvent is preferably one or several of water, methanol, ethanol, acetone, and butanone, and the device used for the liquid mixing preferably matches the device used for dry mixing, and once mixing is complete, the solvent is completely removed by drying at a temperature of 100 to 200°C for 2 to 30 hours, and the present invention does not require a special volume of solvent used in the liquid mixing process, and it is sufficient to be able to uniformly mix raw material M and raw material O.

[0034] In a specific embodiment of the present invention, when a method of supplying after mixing is adopted, the supply rate of raw material MO is preferably 1.7g / min to 1020g / min.

[0035] In the present invention, when adopting a method of supplying raw material M and raw material O separately, the raw materials (i.e., raw material M and raw material O) in other storage tanks are preferably transferred to a combustion reaction vessel at a constant rate, and the present invention controls the transfer rate of raw material M and raw material O so that the mass of raw material O in the reaction vessel is 30% or less of the total mass of raw material M and raw material O. In a specific embodiment of the present invention, when adopting a method of supplying raw material M and raw material O separately, the supply rate of raw material M is preferably 1.7 g / min to 700 g / min, and the supply rate of raw material O is 250 g / min or less, preferably 0.5 to 250 g / min.

[0036] In the present invention, the gas preferably comprises one or more of hydrogen, liquefied natural gas, liquefied petroleum gas, acetylene, and propane, and the auxiliary gas preferably comprises one or two of oxygen and air, and the combustion reaction vessel is preferably a reactor. The present invention preferably first introduces the gas and the auxiliary gas into the reactor to combust, and then introduces the raw material MO or introduces the raw material M and the raw material O respectively. The raw material MO reacts in a high-temperature flame formed by the gas and the auxiliary gas. The raw material MO is instantaneously decomposed under high-temperature conditions rich in oxygen, and the raw material M and oxygen coated in the middle are combusted to release a large amount of heat, causing the temperature to continue rising. The present invention preferably lowers the gas introduction rate to 2% to 10% of the initial introduction rate when the temperature inside the reactor stabilizes. In a specific embodiment of the present invention, the temperature is determined to be stable when the temperature change inside the reactor does not exceed 10℃. Through such operations, the present invention can save gas and lower costs, and simultaneously control the temperature balance inside the reactor. The inflow velocity of the auxiliary gas is preferably calculated according to the chemical metering ratio with the gas, and in a specific embodiment of the present invention, as the usage of the gas decreases, the usage of the auxiliary gas is also reduced, and in a specific embodiment of the present invention, the initial inflow velocity of the gas is preferably 50 m 3 It is / h, and the initial flow velocity of the auxiliary gas is preferably 150 m 3 It is / h, and when the temperature inside the reactor stabilizes, the gas inlet velocity is preferably 2 m 3 At / h, the auxiliary gas inlet velocity is preferably 15 m 3 Lower it to / h.

[0037] In the combustion reaction process, raw material O is vaporized under high-temperature conditions to form nano-level particles or dispersed into nano-level particles by shock waves generated by explosive combustion, and raw material M reacts with oxygen in an oxygen-rich state to aggregate and cool, forming submicron-level particles; therefore, the resulting combustion product is a mixture of nano-level oxide particles and submicron-level oxide particles.

[0038] After obtaining a combustion product, the present invention cools the combustion product and performs fine separation to obtain submicron spherical oxide fillers and nano-spherical oxide fillers. In the present invention, cooling is preferably air cooling, and during the cooling process, nano-level particles and submicron-level particles become spherical due to the action of surface tension, forming nano-spherical oxide particles and submicron spherical oxide particles. In the present invention, the method of fine separation preferably includes one or more of cyclone classification, air stream classification, overflow classification, and sieve classification. The present invention has no special requirements regarding the specific operating conditions of the above methods, and it is sufficient to be able to separate products of different particle sizes by applying conditions known to those skilled in the art. The coarse powder section of the fine separation is a submicron spherical oxide filler, and the fine powder section is a nano-spherical oxide filler. In the present invention, the average particle size of the submicron spherical oxide filler is 0.1 to 1.5 μm, and the average particle size of the nano-spherical oxide filler is 10 to 100 nm.

[0039] The following will clearly and completely explain the technical solution of the present invention in combination with embodiments thereof; it is evident that the described embodiments are only a part of the embodiments of the present invention and do not constitute all embodiments. Based on the embodiments of the present invention, all other embodiments that can be obtained by those skilled in the art without creative effort also fall within the scope of protection of the present invention.

[0040] In the following examples, the gas used is all natural gas, and the auxiliary gas is all oxygen.

[0041] Example 1

[0042] 700g of D 50 Raw Si powder with a g of 5μm and 300g of D 50 Raw SiO2 powder with a particle size of 0.1 μm was homogenized and compounded in an air flow mixer for 3 hours to prepare a mixed raw material Si-SiO2. This mixed raw material was introduced into a high-temperature vessel filled with gas and oxygen to react (the input rate of the mixed raw material was 60 g / min, and the initial gas input rate was 50 m 3 / h, the auxiliary gas injection rate is 150m 3 / h), after 2 hours, the gas injection speed is 2m 3 Reduce to / h, and the auxiliary gas injection rate to 15m 3 The rate was reduced to / h. After cooling the product obtained by the reaction, it was finely separated to obtain submicron spherical silicon dioxide filler (D 50 silver 0.7μm) and nano-spherical silicon dioxide filler (D 50 silver 80nm) was obtained.

[0043] Example 2

[0044] 950g of D 50 Raw Si powder with a g of 300μm and 50g of D 50 Raw SiO2 powder with a particle size of 10 μm was homogenized and compounded in an air flow mixer for 3 hours to prepare a mixed raw material Si-SiO2. This mixed raw material was introduced into a high-temperature vessel filled with gas and oxygen to react (the input rate of the mixed raw material was 60 g / min, and the initial gas input rate was 50 m 3 / h, the auxiliary gas injection rate is 150m 3 / h), after 2 hours, the gas injection speed is 2m 3 Reduce to / h, and the auxiliary gas injection rate to 15m 3The rate was reduced to / h. After cooling the product obtained by the reaction, it was finely separated to obtain submicron spherical silicon dioxide filler (D 50 silver 0.4μm) and nano-spherical silicon dioxide filler (D 50 silver 60nm) was obtained.

[0045] Example 3

[0046] 800g of D 50 Raw material Al powder with a g of 15μm and 200g of D 50 Raw Al2O3 powder with a particle size of 30 nm was homogenized and compounded in a V-type mixer for 3 hours (while being protected by an inert gas) to prepare a mixed raw material Al-Al2O3. This mixed raw material was introduced into a high-temperature vessel filled with gas and oxygen to react (the input rate of the mixed raw material was 60 g / min, and the initial gas input rate was 50 m / min). 3 / h, the auxiliary gas injection rate is 150m 3 / h), after 2 hours, the gas injection speed is 2m 3 Reduce to / h, and the auxiliary gas injection rate to 15m 3 The rate was reduced to / h. After cooling the product obtained by the reaction, it was finely separated to obtain submicron spherical aluminum oxide filler (D 50 silver 0.2μm) and nano-spherical aluminum oxide filler (D 50 silver 50nm) was obtained.

[0047] Example 4

[0048] 700g of D 50 Raw material Al powder with a g of 15μm and 300g of D 50 Raw material Al2O3 powder with a diameter of 40 nm was introduced into high-temperature vessels filled with gas and oxygen, respectively, and reacted (the input rate of Al powder was 42 g / min, the input rate of Al2O3 powder was 18 g / min, and the initial input rate of gas was 50 m 3 / h, the auxiliary gas injection rate is 150m 3 / h), after 2 hours, the gas injection speed is 2m 3 Reduce to / h, and the auxiliary gas injection rate to 15m 3 The rate was reduced to / h. After cooling the product obtained by the reaction, it was finely separated to obtain submicron spherical aluminum oxide filler (D 50 silver 0.4μm) and nano-spherical aluminum oxide filler (D 50 silver 20nm) was obtained.

[0049] Comparative Example 1: Raw Material M Omitted

[0050] 1000g of D 50 Raw Si powder with a particle size of 12 μm is introduced into a high-temperature vessel rich in gas and oxygen and reacted (the Si powder input rate is 60 g / min, and the initial gas input rate is 50 m 3 / h, the auxiliary gas injection rate is 150m 3 / h), after 2 hours, the gas injection speed is 2m 3 Spherical silicon dioxide filler was manufactured by reducing the rate to / h, and D 50 It was 0.8μm.

[0051] Comparative Example 2: Increase the proportion of raw material O

[0052] 500g of D 50 Raw Si powder with a g of 35μm and 500g of D 50 Raw SiO2 powder with a particle size of 3.0 μm was homogenized and compounded at high speed in an air flow mixer for 3 hours to prepare a mixed raw material Si-SiO2. This mixed raw material was introduced into a high-temperature vessel filled with gas and oxygen to react (the input rate of the mixed raw material was 60 g / min, and the initial gas input rate was 50 m 3 / h, the auxiliary gas injection rate is 150m 3 / h), after 2 hours, the gas injection speed is 2m 3 Reduce to / h, and the auxiliary gas injection rate to 15m 3The rate was reduced to / h. After cooling the product obtained by the reaction, it was finely separated to obtain micron spherical silicon dioxide filler (D 50 silver 2.7μm) and nano-spherical silicon dioxide filler (D 50 silver 80nm) was obtained.

[0053] Comparative Example 3: Omission of gas velocity reduction operation

[0054] 700g of D 50 Raw Si powder with a g of 5μm and 300g of D 50 Raw SiO2 powder with a particle size of 0.1 μm was homogenized and compounded at high speed in an air flow mixer for 3 hours to prepare a mixed raw material Si-SiO2. This mixed raw material was introduced into a high-temperature vessel rich in gas and oxygen to react, with the input rate of the mixed raw material being 60 g / min and the gas input rate continuously being 50 m / min. 3 It was maintained at / h, and the auxiliary gas injection rate continued at 150m 3 It was maintained at / h. After cooling the product obtained by the reaction, it was finely separated to obtain submicron spherical silicon dioxide filler (D 50 silver 0.8μm) and nano-spherical silicon dioxide filler (D 50 silver 82nm) was obtained.

[0055] Comparative Example 4: Increasing the particle size of raw material M

[0056] 700g of D 50 Raw material Si with a g of 350μm and 300g of D 50 Mixed raw material Si-SiO2 was prepared by high-speed homogenization and coating of raw material SiO2 with a g of 6 μm in an air flow mixer for 3 hours. This mixed raw material was introduced into a high-temperature vessel filled with gas and oxygen to react (the input rate of the mixed raw material was 60 g / min, and the initial gas input rate was 50 m 3 / h, the auxiliary gas injection rate is 150m 3 / h), after 2 hours, the gas injection speed is 2m3 Reduce to / h, and the auxiliary gas injection rate to 15m 3 The rate was reduced to / h. After cooling the product obtained by the reaction, it was precisely separated into a gray product and D 50 A spherical silicon dioxide filler with a diameter of 60 nm was obtained.

[0057] Performance Test:

[0058] The present invention reduces the reaction activity of the raw materials by complex treatment of raw material M and raw material O, and the reaction activity of the raw materials is characterized using the explosion pressure ratio PR (Pressure ratio, the lower the value, the lower the risk). Since raw material M releases a large amount of heat when reacting with oxygen, the present invention reduces gas to reduce costs and controls the temperature balance inside the container to allow the reaction to proceed more gently. During the reaction process of Examples 1 to 4 and Comparative Examples 1 to 4, the temperature change of the inner wall of the container was monitored, and the particle size distribution was characterized by the particle size distribution of the spherical oxide filler obtained using a laser particlemeter.

[0059] The test results are shown in Table 1.

[0060] Table 1 Test results of Examples 1–4 and Comparative Examples 1–4

[0061]

[0062] According to Table 1, the following applies: (1) In Comparative Example 1, a single Si powder was used as a raw material. Due to the high PR value of the raw material, the reaction was violent and the risk to production safety was high. At the same time, while a submicron-level product could be obtained, it was difficult to obtain a nano-level product. (2) In Comparative Example 2, the proportion of raw material O was increased to 50%. Since the raw material O was not completely vaporized or dispersed, the particle size of Product 1 was coarse and micron-grade, making it difficult to obtain a submicron product. (3) In Comparative Example 3, because the gas was not lowered to the minimum level, product costs increased by 15–25%, and the temperature of the inner wall of the container rose by 15–30%, resulting in higher product costs and hindering continuous production. (4) In Comparative Example 4, the raw material Si powder reached a particle size of 350 μm. Since the reaction was incomplete in the high-temperature zone, it entered the product and turned the product gray.

[0063] In addition, when observing the appearance of the submicron-level and nano-level products obtained in Examples 1 to 4, it was confirmed that all were uniformly spherical.

[0064] The above description is merely a preferred embodiment of the present invention, and a person skilled in the art can make various improvements and modifications without departing from the principles of the present invention, and such improvements and modifications should also be considered within the scope of protection of the present invention.

Claims

Claim 1 A method for simultaneously manufacturing nano and submicron spherical oxide fillers, comprising the step of obtaining a combustion product by combusting a first raw material and a second raw material under conditions in which a gas and an auxiliary gas are present, wherein the first raw material is a metal element powder, a non-metal element powder, or an alloy powder, and the second raw material is an oxide or a composite oxide corresponding to the first raw material, wherein the particle size of the first raw material is 3 to 300 μm, the particle size of the second raw material is 30 nm to 10 μm, and the mass of the second raw material is 30% or less of the total mass of the first raw material and the second raw material, and wherein, after cooling the combustion product, a separation process is performed to obtain a submicron spherical oxide filler having an average particle size of 0.1 to 1.5 μm and a nano spherical oxide filler having an average particle size of 10 to 100 nm. Claim 2 A method for simultaneously manufacturing nano and submicron spherical oxide fillers, characterized in that, in the combustion reaction described in claim 1, the method of introducing the first raw material and the second raw material is to introduce them after mixing the first raw material and the second raw material, and the method of mixing the first raw material and the second raw material is dry mixing or liquid mixing. Claim 3 A method for simultaneously producing nano and submicron spherical oxide fillers according to claim 2, wherein the liquid mixture is characterized by mixing a first raw material, a second raw material, and a solvent, and then drying to obtain a mixed powder. Claim 4 A method for simultaneously producing nano and submicron spherical oxide fillers, characterized in that, in claim 3, the solvent is one or more of water, methanol, ethanol, acetone, and butanone, the drying temperature is within the range of 100 to 200°C, and the drying time is 2 to 30 hours. Claim 5 A method for simultaneously manufacturing nano and submicron spherical oxide fillers according to claim 2, wherein the equipment used for the dry mixing comprises a V-type mixer, a double cone mixer, a pneumatic mixer, a cone mixer, a high-speed mixer, or an air flow mixer. Claim 6 A method for simultaneously manufacturing nano and submicron spherical oxide fillers according to claim 2, characterized in that when the first raw material and the second raw material are mixed and then added, the addition speed is 1.7 g / min to 1020 g / min. Claim 7 A method for simultaneously producing nano and submicron spherical oxide fillers, characterized in that, in the combustion reaction of claim 1, when the first raw material and the second raw material are each introduced, the introduction rate of the first raw material is 1.7 g / min to 700 g / min, and the introduction rate of the second raw material is 250 g / min or less. Claim 8 A method for simultaneously producing nano and submicron spherical oxide fillers according to claim 1, characterized in that, during the combustion reaction, the gas inflow rate is lowered to 2% to 10% of the initial inflow rate after the temperature inside the reactor has stabilized, and the temperature is considered stable when the upper and lower fluctuations of the temperature inside the reactor do not exceed 10℃. Claim 9 In claim 1 or 8, the initial inflow velocity of the gas is 50 m 3 The rate is / h, and after the temperature inside the reactor stabilizes, the gas inflow velocity is 2m 3 A method for simultaneously producing nano and submicron spherical oxide fillers characterized by being reduced to / h. Claim 10 A method for simultaneously producing nano and submicron spherical oxide fillers, characterized in that, in claim 1, the metal element powder comprises one or more of aluminum, magnesium, iron, copper, titanium, zirconium, and zinc, the non-metal element powder is silicon, and the alloy powder comprises one or more of aluminum-iron alloy, aluminum-silicon alloy, aluminum-magnesium alloy, magnesium alloy, and silicon-iron alloy powder. Claim 11 A method for simultaneously producing nano and submicron spherical oxide fillers, wherein the separation method comprises one or more of cyclone classification, airflow classification, overflow classification, and sieve classification. Claim 12 A method for simultaneously producing nano and submicron spherical oxide fillers, characterized in that, in claim 1 or 8, the gas comprises one or more of hydrogen, liquefied natural gas, liquefied petroleum gas, acetylene, and propane, and the auxiliary gas comprises one or two of oxygen and air. Claim 13 delete

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