Broadband-emission yellow-light fluorescent powder and preparation method and application thereof

Abstract

The invention discloses yellow fluorescent powder with broadband emission as well as a preparation method and application of the yellow fluorescent powder, and belongs to the technical field of photoluminescence. The general chemical formula of the yellow fluorescent powder is K < 1-x > Sb < x > Cl, wherein x is more than or equal to 0.005 and less than or equal to 0.3; the yellow light fluorescent powder can emit broadband yellow light with the wavelength of 594 nm under excitation of 365 nm ultraviolet light, the emission peak range is 450-750 nm, the half-peak width reaches 143 nm, and the yellow light fluorescent powder has excellent luminescence performance. The yellow fluorescent powder is synthesized by adopting a room-temperature grinding method, a small amount of absolute ethyl alcohol is used as a solvent, high-temperature treatment is not needed, dependence on reducing or oxidizing atmosphere is avoided, the reaction time is shortened, and the preparation efficiency of the novel fluorescent powder is remarkably improved; meanwhile, the synthesis process is green and environment-friendly, toxic or corrosive solvents are prevented from being used, the development of green chemistry and sustainable manufacturing is met, and a good industrial application prospect is shown.

Description

Technical Field

[0001] This invention belongs to the field of photoluminescent materials technology, specifically relating to a broadband-emitting yellow phosphor, its preparation method, and its application. Background Technology

[0002] Phosphors, as core materials in photoluminescence technology, have significant application value in solid-state lighting, display devices, bioimaging, and optical sensing. Among them, yellow-emitting phosphors have attracted considerable attention due to their ability to effectively adjust color temperature and improve color rendering index in warm white LEDs. However, traditional yellow-emitting phosphors largely rely on rare earth elements (such as europium and cerium), whose scarcity, high cost, and complex purification processes limit their large-scale application. Furthermore, existing non-rare earth yellow-emitting phosphors generally suffer from narrow emission spectra and low luminous efficiency, making it difficult to meet the demands of high color rendering lighting devices.

[0003] In terms of preparation process, traditional phosphors mostly adopt high-temperature solid-state method or hydrothermal method. For example, patent CN 115710506A uses high-temperature solid-state method to prepare Cs2KBi by sintering at 580 ℃ for 2 h. 1-x Sb x Cl6, as in patent CN 119242297 A, is used to prepare K by hydrothermal heating at 180°C for 12 hours. 1-x Sb x Cl-based synthesis methods suffer from drawbacks such as high energy consumption, long reaction cycles, and strong equipment dependence. Although some low-temperature synthesis methods have been proposed to reduce the reaction temperature, they often require the use of toxic organic solvents or inert atmospheres, leading to complex processes and poor environmental compatibility. Furthermore, these methods also face challenges such as low product crystallinity, poor doping uniformity, and unstable luminescence properties, limiting their practical application potential.

[0004] The preparation of fluorescent materials still faces many problems that need to be solved. This invention proposes an innovative room temperature grinding process to solve many of the problems existing in the current preparation process. Summary of the Invention

[0005] This invention aims to overcome the key technical bottlenecks in the preparation of existing yellow phosphors, such as complex processes, high costs, and reliance on rare earth elements. It provides a broadband-emission yellow phosphor, its preparation method, and its applications. The method provided by this invention yields a KCl matrix doped with Sb. 3+ The material is a yellow phosphor; it can achieve broadband yellow light emission under ultraviolet light excitation, and has excellent luminescence performance, good thermal stability and environmental friendliness, making it suitable for high-performance white LEDs and display devices.

[0006] To achieve the above objectives, the present invention provides the following specific technical solutions: This invention provides a method for preparing a broadband-emitting yellow phosphor, comprising the following steps: A potassium-containing compound is added to anhydrous ethanol to obtain a potassium-containing solution; An antimony-containing compound is added to anhydrous ethanol to obtain an antimony-containing solution; An antimony-containing solution is added to a potassium-containing solution and mixed thoroughly to obtain a mixed solution. The molar ratio of the mixed solution is K:Sb:Cl = (1-x):x:1, where 0.005 ≤ x ≤ 0.3. The mixed solution is ground and then heat-treated to obtain yellow phosphor.

[0007] The potassium-containing compound includes any one or more of potassium chlorate, potassium hypochlorite, and potassium chloride, and a mixture thereof in any proportion.

[0008] The antimony-containing compound includes any one or more of oxides, sulfides, and halides, mixed in any proportion.

[0009] The grinding process takes 30 seconds to 10 minutes.

[0010] The heat treatment temperature shown is 30~80 ℃.

[0011] The concentration of the antimony-containing solution is 20-50% mol / L.

[0012] This invention also provides a broadband-emitting yellow phosphor, prepared according to the above-described method for preparing a broadband-emitting yellow phosphor, wherein the general chemical formula of the yellow phosphor is K. 1-x Sb x Cl, where 0.005≤x≤0.3.

[0013] The phosphor emits broadband yellow fluorescence with a wavelength of 594 nm when excited by ultraviolet light.

[0014] The phosphor exhibits an emission peak in the range of 450–750 nm under ultraviolet light excitation, with a full width at half maximum (FWHM) of 143 nm.

[0015] The present invention provides the application of the above-mentioned broadband emission yellow phosphor in solid-state lighting and display devices.

[0016] Compared with the prior art, the beneficial effects of the present invention are as follows: This invention abandons traditional high-temperature solid-state methods and hydrothermal synthesis methods in its preparation process, employing a room-temperature grinding method assisted by anhydrous ethanol. This eliminates the need for high-temperature treatment or inert atmosphere protection, and also avoids the use of corrosive reagents such as hydrochloric acid. The entire reaction process uses only non-toxic, low-cost anhydrous ethanol as the reaction medium and produces no toxic byproducts, thus achieving the desired Sb content. 3+This method enables the rapid synthesis of highly efficient doped and highly crystalline products. The preparation process reduces reaction time to the minute level, significantly improving production efficiency. The resulting phosphor exhibits high-purity yellow light emission under ultraviolet light excitation, and possesses excellent luminous efficiency and good thermal stability. This preparation method aligns with the principles of green chemical synthesis and has the potential for industrial-scale production.

[0017] This invention successfully constructed a novel potassium-based halide fluorescent material system, and developed Sb by controlling the lattice environment through an ion replacement strategy. 3+ Doped K 1-x Sb x This yellow phosphor exhibits a strong and broad emission peak at 594 nm under 365 nm ultraviolet light excitation, significantly improving its luminescence performance. The excitation spectrum of this phosphor effectively covers the 300-400 nm ultraviolet spectral region, highly matching the emission wavelength of conventional ultraviolet LED chips. In summary, this invention represents a significant technological breakthrough in terms of luminous efficiency, spectral characteristics, and environmental friendliness of the process, providing an innovative material solution for the development of next-generation solid-state lighting devices. Attached Figure Description

[0018] To more clearly illustrate the technical solutions of the embodiments of the present invention, the accompanying drawings used in the embodiments will be briefly described below: Figure 1 Sb prepared in Examples 1-9 of this invention 3+ XRD patterns of KCl phosphors with different concentrations of doped KCl phosphors and corresponding standard KCl cards; Figure 2 Sb prepared in Examples 1-9 of this invention 3+ Photoluminescence emission spectra of KCl phosphors with different concentrations of doped phosphors at room temperature, with a wavelength of 594 nm; Figure 3 Sb prepared in Example 5 of this invention 3+ Chromaticity diagram of KCl-doped phosphor. Detailed Implementation

[0019] To make the objectives, technical solutions, and advantages of the embodiments of the present invention clearer, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some, not all, of the embodiments of the present invention. The components of the embodiments of the present invention described and shown in the accompanying drawings can generally be arranged and designed in various different configurations. Therefore, the following detailed description of the embodiments of the present invention provided in the accompanying drawings is not intended to limit the scope of the claimed invention, but merely to illustrate selected embodiments of the invention. All other embodiments obtained by those skilled in the art based on the embodiments of the present invention without inventive effort are within the scope of protection of the present invention.

[0020] This invention achieves its goal through the rational design of Sb 3+ By employing a room-temperature grinding method with KCl doping, the technical challenges of low efficiency and complex processes in non-rare-earth yellow phosphors have been successfully overcome, providing a feasible solution for low-cost, environmentally friendly, high-performance phosphors. The entire preparation process eliminates corrosive reagents such as hydrochloric acid that may be used in traditional methods, using only anhydrous ethanol as the reaction medium, significantly improving the safety and environmental friendliness of the process, and demonstrating good prospects for industrial application.

[0021] To more clearly illustrate the purpose, technical solution, and beneficial effects of this invention, the following detailed description is provided in conjunction with specific embodiments. Unless otherwise specified, all raw materials and reagents used are available through conventional commercial channels; the testing and analytical methods involved are standard methods commonly used in the field.

[0022] Example 1 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.995 Sb 0.005 Cl (x=0.5%), prepared as follows: Weigh 0.995 mmol of high-purity (99%) KCl and pour it into a mortar. Add an appropriate amount of anhydrous ethanol and grind for 9 min to mix thoroughly to obtain a KCl solution. Separately, dissolve 2 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 20% mol / L SbCl3 solution. Add 25 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution and continue grinding for 2 min. Then transfer the solution to a 60 ℃ oven and dry for 15 min to obtain broadband emission KCl. 0.995 Sb 0.005 Cl yellow fluorescent powder.

[0023] The K prepared in this embodiment 0.995 Sb0.005 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0024] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment are consistent with those of the KCl standard card PDF#00-041-1476, and other impurity phases were detected.

[0025] Depend on Figure 2 It can be seen that, under 365 nm ultraviolet light excitation, the emission peak of the yellow phosphor in this embodiment is located near 594 nm, and the luminescence intensity is relatively weak.

[0026] Example 2 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.99 Sb 0.01 Cl (x=1%), prepared by the following method: Weigh 0.99 mmol of KCl into a mortar, add anhydrous ethanol, and grind for 8 min to obtain a homogeneous KCl solution. Separately, dissolve 2 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 20% mol / L SbCl3 solution. Add 50 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution, continue grinding for 3 min, and then place it in a 45 ℃ oven to dry for 30 min to obtain broadband emission KCl. 0.99 Sb 0.01 Cl yellow fluorescent powder.

[0027] The K prepared in this embodiment 0.99 Sb 0.01 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0028] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment are consistent with those of the KCl standard card PDF#00-041-1476, and no other impurities are observed.

[0029] Depend on Figure 2 It can be seen that, under 365 nm ultraviolet light excitation, the emission peak of the yellow phosphor in this embodiment is located near 594 nm, and the luminescence intensity is slightly enhanced, but still very weak.

[0030] Example 3 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.97 Sb 0.03 Cl (x=3%), prepared by the following method: Weigh 0.97 mmol of KCl into a mortar, add anhydrous ethanol, and grind for 8 min to obtain a homogeneous KCl solution. Separately, dissolve 3 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 30% mol / L SbCl3 solution. Add 100 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution, continue grinding for 6 min, and then place it in a 30 ℃ oven to dry for 40 min to obtain broadband emission KCl. 0.97 Sb 0.03 Cl yellow fluorescent powder.

[0031] The K prepared in this embodiment 0.97 Sb 0.03 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0032] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment are consistent with those of the KCl standard card PDF#00-041-1476, and no other impurities are observed.

[0033] Depend on Figure 2 It can be seen that, under 365 nm ultraviolet light excitation, the emission peak of the yellow phosphor in this embodiment is located near 594 nm, and the luminescence intensity is further enhanced, but still relatively low.

[0034] Example 4 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.95 Sb 0.05 Cl (x=5%), prepared by the following method: Weigh 0.95 mmol of KCl into a mortar, add anhydrous ethanol, and grind for 7 min to obtain a homogeneous KCl solution. Separately, dissolve 3 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 30% mol / L SbCl3 solution. Add 167 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution, grind for 6 min, and then place it in a 60 ℃ oven to dry for 10 min to obtain broadband emission KCl. 0.95 Sb 0.05 Cl yellow fluorescent powder.

[0035] The K prepared in this embodiment 0.95 Sb 0.05 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0036] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment are consistent with those of the KCl standard card PDF#00-041-1476, and no other impurities were observed.

[0037] Depend on Figure 2 It can be seen that, in this embodiment, the yellow phosphor exhibits a significantly enhanced 594 nm emission peak under 365 nm ultraviolet light excitation, indicating that with the increase of Sb... 3+ Increasing the doping concentration improves the luminescence performance.

[0038] Example 5 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.93 Sb 0.07 Cl (x=7%), prepared by the following method: Weigh 0.93 mmol of KCl into a mortar, add anhydrous ethanol, and grind for 5 min to obtain a homogeneous KCl solution. Separately, dissolve 4 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 40% mol / L SbCl3 solution. Add 175 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution, grind for 7 min, and then place it in an 80 ℃ oven to dry for 5 min to obtain broadband emission KCl. 0.93 Sb 0.07 Cl yellow fluorescent powder.

[0039] The K prepared in this embodiment 0.93 Sb 0.07 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0040] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment are consistent with those of the KCl standard card PDF#00-041-1476, and no other impurities were observed.

[0041] Depend on Figure 2 It can be seen that, in this embodiment, the intensity of the 594 nm emission peak of the yellow phosphor continues to increase under 365 nm ultraviolet light excitation, indicating that Sb 3+ Increasing the doping concentration is beneficial to improving luminescence performance.

[0042] Example 6 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.90 Sb 0.10 Cl (x=10%) is prepared as follows: Weigh 0.90 mmol of KCl into a mortar, add anhydrous ethanol, and grind for 6 min to obtain a homogeneous KCl solution. Separately, dissolve 4 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 40% mol / L SbCl3 solution. Add 250 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution, grind for 8 min, and then place it in a 70 ℃ oven to dry for 8 min to obtain broadband emission KCl. 0.90 Sb 0.10 Cl yellow fluorescent powder.

[0043] The K prepared in this embodiment 0.90 Sb 0.10 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0044] Depend on Figure 1 It can be seen that, in addition to conforming to the KCl standard card PDF#00-041-1476, the X-ray diffraction peaks of the yellow phosphor in this embodiment also show a small amount of K3SbCl6 impurity phase.

[0045] Depend on Figure 2 It can be seen that the intensity of the 594 nm emission peak of the yellow phosphor in this embodiment is further enhanced under 365 nm ultraviolet light excitation.

[0046] Example 7 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.85 Sb 0.15 Cl (x=15%), prepared by the following method: Weigh 0.85 mmol of KCl and pour it into a mortar. Add anhydrous ethanol and grind for 5 min to mix evenly to obtain a KCl solution. Separately, dissolve 4 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 40% mol / L SbCl3 solution. Add 375 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution. Grind for 6 min and then place it in a 30 ℃ oven to dry for 40 min to obtain a broadband-emitting yellow phosphor.

[0047] The K prepared in this embodiment 0.85 Sb 0.15 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0048] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment not only match those of the KCl standard card PDF#00-041-1476, but also generate obvious K3SbCl6 impurity peaks.

[0049] Depend on Figure 2 It can be seen that, in this embodiment, the intensity of the 594 nm emission peak of the yellow phosphor continuously increases under 365 nm ultraviolet light excitation, indicating that the high concentration of Sb 3+ Doping can further improve luminescence efficiency.

[0050] Example 8 Sb 3+ Preparation of KClO3-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.80 Sb 0.20 Cl (x=20%), prepared by the following method: Weigh 0.80 mmol of KCl and pour it into a mortar. Add anhydrous ethanol and grind for 5 min to mix evenly to obtain a KClO3 solution. Separately, dissolve 5 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 50% mol / L SbCl3 solution. Add 400 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution. Grind for 9 min and then place it in a 45 ℃ oven to dry for 30 min to obtain a broadband-emitting yellow phosphor.

[0051] The K prepared in this embodiment 0.80 Sb 0.10 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0052] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment mainly correspond to the K3SbCl6 standard card PDF#00-024-0833, while also containing a small amount of SbCl3 impurity phase.

[0053] Depend on Figure 2 It can be seen that the intensity of the 594 nm emission peak of the yellow phosphor in this embodiment continues to increase under 365 nm ultraviolet light excitation.

[0054] Example 9 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.70 Sb 0.30 Cl (x=30%) is prepared as follows: Weigh 0.70 mmol of KCl and pour it into a mortar. Add anhydrous ethanol and grind for 4 min to mix evenly to obtain a KCl solution. Separately, dissolve 5 mmol of SbCl3 in 10 mL of anhydrous ethanol to prepare a 50% mol / L SbCl3 solution. Add 599 μL of the SbCl3 solution dropwise into the mortar containing the KCl solution. Grind for 10 min and then place it in a 50 ℃ oven to dry for 25 min to obtain a broadband-emitting yellow phosphor.

[0055] The K prepared in this embodiment 0.70 Sb 0.30 The XRD pattern of the Cl yellow phosphor is shown below. Figure 1 The emission spectrum is shown below. Figure 2 .

[0056] Depend on Figure 1 It can be seen that the X-ray diffraction peaks of the yellow phosphor in this embodiment mainly correspond to the K3SbCl6 standard card PDF#00-024-0833, indicating an increase in the content of SbCl3 impurity phase.

[0057] Depend on Figure 2 It can be seen that, in this embodiment, the yellow phosphor reaches its maximum emission peak intensity at 594 nm under 365 nm ultraviolet light excitation, indicating that Sb 3+ The doping concentration has reached the upper limit of the optimal range.

[0058] Example 10 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.80 Sb 0.20 Cl (x=20%), prepared by the following method: Weigh 0.80 mmol of KClO3 into a mortar, add hydrochloric acid, and grind for 4 min to mix thoroughly to obtain a K-containing solution. + A solution containing ions; separately, 2.5 mmol of Sb₂O₃ was dissolved in 10 mL of HCl to prepare a 50% mol / L solution containing Sb. 3+ Solution containing ions; take 400 μL of Sb-containing solution. 3+ The solution of ions is added dropwise into a mortar containing KClO3 solution, and after grinding for 9 minutes, it is placed in a 50 °C oven to dry for 30 minutes to obtain a broadband-emitting yellow phosphor.

[0059] Example 11 Sb 3+ Preparation of KCl-doped yellow phosphor The chemical formula of the antimony ion-doped potassium chloride luminescent material prepared in this embodiment is: K 0.80 Sb 0.20 Cl (x=20%), prepared by the following method: Weigh 0.80 mmol of KClO and pour it into a mortar. Add hydrochloric acid and grind for 4 minutes to mix thoroughly to obtain a K-containing solution. + A solution containing ions; separately, 2.5 mmol of Sb₂S₃ was dissolved in 10 mL of HCl to prepare a 50% mol / L solution containing Sb. 3+ Solution containing ions; take 400 μL of Sb-containing solution. 3+ The solution of ions is added dropwise into a mortar containing KClO solution, and after grinding for 9 minutes, it is placed in a 50 °C oven to dry for 30 minutes to obtain a broadband-emitting yellow phosphor.

[0060] Structural and property analysis of yellow phosphor: Figure 1 The Sb prepared in Examples 1-9 3+ X-ray diffraction patterns of yellow phosphors doped with KCl at different concentrations. Figure 1 It can be seen that in Sb 3+ When the doping concentration x is within the range of 0.005 ≤ x ≤ 0.07, the XRD pattern of the obtained sample is highly consistent with the standard diffraction card of KCl (PDF#00-041-1476), and no obvious impurity phase diffraction peaks are detected, indicating that Sb 3+ Successful entry into the KCl lattice did not trigger a significant structural phase transition. This result demonstrates that the room-temperature synthesis method employed in Examples 1-5 of this invention can yield single-phase KCl with high crystallinity. 1-x Sb x Cl material, and Sb 3+ The ions exhibit good solid solubility at low doping concentrations. When Sb...3+ When the doping amount is further increased to 0.07 < x ≤ 0.15 (corresponding to Examples 6 and 7), in addition to the characteristic diffraction peaks of the KCl matrix retained in the XRD pattern, extra diffraction peaks attributed to K3SbCl6 also appear, and its standard card is PDF#00-024-0833. This indicates that at a relatively high Sb 3+ concentration, a second phase begins to form in the system, and the product transforms from a single-phase structure to a multi-phase coexistence. This phenomenon may stem from Sb 3+ ions exceeding the maximum solid solubility in the KCl lattice, resulting in their precipitation in the form of an independent compound, thereby triggering a side reaction to generate the K3SbCl6 compound. As the Sb 3+ doping amount is further increased to 0.15 < x ≤ 0.3 (corresponding to Examples 8 and 9), the XRD pattern mainly shows the diffraction characteristics of K3SbCl6, accompanied by a small amount of residual SbCl3 phase, indicating that it is difficult to maintain the original KCl structure at this time.

[0061] Figure 2 The emission spectra of the phosphors prepared in Examples 1 - 9 under ultraviolet light excitation are shown. The results show that all samples can effectively convert ultraviolet light into yellow light emission, with emission peaks in the range of 450 - 750 nm under ultraviolet light excitation, and its full width at half maximum reaches 143 nm, indicating its excellent photoluminescence performance. As the Sb 3+ ion doping concentration increases, the luminescence intensity of the phosphor shows a gradually increasing trend. Specifically, within the range of 0.005 ≤ x ≤ 0.1, the luminescence intensity increases significantly with the increase of the Sb 3+ content. This phenomenon is mainly attributed to the introduction of Sb 3+ causing local lattice distortion, thereby changing the local environment around the luminescence center, enhancing the radiation transition probability of Sb 3+ and possibly suppressing the non-radiative recombination process, thus improving the overall luminescence efficiency. When the doping concentration continues to increase to x > 0.1, the luminescence intensity continues to increase, but the increase amplitude tends to flatten.

[0062] Figure 3 is the CIE chromaticity diagram of the phosphor obtained in Example 5. The results show that the emitted light of all samples is high-purity yellow light, and its chromaticity coordinates are (0.4911, 0.4813), located in the yellow light region of the standard CIE chromaticity diagram.

[0063] This invention designs and develops a Sb 3+ doped yellow phosphor based on the KCl matrix (chemical formula is K 1- x Sb xBy employing an ion-substitution strategy to modulate the lattice environment, the luminescent properties of Sb were significantly enhanced. This preparation process utilizes anhydrous ethanol-assisted room-temperature milling, eliminating the need for high-temperature treatment or inert atmosphere protection, to achieve Sb... 3+ This invention enables the rapid synthesis of highly efficient doped and highly crystalline products (reaction time reduced to minutes, superior to the solution method in patent CN116240017B). The obtained phosphor exhibits high-purity yellow light emission under ultraviolet light excitation, while also possessing excellent luminous efficiency and good thermal stability. This invention not only achieves a new breakthrough in material design but also provides a practical new path for green and low-cost preparation technology, offering an innovative solution for the industrialization of next-generation high-performance, environmentally friendly fluorescent materials.

[0064] The endpoints and any values ​​of the ranges disclosed in this invention are not limited to the precise ranges or values; these ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of the various ranges, the endpoint values ​​of the various ranges and individual point values, and individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed herein. In the following, various technical solutions can, in principle, be combined with each other to obtain new technical solutions, which should also be considered as specifically disclosed herein.

[0065] The above embodiments are only used to illustrate the technical solutions of the present invention and not to limit it. Although the present invention has been described in detail with reference to the above embodiments, those skilled in the art can still make modifications or equivalent substitutions to the specific implementation of the present invention. Any modifications or equivalent substitutions that do not depart from the spirit and scope of the present invention are within the protection scope of the claims of the present invention pending approval.

Claims

1. A method for preparing a broadband-emitting yellow phosphor, characterized in that, Includes the following steps: A potassium-containing compound is added to anhydrous ethanol to obtain a potassium-containing solution; An antimony-containing compound is added to anhydrous ethanol to obtain an antimony-containing solution; An antimony-containing solution is added to a potassium-containing solution and mixed thoroughly to obtain a mixed solution. The molar ratio of the mixed solution is K:Sb:Cl = (1-x):x:1, where 0.005 ≤ x ≤ 0.

3. The mixed solution is ground and then heat-treated to obtain yellow phosphor.

2. The method for preparing the broadband-emitting yellow phosphor according to claim 1, characterized in that, The potassium-containing compound includes any one or more of potassium chlorate, potassium hypochlorite, and potassium chloride, and a mixture thereof in any proportion.

3. The method for preparing the broadband-emitting yellow phosphor according to claim 1, characterized in that, The antimony-containing compound includes any one or more of oxides, sulfides, and halides, mixed in any proportion.

4. The method for preparing the broadband-emitting yellow phosphor according to claim 1, characterized in that, The grinding process takes 30 seconds to 10 minutes.

5. The method for preparing the broadband-emitting yellow phosphor according to claim 1, characterized in that, The heat treatment temperature shown is 30~80 ℃.

6. The method for preparing the broadband-emitting yellow phosphor according to claim 1, characterized in that, The concentration of the antimony-containing solution is 20-50% mol / L.

7. A broadband-emitting yellow phosphor, characterized in that, The yellow phosphor with broadband emission is prepared according to any one of claims 1-6, wherein the general chemical formula of the yellow phosphor is K. 1-x Sb x Cl, where 0.005≤x≤0.

3.

8. The broadband-emitting yellow phosphor according to claim 7, characterized in that, The phosphor emits broadband yellow fluorescence with a wavelength of 594 nm when excited by ultraviolet light.

9. The broadband-emitting yellow phosphor according to claim 7, characterized in that, The phosphor exhibits an emission peak in the range of 450–750 nm under ultraviolet light excitation, with a full width at half maximum (FWHM) of 143 nm.

10. The application of the broadband-emitting yellow phosphor of claim 7 in solid-state lighting and display devices.

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