Spinel-perovskite dual-phase high-entropy ceramic powder material and preparation method thereof

Abstract

The application relates to a spinel-perovskite dual-phase high-entropy ceramic powder material, which has a chemical formula AMn x O y wherein A is three transition metal elements selected from Cu, Ni, Co, Zn and Mg and one rare earth element selected from La, Pr and Nd, the elements are in equal molar ratio, 1 < x < 2 and 3 < y < 4, the material has a face-centered cubic crystal structure spinel phase and a perovskite phase. Meanwhile, the application also discloses a preparation method of the high-entropy ceramic powder material. The high-entropy ceramic powder material has the characteristics of two-phase coexistence, high purity, small particle size (100-400 nm) and uniform element distribution, and has excellent solar absorptivity (>0.87), infrared emissivity (>0.90) and high-temperature thermal stability (1600 DEG C), and can be widely used in the field of high-temperature thermal radiation, including aerospace, industrial kiln, power station boiler and the like, as an infrared radiation material and a solar energy absorption material.

Description

TECHNICAL FIELD

[0001] The present application relates to the field of infrared radiation heating / cooling materials and solar energy absorbing materials, in particular to a spinel-perovskite dual-phase high-entropy ceramic powder material and a preparation method thereof. BACKGROUND

[0002] As a new star in the field of ceramics, high-entropy ceramics not only have simple structure and excellent performance, but also have unique high-entropy effect similar to high-entropy alloys, which has attracted extensive attention of domestic researchers. The design concept of high-entropy comes from high-entropy alloys, that is, the use of multi-component solid solution to increase the configurational entropy in the system, thereby reducing the Gibbs free energy, and ultimately improving the stability of the phase structure. In 2015, Rost et al. prepared high-entropy oxides [(Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )O] for the first time, introducing the concept of "high-entropy" from the alloy field to the inorganic non-metal field (C.M. Rost, E. Sachet, T. Borman, A. Moballegh, E.C. Dickey, D Hou, J.L. Jones, S. Curtarolo, J.-P. Maria, Nat. Commun. 6 (2015) 8485.). At present, a large number of researches have been carried out on high-entropy materials. With the help of high entropy value, low Gibbs free energy and a large number of lattice distortions, high-entropy materials exhibit excellent performance in electricity, light, magnetism and other aspects, and their application range can cover almost the entire industrial field such as high temperature and high heat, energy and battery, catalysis, machinery and wave absorption.

[0003] At present, the high-entropy ceramic materials with solar energy absorption / infrared radiation performance reported in the literature at home and abroad or published in Chinese invention patents are mostly spinel phase single-phase materials. In 2021, Gao Xianghu et al. applied for a Chinese invention patent (application publication number CN202110799888.X) "Preparation method of high-entropy oxide with good infrared radiation performance", which used a method combining mechanical wet grinding and solid phase synthesis to prepare single-phase spinel phase high-entropy oxide, which had high infrared emissivity and good thermal stability.

[0004] In recent years, a variety of dual-phase high-entropy ceramic materials have been reported. In 2022, G Dai et al. prepared a dual-phase high-entropy oxide material (Fe 0.2x , Co 0.2 , Ni 0.2 , Cr 0.2 , Mn 0.2)3O4(x=1~5), spinel phase and alloy phase coexist, specifically, first, Fe2O3, Co3O4, NiO, Cr2O3 and MnO2 with a molar ratio of x:1:1:1:1 are mixed uniformly by mechanical ball milling method, sieved and uniaxially pressed into a disc under a pressure of 30 MPa, then heated to 1000℃ at a heating rate of 10℃ / min under hydrogen atmosphere and calcined for 3 hours, finally the sample is cooled to room temperature with the furnace to obtain the dual-phase high-entropy oxide (G. Dai, R. Deng, T. Zhang, et al. Quantitative evaluation of loss capability for in situ conductive phase enhanced microwave absorption of high-entropy transition metal oxides[J]. Adv. Funct. Mater. 2022, 32, 2205325). Feng Jing et al. applied for a Chinese invention patent (application publication number CN 114773059 A) “A symbiotic dual-phase high-entropy ceramic and its preparation method and application”, which adopts ball milling method and spark plasma sintering process to prepare the dual-phase high-entropy ceramic material. However, at present, there is no report on the preparation of spinel / perovskite dual-phase high-entropy ceramic material by solid phase synthesis method. SUMMARY

[0005] The technical problem to be solved by the present application is to provide a spinel-perovskite dual-phase high-entropy ceramic powder material with good performance.

[0006] Another technical problem to be solved by the present application is to provide a preparation method of the spinel-perovskite dual-phase high-entropy ceramic powder material.

[0007] To solve the above problems, the spinel-perovskite dual-phase high-entropy ceramic powder material according to the present application has the following characteristics: the chemical formula of the dual-phase high-entropy ceramic powder material is AMn x O y , wherein A is three transition metal elements selected from Cu, Ni, Co, Zn and Mg and one rare earth element selected from La, Pr and Nd, and each element is in equimolar ratio, 1<x<2, 3<y<4, and it has a face-centered cubic crystal structure spinel phase and a perovskite phase.

[0008] The solar absorption rate of the dual-phase high-entropy ceramic powder material is greater than 0.87 in the range of 0.3~2.5μm, and the infrared emissivity is greater than 0.90 in the range of 2~22μm.

[0009] The particle size of the dual-phase high-entropy ceramic powder material is in the range of 100-400 nm.

[0010] A preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material as described above, comprising the following steps:

[0011] Step 1: taking AOx powder and MnO2 powder as raw materials, the molar ratio of metal elements being 1:4-8, the AOx being one of CuO, NiO, CoO, ZnO and MgO powder, and the La2O3, Pr6O 11 , Nd2O3 powder, and each element being in an equimolar ratio; the raw materials are mixed by ball milling, dried, and ground to obtain a mixture powder;

[0012] Step 2: the mixture powder is subjected to staged calcination in an air atmosphere, and is cooled and ground to obtain a high-entropy ceramic powder material having a spinel and perovskite dual-phase coexisting structure.

[0013] The ball milling condition in step 1 refers to ball milling by using a planetary ball mill, the ball milling solvent being ultrapure water, the ball milling rotation speed being 300-500 r / min, the ball milling time being 5-10 hours, and the mass ratio of ball, solvent and water being 2-5:1:3.

[0014] The drying condition in step 1 refers to a temperature of 80-100℃ and a drying time of 12-24 hours.

[0015] The staged calcination condition in step 2 refers to first heating at 5 ℃ / min to 500 ℃, and then continuously heating at 2-5 ℃ / min, the calcination temperature range being 500-1400℃, and the calcination time being 1-10 hours.

[0016] The cooling mode in step 2 is one of furnace cooling, air quenching cooling and liquid nitrogen quenching cooling.

[0017] Compared with the prior art, the present application has the following advantages:

[0018] 1. The high-entropy ceramic material has two crystal structure compositions of cubic spinel phase and perovskite phase, wherein the spinel phase is of Fd-3m space group, the A ion is in a coordination structure with 4 oxygen ions and located in a tetrahedral gap, and the B ion is in a coordination structure with 6 oxygen atoms and located in an octahedral gap; the perovskite phase is of Pbnm space group, the A site is a rare earth element, the cation is in a 12-coordination structure and located in a cavity composed of octahedrons; the B site is a transition metal element, and the transition metal ion forms an octahedral coordination with six oxygen ions. The two phases coexist and can inhibit the growth of crystal grains, so that the ceramic particles have a smaller size (100-400 nm), and have the characteristics of high purity, stable phase structure and uniform element distribution.

[0019] 2. The high-entropy ceramic material has high-temperature-resistant rare earth elements introduced and high-entropy design at A sites, the configurational entropy of the high-entropy ceramic material increases with the introduction of the main components, thereby reducing the Gibbs free energy, and the high-entropy ceramic material has excellent thermal stability and high infrared emissivity (above 0.90) after long-time high-temperature calcination, and the highest use temperature can reach 1600 DEG C.

[0020] 3. The high-entropy ceramic material has high infrared emissivity in air, and the emissivity reaches above 0.9 in the 2-22 mu m wave band, and the solar absorptivity reaches above 0.87 in the 0.3-2.5 mu m wave band. Compared with the single-phase spinel high-entropy ceramic, the above-mentioned double-phase high-entropy ceramic material has higher solar absorptivity and infrared emissivity, and the reasons mainly include the following points:

[0021] (1) The rare earth elements are introduced, and the perovskite structure is formed with the Mn elements, the serious lattice distortion is caused by the ion radius difference of multiple elements, the lattice asymmetric vibration is increased, the vibration absorption is enhanced, and thereby the solar absorptivity and infrared emissivity in the middle infrared wave band (2-22 mu m) are improved;

[0022] (2) The impurity energy level is formed near the Fermi level by doping ions with different valence states and valence bond structures, transition metal elements 3d orbits and rare earth elements 4f orbits, the concentration of free carriers (electrons and holes) in the valence band and the f-electron layer transition (f-f) and interlayer transition (f-d) are enhanced, the intrinsic band gap of the double-phase high-entropy ceramic material is effectively reduced (<0.26 eV), and thereby the solar absorptivity and infrared emissivity in the near-infrared wave band (0.3-2.5 mu m) are improved;

[0023] (3) The double-phase high-entropy material belongs to a nano material, the size is small (100-400 nm), the number of grain boundaries is increased, the defect structure is increased, and the selectivity to thermal radiation is reduced. The spinel and perovskite phases coexist, and the solar absorptivity and infrared emissivity of the material can be significantly improved by the synergistic effect.

[0024] 4. The high-entropy ceramic material is calcined by mechanical wet grinding and solid-phase synthesis, the metal elements can be fully mixed, the operation is simple, the production cycle is short, and the industrial production can be realized, and the obtained material can be widely used in the field of high-temperature thermal radiation, including aerospace, industrial kiln, power station boiler and the like. BRIEF DESCRIPTION OF DRAWINGS

[0025] The specific embodiments of the present application will be further described in detail below with reference to the accompanying drawings.

[0026] Figure 1XRD pattern of the present application example 1 (Cu, Ni, La, Mg)Mn x O y .

[0027] Figure 2 XRD pattern of the present application example 2 (Cu, Zn, Nd, Co)Mn x O y .

[0028] Figure 3 XRD pattern of the present application example 3 (Cu, Ni, La, Co)Mn x O y .

[0029] Figure 4 EDS result of the present application example 3 (Cu, Ni, La, Co)Mn x O y .

[0030] Figure 5 SEM result of the present application example 3 (Cu, Ni, La, Co)Mn x O y .

[0031] Figure 6 Solar absorption spectrum of the present application example 3 (Cu, Ni, La, Co)Mn x O y in 0.3-2.5 μm waveband.

[0032] Figure 7 XRD pattern of the present application example 3 (Cu, Ni, La, Co)Mn x O y after thermal stability test.

[0033] Figure 8 XRD result of the present application example 4 (Cu, Ni, Pr, Co)Mn x O y . DETAILED DESCRIPTION

[0034] A spinel-perovskite dual-phase high-entropy ceramic powder material, the chemical formula of the dual-phase high-entropy ceramic powder material is AMn x O y , wherein A is three transition metal elements in Cu, Ni, Co, Zn, Mg and one rare earth element in La, Pr, Nd, and each element is in equimolar ratio, 1

[0035] The solar absorption rate of the dual-phase high-entropy ceramic powder material is greater than 0.87 in the range of 0.3-2.5 μm, and the infrared emissivity is greater than 0.90 in the range of 2-22 μm. The particle size is in the range of 100-400 nm.

[0036] A preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material, comprising the following steps:

[0037] Step 1: taking AOx powder and MnO2 powder as raw materials, the molar ratio of metal elements being 1:4-8, AOx being three of CuO, NiO, CoO, ZnO and MgO powder, and one of La2O3, Pr6O 11 , and Nd2O3 powder, and each element being in an equimolar ratio; each raw material is mixed by a planetary ball mill, the ball milling solvent being ultrapure water, the ball milling rotation speed being 300-500 r / min, the ball milling time being 5-10 hours, and the mass ratio (g / g) of ball milling water being 2:1:3. Then, after drying at 80-100 ℃ for 12-24 hours, the mixture powder is obtained by grinding.

[0038] Step 2: the mixture powder is calcined in air atmosphere, the temperature is raised to 500 ℃ at a rate of 5 ℃ / min, and then the temperature is continuously raised at a rate of 2-5 ℃ / min, the calcination temperature range being 500-1400 ℃, and the calcination time being 1-10 hours. After calcination, one of furnace cooling, air quenching and liquid nitrogen quenching is used for cooling, and the high-entropy ceramic powder material with spinel and perovskite dual-phase coexisting structure is obtained by grinding.

[0039] Example 1

[0040] A preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material, comprising the following steps:

[0041] Step 1: CuO (0.9944 g), MgO (0.5038 g), La2O3 (2.0366 g), NiO (0.9336 g) and MnO2 (4.347 g) powder are weighed in a molar ratio of 1:1:1:1:4, respectively, and mixed by a planetary ball mill, the ball milling solvent being ultrapure water, the mass ratio (g / g) of ball milling water being 2:1:3, 1 hour of ball milling is first performed at a rotation speed of 300 r / min, then the ball milling is paused for 10 min, which is one ball milling cycle, 1 hour of ball milling is then performed at a rotation speed of 300 r / min, and the ball milling is repeated for a total of 5 hours. Then, after drying at 80-100 ℃ for 12-24 hours, the mixture powder is obtained by grinding.

[0042] Step 2: The mixture powder is calcined in air atmosphere, the temperature is raised to 500 ℃ at a rate of 5 ℃ / min, and the calcination time is 1 hour. After the calcination is completed, the furnace is cooled down, and the dual-phase (Cu, Ni, La, Mg)Mn x O y High-entropy ceramic powder material, 1 < x < 2, 3 < y < 4.

[0043] The obtained (Cu, Ni, La, Mg)Mn x O y The high-entropy ceramic powder material is subjected to X-ray diffraction test, and the result is shown in FIG. 2. The spectrum is very consistent with the crystal form of the CuMn2O4 spectrum (PDF #34-1400) with a spinel structure and the LaCrO3 spectrum (PDF #24-1016) with a perovskite structure in the ICDD database (the LaCrO3 spectrum represents a class of perovskite structures), indicating that the high-entropy ceramic material prepared in the embodiment coexists with spinel and perovskite structures, and the dual-phase coexists. Figure 1

[0044] A Lambda 950 ultraviolet / visible / near-infrared spectrophotometer (with a 150 mm integrating sphere) manufactured by PerkinElmer Company of the United States is used to evaluate the solar absorptivity of the material, the absorptivity of the material in the 0.3-2.5 μm wave band is measured, and then the solar absorptivity is calculated according to the calculation formula in the international standard ISO 9845-1 (1992). A TSS-5X-2 infrared emissivity detector manufactured by Senor Company of Japan is used to evaluate the infrared emissivity of the material, and the normal infrared emissivity of the material in the 2-22 μm wave band is measured. The dual-phase high-entropy ceramic powder material is placed in an air atmosphere of a box furnace, and a thermal stability experiment is performed at 1600 ℃ for 200 h.

[0045] 0.2 g (Cu, Ni, La, Mg)Mn x O y The high-entropy ceramic powder material is measured to have a normal infrared emissivity of 0.90 in the 2-22 μm wave band and a solar absorptivity of 0.871 in the 0.3-2.5 μm wave band; after the thermal stability experiment, the material is measured to have a normal infrared emissivity of 0.91 in the 2-22 μm wave band and a solar absorptivity of 0.878 in the 0.3-2.5 μm wave band.

[0046] Example 2

[0047] A preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material, comprising the following steps:

[0048] ​Step 1: Weigh out CuO (0.9944 g), CoO (0.9366 g), Nd₂O₃ (2.1030 g), ZnO (1.0174 g), and MnO₂ (6.5200 g) powders with a metal atomic molar ratio of 1:1:1:1:6. Mix them using a planetary ball mill with ultrapure water as the milling solvent. The mass ratio of ball to material to water (g / g) is 2:1:3. Mill for 1 hour at 400 r / min, then pause for 10 minutes, completing one milling cycle. Repeat this 10-minute pause for another hour at 400 r / min, for a total of 5 hours. Then dry the mixture at 80-100℃ for 12-24 hours before grinding to obtain the final powder mixture.

[0049] Step 2: The mixed powder was calcined in stages in air atmosphere, with the temperature increased to 500℃ at a rate of 5℃ / min, followed by a further increase at a rate of 2℃ / min, maintaining a calcination temperature range of 800℃ for 3 hours. After calcination, the powder was cooled in the furnace and ground to obtain the biphase (Cu, Zn, Nd, Co)Mn. x O y High-entropy ceramic powder materials, 1 <x<2,3<y<4。

[0050] The obtained (Cu, Zn, Nd, Co)Mn x O y X-ray diffraction testing was performed on the high-entropy ceramic powder material, and the results are as follows: Figure 2 As shown, the spectral line is in very good agreement with the crystal structure of CuMn2O4 (PDF#34-1400) with spinel structure and LaCrO3 (PDF#24-1016) with perovskite structure in the ICDD database (LaCrO3 spectral line represents a type of perovskite structure), indicating that the high-entropy ceramic material prepared in this embodiment has a two-phase coexistence structure.

[0051] The absorptivity in the 0.3~2.5 μm band, the normal infrared emissivity in the 2~22 μm band, and the thermal stability experiments were the same as in Example 1.

[0052] Take 0.2 g of (Cu, Zn, Nd, Co)Mn x O y The high-entropy ceramic powder material has a normal infrared emissivity of 0.90 in the 2-22 μm wavelength range and a solar energy absorptivity of 0.875 in the 0.3-2.5 μm wavelength range. After thermal stability testing, the high-entropy ceramic powder material has a normal infrared emissivity of 0.90 in the 2-22 μm wavelength range and a solar energy absorptivity of 0.878 in the 0.3-2.5 μm wavelength range.

[0053] Example 3

[0054] A preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material, comprising the following steps:

[0055] Step 1: CuO (0.9944 g), CoO (0.9366 g), La2O3 (2.0366 g), NiO (0.9336 g) and MnO2 (8.693 g) powders are weighed in a molar ratio of 1:1:1:1:8, respectively, and are mixed by a planetary ball mill, with ultrapure water as the ball milling solvent, a mass ratio (g / g) of ball to water of 2:1:3, 1 hour of ball milling at a speed of 500 r / min, then a pause of 10 min, and then 1 hour of ball milling at a speed of 500 r / min, for a total of 10 hours of ball milling. After drying at 80-100℃ for 12-24 hours, the mixture powder is obtained.

[0056] Step 2: The mixture powder is calcined in air in stages, with a temperature rise of 5 ℃ / min to 500 ℃, and then a temperature rise of 4 ℃ / min, a calcination temperature range of 1400℃, and a calcination time of 10 hours. After cooling in the furnace, the dual-phase (Cu, Ni, La, Co)Mn x O y High-entropy ceramic powder material, 1 < x < 2, 3 < y < 4.

[0057] The obtained (Cu, Ni, La, Co)Mn x O y High-entropy ceramic powder material is subjected to X-ray diffraction testing, and the results are shown in Figure 3 The spectrum is very consistent with the crystal form of the CuMn2O4 spectrum (PDF#34-1400) with a spinel structure and the LaCrO3 spectrum (PDF#24-1016) with a perovskite structure in the ICDD database (the LaCrO3 spectrum represents a class of perovskite structures), indicating that the dual-phase coexistence structure of the high-entropy ceramic material prepared in this embodiment is obtained.

[0058] Figure 4 The SEM image of the (Cu, Ni, La, Co)Mn x O y High-entropy ceramic powder material is shown in the SEM image, and the powder particle size is between 200-500 nm.

[0059] Figure 5 The SEM image of the (Cu, Ni, La, Co)Mn x O yThe EDS result of the high-entropy ceramic powder material shows that the molar ratio of each metal element in the material conforms to the original component design, and is a typical high-entropy compound state.

[0060] The absorption rate in the 0.3-2.5 μm wave band, the normal infrared emissivity in the 2-22 μm wave band, and the thermal stability experiment are the same as in Embodiment 1.

[0061] 0.2 g (Cu, Ni, La, Co)Mn x O y The high-entropy ceramic powder material has a normal infrared emissivity of 0.93 in the 2-22 μm wave band and a solar energy absorption rate of 0.905 in the 0.3-2.5 μm wave band. After the thermal stability experiment, the material has a normal infrared emissivity of 0.92 in the 2-22 μm wave band and a solar energy absorption rate of 0.912 in the 0.3-2.5 μm wave band.

[0062] Figure 6 (Cu, Ni, La, Co)Mn x O y The solar energy absorption spectrum of the high-entropy ceramic powder material in the 0.3-2.5 μm wave band shows that the dual-phase high-entropy ceramic has a high solar energy absorption rate in the wave band.

[0063] Figure 7 (Cu, Ni, La, Co)Mn x O y The XRD patterns of the high-entropy ceramic powder material before and after the 1600℃ thermal stability experiment show that the dual-phase high-entropy material does not change phase after the 1600℃ thermal stability experiment, indicating that the material has good thermal stability, which is due to the large configurational entropy in the high-entropy effect, making the material form a stable solid solution structure.

[0064] Embodiment 4

[0065] A preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material, comprising the following steps:

[0066] Step 1: CuO (0.9944 g), CoO (0.9366 g), Pr6O 11Powders of NiO (2.1280 g), NiO (0.9336 g), and MnO2 (8.693 g) were ball-milled using a planetary ball mill with ultrapure water as the milling solvent. The mass ratio of ball to powder (g / g) was 2:1:3. The milling was performed for 1 hour at 500 r / min, followed by a 10-min pause, constituting one milling cycle. This was repeated for another hour at 500 r / min, for a total of 5 hours of milling. The mixture was then dried at 80–100℃ for 12–24 hours and then ground to obtain the final powder.

[0067] Step 2: The mixed powder was calcined in stages in air atmosphere, with the temperature increased to 500℃ at a rate of 5℃ / min, followed by a further increase at a rate of 4℃ / min, for a total calcination temperature range of 1000℃ and a calcination time of 5 hours. After calcination, the powder was cooled in the furnace and ground to obtain the two-phase (Cu, Ni, Pr, Co)Mn. x O y High-entropy ceramic powder materials, 1 <x<2,3<y<4。

[0068] The obtained (Cu, Ni, Pr, Co)Mn x O y X-ray diffraction testing was performed on the high-entropy ceramic powder material, and the results are as follows: Figure 8 As shown, the spectral line is in very good agreement with the crystal structure of CuMn2O4 (PDF#34-1400) with spinel structure and LaCrO3 (PDF#24-1016) with perovskite structure in the ICDD database (LaCrO3 spectral line represents a type of perovskite structure), indicating that the high-entropy ceramic material prepared in this embodiment has a two-phase coexistence structure.

[0069] The absorptivity in the 0.3~2.5 μm band, the normal infrared emissivity in the 2~22 μm band, and the thermal stability experiments were the same as in Example 1.

[0070] Take 0.2 g of (Cu, Ni, Pr, Co)Mn x O y The high-entropy ceramic powder material has a normal infrared emissivity of 0.92 in the 2-22 μm band and a solar absorptivity of 0.895 in the 0.3-2.5 μm band. After thermal stability testing, the material has a normal infrared emissivity of 0.91 in the 2-22 μm band and a solar absorptivity of 0.915 in the 0.3-2.5 μm band.

[0071] In summary, the material obtained in Examples 1-4 has an infrared emissivity of 0.90 or more in the 2-22 μm band, and a solar absorptivity of 0.87-0.92 in the 0.3-2.5 μm band. Long-term thermal stability experiments show that the crystal structure of the material is stable, and the fluctuations in solar absorptivity and infrared emissivity are about 0.01-0.02. The above data show that the high-entropy ceramic powder material prepared by the present application has high solar absorptivity and infrared emissivity, and good thermal stability in air, thus ensuring the light-heat conversion efficiency of the solar absorber material and the heating / cooling efficiency of the infrared radiation material.

[0072] The above merely illustrates the best embodiments of the present application, but should not be understood as limiting the claims. The present application is not limited to the above embodiments, and the specific structure allows variations. Any variations made within the protection scope of the independent claims of the present application are within the protection scope of the present application.

Claims

1. A spinel-perovskite dual-phase high-entropy ceramic powder material, characterized in that: The chemical formula of the dual-phase high-entropy ceramic powder material is AMn x O y , where the A site is composed of three transition metal elements selected from Cu, Ni, Co, Zn, Mg and one rare earth element selected from La, Pr, Nd, and the elements are in equimolar ratio, 1 < x < 2, 3 < y < 4, and it has a face-centered cubic crystal structure spinel phase and perovskite phase; the solar absorptance of the dual-phase high-entropy ceramic powder material is greater than 0.87 in the range of 0.3 - 2.5 μm, and the infrared emissivity is greater than 0.90 in the range of 2 - 22 μm; and it still has a relatively high infrared emissivity of more than 0.90 after long-term high-temperature calcination, and the maximum service temperature can reach 1600 °C; the particle size of the dual-phase high-entropy ceramic powder material is in the range of 100 - 400 nm.

2. The preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material as described in claim 1, comprising the following steps: Step 1: Using AOx powder and MnO2 powder with a metal element molar ratio of 1:4~8 as raw materials, AOx is three of CuO, NiO, CoO, ZnO, and MgO powders, and La2O3 and Pr6O. 11 The raw materials are one of Nd2O3 powder, and the elements are in equimolar ratio; the raw materials are ball-milled, dried and ground to obtain the mixture powder. Step 2: The mixed powder is calcined in stages in an air atmosphere, and after cooling and grinding, a high-entropy ceramic powder material with a dual-phase structure of spinel and perovskite is obtained.

3. The method for preparing a spinel-perovskite dual-phase high-entropy ceramic powder material as described in claim 2, characterized in that: The conditions for ball milling in step 1 refer to using a planetary ball mill, using ultrapure water as the ball milling solvent, a ball milling speed of 300-500 r / min, a ball milling time of 5-10 hours, and a ball-to-water mass ratio of 2-5:1:

3.

4. The preparation method of a spinel-perovskite dual-phase high-entropy ceramic powder material as described in claim 2, characterized in that: The drying conditions in step 1 refer to a temperature of 80~100℃ and a drying time of 12~24 hours.

5. The method for preparing a spinel-perovskite dual-phase high-entropy ceramic powder material as described in claim 2, characterized in that: The conditions for segmented calcination in step 2 are as follows: first, the temperature is increased to 500℃ at a rate of 5℃ / min, and then the temperature is increased at a rate of 2~5℃ / min. The calcination temperature range is 500~1400℃, and the calcination time is 1~10 hours.

6. The method for preparing a spinel-perovskite dual-phase high-entropy ceramic powder material as described in claim 2, characterized in that: The cooling method in step 2 is one of furnace cooling, air quenching cooling, and liquid nitrogen quenching cooling.

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