CN102977884B - 荧光材料与白光发光装置 - Google Patents
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Abstract
本发明提供一种荧光材料,如下具有化学式:(Sr1-a-b-cMaTmbEuc)3Si1-dGedO5,其中:Sr、M、Tm、及Eu为二价金属离子,且M是Ca、Ba、Mg、或上述的组合;Si及Ge为四价离子;0≤a≤0.5;0≤b≤0.03;0<c≤0.1;以及0<d≤0.005。上述荧光材料可与黄色荧光材料搭配蓝光激发光源,以形成暖色系的白光发光装置。
Description
技术领域
本发明是关于一种荧光材料,更特别关于此种材料于白光发光装置的应用。
背景技术
利用具省电、低污染与寿命长等优点的白光发光二极管(light emittingdiodes;LEDs)作为照明光源已是现代照明主要发展趋势。为取得理想的照明光源,除LED本身亮度外,所选用的荧光体亦为影响光源整体发光效率的关键因素。
目前市面上常见白光LED为蓝色LED(发射波长为460-480nm)配合黄色荧光粉,因缺乏红色成份,其演色性较差。故搭配红色、黄色荧光粉及组合的白光LED将比只含有单一黄色荧光粉的白光LED具更高演色性。但目前市面常见的蓝光激发的红色荧光粉以氮化物及硫化物为主(发射波长为620-650nm),氮化物最大优点是稳定度高,但其原料为氮化锶及氮化钡,再加上有些氮化物荧光粉甚至需要高温高压制程,所以成本极为高昂。硫化物虽然成本较低,但其具极差的化学稳定性,故不适合做为LED的荧光粉。近来利用硅酸盐材料的桔红色荧光粉搭配黄色荧光粉及蓝色LED而成的高演色性白光LED,则是不错的选择。目前市面上常见硅酸盐桔红光荧光粉为BOS系列的BOS600(CaSr)2SiO4:Eu2+荧光粉(发射波长为580-600nm),其成本较低发光效率也不差,化学稳定性也优于硫化物,但缺点是热稳定性仍不够好。综上所述,目前亟需发光效率不差、成本低、及热稳定性佳的桔红色荧光粉。
发明内容
本发明的目的在于提供一发光效率不差、成本低、及热稳定性佳的桔红色荧光粉,其可与黄色荧光材料搭配蓝光激发光源,以形成暖色系的白光发光装置。
本发明一实施方式提供一种荧光材料,具有化学式如下:(Sr1-a-b-cMaTmbEuc)3Si1-dGedO5;其中Sr、M、Tm、及Eu为二价金属离子,且M是Ca、Ba、Mg、或上述的组合;Si及Ge为四价离子;0≤a≤0.5;0≤b≤0.03;0<c≤0.1;以及0<d≤0.005。
本发明一实施方式提供一种白光发光装置,包括蓝光激发光源;以及黄色荧光材料与上述的荧光材料。
本发明的优点在于:本发明的荧光材料通过在现有的桔黄光荧光材料的主体Sr3SiO5中另外掺杂元素来增加其发光效率,因而成本低且热稳定性佳;本发明的这一桔红色荧光粉可与黄色荧光材料搭配蓝光激发光源,形成暖色系的白光发光装置。
附图说明
图1a是本发明一实施例中,不同Si/Ge 比例的荧光材料(Sr0.99Eu0.01)3Si1-dGedO5的吸收光谱;
图1b是本发明一实施例中,不同Si/Ge比例的荧光材料(Sr0.99Eu0.01)3Si1-dGedO5的发射光谱;
图2a是本发明一实施例中,不同Sr/Tm及Si/Ge比例的荧光材料(Sr0.99-bTmbEu0.01)3Si1-dGedO5的吸收光谱;
图2b是本发明一实施例中,不同Sr/Tm及Si/Ge比例的荧光材料(Sr0.99-bTmbEu0.01)3Si1-dGedO5的发射光谱;
图3是本发明一实施例中,不同Sr/Ba/Tm及Si/Ge比例的荧光材料(Sr0.99-a-bBaaTmbEu0.01)3Si1-dGedO5的发射光谱;
图4是本发明一实施例中,(Sr0.86Ba0.1Tm0.003Eu0.01)3Si0.999Ge0.001O5的X-ray绕射图;以及
图5是本发明一实施例中,黄色荧光材料YAG、(Sr0.757Ba0.23Tm0.003Eu0.01)3Si0.999Ge0.001O5、蓝光LED、及上述三者组合成的白光发光装置的CIE坐标。
具体实施方式
本发明提供一系列硅酸盐荧光材料,其化学式如式1:
(Sr1-a-b-cMaTmbEuc)3Si1-dGedO5 (式1)
在式1中,Sr、M、Tm、及Eu为二价金属离子,且M为Ca、Ba、Mg、或上述的组合。Si与Ge为四价离子。其中,0≤a≤0.5;0≤b≤0.03;0<c≤0.1;以及0<d≤0.005。上述荧光材料的主要机制为在原来桔黄光荧光材料的主体Sr3SiO5中,另外掺杂元素来增加其发光效率。
若式1中的荧光材料化学式中的a=b=0时,上述的荧光材料的化学式为(Sr1-cEuc)3Si1-dGedO5,其发射光谱为580nm±5nm。
若式1中的荧光材料化学式中的a=0,且0<b≤0.03时,上述的荧光材料的化学式为(Sr1-b-cTmbEuc)3Si1-dGedO5,其发射光谱为580nm±5nm。
若式1中的荧光材料化学式中的M为Ba,0.1≤a≤0.5,且0<b≤0.03及0<d≤0.005时,上述的荧光材料的化学式为(Sr1-a-b-cBaaTmbEuc)3Si1-dGedO5,其发射光谱为600nm±5nm。
上述荧光材料可与黄色荧光材料如Y3Al5O12:Ce(简称YAG)、Tb3Al5O12:Ce、(BaSr)2SiO4:Eu、或上述的组合结合,搭配蓝光的激发光源如发光二极管或激光二极管,即完成白光发光装置。在本发明一实施方式中,此白光发光装置为暖色系的白光发光装置。
此外,本发明也提供上述硅酸盐荧光材料的制造方法,包含以下步骤:首先,混合以下成份得到混合物:(1)具有锶的含氧化合物;(2)具有硅的含氧化合物;(3)具有锗的含氧化合物;(4)具有铕的含氧化合物;与(5)具有铥及/或M的含氧化合物。接着对混合物进行烧结,且烧结温度介于1300℃-1600℃之间。当混合物升温至烧结温度后,维持在烧结温度下1至4小时,以烧结混合物。根据本发明的实施方式,含氧化合物可为氧化物、碳酸化合物、或硝酸化合物。
为了让本发明的上述和其它目的、特征、和优点能更明显易懂,下文特举数实施例配合所附附图,作详细说明如下:
【实施例】
实施例1
依化学剂量比例取氧化锶、氧化铕、氧化硅、及氧化锗,均匀混合后研磨10分钟,并放入坩锅,置入高温炉,于5%的氢气与95%氮气(体积比)的混合气体下加热至1300℃~1600℃烧结,以制备不同Si/Ge比例的(Sr0.99Eu0.01)3Si1-dGedO5,其中d分别为0、0.001、0.01、及0.05。图1a是不同Si/Ge比例的荧光材料(Sr0.99Eu0.01)3Si1-dGedO5的吸收光谱而图1b是不同Si/Ge比例的荧光材料(Sr0.99Eu0.01)3Si1-dGedO5的发射光谱。当d为0时,(Sr0.09Eu0.01)3SiO5的激发波段介于深紫外光的250nm至绿光的550nm左右,发射光谱则为桔黄的580nm左右。当Ge的掺杂量d=0.001时,其激发波段和发光波长并无改变,但可增加发光效率。适量添加Ge可增加长波段的激发效率,如图1a所示。
实施例2
依化学剂量比例取氧化锶、氧化铕、氧化硅、氧化锗、及氧化铥,均匀混合后研磨10分钟,并放入坩锅,置入高温炉,于5%的氢气与95%氮气的混合气体下加热至1300℃~1600℃烧结,以制备不同Sr/Tm及Si/Ge比例的(Sr0.99-bTmbEu0.01)3Si1-dGedO5,其中(b,d)分别为(0,0)、(0.003,0)、(0,0.01)、及(0.003,0.001)。图2a是不同Sr/Tm及Si/Ge比例的荧光材料(Sr0.99-bTmbEu0.01)3Si1-dGedO5的吸收光谱,而图2b是不同Sr/Tm及Si/Ge比例的荧光材料(Sr0.99-bTmbEu0.01)3Si1-dGedO5的发射光谱。由图2b可知,不论添加Ge或Tm均能增加发光效率,但同时适量添加二种元素则可进一步增加荧光材料的发光效率。
实施例3
依化学剂量比例取氧化锶、氧化铕、氧化硅、氧化锗、氧化铥及氧化钡,均匀混合后研磨10分钟,并放入坩锅,置入高温炉,于5%的氢气与95%氮气的混合气体下加热至1300℃~1600℃烧结,以制备不同Sr/Ba/Tm及Si/Ge比例的(Sr0.99-a-bBaaTmbEu0.01)3Si1-dGedO5,其中(a,b,d)分别为(0,0,0)、(0,0.003,0.001)、(0.1,0.003,0.001)、(0.17,0.003,0.001)、及(0.23,0.003,0.001)。图3是不同Sr/Ba/Tm及Si/Ge比例的荧光材料(Sr0.99-a-bBaaTmbEu0.01)3Si1-dGedO5的发射光谱。
因蓝光激发黄光荧光粉的白光LED需要桔红色荧光粉来增加其演色性,进一步添加碱土金属元素Ba的添加来位移发光波长,如图3所示。掺杂Tm及Ge可增加发光效率,而掺杂Ba可位移发光。无掺杂的荧光材料发射580nm左右的桔黄光,而添加Ba的荧光材料的放射光谱将位移至597nm的桔红光。图4则为上述产物的X光衍射图。由图中得知除了少许不发光原料的SiO2的相,绝大部分是由Sr3SiO5所组成。另上述的桔红色的荧光材料搭配黄色的荧光材料YAG及蓝光LED时,可形成色温3000K的暖白光LED,如图5所示。
虽然本发明已以数个较佳实施例揭露如上,然其并非用以限定本发明,任何熟习此技艺者,在不脱离本发明的精神和范围内,当可作任意的更动与润饰,因此本发明的保护范围当视后附的权利要求书所界定的范围为准。
Claims (5)
1.一种荧光材料,具有化学式如下:
(Sr1-a-b-cMaTmbEuc)3Si1-dGedO5;
其中Sr、M、Tm、及Eu为二价金属离子,且M是Ca、Ba、Mg、或上述的组合;
Si及Ge为四价离子;
0≤a≤0.5;0<b≤0.03;0<c≤0.1;以及0<d≤0.005。
2.如权利要求1所述的荧光材料,具有化学式如下:
(Sr1-b-cTmbEuc)3Si1-dGedO5,其发射光谱为580nm±5nm;
其中0<b≤0.03。
3.如权利要求1所述的荧光材料,具有化学式如下:
(Sr1-a-b-cBaaTmbEuc)3Si1-dGedO5,其发射光谱为600nm±5nm;
其中0.1≤a≤0.5;0<b≤0.03及0<d≤0.005。
4.一种白光发光装置,包括:
一蓝光激发光源;以及
一黄色荧光材料与权利要求1所述的荧光材料。
5.如权利要求4所述的白光发光装置,其中所述黄色荧光材料为Y3Al5O12:Ce、Tb3Al5O12:Ce、(BaSr)2SiO4:Eu、或上述的组合。
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US20130057139A1 (en) | 2013-03-07 |
US8721924B2 (en) | 2014-05-13 |
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