CN1381072A - 基于发光二极管的发射白光的照明设备 - Google Patents

基于发光二极管的发射白光的照明设备 Download PDF

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CN1381072A
CN1381072A CN01801487A CN01801487A CN1381072A CN 1381072 A CN1381072 A CN 1381072A CN 01801487 A CN01801487 A CN 01801487A CN 01801487 A CN01801487 A CN 01801487A CN 1381072 A CN1381072 A CN 1381072A
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A·埃伦斯
F·杰尔曼
F·库默
M·奥斯特塔格
F·茨瓦施卡
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Abstract

在一种发射白光的光转换二极管(LED)中,采用一种氯硅酸盐荧光剂,这种荧光剂中除了Ca和Mg以外还包含掺杂的铕,在该LED中也采用稀土,特别是Y和/或Tb的石榴石荧光剂,以这种方式,能够获得高的色彩再现和在不同温度条件下的高度稳定的照明性能。

Description

基于发光二极管的发射白光的照明设备
                        技术领域
本发明涉及基于发光二极管的发射白光的照明设备，其中LED主要发射UV辐射或蓝光。此外，还采用至少一种发射黄光的荧光剂和一种发射绿光的荧光剂对主辐射进行部分转换。所采用的黄色荧光剂是Ce-活化的柘榴石，特别是包含Y和/或Tb的柘榴石。所采用的绿色荧光剂是Eu-活化的钙-镁-氯硅酸盐(Ca8Mg(SiO4)4Cl2)。
                        现有技术
电化学会志(J.Electrochem.Soc.)1992，p.622已公开一种氯硅酸盐荧光剂和它对UV和蓝光激发的应用，这种荧光剂中掺杂Eu(掺杂Eu2+的Ca8Mg(SiO4)4Cl2荧光剂的发光性能和能量转换)。它发出的光在光谱的绿色区域。该文没有说明这种荧光剂的具体应用领域。
发射白光的发光转换-LED，目前是将在约460nm发射的蓝色Ga(In)N LED与发射黄光的YAG：Ce3+荧光剂结合起来生产的(美国专利5,998,925和欧洲专利862 794)。然而，由于缺乏颜色成分(主要是红色成分)，造成差的色彩再现，所以这些发射白光的LED只能有限地应用于一般照明目的。另一种方法是混合三种颜色RGB(红、绿、蓝)，它们合起来产生白光，参见例如WO 98/39805。
                      发明概述
本发明的目的是提供一种按照权利要求1的前述部分的基于LED的照明设备，该设备发射白光，特别是具有高的色彩再现。
这些目的是利用权利要求1的特征部分实现的。在从属 中，给出特别有利的实施方案。
以前制造发射白光的LED的方法，主要是基于RGB配料，即基于三种颜色，也就是红、绿和蓝的混合物，在这种情况下，该后一种成分可由荧光剂或由LED的主发射提供。第二种简化的方法中，如在序言中所讨论的，是基于混合蓝色和黄色(BG配料)。
根据本发明，首次采用基于BGG混合物——即蓝、黄、和绿色的组合——的全新概念。最重要的因素是，黄色荧光剂的光带是如此之宽，以致它们在光谱的红色区域也有足够的发射比例，特别是其在可见光区域总发射比例的至少20％处在≥620nm的光谱区域。
已经证明，Ce-活化的稀土(RE)柘榴石是一种特别适宜的发射黄光的荧光剂，其中RE优选自Y、Tb、Gd、Lu和/或La。Y和Tb组合是优选的。在这种情况下，为了达到足够的红色比例，Tb引起的长波位移具有特别有利的作用。
优选特别适合发射绿光的荧光剂(其发射波长峰值位于500-525nm区域)的CaMg氯硅酸盐结构根据本发明它掺杂以铕(Eu)。如果适宜，还可将少量的其它掺杂剂，特别是锰(Mn)，以小比例加入，用于细调。另一种方案是SrAl2O4：Eu2+或Sr4Al14O25：Eu2+类型的绿色荧光剂。
在色图中，绿色荧光剂的色品位置与黄色荧光剂的色品位置以及蓝色LED的色品位置(或蓝色荧光剂颜色的色品位置)一起，封闭成很宽的三角形，产生适合特殊要求的更多的可能性。相比之下，不同的柘榴石的色品位置变化的范围明显较小。因此，对于可能达到的色温也可在很宽的范围，一般在4000-10 000K内散射。
在开发发射白光的照明设备方面，本发明是特别有利的。这是一种既基于LED阵列又基于单个LED的照明设备，或者是一种直接进行发光转换的LED，其中的荧光剂直接或间接地与芯片接触，即将荧光剂直接施加到芯片上，或嵌在包围它的树脂中。
将发射发射波长(峰)为300-470nm的发UV或蓝光(在本说明书中全都称作“短波”光)的LED，与根据本发明的荧光剂混合物组合起来，可以产生白光，这种荧光剂混合物能完全或部分地吸收LED的辐射，并且本身在光谱范围内发光，它与LED光的加成混合物产生有优良色彩再现的白光。可能还需要加入另一种发射蓝光的荧光剂成分(例如BAM)。在UV-LED的情况下，在发射波长(峰)约330-350nm处，和在蓝色LED的情况下，在发射波长(峰)约450-470nm处，达到特别有效的激发。
例如，通过混合20-50重量％的氯硅酸盐荧光剂，结果改善了基于柘榴石荧光剂的这种已知的白色LED的色彩再现。发射黄光的荧光剂是按照通式RE3(Al，Ga)5O12：Ce的稀土(RE)Y、Gd、Lu、La和/或Tb的柘榴石，特别是按照通式YAG：Ce或TbAG：Ce，其中特别是RE＝Y和/或Tb。
从科学文献中获悉荧光剂Ca8Mg(SiO4)4Cl2：Eu2+，但该文献并没有指出这种荧光剂的具体应用。根据本发明，这种荧光剂在白色LED的应用中有好的性能，基于三色混合物的荧光剂是特别方便的，这种混合物是由主UV光源(300-390nm)激发的。然而，它也适合在有蓝色主光源(430-470nm)的白色LED中的特殊应用。铕的比例x，在x＝0.005至x＝1.6之间，特别是在x＝0.01至x＝1.0之间是有利的。在这种情况下，具有经验式Ca8-xEuxMg(SiO4)4Cl2。
除了Eu以外，加入少量的Mn(达到Eu mol比例约20％)作为另一种掺杂剂，能有目的的将发射从光谱的绿色区域移向长波区域，即进入光谱的黄色区域。这具有使发射更适于人眼的优点，因此也改善了视觉的有效效果。Mn的比例y，至多为y＝0.1。在不加锰的情况下，特别优选铕的比例为x＝0.05至x＝0.8。
当在光源中，特别是在LED中使用时，铕的浓度影响发射光的色品位置。这种荧光剂的色品位置，可采用二种浓度Eu∶Mn的比例另行细调，这简化或最佳化LED中其它(黄色或蓝色)荧光剂的匹配。
例如在设备中也可采用根据本发明的荧光剂也可用于其中LED阵列(UV或蓝色主发射)照射透明板上的荧光剂的设备，或其中各个LED照射涂敷在透镜上的荧光剂的设备。
为产生有高的色彩再现的白色LED，采用根据本发明的荧光剂是特别方便的。为此，可以单独地或以混合物的形式施加这些荧光剂，如果适宜，可将这些荧光剂与尽可能是透明的粘合剂混合(欧洲专利862 794)。这些荧光剂能全部或部分地吸收发射UV/蓝光的LED的光，并在光谱的其它区域(主要是黄色和绿色)，以足够宽的带(即具有显著的红色比例)再发射光，形成具有所需色品位置的总发射。迄今为止，几乎没有任何如这里所述的以其组合形式的荧光剂那样好的能满足这些要求的荧光剂。它们具有高的量子效率(约70％)，同时，其发射光谱是基于眼睛灵敏度那样的明亮。色品的位置可在很宽的范围内调节。
适宜的光源是一种LED(发光二极管)，它产生白光，是通过直接将发射绿光或发射黄光的荧光剂与在光谱蓝色区域(430-470nm)的主辐射混合，或利用多种荧光剂(采用三种荧光剂混合形成的BGG)，将主发射的UV辐射转换成白色。在本文中，术语蓝、黄和绿的含义，一般应理解为在蓝色区域：430-470nm，绿色区域：490-525nm，和黄色区域：545-590nm发射最大。
所采用的主光源是发射UV或发射蓝光芯片的辐射。采用在330-370nm发射最大的UV-LED能得到特别好的结果。特别是在考虑到柘榴石和氯硅酸盐的激发光谱时，在355-365nm得到了最佳结果。这里所用的蓝色荧光剂是例如BAM。在蓝色芯片的情况下，采用峰值波长430-470nm能获得特别好的结果。特别是在考虑到柘榴石和氯硅酸盐的激发光谱时，在445-460nm得到了最佳结果。
色彩再现特别优良的方案是将二种荧光剂结合使用，即一种Tb含量高的荧光剂，优选纯的TbAG：Ce与氯硅酸盐：Eu结合起来。温度稳定性特别好的方案是将二种荧光剂结合使用，即一种Y含量高的荧光剂，优选纯的YAG：Ce与氯硅酸盐：Eu结合起来。
特别适合作为主辐射的发射UV或蓝色辐射(为了简化起见，下面称作短波辐射)的LED是Ga(In)N-LED，或采用另一种方案，是在发射区域300-470nm发射其它短波的LED。特别推荐主发射区域在UV区域(320-360nm)和在蓝色区域(430-470nm)，因为这是效率最高的区域。
                        附图
下面将参照若干典型的实施方案更详细地说明本发明。在附图中：
图1示出掺杂铕的氯硅酸盐的激发光谱和发射光谱；
图2示出另一种掺杂铕的氯硅酸盐的反射光谱和发射光谱；
图3示出一种作为白光光源(LED)使用的半导体元件；
图4示出图3中的LED的发射光谱，这种LED采用根据本发明的荧光剂TbAG和CS：Eu；
图5示出另一种LED的发射光谱，这种LED采用根据本发明的荧光剂TbAG和CS：Eu；
图6示出一种LED的温度行为，该LED采用根据本发明的荧光剂YAG和CS：Eu；
图7示出一种LED的发射光谱，该LED采用根据本发明的荧光剂YAG和CS：Eu；
图8示出一种采用根据本发明的荧光剂的照明设备。
                         对附图的说明
下文采用实例对掺杂Eu和掺杂Mn的氯硅酸盐Ca8Mg(SiO4)4Cl2：(Eu2+，Mn2+)的合成进行更详细地说明。然后在若干典型测定的基础上，证明这种荧光剂的适宜性。
荧光剂粉末是采用高温固体反应生产的。为此所举的实例是，将高纯度的原料CaCO3、MgO、SiO2、和CaCl2，按照摩尔比7∶1∶4∶1.5混合起来。为了掺杂，加入少量的Eu2O3或MnCO3，取代相应摩尔量的CaCO3。这相应于经验式Ca8-x-yEuxMnxMg(SiO4)4Cl2加0.5CaCl2。
在将各个成分充分混合之后，在还原性气氛(H2/N2)中，在1000-1200℃下将该粉末加热1-4小时，使其反应以得上述的化合物。为了除去过量的CaCl2和其它能水溶的夹杂相，可采用充分脱离子的水再次洗涤该粉末。获得的荧光剂粉末在波长约400nm的短波区域激发时具有高量子效率(一般约70％)。
图1示出掺杂铕的粉末典型的激发光谱和发射光谱。加入的Eu2O3的量为0.03摩尔，即x＝0.06。从该图可以看到，在300-470nm非常宽的波长范围内，主要是360-400nm范围内的有效激发十分清晰。在更大的波长下，由于Eu2+吸收带引起激发性能的下降。然而，测定的460nm下的量子效率仍可与在400nm或甚至更短波长(短到约340nm)下的量子效率相当。
发射光谱表明在约507nm具有最大的Eu2+发射带。这种发射眼睛看上去是绿色的。如果需要，共掺杂少量的锰，可使这种荧光剂的发射行为与眼睛的灵敏度更好地适配。
图2示出掺杂Eu的氯硅酸盐Ca8Mg(SiO4)4Cl2：Eu2+(简缩为CS：Eu)的另一个典型的实施方案。加入的Eu2O3量为0.2摩尔，即x＝0.4。峰的波长为509nm，平均波长为522nm。色坐标是x＝0.185，y＝0.615。采用图2a中任选的单位，表示在400nm照射时的发射。此外，在图2b中还示出反射率(以％表示)。
为了与GaInN-芯片一起用于白色LED，作为实例，采用与在美国专利5,998,925中所述相似的结构。在图3中详细地示出用于白光的这种类型的光源结构。这种光源是一种InGaN型的半导体元件(芯片1)，峰的发射波长为450nm，它具有第一和第二个电连接件2，3，并嵌在不透光的底外壳8中间隙9的区域内，连接件3中之一通过焊接导线14与芯片1连接。该间隙具有壁17，壁17用作芯片1蓝色主辐射的反射器。间隙9中充满封装化合物5，其主要成分是铸塑环氧树脂(80-90重量％)和荧光剂颜料6(＜15重量％)。此外，其它少量的成分是甲基醚和一种高度分散的硅胶。
第二个实施方案的氯硅酸盐荧光剂(CS：Eu)与TbAG：Ce一起作为荧光剂颜料。(CS：Eu)与TbAG的混合比例是4∶6(重量比例)。这个实施方案的特征是特别高的色彩再现，其Ra＝85。在图4中示出这个实施方案的发射光谱。
常规方法(BG)和根据本发明的方法(BGG)的直接对比，得到以下结果：所选的BG方法，是将发射蓝光的InGaN芯片(峰为450nm)与常规的YAG：Ce结合起来。所选的根据本发明的BGG方法，是将相同的LED与TbAG：Ce和CS：Eu结合起来。在每一种情况下，这都会导致在x＝0.322，y＝0.366的色品位置上的色温达到6000K。简单的BG方法色彩再现只达到Ra＝72时，而BGG方法的色彩再现达到Ra＝80。红色再现也有明显的改善，即从R9＝-22到R9＝10。在图5中示出BGG方法的发射光谱。
另一个优选的白色LED的实施方案，除了采用InGaN芯片(在450nm发射蓝色)以外，还采用上述的氯硅酸盐荧光剂(CS：Eu)与YAG：Ce组合。如从图6所看到的，这个实施方案的特征是，这二种荧光剂具有极其相似的温度衰减行为。在容许采用的范围内(达到约100℃)，这二种荧光剂的温度衰减行为实际上是相同的，仅仅是略微与温度有关。为了与研究的混合柘榴石(Y0.33Gd0.63Ce0.04)Al5O12对比的其它柘榴石，具有明显较差的温度常数(在图6中，这种混合的柘榴石被称作(Y，Gd)AG：Ce)。因此，在这个实施方案中，在不同的温度条件下，能确保色品位置和其它照明数据特别稳定，这个实施方案包含高含量的Y(或采用Tb代替)作为RE(至少60摩尔％的RE晶格位置)。在图7中示出这个实施方案的发射光谱。它相应于色温8000K，和坐标为x＝0.294，y＝0.309的色品位置。色彩再现Ra＝77。这二种荧光剂的混合比例为4.6∶1。
图8示出一个作为发光设备的表面照明灯具20。它包括公共底座21，立方形的外壳22通过粘接固定在底座上。其上面具有一个公共顶盖23。这个立方形的外壳具有一些凹坑，其中容纳单个的半导体元件24。它们是发射UV的LED，发射峰为360nm。采用一些转换层25，将其转换成白光，转换层配置在UV辐射可达到的所有表面上。这些表面包括外壳侧壁、顶盖、和底部的内表面。转换层25由三种荧光剂组成，在采用根据本发明的荧光剂时，这三种荧光剂能在黄色、绿色和蓝色光谱区发射。

Claims (10)

1.一种发射白光的照明设备，其具有至少一个作为光源的LED，该LED在300-470nm区域发出主辐射，采用暴露在LED主辐射中的荧光剂，将这种辐射部分或全部转换成长波辐射，这种设备的特征在于，至少借助一种发射绿色的荧光剂，和至少一种发射黄色的荧光剂进行转换，前者来源于Eu-活化的钙镁氯硅酸盐类，后者来源于Ce-活化的稀土柘榴石类。
2.权利要求1的发射白光的照明设备，其特征在于，发射绿光的荧光剂满足了经验式Ca8-x-yEuxMnyMg(SiO4)4Cl2，式中x＝0.005至x＝1.6，y＝0至y＝0.1(在每一种情况下，都包括截止值)。
3.权利要求1的发射白光的照明设备，其特征在于，发射黄光的荧光剂，是按照通式RE3(Al，Ga)5O12：Ce的稀土(RE)Y、Gd、Lu、La和/或Tb的柘榴石，特别是按照通式YAG：Ce或TbAG：Ce，式中RE＝Y和/或Tb。
4.权利要求1的发射白光的照明设备，其特征在于，发射的主辐射在波长范围330-370nm，该主辐射照射到在蓝色区域(430-470nm)、绿色区域(490-525nm)、和黄色区域(545-590nm)有最大发射的三种荧光剂上。
5.权利要求1的发射白光的照明设备，其特征在于，发射的主辐射在蓝色波长范围430-470nm，如前述权利要求之一所述，该主蓝色辐射照射到在黄色区域(545-590nm)、和在绿色区域(490-525nm)有最大发射的二种荧光剂上。
6.权利要求1中所述的发射白光的发光转换LED，其特征在于，采用发射短波光的二极管，特别是基于Ga(In)N的二极管作为主辐射源。
7.权利要求1的发射白光的照明设备，其特征在于，在不另外采用锰的条件下，铕的比例为x＝0.1至x＝1.0。
8.权利要求1的发射白光的照明设备，其特征在于，这种照明设备是一种发光转换LED，其中荧光剂直接或间接地与芯片接触。
9.权利要求1的发射白光的照明设备，其特征在于，这种照明设备是一种LED阵列。
10.权利要求9的发射白光的照明设备，其特征在于，将至少一种荧光剂配置在一种光学装置上，该光学装置配置在LED阵列的前面。
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