CN115710502A - Yb 3+ Doped CsPbBr 3 PMSCs and preparation method and application thereof - Google Patents
Yb 3+ Doped CsPbBr 3 PMSCs and preparation method and application thereof Download PDFInfo
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Abstract
Yb of the invention 3+ Doped CsPbBr 3 PMSCs, a preparation method and application thereof, belonging to the technical field of photoelectric material preparation. The preparation method comprises the following steps: weighing CsBr and PbBr in proportion 2 Then dissolving the mixed solution in a solvent to obtain a mixed solution 1; sequentially adding oleic acid and oleylamine into the mixed solution 1 according to a ratio, and dissolving to obtain a mixed solution 2; weighing Yb in proportion 3+ Adding the compound into the mixed solution 2, and dissolving to obtain a precursor solution; injecting the precursor solution into an antisolvent to obtain Yb 3+ Doped CsPbBr 3 PMSCs solution; high speed centrifugal washing of purified Yb 3+ Doped CsPbBr 3 PMSCs solution. Yb of the invention 3+ Doped CsPbBr 3 PMSCs with high efficiency dual emission and high fluorescence quantum yieldThe product has the advantages of excellent stability, and can be applied to the near infrared light emitting field and photoelectric devices.
Description
Technical Field
The invention belongs to the technical field of photoelectric material preparation, and particularly relates to Yb 3+ Doped CsPbBr 3 PMSCs and a preparation method and application thereof.
Background
The low-dimensional Perovskite Magic-Sized Clusters (PMSCs) material has the unique advantages of adjustable luminescent color, excellent charge transmission performance, high narrow-band emission color purity, remarkable light quantum effect and the like, and has great development potential in the fields of bioluminescence imaging, cell marking, ultra-high definition display, biochemical sensors, photocatalysis and the like. However, the PMSCs have the defects of poor stability and storage performance of more surface defects in the environment due to larger specific surface area, containing toxic heavy metal lead element and only covering the visible light region in the spectral range, so that the design, development and application of PMSCs-based photoelectric devices in the future are seriously challenged.
In structure and performance, the PMSCs material has the unique properties of small size (2 nm), narrow fluorescence half-peak width (FWHM < 15 nm), obvious quantum confinement effect, high specific surface area, more surface defects and the like, so that the structural performance of the PMSCs material can be modified. At present, csPbBr is concerned 3 The relevant research on PMSCs has mainly focused on the relevant research on unique size, composition, stability and optoelectronic properties. By the pair CsPbBr 3 PMSCs are modified and studied, and the transition metal Mn with high fluorescence quantum yield and high transition metal Mn can be prepared 2+ Doping and small-size (2 nm) samples, but the technology of the existing doped PMSCs has not broken through the technical bottleneck of near-infrared luminescence.
The lanthanide rare earth ion doped low-dimensional PMSCs material not only has the intrinsic excellent physical and chemical properties of the PMSCs material, but also has the unique optical, electrical, magnetic and catalytic properties endowed by the special 4 f-valent electronic configuration of the lanthanide rare earth ion, and can create new emission characteristics, enhance stability, reduce defect state density and the like, so that the lanthanide rare earth ion and the PMSCs material can be used for designing and preparing a novel photoelectric functional material with excellent photoelectric properties and stability under the synergistic effect. This study focused on CsPbBr 3 PMSCs were studied, composition CsPbBr 3 PMSCs are structurally defined by Cs + 、Pb 2+ And halide ion Br - Composition is carried out; structurally, lanthanide rare earth ions are generally introduced into the A, B or B sites of perovskites, widening CsPbBr 3 The luminescent spectrum range of PMSCs is from original ultraviolet region to ultraviolet regionNear infrared region, which improves the photoelectric application range of the material; csPbBr with quantum confinement effect on physical and chemical properties compared with large-sized perovskite blocks and perovskite thin films 3 The PMSCs material can effectively reduce surface defects by combining a surface passivation strategy and a doping substitution strategy due to the existence of larger exciton binding energy, and effectively improve the stability, toxicity and photoelectric properties of the material. Furthermore, compared to organic-inorganic hybrid perovskites, inorganic CsPbBr 3 The PMSCs have temperature and H resistance due to the absence of organic components 2 O and O 2 Stronger stability. Thus, inorganic CsPbBr 3 The preparation and synthesis process of PMSCs has very wide market prospect for promoting the application in the field of novel photoelectric devices. The lanthanide rare earth ions have extremely rich energy levels and 4f electron transition effects, so that the rare earth doped material shows quantum behaviors and photoelectric characteristics with wide spectral range and rich connotation. By doping substitution strategies CsPbBr 3 The PMSCs can realize absorption and emission in ultraviolet and near infrared regions, and further effectively improve and expand photoelectric application of the PMSCs. However, no relevant research on lanthanide rare earth doped PMSCs is reported at present.
Therefore, the lanthanide rare earth ion doped PMSCs have important research significance and practical value for preparing high-quality perovskite type up-conversion nano material devices.
Disclosure of Invention
The invention aims to overcome the defects in the prior art and provides Yb with high efficiency, double emission, high fluorescence quantum yield and excellent stability 3+ Doped CsPbBr 3 PMSCs, preparation method and application thereof, and realization of CsPbBr 3 The stable storage of PMSCs in the external environment and the stable luminescence in the near infrared region are realized, so that the purpose of reaction to generate CsPbBr with excellent stability and optical performance is achieved 3 Target of PMSCs.
To achieve the above object, the present invention provides Yb 3+ Doped CsPbBr 3 The preparation method of PMSCs comprises the following steps:
weighing CsBr and PbBr in proportion 2 Then dissolving the mixed solution in a solvent to obtain a mixed solution 1;
sequentially adding oleic acid and oleylamine into the mixed solution 1 according to a ratio, and dissolving to obtain a mixed solution 2;
weighing Yb in proportion 3+ Adding the compound into the mixed solution 2, and dissolving to obtain a precursor solution;
injecting the precursor solution into an antisolvent to obtain Yb 3+ Doped CsPbBr 3 PMSCs solution;
high speed centrifugal washing to purify the Yb 3+ Doped CsPbBr 3 Obtaining Yb from PMSCs solution 3+ Doped CsPbBr 3 PMSCs。
Preferably, csBr and PbBr 2 The mass ratio of (1) to (0.5) is: 1, the solvent is dimethyl sulfoxide or N, N-dimethylformamide, pbBr 2 And the addition amount of the solvent was 0.02mmol: (0.1-1.1) mL.
Preferably, oleic acid and PbBr 2 The ratio of the amounts of the substances (1) to (0.2 to 0.8): 1, oleylamine and PbBr 2 The ratio of the amounts of the substances (1) to (0.6): 1.
preferably, yb is a rare earth containing lanthanum 3+ Compound of (2) and PbBr 2 The ratio of the amounts of the substances (1) is (0.04-0.1): 1.
Preferably, the antisolvent is any one of n-hexane, toluene, dichloromethane and chloroform, and the volume ratio of the precursor solution to the antisolvent is (0.1-0.5): (2-10).
Preferably, the high-speed centrifugation is carried out at a rotating speed of 6000-12000 r/min for multiple times of 15-20min, and supernatant is taken after each time of high-speed centrifugation to obtain separated and purified Yb 3+ Doped CsPbBr 3 PMSCs, which are stored in a refrigerator at 0-5 ℃.
Preferably, the dissolving treatment is stirring dissolving at normal temperature; containing Yb 3+ Is Yb (NO) 3 ) 3 ·5H 2 O、 Yb 2 (SO 4 ) 3 、YbBr 3 、YbCl 3 And YbI 3 Or a mixture of two.
The invention also provides Yb prepared by the preparation method 3+ Doped CsPbBr 3 PMSCs。
The invention also provides Yb prepared by the preparation method 3+ Doped CsPbBr 3 PMSCs or Yb as described above 3+ Doped CsPbBr 3 Application of PMSCs in the near-infrared light emitting field.
The invention also provides a photoelectric device comprising Yb prepared by the preparation method 3+ Doped CsPbBr 3 PMSCs, or Yb as described above 3+ Doped CsPbBr 3 PMSCs。
The invention adopts the technical scheme that the method has the advantages that:
yb of the invention 3+ Doped CsPbBr 3 The preparation method of PMSCs adopts the technical process of ligand assisted reprecipitation (LAPR) at normal temperature and uses CsBr and PbBr 2 Oleic acid and oleylamine are used as surface passivation ligands and contain lanthanum rare earth Yb 3+ The compound of (1) is a doping compound. wherein-COO is added to oleic acid - Can effectively passivate Cs + And Pb 2+ Addition of oleylamine-NH 3 + Can effectively passivate Br - Doping with lanthanide-containing rare earth ions Yb 3+ The compound can effectively replace CsPbBr 3 Pb in the Structure of PMSCs 2+ . Moreover, the oleic acid and oleylamine ligands not only can passivate surface defects and play a role in stabilizing CsPbBr 3 The action of PMSCs can also control CsPbBr 3 The growth speed of PMSCs inhibits cluster nucleation; by pairing ligands and Yb-containing compounds 3+ The addition amount of the compound and the dropping time of the anti-solvent are finely regulated, so that the Yb with good stability and optical performance is generated by controlling the reaction 3+ Doped CsPbBr 3 PMSCs; the preparation method has the characteristics of simple process, easy operation and solution-soluble processing.
Yb of the invention 3+ Doped CsPbBr 3 The PMSCs and lanthanide rare earth ions are doped into the PMSCs structure due to the abundant 4f energy level and electron configuration, so that the stability and the photoelectric performance of the PMSCs can be remarkably improved, and the characteristics are mainly that electrons in a 4f shell layer are effectively shielded by electrons in external 5s and 5p shell layers. And, rare earthThe half-peak width of the emission peak of ion luminescence is narrow, the luminescence decay life is long and can reach several microseconds, the luminescence range of the PMSCs can be effectively widened, and the optical performance of the PMSCs is further improved. Pb present in PMSCs 2+ Is toxic heavy metal ion and can not reverse environmental pollution, the invention mainly adopts Yb 3+ Has strong light absorption advantage to near infrared light and is based on Yb 3+ Ratio of Pb to Pb 2+ Small ion radius, and can effectively dope and replace Pb 2+ The shrinkage of the PMSCs structure is caused to increase the binding energy between the negative ions and the positive ions in the structure, so that the enhancement of intrinsic luminescence of the PMSCs is effectively regulated and controlled, the stability of the PMSCs structure is improved, the toxicity of lead-containing elements is reduced, and the spectrum application range is widened.
The invention passes Yb 3+ Doping of lanthanide rare earth ions, and f → f transition based on rare earth ions can effectively realize CsPbBr 3 The PMSCs can efficiently emit light in a near-infrared band, can be applied to the field of near-infrared light emission, and also provides a new method and a new idea for designing and developing a high-efficiency multifunctional perovskite cluster-based photoelectric device.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the embodiments or the prior art descriptions will be briefly described below, it is obvious that the drawings in the following description are only some embodiments of the present invention, and other drawings can be obtained by those skilled in the art without creative efforts.
FIG. 1 shows Yb in example 1 of the present invention 3+ Doped CsPbBr 3 The ultraviolet absorption spectrum and the fluorescence emission spectrum of PMSCs are tested, wherein (a) is Yb 3+ Doped CsPbBr 3 Ultraviolet absorption spectrum and fluorescence emission spectrum of PMSCs in ultraviolet-visible light range, and (b) Yb 3+ Doped CsPbBr 3 Fluorescence emission spectra of PMSCs in the near infrared range;
FIG. 2 shows Yb in comparative example 1 of the present invention 3+ Doped CsPbBr 3 Ultraviolet absorption spectra of Perovskite Quantum Dots (PQDs) in the wavelength range of 350-650nmA fluorescence emission spectrum test result graph;
FIG. 3 shows the undoped CsPbBr in comparative example 2 according to the present invention 3 Testing result graphs of ultraviolet absorption spectra and fluorescence emission spectra of PMSCs in the wavelength range of 350-650 nm;
FIG. 4 is a graph of the stability of the fluorescence quantum yield over time for the products prepared in examples 1 to 4 according to the invention and in comparative examples 1 to 3, in which (a) is a graph corresponding to Yb prepared in examples 1 to 4 3+ Doped CsPbBr 3 PMSCs, the (b) diagram corresponds to the products prepared in comparative examples 1-3.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be obtained by a person skilled in the art without making any creative effort based on the embodiments in the present invention, belong to the protection scope of the present invention.
The invention provides a Yb 3+ Doped CsPbBr 3 The preparation method of PMSCs comprises the following steps:
weighing CsBr and PbBr in proportion 2 Then dissolving the mixed solution in a solvent to obtain a mixed solution 1;
sequentially adding oleic acid and oleylamine into the mixed solution 1 according to a ratio, and dissolving to obtain a mixed solution 2;
weighing Yb in proportion 3+ Adding the compound of (2) into the mixed solution 2, and dissolving to obtain a precursor solution;
injecting the precursor solution into an antisolvent to obtain Yb 3+ Doped CsPbBr 3 PMSCs solution;
high speed centrifugal washing to purify the Yb 3+ Doped CsPbBr 3 Obtaining Yb from PMSCs solution 3+ Doped CsPbBr 3 PMSCs。
Wherein CsBr and PbBr 2 The mass ratio of (2) is (0.5-1.2): 1, preferably 0.8 to 1.1. The solvent is dimethyl sulfoxide (DMSO) or N, N-Dimethylformamide (DMF), pbBr 2 And the addition amount of the solvent was 0.02mmol: (0.1-1.1) mL, when PbBr is present 2 When the amount of the substance(s) is 0.02mmol, the solvent addition volume is preferably 0.1mL, 0.3mL, 0.5mL, 0.7mL, 0.9mL or 1.1mL, more preferably 0.3mL, 0.5mL or 0.7mL. CsBr and PbBr 2 The dissolution of (2) is stirring dissolution at normal temperature, and the stirring time is about 20min.
Oleic acid and PbBr 2 The ratio of the amounts of the substances (1) to (0.2 to 0.8): 1, preferably (0.4 to 0.7): 1; oleylamine and PbBr 2 The ratio of the amounts of the substances (1) to (0.6): 1, preferably (0.2 to 0.4): 1. the oleic acid and oleylamine are dissolved by stirring at normal temperature for about 30min.
Yb containing lanthanide series rare earth 3+ Compound of (2) and PbBr 2 The ratio of the amounts of the substances (1) is (0.04-0.1): 1, preferably (0.05 to 0.08): 1. containing Yb 3+ The compound of (A) can be selected from Yb (NO) 3 ) 3 ·5H 2 O、Yb 2 (SO 4 ) 3 、 YbBr 3 、YbCl 3 And YbI 3 One or a mixture of two. Containing Yb 3+ The compound (2) is dissolved by stirring at normal temperature for about 10min.
The anti-solvent is any one of n-hexane, toluene, dichloromethane and trichloromethane, and toluene or dichloromethane is preferred. The volume ratio of the precursor solution to the antisolvent is (0.1-0.5): (2 to 10), preferably (0.2 to 0.5): (4-8). The method for injecting the precursor solution into the anti-solvent specifically comprises the following steps: and (3) placing the glass bottle with the anti-solvent of the stirrer on a stirring table for stirring, measuring the precursor solution by using a pipettor, quickly injecting the precursor solution into the anti-solvent at one time, and quickly stirring for 5-10min at normal temperature.
The high-speed centrifugation is carried out at a rotating speed of 6000-12000 r/min, preferably 8000-10000 r/min, the high-speed centrifugation is carried out for a plurality of times, each time is 15-20min, supernatant fluid is taken after each high-speed centrifugation, and separated and purified Yb is obtained 3+ Doped CsPbBr 3 PMSCs, which are stored in a refrigerator at 0-5 ℃.
The invention also provides Yb prepared by the preparation method 3+ Doped CsPbBr 3 PMSCs。
The invention also provides Yb prepared by the preparation method 3+ Doped CsPbBr 3 PMSCs or Yb as described above 3+ Doped CsPbBr 3 Application of PMSCs in the near-infrared light emitting field.
The invention also provides a photoelectric device comprising Yb prepared by the preparation method 3+ Doped CsPbBr 3 PMSCs, or Yb as described above 3+ Doped CsPbBr 3 PMSCs。
Example 1
Yb (Yb) 3+ Doped CsPbBr 3 PMSCs, the preparation process is as follows:
weighing the materials in a glove box according to the weight ratio of 1:1 cesium bromide (CsBr) and lead bromide (PbBr) 2 ) Then transferred in dimethyl sulfoxide (DMSO) solvent and stirred rapidly until completely dissolved, wherein PbBr 2 The amount of the substance is 0.02mmol, and the volume of the dimethyl sulfoxide (DMSO) solvent is 0.5mL, so as to obtain a mixed solution 1;
then, the organic carboxylic acid Oleic Acid (OA) and the organic amine oleylamine (OAm) were added to the mixed solution 1 in order and rapidly stirred until dissolved, wherein the amount of the added Oleic Acid (OA) and PbBr were added 2 The mass ratio of 0.5:1, the addition amount of organic amine oleylamine (OAm) and PbBr 2 The mass ratio of the substances is 0.3:1, obtaining a mixed solution 2;
subsequently, a certain amount of Yb is incorporated 3+ Rare earth compound YbBr 3 Adding into the mixed solution 2 and rapidly stirring until the mixed solution is dissolved, wherein YbBr 3 Addition amount of (B) and PbBr 2 The mass ratio of the substances is 15:1, obtaining a precursor solution;
rapidly injecting the precursor solution into a dichloromethane antisolvent which is rapidly stirred according to the volume ratio of the precursor solution to the antisolvent dichloromethane being 1; covering and stirring at room temperature for 5-10min to obtain Yb 3+ Doped CsPbBr 3 PMSCs solution;
yb obtained by the reaction 3+ Doped CsPbBr 3 PMSCs solution at speed of rotationCentrifuging at 10000r/min for 10min to obtain supernatant, centrifuging for 3 times to obtain purified Yb 3+ Doped CsPbBr 3 And (5) storing the PMSCs in a refrigerator at 0-5 ℃.
Example 2
Yb (Yb) 3+ Doped CsPbBr 3 PMSCs, the preparation process of which differs from example 1 only in that: the solvent is N, N-Dimethylformamide (DMF), the anti-solvent is toluene, and the control of other processes is the same.
Example 3
Yb (Yb) 3+ Doped CsPbBr 3 PMSCs, the preparation process of which differs from example 1 only in that: the addition amount of organic amine (OAm) and PbBr 2 The mass ratio of the substances is 0.4:1, the other process controls are the same.
Example 4
Yb (Yb) 3+ Doped CsPbBr 3 PMSCs, the preparation process of which differed from example 1 only in that: ybBr 3 Addition amount of (B) and PbBr 2 The mass ratio of the substances is 10:1, the other process controls are the same.
Comparative example 1
Yb (Yb) 3+ Doped CsPbBr 3 PQDs, the preparation of which differs from example 1 only in that: the organic carboxylic acid Oleic Acid (OA) was not added, and the other process controls were the same.
Comparative example 2
Undoped CsPbBr 3 PMSCs, the preparation process of which differs from example 1 only in that: containing Yb 3+ Is Yb (NO) 3 ) 3 ·5H 2 O, the other process controls are the same.
Comparative example 3
Yb (Yb) 3+ Doped CsPbBr 3 PQDs, the preparation of which differs from example 1 only in that: no organic amine oleylamine (OAm) was added and the other process controls were the same.
The performance tests and results are as follows:
(1) Ultraviolet absorption spectrum and fluorescence emission spectrum tests were performed on the products prepared in example 1, comparative example 1 and comparative example 2 using an ultraviolet-visible-near infrared spectrophotometer and a fluorescence spectrophotometer instrument.
FIG. 1 shows Yb in example 1 3+ Doped CsPbBr 3 The ultraviolet absorption spectrum and the fluorescence emission spectrum of PMSCs are tested, wherein (a) is Yb 3+ Doped CsPbBr 3 Ultraviolet absorption spectrum and fluorescence emission spectrum of PMSCs in ultraviolet-visible light range (b) is Yb 3+ Doped CsPbBr 3 Fluorescence emission spectra of PMSCs in the near infrared range. As can be seen from the figure, yb in example 1 3+ Doped CsPbBr 3 Characteristic peaks of an ultraviolet absorption spectrum and a fluorescence emission spectrum of the PMSCs are 418nm and 420/978 nm respectively.
FIG. 2 shows Yb in comparative example 1 3+ Doped CsPbBr 3 The ultraviolet absorption spectrum and the fluorescence emission spectrum of the PQDs in the wavelength range of 350-650nm are tested to obtain a result graph, and the characteristic peaks of the ultraviolet absorption spectrum and the fluorescence emission spectrum are 508nm and 519nm respectively.
FIG. 3 shows CsPbBr undoped in comparative example 2 3 And (3) testing results of the ultraviolet absorption spectrum and the fluorescence emission spectrum of the PMSCs in the wavelength range of 350-650nm, wherein characteristic peaks of the ultraviolet absorption spectrum and the fluorescence emission spectrum of the PMSCs are respectively 510nm and 515nm.
(2) The fluorescence quantum yield of the stability of the products prepared in examples 1 to 4 and comparative examples 1 to 3 was tested using a fluorescence spectrophotometer, and the experimental conditions for stability were: the relative air humidity at room temperature was 80%. Table 1 shows the initial values of fluorescence quantum yields and the values after one month (30 days) for the stability of the products prepared in examples 1 to 4 and comparative examples 1 to 3.
TABLE 1 results of fluorescence quantum yield test for stability of products prepared in examples 1 to 4 and comparative examples 1 to 3
| Initial value of fluorescence quantum yield% | Fluorescence quantum yield after one month% | |
| Example 1 | 90％ | 88％ |
| Example 2 | 89％ | 87％ |
| Example 3 | 87％ | 85％ |
| Example 4 | 85％ | 80％ |
| Comparative example 1 | 8％ | 1％ |
| Comparative example 2 | 76％ | 28％ |
| Comparative example 3 | 12％ | 3％ |
Changes over time in the fluorescence quantum yield of the stability of the products prepared in examples 1 to 4 and comparative examples 1 to 3The curve is shown in FIG. 4, in which (a) is the Yb prepared in examples 1 to 4 3+ Doped CsPbBr 3 The initial value of the fluorescence quantum yield of the PMSCs test for one month (30 days) was reduced from the initial 90%, 89%, 87% and 85% to 88%, 87%, 85% and 80%, respectively, showing good stability. (b) The figure shows CsPbBr prepared in comparative examples 1 to 3 3 The initial value of the fluorescence quantum yield of PQDs tested for one month (30 days) is respectively reduced from initial 8%, 76% and 12% to 1%, 28% and 3%, and the PQDs are not good in stability and are easy to decompose. In the preparation processes of comparative example 1 and comparative example 3, as the ligands of Oleic Acid (OA) and oleylamine (OAm) are not added respectively, the synergistic action of the ligands is avoided, the passivated surface defects only exist in the presence of single ligand passivated surface defects, and the sample is difficult to control and synthesize CsPbBr 3 PMSCs to generate CsPbBr with poor stability 3 PQDs. Comparative example 2 since Yb is contained 3+ Compound YbBr 3 Replacement by Yb (NO) 3 ) 3 ·5H 2 O, reaction to produce undoped CsPbBr 3 PMSCs, surface ligands, although passivating surface defects and having a certain surface coating stabilizing effect, failed to synthesize Yb 3+ Doped CsPbBr 3 PMSCs。
(3) The products prepared in example 1 and comparative example 2 were subjected to stability tests in the polar solvent isopropanol, wherein the ratio of the volume of the sample solution to the volume of isopropanol was 1.
As a result of stability analysis, the initial values of the fluorescence quantum yields of the samples of example 1 and comparative example 2 were reduced from 90% and 76% to 82% and 21%, respectively. Yb in example 1 3+ Doped CsPbBr 3 The stability and optical property of the PMSCs sample are obviously superior to those of the undoped CsPbBr 3 PMSCs sample, indicating lanthanide rare earth Yb 3+ Doping can effectively improve CsPbBr 3 Stability and optical properties of PMSCs.
The invention adopts the technical scheme that the method has the advantages that:
yb of the invention 3+ Doped CsPbBr 3 The preparation method of PMSCs adopts a technical process of ligand assisted reprecipitation (LAPR) at normal temperature and uses CsBr and PbBr 2 Oleic Acid (OA) and oleylamine (OAm) as raw materials for surface passivationLigand of Yb-containing 3 + The compound of (A) is a rare earth doped compound, and-COO is added into oleic acid - Can effectively passivate Cs + And Pb 2+ Addition of oleylamine-NH 3 + Can effectively passivate Br - Doped with Yb 3+ The compound can effectively replace CsPbBr 3 Pb in PMSCs Structure 2+ The oleic acid and oleylamine ligand can passivate surface defects to achieve the purpose of stabilizing PMSCs, can control the growth speed of the PMSCs, and inhibits cluster nucleation to achieve the effect of stabilizing the structure of the PMSCs; by pairing ligands and Yb-containing compounds 3+ The addition amount of the compound and the dropping time of the anti-solvent are finely regulated, so that Yb with good stability and optical performance is generated by reaction 3+ Doped CsPbBr 3 PMSCs; the preparation method has the characteristics of simple process, easy operation and solution-soluble processing.
Yb of the invention 3+ Doped CsPbBr 3 The PMSCs and lanthanide rare earth ions are doped into the PMSCs structure due to the abundant 4f energy level and electron configuration, so that the stability and the photoelectric performance of the PMSCs can be remarkably improved, and the characteristics are mainly due to the fact that electrons in a 4f shell layer are effectively shielded by electrons in external 5s and 5p shell layers. Moreover, the half-peak width of the emission peak of the rare earth ion luminescence is narrow, the luminescence decay life is long and can reach several microseconds, the luminescence range of the PMSCs can be effectively widened, and the fluorescence quantum yield of the PMSCs is improved. Pb present in PMSCs 2+ Is toxic heavy metal ion and can not reverse environmental pollution, the invention mainly adopts Yb 3+ Has strong light absorption advantage to near infrared light and is based on Yb 3+ Specific ratio of Pb to Pb 2+ Small ion radius, and can effectively dope and replace Pb 2+ The structure of the PMSCs is contracted to increase the binding energy between negative ions and positive ions in the structure, so that the intrinsic luminescence of the PMSCs is effectively regulated and controlled to be enhanced, the stability of the PMSCs structure is improved, the toxicity of lead-containing elements is reduced, and the spectrum application range is widened.
The invention passes through Yb 3+ Doping lanthanide rare earth ions, and f → f transition based on the rare earth ions can effectively realize high-efficiency luminescence of PMSCs in near-infrared band, can be applied to the near-infrared luminescence field, and alsoThe design and development of the high-efficiency multifunctional perovskite cluster-based photoelectric device provide a new method and a new idea.
Finally, it should be noted that: the above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; while the invention has been described in detail and with reference to the foregoing embodiments, it will be understood by those skilled in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some or all of the technical features may be equivalently replaced; and the modifications or the substitutions do not make the essence of the corresponding technical solutions depart from the scope of the technical solutions of the embodiments of the present invention.
Claims (10)
1. Yb (molybdenum) 3+ Doped CsPbBr 3 The preparation method of PMSCs is characterized by comprising the following steps:
weighing CsBr and PbBr in proportion 2 Then dissolving the mixed solution in a solvent to obtain a mixed solution 1;
sequentially adding oleic acid and oleylamine into the mixed solution 1 according to a ratio, and dissolving to obtain a mixed solution 2;
weighing Yb in proportion 3+ Adding the compound into the mixed solution 2, and dissolving to obtain a precursor solution;
injecting the precursor solution into an antisolvent to obtain Yb 3+ Doped CsPbBr 3 PMSCs solution;
high speed centrifugal washing to purify the Yb 3+ Doped CsPbBr 3 Obtaining Yb from PMSCs solution 3+ Doped CsPbBr 3 PMSCs。
2. Yb according to claim 1 3+ Doped CsPbBr 3 The preparation method of PMSCs is characterized in that CsBr and PbBr 2 The mass ratio of (2) is (0.5-1.2): 1, the solvent is dimethyl sulfoxide or N, N-dimethylformamide, pbBr 2 And the addition amount of the solvent was 0.02mmol: (0.1-1.1) mL.
3. Yb according to claim 1 3+ CsPb dopingBr 3 The preparation method of PMSCs is characterized in that oleic acid and PbBr 2 The ratio of the amounts of the substances (1) to (0.2 to 0.8): 1, oleylamine and PbBr 2 The ratio of the amounts of the substances (1) to (0.6): 1.
4. yb according to claim 1 3+ Doped CsPbBr 3 A process for producing PMSCs characterized by containing Yb 3+ Compound of (2) and PbBr 2 The ratio of the amounts of the substances (1) is (0.04-0.1): 1.
5. yb according to claim 1 3+ Doped CsPbBr 3 The preparation method of PMSCs is characterized in that the antisolvent is any one of n-hexane, toluene, dichloromethane and chloroform, and the volume ratio of the precursor solution to the antisolvent is (0.1-0.5): (2-10).
6. Yb according to claim 1 3+ Doped CsPbBr 3 The preparation method of PMSCs is characterized in that the rotating speed of high-speed centrifugation is 6000-12000 r/min, the high-speed centrifugation is carried out for a plurality of times, each time is 15-20min, supernatant fluid is taken after each high-speed centrifugation, and separated and purified Yb is obtained 3+ Doped CsPbBr 3 PMSCs, which are stored in a refrigerator at 0-5 ℃.
7. Yb according to claim 1 3+ Doped CsPbBr 3 The preparation method of PMSCs is characterized in that the dissolving treatment is stirring and dissolving at normal temperature; containing Yb 3+ Is Yb (NO) 3 ) 3 ·5H 2 O、Yb 2 (SO 4 ) 3 、YbBr 3 、YbCl 3 And YbI 3 One or a mixture of two.
8. Yb produced by the production method according to any one of claims 1 to 7 3+ Doped CsPbBr 3 PMSCs。
9. A process according to any one of claims 1 to 7Yb produced by the method 3+ Doped CsPbBr 3 PMSCs or Yb according to claim 8 3+ Doped CsPbBr 3 The PMSCs are applied to the near-infrared light emitting field.
10. An optoelectronic device, characterized by: the photoelectric device comprises Yb produced by the production method according to any one of claims 1 to 7 3+ Doped CsPbBr 3 PMSCs, or Yb according to claim 8 3+ Doped CsPbBr 3 PMSCs。
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