白光LED用红、白荧光粉的合成与光谱性能研究
摘要
白光LED具有体积小、节能、环保、寿命长等优点,被称为第四代照明光源。目前,最成熟的白光LED实现方法是荧光粉转换法,备受各国和研究者们的关注。而荧光粉作为白光LED的重要组成部分,直接影响着白光LED的发展与应用。目前白光LED用荧光粉的研究与发展主要存在以下一些问题：一是缺少能被蓝光和紫外或近紫外有效激发的红色荧光粉,导致白光LED显色指数低,发光不稳定；二是急需寻找性能优异,稳定的单基质白光荧光粉,为白光LED的实现寻找一条新的切实可行的方法。此外,工业上荧光粉的生产主要是高温固相法,能耗大,颗粒形貌不可控等,已逐渐不能满足当今发展的需求。因此开发新型的白光LED用各色荧光粉并寻找新型的高效合成方法具有很大的理论研究意义和实际应用价值。
本论文一方面用低温熔盐法合成了能被蓝光和紫外或近紫外有效激发的白光LED用红色荧光粉；另一方面用高温固相法合成了可被紫外激发的单基质LED用白光荧光粉；同时还研究了它们的光谱性能。本论文的主要内容如下：
(1)用低温熔盐法合成了性能优异的能被蓝光和紫外激发的Y203：Eu红色荧光粉。研究了不同烧结温度、烧结时间、熔盐使用量、Eu3+掺杂浓度等对Y2O3:Eu发光性能的影响,找出了最佳合成条件。
(2)用共沉淀-熔盐法合成了颗粒分散均匀能被蓝光和紫外有效激发的Y2O3:Eu红色荧光粉。研究合成温度、不同熔盐体系对产物性能的影响,并对其中一些发光机理进行了探讨。
(3)用低温表面活性剂辅助共沉淀-熔盐法合成了性能优异的白光LED用Y2O3:Eu红色荧光粉。研究了不同烧结温度、表面活性剂使用量对产物光谱特性的影响,并对相应的机理进行了探讨。
(4)采用低温熔盐法合成了新型的能被蓝光和紫外有效激发的Y2O3:Eu, Bi高效红色荧光粉。考察了Bi3+掺杂浓度对产物发光性能的影响及其变化规律,并进一步探讨了光谱与能量传递机制。
(5)用传统的高温固相法合成了新型的单基质Ca9Y(PO4)7:Tm3+, Dy3+白光荧光粉。研究了Ca9Y(PO4)7:Tm3+, Dy3+的发光机理并考察了Tm3+和Dy3+掺杂浓度对产物光谱、色坐标等的影响。
White light-emitting diodes (LED) have been called as the fourth generation solid-state lighting source due to their small volume, energy-saving, environment-friendly, and long lifetime. Recently, phosphor-converted (pc) method is the most common to fabricate white LED, which has attracted considerable intentions of researchers and countries. As the important ingredient in pc-white LED, phosphor affects the development and application of white LED directly. With the development of phosphor for white LED in modern industry, there are several urgent problems needed to be solved. First of all, the absence of red phosphor which can be effectively excited by blue and ultraviolet or near ultraviolet light leads to low color render indexing and the unstable of luminescence. Secondly, it is an urgent need to develop single-phased white-emitting phosphors, which would provide a new and feasible method for the fabrication of white LED. In addition, the commercial phosphors are generally prepared by conventional high temperature solid state reaction which gradually cannot meet the demand of development in the area of light and display because of energy-consuming and uncontrollable for the shape of particles. Therefore, it is great meaningful to develop new good properties of different color-emitting phosphors and propose a novel energy-saving way for the parparation of phophors.
In this article, on the one hand, red phosphors, which can be pumped by blue and ultraviolet or near ultraviolet effectively, have been prepared by molten salt synthesis method in low temperature. On the other hand, a single-phazed white-emitting phosphor for white LED has been synthesized by high temperature solid state reaction. Furthermore, the corresponding luminescence properties are also investigated. The main contents in our work are listed in the followings:
(1) Good property of Y2O3:Eu red phosphor has been successfully fabricated by molten salt synthesis method and can be excited by blue as well as ultraviolet light effectively. The effect of annealed temperature, annealed time, molten salt content, Eu3+ doping concentration on the luminescence properties of Y2O3:Eu are discussed and the optimal synthesis conditions are also figured out.
(2) Y2O3:Eu red phosphor has been successfully prepared via co-precipitation-molten salt synthesis method and can be pumped by blue as well as ultraviolet light effectively. The dependence of luminescence properties on calcined temperature and fluxes are studied. The luminescence mechanisms are also discussed.
(3) Y2O3:Eu red phosphor for white LED has been successfully prepared by surfactant assisted co-precipitation-molten salt synthesis method in low temperature. Annealed temperature and surfactant concentration are explored in the effect of luminescence properties of products and the corresponding mechanisms are investigated.
(4) A new and high performance of Y2O3:Eu, Bi red phosphor, which can be monitered by blue and ultraviolet light effectively, has been fabricated via molten salt synthesis method. The luminescence properties of as-synthesized samples are discussed with respect to different Bi3+ doping concentrations. More importantly, the mechanisms about luminescence and energy transferring in Y2O3:Eu, Bi are studied.
(5) A novel single-phased Ca9Y(PO4)7:Tm3+, Dy3+ white-emitting phosphor has been successfully synthesized by high temperature solid state reaction. The luminescence mechanisms of as-prepared specimens are discussed. In addition to this, the effect of Tm3+ and Dy3+ doping concentrations on the luminescence properties and color coordinate of as-fabricated products are also investigated.
本论文一方面用低温熔盐法合成了能被蓝光和紫外或近紫外有效激发的白光LED用红色荧光粉；另一方面用高温固相法合成了可被紫外激发的单基质LED用白光荧光粉；同时还研究了它们的光谱性能。本论文的主要内容如下：
(1)用低温熔盐法合成了性能优异的能被蓝光和紫外激发的Y203：Eu红色荧光粉。研究了不同烧结温度、烧结时间、熔盐使用量、Eu3+掺杂浓度等对Y2O3:Eu发光性能的影响,找出了最佳合成条件。
(2)用共沉淀-熔盐法合成了颗粒分散均匀能被蓝光和紫外有效激发的Y2O3:Eu红色荧光粉。研究合成温度、不同熔盐体系对产物性能的影响,并对其中一些发光机理进行了探讨。
(3)用低温表面活性剂辅助共沉淀-熔盐法合成了性能优异的白光LED用Y2O3:Eu红色荧光粉。研究了不同烧结温度、表面活性剂使用量对产物光谱特性的影响,并对相应的机理进行了探讨。
(4)采用低温熔盐法合成了新型的能被蓝光和紫外有效激发的Y2O3:Eu, Bi高效红色荧光粉。考察了Bi3+掺杂浓度对产物发光性能的影响及其变化规律,并进一步探讨了光谱与能量传递机制。
(5)用传统的高温固相法合成了新型的单基质Ca9Y(PO4)7:Tm3+, Dy3+白光荧光粉。研究了Ca9Y(PO4)7:Tm3+, Dy3+的发光机理并考察了Tm3+和Dy3+掺杂浓度对产物光谱、色坐标等的影响。
White light-emitting diodes (LED) have been called as the fourth generation solid-state lighting source due to their small volume, energy-saving, environment-friendly, and long lifetime. Recently, phosphor-converted (pc) method is the most common to fabricate white LED, which has attracted considerable intentions of researchers and countries. As the important ingredient in pc-white LED, phosphor affects the development and application of white LED directly. With the development of phosphor for white LED in modern industry, there are several urgent problems needed to be solved. First of all, the absence of red phosphor which can be effectively excited by blue and ultraviolet or near ultraviolet light leads to low color render indexing and the unstable of luminescence. Secondly, it is an urgent need to develop single-phased white-emitting phosphors, which would provide a new and feasible method for the fabrication of white LED. In addition, the commercial phosphors are generally prepared by conventional high temperature solid state reaction which gradually cannot meet the demand of development in the area of light and display because of energy-consuming and uncontrollable for the shape of particles. Therefore, it is great meaningful to develop new good properties of different color-emitting phosphors and propose a novel energy-saving way for the parparation of phophors.
In this article, on the one hand, red phosphors, which can be pumped by blue and ultraviolet or near ultraviolet effectively, have been prepared by molten salt synthesis method in low temperature. On the other hand, a single-phazed white-emitting phosphor for white LED has been synthesized by high temperature solid state reaction. Furthermore, the corresponding luminescence properties are also investigated. The main contents in our work are listed in the followings:
(1) Good property of Y2O3:Eu red phosphor has been successfully fabricated by molten salt synthesis method and can be excited by blue as well as ultraviolet light effectively. The effect of annealed temperature, annealed time, molten salt content, Eu3+ doping concentration on the luminescence properties of Y2O3:Eu are discussed and the optimal synthesis conditions are also figured out.
(2) Y2O3:Eu red phosphor has been successfully prepared via co-precipitation-molten salt synthesis method and can be pumped by blue as well as ultraviolet light effectively. The dependence of luminescence properties on calcined temperature and fluxes are studied. The luminescence mechanisms are also discussed.
(3) Y2O3:Eu red phosphor for white LED has been successfully prepared by surfactant assisted co-precipitation-molten salt synthesis method in low temperature. Annealed temperature and surfactant concentration are explored in the effect of luminescence properties of products and the corresponding mechanisms are investigated.
(4) A new and high performance of Y2O3:Eu, Bi red phosphor, which can be monitered by blue and ultraviolet light effectively, has been fabricated via molten salt synthesis method. The luminescence properties of as-synthesized samples are discussed with respect to different Bi3+ doping concentrations. More importantly, the mechanisms about luminescence and energy transferring in Y2O3:Eu, Bi are studied.
(5) A novel single-phased Ca9Y(PO4)7:Tm3+, Dy3+ white-emitting phosphor has been successfully synthesized by high temperature solid state reaction. The luminescence mechanisms of as-prepared specimens are discussed. In addition to this, the effect of Tm3+ and Dy3+ doping concentrations on the luminescence properties and color coordinate of as-fabricated products are also investigated.
引文
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