Cs2AgCl3 full-inorganic lead-free perovskite and green and efficient synthesis method thereof

Abstract

The invention discloses a Cs2AgCl3 full-inorganic lead-free perovskite and a green and efficient synthesis method thereof, and the green and efficient synthesis method comprises the following steps: mixing a CsCl aqueous solution with AgCl, and then carrying out ultrasonic dispersion and drying to obtain the Cs2AgCl3 full-inorganic lead-free perovskite. The synthesis method has the characteristics of greenness, high efficiency, simplicity and convenience in operation and mild reaction conditions, a large amount of pure-phase all-inorganic lead-free perovskite Cs2AgCl3 can be synthesized at normal temperature and normal pressure, and a new method is provided for synthesizing pure-phase substances.

Description

Technical Field

[0001] The invention relates to a metal halide perovskite composition, and in particular to a Cs2AgCl3 all-inorganic non-lead perovskite and a green and efficient synthesis method thereof. Background Art

[0002] Silver-based metal halide materials Cs-Ag-X (X = Cl, Br, I) present a 0D / 1D / 2D crystal structure similar to Cs-Cu-X in molecular dimensions, and have potential application prospects in the fields of ionic conductivity and photonic crystals. In addition, silver-based electrical contact materials have been widely used in electrical contact materials due to their unique excellent properties. The research and application of silver-based metal halide materials are constantly progressing, showing great potential in the field of optoelectronic devices.

[0003] Traditional methods for synthesizing non-lead metal halide materials, such as high-temperature solid-phase synthesis, solvothermal method, and organic solvent-assisted synthesis, can produce materials with excellent performance, but these methods often rely on toxic organic solvents, which not only pollutes the environment, but also makes the synthesis process complicated and costly. Therefore, the development of a green and sustainable synthesis strategy is crucial for the practical application of non-lead metal halide materials. In this context, aqueous phase synthesis has emerged as an environmentally friendly synthesis strategy. Due to its advantages such as simple operation, low cost, and environmental friendliness, aqueous phase synthesis is considered to be an ideal synthesis method. As a solvent, water has the characteristics of high heat capacity, high solubility, and easy handling, which gives it unique advantages in the synthesis process. The aqueous phase synthesis method uses water as a solvent and can synthesize a variety of metal halide materials by precisely controlling the reaction conditions, such as pH, temperature, and reaction time. Compared with traditional organic solvents, the aqueous phase synthesis method is not only environmentally friendly, but also can reduce the use of harmful solvents and reduce production costs, while improving the stability and adjustability of materials, providing a new way for the preparation of non-lead metal halide materials. Summary of the invention

[0004] The purpose of the present invention is to provide a Cs2AgCl3 all-inorganic non-lead perovskite and a green and efficient synthesis method thereof. The synthesis method is green and efficient, easy to operate, and has mild reaction conditions. The pure phase all-inorganic non-lead perovskite Cs2AgCl3 can be synthesized in large quantities at room temperature and pressure.

[0005] The technical solution of the present invention is as follows:

[0006] A green and efficient synthesis method for Cs2AgCl3 all-inorganic non-lead perovskite comprises the following steps: mixing a CsCl aqueous solution with AgCl powder in a molar ratio of 2:1 to form an aqueous solution with a precipitate, ultrasonically dispersing the solution at room temperature, and drying the solution, wherein the ultrasonic dispersion time is 10 to 30 minutes.

[0007] In some preferred implementations, the concentration of the CsCl aqueous solution is 0.5 to 4 mol / L.

[0008] In some preferred implementations, the drying temperature is 30 to 70 degrees Celsius.

[0009] In some preferred implementations, the green and efficient synthesis method further comprises grinding into microcrystals with an agate mortar after drying, collecting, and storing in a drying oven.

[0010] In some preferred implementations, the purity of CsCl is ≥99.999%, and the purity of AgCl is ≥99.99%.

[0011] In some preferred implementations, the solvent of the CsCl aqueous solution is deionized water.

[0012] A Cs2AgCl3 all-inorganic non-lead perovskite is prepared by the above-mentioned green and efficient synthesis method, has a space group of Pnma, and belongs to the orthorhombic crystal system.

[0013] The present invention has at least the following beneficial effects:

[0014] 1. The present invention does not require the addition of any solvent other than water, nor does it require any large-scale equipment, and is green and environmentally friendly.

[0015] 2. The synthesis method of the present invention is simple and easy to realize industrial large-scale production, providing a new method for synthesizing pure phase substances.

[0016] 3. The Cs2AgCl3 all-inorganic non-lead perovskite prepared by the above method can be excited by 258-nanometer ultraviolet light at room temperature, emitting a peak at 610 nanometers, covering broadband luminescence characteristics from 400 to 850 nanometers. BRIEF DESCRIPTION OF THE DRAWINGS

[0017] Figure 1 The X-ray diffraction pattern of the Cs2AgCl3 all-inorganic non-lead perovskite prepared in Example 1;

[0018] Figure 2 The photoluminescence spectrum of the Cs2AgCl3 all-inorganic non-lead perovskite prepared in Example 1;

[0019] Figure 3 The diffuse reflectance spectrum of the Cs2AgCl3 all-inorganic non-lead perovskite prepared in Example 1;

[0020] Figure 4 The X-ray diffraction patterns of Cs2AgCl3 all-inorganic non-lead perovskite prepared at different drying temperatures in Example 2;

[0021] Figure 5 The photoluminescence spectra of Cs2AgCl3 all-inorganic non-lead perovskite prepared at different drying temperatures in Example 2;

[0022] Figure 6 The X-ray diffraction patterns of Cs2AgCl3 all-inorganic non-lead perovskite prepared in Example 3 at different CsCl aqueous solution concentrations;

[0023] Figure 7 The photoluminescence spectra of Cs2AgCl3 all-inorganic non-lead perovskite prepared in Example 3 at different CsCl aqueous solution concentrations. DETAILED DESCRIPTION

[0024] The technical solution of the present invention is further illustrated and described below through specific implementation methods.

[0025] In the following examples, the water used can be one or more of distilled water, purified water, and drinking water; unless otherwise specified, the detection methods in the following examples are conventional detection methods; unless otherwise specified, the reagents in the following examples are purchased from commercial channels. Hereinafter, Cs2AgCl3 all-inorganic non-lead perovskite is referred to as Cs2AgCl3.

[0026] Example 1

[0027] S1. Dissolve 3.3 mmol of CsCl in 5 ml of deionized water to form a 0.66 mol / L CsCl aqueous solution.

[0028] S2. Mix 3 ml of 0.66 mol / L CsCl aqueous solution and 1 mmol of AgCl powder in a clean glass bottle to form an aqueous solution with a precipitate, and disperse it under ultrasound for 30 minutes.

[0029] S3. Dry the obtained aqueous solution with precipitate in an oven at 50 degrees Celsius for 6 hours. After drying, grind into microcrystals using an agate mortar, collect, and store in a drying oven.

[0030] This embodiment is the best embodiment.

[0031] The Cs2AgCl3 material obtained by the present invention is subjected to X-ray diffraction spectrum, photoluminescence spectrum and diffuse reflectance spectrum tests. The X-ray diffraction spectrum of the product is as follows: Figure 1 As shown. Figure 1It can be seen that the material can synthesize Cs2AgCl3 at 50 degrees Celsius; the photoluminescence spectrum is as follows Figure 2 As shown, the luminescence center is 618 nanometers and the half-peak width is 235 nanometers; the diffuse reflectance spectrum is as follows Figure 3 As shown, the material has certain light absorption characteristics between 200 and 450 nanometers.

[0032] Example 2

[0033] S1. Dissolve 3.3 mmol of CsCl in 5 ml of deionized water to form a 0.66 mol / L CsCl aqueous solution.

[0034] S2. Mix 3 ml of 0.66 mol / L CsCl aqueous solution and 1 mmol of AgCl powder in a clean glass bottle to form an aqueous solution with a precipitate, and disperse it under ultrasound for 30 minutes.

[0035] S3. Dry the obtained aqueous solution with precipitate in an oven at 30 degrees Celsius, 40 degrees Celsius, 50 degrees Celsius, 60 degrees Celsius and 70 degrees Celsius for 6 hours. After drying, grind into microcrystals using an agate mortar, collect, and store in a drying oven.

[0036] The Cs2AgCl3 material obtained by the present invention is subjected to X-ray diffraction and photoluminescence spectrum tests. The X-ray diffraction spectrum of the product is as follows: Figure 4 As shown. Figure 4 It can be seen that the material can synthesize Cs2AgCl3 at 30 to 70 degrees Celsius; the photoluminescence spectrum is shown in Figure 5 As shown by Figure 5 It can be seen that the photoluminescence intensity of the product is the strongest at 50 degrees Celsius. Therefore, the optimal temperature for drying water is 50 degrees Celsius.

[0037] Example 3

[0038] S1. Dissolve 20 mmoles of CsCl in 5 ml of deionized water to form a 4 mol / L CsCl aqueous solution; dissolve 10 mmoles of CsCl in 5 ml of deionized water to form a 2 mol / L CsCl aqueous solution; dissolve 5 mmoles of CsCl in 5 ml of deionized water to form a 1 mol / L CsCl aqueous solution. Dissolve 3.3 mmoles of CsCl in 5 ml of deionized water to form a 0.66 mol / L CsCl aqueous solution. Dissolve 2.5 mmoles of CsCl in 5 ml of deionized water to form a 0.5 mol / L CsCl aqueous solution.

[0039] S2. Mix 0.5 ml of a 4 mol / L (1 ml of 2 mol / L, 2 ml of 1 mol / L, 3 ml of 0.66 mol / L or 4 ml of 0.25 mol / L) CsCl aqueous solution with 1 mmol of AgCl powder in a clean glass bottle to form an aqueous solution with a precipitate, and disperse under ultrasound for 30 minutes.

[0040] S3. Dry the obtained aqueous solution with precipitate in an oven at 50 degrees Celsius for 6 hours. After drying, grind into microcrystals using an agate mortar, collect, and store in a drying oven.

[0041] The Cs2AgCl3 material obtained by the present invention is subjected to X-ray diffraction and photoluminescence spectrum tests. The X-ray diffraction spectrum of the product is as follows: Figure 6 As shown. Figure 6 It can be seen that Cs2AgCl3 perovskite materials can be successfully synthesized at a CsCl aqueous solution concentration of 0.5 to 4 mol / L. The photoluminescence spectrum of the synthesized Cs2AgCl3 under 258 nm excitation is shown in Figure 7 As shown. Figure 7 It can be seen that the photoluminescence intensity of the product is the largest at a CsCl aqueous solution concentration of 0.66 mol / L. Therefore, the optimal CsCl aqueous solution concentration for synthesizing Cs2AgCl3 is 0.66 mol / L.

[0042] The above description is only a preferred embodiment of the present invention, and therefore cannot be used to limit the scope of the present invention. That is, equivalent changes and modifications made according to the patent scope of the present invention and the contents of the specification should still fall within the scope of the present invention.

Claims

1. A green and efficient method for synthesizing Cs2AgCl3 all-inorganic non-lead perovskite, characterized in that: The method comprises the following steps: mixing a CsCl aqueous solution and AgCl powder in a molar ratio of 2:1 to form an aqueous solution with precipitation, ultrasonically dispersing the solution at room temperature, and drying the solution, wherein the ultrasonic dispersing time is 10 to 30 minutes.

2. The green and efficient synthesis method as claimed in claim 1, characterized in that: The concentration of the CsCl aqueous solution is 0.5 to 4 mol / L.

3. The green and efficient synthesis method as claimed in claim 1, characterized in that: The drying temperature is 30 to 70 degrees Celsius.

4. The green and efficient synthesis method as claimed in claim 1, characterized in that: It also includes grinding it into microcrystals using an agate mortar after drying, collecting it, and storing it in a drying oven.

5. The green and efficient synthesis method as claimed in claim 1, characterized in that: The purity of the CsCl is ≥99.999%, and the purity of the AgCl is ≥99.99%.

6. The green and efficient synthesis method as claimed in claim 1, characterized in that: The solvent of the CsCl aqueous solution is deionized water.

7. A Cs2AgCl3 all-inorganic non-lead perovskite, characterized in that: The invention is prepared by the green and efficient synthesis method described in any one of claims 1 to 6, and its space group is Pnma, belonging to the orthorhombic crystal system.

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