發(fā)布時(shí)間：2018-07-05 09:02

  本文選題：硅鋁酸鹽 + 熒光粉��； 參考：《吉林大學(xué)》2016年博士論文

【摘要】：近年來,白光發(fā)光二極管由于具有高發(fā)光效率、節(jié)能、環(huán)保、使用方便和壽命長等的優(yōu)點(diǎn)而受到廣泛的關(guān)注和研究。發(fā)光二極管實(shí)現(xiàn)白光最普遍的方式是二極管芯片與熒光粉相結(jié)合。白光發(fā)光二極管的實(shí)現(xiàn)方式通常有兩種方法:一種是藍(lán)光芯片與黃色熒光粉Y3Al5O12:Ce組合,然而較高的猝滅溫度和低顯色性限制了其在照明領(lǐng)域的發(fā)展。另一種是紫外芯片與三基色熒光粉組合,這種方法可以克服以上不足并得到廣泛應(yīng)用。此種方法產(chǎn)生的白光均是由熒光粉發(fā)射復(fù)合而成,因此其具有高光效和高顯色指數(shù)的優(yōu)點(diǎn)。此外,單相多色熒光粉在其基礎(chǔ)上可進(jìn)一步提高發(fā)光效率和顯色指數(shù),因此,研發(fā)高穩(wěn)定性和吸收較強(qiáng)紫外光的三色熒光粉或是單相多色發(fā)光熒光粉具有重大意義。在本論文中,我們合成了一系列以硅鋁酸鹽為基質(zhì)的三色熒光粉和單相多色發(fā)光熒光粉,并研究了這些熒光粉的發(fā)光特性、能量傳遞及其在發(fā)光二極管器件上的應(yīng)用。得到研究成果如下:1.通過高溫固相法合成了新穎綠色熒光粉Ca2Mg0.5Al Si1.5O7:Eu2+。在368 nm激發(fā)下,該熒光粉可發(fā)射出峰值在525 nm左右的綠光。Eu2+離子的猝滅濃度和離子間的臨界距離分別為1.5 mol%和13.40?。熱活化能值為0.5432 e V,熒光粉的熒光壽命值為0.57μs。在綠色熒光粉Ca2Mg0.5Al Si1.5O7:Eu2+的基礎(chǔ)上共摻Ce3+離子通過高溫固相法合成了Ca2Mg0.5Al Si1.5O7:Ce3+,Eu2+藍(lán)-綠色多色發(fā)光熒光粉。研究其發(fā)光性質(zhì),發(fā)射光譜中409和525 nm的兩處發(fā)射峰分別歸屬于Ce3+和Eu2+離子的d-f電子躍遷。研究了Ce3+到Eu2+的能量傳遞,證明其是偶極-偶極的能量傳遞機(jī)理。進(jìn)一步研究表明,在350 nm激發(fā)下通過改變Ce3+/Eu2+的相對摻雜濃度比例,熒光粉Ca2Mg0.5Al Si1.5O7:Ce3+,Eu2+可實(shí)現(xiàn)藍(lán)-綠光多色發(fā)光,這表明該熒光粉在白光發(fā)光二極管領(lǐng)域具有潛在的應(yīng)用價(jià)值。2.在熒光粉Ca2Mg0.5Al Si1.5O7:Ce3+,Eu2+的基礎(chǔ)上,改變各元素的化學(xué)計(jì)量比,通過高溫固相法合成了光色可調(diào)的單相熒光粉Ca2Mg0.25Al1.5Si1.25O7:Ce3+,Tb3+和Ca2Mg0.25Al1.5Si1.25O7:Ce3+,Eu2+。研究了Ce3+到Eu2+和Ce3+到Tb3+的能量傳遞,確定它們的能量傳遞機(jī)理分別為偶極-偶極和偶極-四極的機(jī)理。通過改變Ce3+/Eu2+和Ce3+/Tb3+的相對摻雜濃度比例可實(shí)現(xiàn)熒光粉Ca2Mg0.25Al1.5Si1.25O7:Ce3+,Eu2+/Tb3+藍(lán)到綠光的多色發(fā)光,表明這兩種熒光粉可作為白光發(fā)光二極管用光色可調(diào)熒光粉。3.采用高溫固相法合成了一系列Ca2Mg0.75Al0.5Si1.75O7:Ln(Ln=Ce3+,Dy3+,Eu3+,Sm3+)的熒光粉,實(shí)現(xiàn)了三色光和白光發(fā)射。將已制備的熒光粉與紫外芯片相結(jié)合,封裝成藍(lán)、紅和白光發(fā)光二極管器件,并對器件的發(fā)光效率、國際照明協(xié)會(huì)色度坐標(biāo)、色溫和顯色指數(shù)等性能進(jìn)行測試,結(jié)果表明這些熒光粉為可應(yīng)用于白光發(fā)光二極管的紅、藍(lán)和白光熒光粉。4.合成了光色可調(diào)的單相白光熒光粉Ca20Al26Mg3Si3O68:Ce3+,Dy3+和黃-紅光多色發(fā)光熒光粉Ca20Al26Mg3Si3O68:Dy3+,Eu3+,并研究其發(fā)光性質(zhì)。對于熒光粉Ca20Al26Mg3Si3O68:Ce3+,Dy3+,在紫外光激發(fā)下,其發(fā)射光譜由407和577 nm兩處發(fā)射峰組成,分別歸屬于Ce3+和Dy3+的電子躍遷。更重要的是,通過激發(fā)和發(fā)射光譜及熒光壽命證明了Ce3+到Dy3+的有效的能量傳遞的存在。最后,通過改變Ce3+/Dy3+的相對摻雜濃度實(shí)現(xiàn)該熒光粉藍(lán)光-白光的多色發(fā)光,表明該熒光粉在白光發(fā)光二極管中具有潛在的應(yīng)用價(jià)值。在Ca20Al26Mg3Si3O68:Dy3+,Eu3+體系中,對熒光粉Ca20Al26Mg3Si3O68:Dy3+和Ca20Al26Mg3Si3O68:Eu3+分別進(jìn)行了X射線光電子能譜分析和位置選擇性光譜的測試來驗(yàn)證Dy3+和Eu3+的摻雜位置。進(jìn)一步證明和研究了Dy3+到Eu3+的能量傳遞。結(jié)果表明該熒光粉為在白光發(fā)光二極管領(lǐng)域具有潛在應(yīng)用價(jià)值的黃-紅光熒光粉。5.合成了一系列的Ln(Ln=Ce3+,Tb3+,Eu3+)分別單摻基質(zhì)Ca2Mg0.5Al Si1.5O7,Ca2Mg0.25Al1.5Si1.25O7,Ca2Mg0.75Al0.5Si1.75O7和Ca20Al26Mg3Si3O68的三色熒光粉。并研究了這些熒光粉的發(fā)光性質(zhì)及其在發(fā)光二極管器件上的應(yīng)用。通過對比發(fā)光強(qiáng)度,選出發(fā)光性最優(yōu)良的三色熒光粉并進(jìn)行封裝器件的測試,最后結(jié)果表明這些熒光粉為可應(yīng)用于白光發(fā)光二極管的三色熒光粉。
[Abstract]:In recent years, white light emitting diode has been widely concerned and studied because of its advantages of high luminous efficiency, energy saving, environmental protection, convenient use and long life. The most common way to realize white light by LEDs is the combination of diode chips and phosphor. The implementation of white light diodes usually has two methods: one is blue. The optical chip is combined with the yellow phosphor Y3Al5O12:Ce, but the high quenching temperature and low chromaticity limit its development in the lighting field. The other is the combination of UV chip and three color phosphor. This method can overcome the above shortcomings and be widely used. The production of white light is made of phosphor powder. Therefore, it has the advantages of high light efficiency and high color rendering index. In addition, the single-phase polychromatic phosphor can further improve the luminous efficiency and color rendering index. Therefore, it is of great significance to develop high stability and absorption of strong ultraviolet light powder or single phase polychromatic phosphor. In this paper, we have synthesized a system The three color phosphors and single-phase polychromatic phosphor phosphors based on Aluminosilicate are listed, and the luminescence characteristics, energy transfer and their application on the light emitting diode are studied. The results are as follows: 1. the novel green fluorescent powder Ca2Mg0.5Al Si1.5O7:Eu2+. was synthesized by high temperature solid phase method under the excitation of 368 nm. The fluorescence powder can emit the quenching concentration of the green light.Eu2+ ion with a peak of about 525 nm and the critical distance between the ions is 1.5 mol% and 13.40? The thermal activation energy is 0.5432 e V, and the fluorescence lifetime value of the phosphor is 0.57 U S. on the basis of the green phosphor Ca2Mg0.5Al Si1.5O7:Eu2+, and the Ce3+ ions are synthesized by the high temperature solid state method. 2Mg0.5Al Si1.5O7:Ce3+, Eu2+ blue green polychromatic phosphor. Study its luminescence properties. The two emission peaks of 409 and 525 nm in emission spectra belong to d-f electron transition of Ce3+ and Eu2+ ions respectively. The energy transfer of Ce3+ to Eu2+ is studied. It is proved that it is the energy transfer mechanism of dipole dipole. Further research shows that it is excited under 350 nm. By changing the ratio of relative doping concentration of Ce3+/Eu2+, phosphor Ca2Mg0.5Al Si1.5O7:Ce3+, Eu2+ can realize blue green light polychromatic luminescence, which shows that the phosphor has potential application value in the field of white light emitting diode (.2.), on the basis of phosphor Ca2Mg0.5Al Si1.5O7:Ce3+, Eu2+, change the chemometric ratio of each element, through high temperature. The solid phase method has synthesized a light colored single-phase phosphor Ca2Mg0.25Al1.5Si1.25O7:Ce3+, Tb3+ and Ca2Mg0.25Al1.5Si1.25O7:Ce3+. Eu2+. studies the energy transfer of Ce3+ to Eu2+ and Ce3+ to Tb3+, and determines that their energy transfer mechanism is the mechanism of dipole dipole and dipole quadrupole respectively. By changing the relative concentration of Ce3+/Eu2+ and Ce3+/Tb3+, the relative doping concentration of Ce3+/Eu2+ and Ce3+/Tb3+ is changed. The ratio can realize phosphor Ca2Mg0.25Al1.5Si1.25O7:Ce3+, Eu2+/Tb3+ blue to green light, which shows that the two phosphors can be used as white light emitting diodes with light color tunable phosphor.3. to synthesize a series of Ca2Mg0.75Al0.5Si1.75O7:Ln (Ln=Ce3+, Dy3+, Eu3+, Sm3+) Phosphors by high temperature solid phase method, and realize the three color light and white. Light emission. The prepared phosphors are combined with UV chips and packaged into blue, red and white light emitting diodes. The luminescence efficiency of the devices, the chromaticity coordinates of the International Lighting Association, color temperature and color rendering index are tested. The results show that these phosphors are red, blue and white light phosphors that can be used in white light emitting diodes. .4. syntheses the light color adjustable single-phase white phosphor Ca20Al26Mg3Si3O68:Ce3+, Dy3+ and yellow red light polychromatic phosphor Ca20Al26Mg3Si3O68:Dy3+, Eu3+, and study its luminescence properties. The emission spectra of phosphor Ca20Al26Mg3Si3O68:Ce3+, Dy3+, under ultraviolet light, are composed of 407 and 577 nm two emission peaks, belonging to Ce3+, respectively. More importantly, the existence of effective energy transfer from Ce3+ to Dy3+ is demonstrated by excitation and emission spectra and fluorescence lifetime. Finally, the polychromatic luminescence of the phosphor white light is realized by changing the relative doping concentration of the Ce3+/Dy3+, which indicates that the phosphor has potential applications in the white light emitting diode. Value. In the Ca20Al26Mg3Si3O68:Dy3+, Eu3+ system, the X ray photoelectron spectroscopy and the position selective spectra of the phosphor Ca20Al26Mg3Si3O68:Dy3+ and Ca20Al26Mg3Si3O68:Eu3+ were tested to verify the doping position of Dy3+ and Eu3+. The energy transfer of Dy3+ to Eu3+ was further proved and studied. The results showed that the phosphor was the powder. A series of Ln (Ln=Ce3+, Tb3+, Eu3+) mixed with Ca2Mg0.5Al Si1.5O7, Ca2Mg0.25Al1.5Si1.25O7, Ca2Mg0.75Al0.5Si1.75O7 and Ca20Al26Mg3Si3O68 were synthesized in the yellow red light phosphor.5., which is of potential value in the field of white light emitting diodes. The luminescence properties of these phosphors and their luminescence are studied. The application of the diode device. By comparing the luminescence intensity, the best luminescent three color phosphors are selected and the test of the packaging devices is carried out. Finally, the results show that these phosphors are three color phosphors which can be used in white light emitting diodes.
【學(xué)位授予單位】：吉林大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2016
【分類號】：TN312.8;TQ422
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本文編號：2099687