CN111748341B - 吩噻嗪弱光上转换体系及其制备方法与应用 - Google Patents
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Abstract
本发明公开了吩噻嗪弱光上转换体系及其制备方法与应用,将发光剂、吩噻嗪盐在DMF溶剂中混合,得到吩噻嗪弱光上转换体系。本发明的目的报道一类即不含贵金属也不含重原子的吩噻嗪盐作为敏化剂,与红荧烯发光剂组成二元体系,可将655 nm的近红外光转化为~560 nm的黄光,这种红‑转‑黄上转换发光与硅电池耦合,可使硅电池的光电流密度提高。
Description
技术领域
本发明涉及一类不基于重原子效应(即不含重金属元素也不含卤素重原子)的三线态敏化技术,属于有机弱光上转换领域;具体涉及纯有机染料吩噻嗪盐敏化红荧烯实现红-转-黄弱光上转换。
背景技术
在三线态-三线态湮灭上转换(TTA-UC)过程中,首先是敏化剂吸收较低能量的光子,继而发生系间窜跃、三线态-三线态能量转移等微观过程,最后产生高能量上转换光子。可见,敏化剂的作用至关重要。有效的敏化剂应当具有大的系间窜跃几率、高的三线态能级和长的三线态寿命(后两者可确保大的三线态-三线态能量转移)。目前最常用的敏化剂为贵金属配合物,其原因在于贵金属配合物系间窜跃几率为100%,敏化效果好,上转换效率高;然而,贵金属敏化剂制备困难,产率低造价高。因此,含碘或溴的卤素敏化剂通常作为贵金属配合物的替代品,其原理也是在于重原子效应,且含碘或溴的卤素敏化剂在制备过程中存在着环境污染问题,因此,不含重原子的(heavy-atom-free)有机敏化剂的研发最受青睐。
目前,已报道的不含重原子(heavy-atom-free)的有机敏化剂仅三例。如2009年Castellano报道的2,3-丁二酮作为敏化剂,与激光染料2,5-二苯恶唑(PPO)为发光剂,在脱气的苯中实现了由442 nm的蓝光上转换为360 nm的紫外光;2016年马玉国利用咔唑基二氰基苯(CDCB)作为敏化剂,与2,7-二叔丁基苝(DBP)为发光剂复配,也实现了蓝光-转-紫外光上转换。2013年赵建章报道一种含氟的Bodipy二聚体作为敏化剂,与发光剂苝衍生物复配,实现了绿-转-蓝上转换。然而,目前尚未见非重原子敏化剂用于近红光-转-黄光的上转换报道。由于近红外光的上转换在利用太阳能方面具有潜在的应用价值,且使用不含重金属的有机化合物作为敏化剂具有成本低和环境友好等特点,具有更为重要的应用价值。
发明内容
本发明的目的报道一类即不含贵金属也不含重原子的吩噻嗪盐作为敏化剂,与红荧烯发光剂组成二元体系,可将655 nm的近红外光转化为~560 nm的黄光,这种红-转-黄上转换发光与硅电池耦合,可使硅电池的光电流密度提高1.4 mA/cm2。
本发明采用如下技术方案:
吩噻嗪弱光上转换体系,包括发光剂、吩噻嗪盐;进一步包括溶剂。
本发明公开了上述吩噻嗪弱光上转换体系的制备方法,包括以下步骤,将发光剂、吩噻嗪盐在溶剂中混合,经过氩气除氧,得到吩噻嗪弱光上转换体系。
优选的,发光剂为红荧烯,吩噻嗪盐为敏化剂,溶剂为DMF组成。
本发明中,将吩噻嗪弱光上转换体系装入比色皿中,在激发光照射下得到上转换光谱;激发光由655 nm半导体激光器发出,激发光强度为200~2000mW·cm2。
本发明中,所述敏化剂吩噻嗪盐的化学结构式如下:
所述发光剂的化学结构式如下:
本发明中,发光剂、吩噻嗪盐的摩尔比为0.5~3.5∶1。
本发明中,所述吩噻嗪弱光上转换体系的激发光波长为655nm,激发光强度为200~2000mW/cm2。
近年来,曾见报道三例非重原子(heavy-atom-free)的敏化剂材料,用于蓝光-转-紫外光或绿光-转-蓝光的上转换,尚未见非重原(heavy-atom-free)的敏化剂近红光-转-短波长的上转换报道,本发明首次公开了吩噻嗪弱光上转换体系可以实现近红光-转-黄光的上转换,由于近红外光的上转换在利用太阳能方面具有潜在的应用价值,且使用不含重金属的有机化合物作为敏化剂具有成本低和环境友好等特点,其应用前景更为诱人。
本发明将红荧烯与吩噻嗪盐(吩噻嗪A或吩噻嗪B或与吩噻嗪M)在DMF溶剂混合,通氩气除氧后,在655 nm半导体激光器激发下,可获得红-转-黄上转换上转换,发光峰位在~560 nm。
本发明公开了不含重原子效应的吩噻嗪盐作为三线态敏化剂,可以敏化红荧烯(作为发光剂),实现了吸收长波长(红光)转换为短波长(黄光)的TTA-UC上转换;在655nm激发光激发下,三种敏化剂敏化红荧烯,得出红-转-黄上转换效率(UC,%)顺序为:吩噻嗪A(0.085)>吩噻嗪B(0.083)>吩噻嗪M(0.049)。
附图说明
图1固定敏化剂浓度(200μm),上转换强度与发光剂浓度之间的关系(DMF),其中a、b、c分别对应吩噻嗪 A、吩噻嗪 B、吩噻嗪 M;
图2吩噻嗪与红荧烯二元体系随功率密度变化的上转换光谱图(DMF);
图3上转换体系与硅电池耦合示意图;
图4上转换体系硅电池的吸收光谱;
图5在655nm半导体激光器激发下,红-转-黄上转换驱动硅电池光电流曲线。
具体实施方式
下面结合附图以及实施例对本发明作进一步描述:
本实施例中,紫外-可见吸收光谱是在SHIMADZU UV2600型紫外-可见吸收光谱仪上测定的;荧光光谱是在Edinburgh FLS-920型荧光光谱仪上测定的。三线态-三线态湮灭上转换光谱是用SpectraScanPR655光谱仪测定的,用655 nm半导体激光器作为激发光源,比色皿规格为1 cm (长)×1cm(宽)×3cm(高);溶剂为光谱纯的DMF,其中DMF体系中需要氩气氛。
实施例:
吩噻嗪A-红荧烯双组份体系配制:按吩噻嗪A-红荧烯1:1摩尔比将吩噻嗪A溶液(DMF,1×10-2 mol/L)和红荧烯溶液(DMF,1×10-3 mol/L)加入到5mL容量瓶中,振荡混合,然后用DMF溶剂稀释定容至5mL,得到混合溶液,除氧得到吩噻嗪弱光上转换体系,其中,敏化剂吩噻嗪A的浓度固定为200μm。然后,按照同样的方法分别配制得到1:1.5、1:2和1:2.5 摩尔比例的吩噻嗪A-红荧烯双组份体系(其中,敏化剂吩噻嗪A的浓度固定为200μm)。
按照上述的方法,将吩噻嗪B替代吩噻嗪A,分别得到吩噻嗪B-红荧烯1:1、1:1.5、1:2和1:2.5 摩尔比例的吩噻嗪B-红荧烯双组份体系(其中,敏化剂吩噻嗪B的浓度固定为200μm)。
按照上述的方法,将吩噻嗪M替代吩噻嗪A,分别得到吩噻嗪M-红荧烯1:1、1:1.5、1:2和1:2.5 摩尔比例的吩噻嗪M-红荧烯双组份体系(其中,敏化剂吩噻嗪M的浓度固定为200μm)。
所述吩噻嗪盐敏化剂(吩噻嗪 A、吩噻嗪 B与吩噻嗪 M)的化学结构式如下:
所述发光剂红荧烯的化学结构式如下:
分别将三种敏化剂(吩噻嗪 A、吩噻嗪 B、吩噻嗪 M)与红荧烯复配,得到吩噻嗪弱光上转换体系,然后拧紧比色皿帽盖,测其上转换性能,结果如图1所示。
图2为敏化剂吩噻嗪A(吩噻嗪A/红荧烯=200μm /0.5mM)、吩噻嗪B(吩噻嗪B/红荧烯=200μm /0.6 mM)、吩噻嗪M(吩噻嗪M/红荧烯=200μm /0.5 mM)与发光剂红荧烯随功率密度变化的上转换光谱。据此,根据公式(2)计算得上转换效率。
公式(1)中,Ar和As分别是参考物质(酞菁锌)和样品(敏化剂)的吸光度。Fs代表上转换荧光强度,而Fr代表酞菁锌的下转换荧光强度。Fr是酞菁锌(在DMSO中为20%)的荧光量子产率。ηs和ηr分别是发光剂/敏化剂双组份溶液和酞菁锌溶液的折射率。该方程乘以2倍,这说明需要吸收两个的光子才能产生一个上转换的光子。公式(2)中,ε为敏化剂在激发光处(655 nm)的摩尔吸光系数,η为二元体系的总上转换能力。计算结果列于表1。
采用常规方法,将上转换体系(吩噻嗪M/红荧烯二元体系)与硅电池耦合,其示意图见图3。用655 nm半导体激光器激发二元体系,使后者发出563 nm的黄光,该黄光可被硅电池吸收(见图4,硅电池的吸收光谱)。为了排除其它波长的光对测试的干扰,测试是在暗室里进行的,同时在硅电池的前端放上655 nm滤光片,该滤光片能够滤去655~660 nm波段的光。
测试的光电流曲线见图5所示。可见,吩噻嗪M(200μm)/红荧烯(0.5mM)的黄光辐照的硅电池的光电流密度为1.5 mA/cm2,而吩噻嗪M (300μm)/红荧烯(0.5mM)的黄光辐照的硅电池的光电流为1.6 mA/cm2。同时,用655nm激光器辐照空白对照样(即没有吩噻嗪/红荧烯的DMF空白溶剂),发现光电流曲线微乎其微,这说明吩噻嗪M/红莹烯的黄光上转换强度与硅电池耦合具有明显的光电转换效果。
Claims (7)
2.根据权利要求1所述的应用,其特征在于,敏化剂与发光剂的摩尔比为1∶0.5~3.5。
3.吩噻嗪弱光上转换体系,其特征在于,所述吩噻嗪弱光上转换体系包括发光剂红荧烯、权利要求1所述吩噻嗪盐。
4.根据权利要求3所述吩噻嗪弱光上转换体系,其特征在于,发光剂、吩噻嗪盐的摩尔比为1~3.5∶1。
5.根据权利要求3所述吩噻嗪弱光上转换体系,其特征在于,所述上转换体系的激发光波长为655 nm,激发光强度200~2000mW×cm2。
6.权利要求3所述吩噻嗪弱光上转换体系的制备方法,其特征在于,包括以下步骤,将发光剂、吩噻嗪盐在DMF溶剂中混合,得到吩噻嗪弱光上转换体系。
7.权利要求3所述吩噻嗪弱光上转换体系在制备近红光-转-黄光材料中的应用。
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