阳离子铱(III)配合物掺杂的SiO2微粉的制备及在发光二极管中的应用

doi:10.15541/jim20150179

无机材料学报 ›› 2015, Vol. 30 ›› Issue (11): 1195-1200.DOI: 10.15541/jim20150179 CSTR: 32189.14.10.15541/jim20150179

阳离子铱(III)配合物掺杂的SiO₂微粉的制备及在发光二极管中的应用

孟国云, 陈泽宇, 刘永, 魏丽莹, 汪正良, 唐怀军

(云南民族大学化学与生物技术学院, 云南省高校民族地区资源清洁转化重点实验室, 云南省生物高分子功能材料工程技术研究中心, 昆明 650500)

收稿日期:2015-04-13 修回日期:2015-05-24 出版日期:2015-11-20 网络出版日期:2015-10-20
作者简介:孟国云(1988–), 男, 硕士研究生. E-mail: mengguoyun@sina.com
基金资助:
国家自然科学基金(21262046, 21261027);云南省教育厅理工重点资助项目(2011Z003)

Cationic Iridium(Ⅲ) Complex Doped in SiO₂ Micropowder: Preparation and Application in Light-emitting Diodes

MENG Guo-Yun, CHEN Ze-Yu, LIU Yong, WEI Li-Ying, WANG Zheng-Liang, TANG Huai-Jun

(Key Laboratory of Resource Clean Conversion in Ethnic Regions, Education Department of Yunnan, and Engineering Research Center of Biopolymer Functional Materials of Yunnan, School of Chemistry and Biotechnology, Yunnan Minzu University, Kunming 650500, China)

Received:2015-04-13 Revised:2015-05-24 Published:2015-11-20 Online:2015-10-20
About author:MENG Guo-Yun. E-mail: mengguoyun@sina.com
Supported by:
National Natural Science Foundation of China (21262046, 21261027);Key Scientific Research Fund of Yunnan Province Education Department (2011Z003)

摘要/Abstract

摘要：

将硅酸乙酯水解得SiO₂溶胶, 陈化1 d后掺入15.0wt%阳离子铱(III)配合物[Ir(ppy)₂(o-phen)][PF₆](ppy: 2-苯基吡啶; o-phen: 1-乙基-2-(4-(5-(4-叔丁基苯基)-1, 3, 4-噁二唑-2-基)-苯基)-1H-咪唑并[4, 5-f][1, 10]菲啰啉), 45 ℃恒温3 d后室温放置10 d得干凝胶, 再经研磨和150 ℃干燥8 h制得黄色发光微粉。将所得的发光微粉按6.0、9.0、12.0、15.0、18.0和21.0wt%掺入到环氧树脂中, 作为下转换发光材料涂敷在395 nm发射的InGaN芯片上制备成LED器件。掺入12wt% SiO₂微粉的LED发光性能最佳, 在40.0 mA正向电流和5 V反向电压下, 该LED达到最大发光效率51.9 lm/W, CIE色坐标为(0.42, 0.42)。

关键词: 阳离子铱(III)配合物, 发光二极管, 下转换发光材料, 溶液-凝胶法

Abstract:

A silica sol was prepared from tetraethyl orthosilicate by hydrolysis method, then 15wt% cationic iridium(III) complex [Ir(ppy)₂(o-phen)][PF₆] (ppy: 2-phenylpyridine, o-phen: 1-Ethyl-2-(4-(5-(4-tert-butylphenyl)-1, 3, 4-oxadiazol- 2-yl)phenyl)-1H-imidazo[4, 5-f][1, 10]phenanthroline) was doped after the sol being aged for 1 d. The sol was turned into xerogel after it was heated at 45 ℃ for 3 d and kept at room temperature for 10 d, then the yellow luminescent micropowder was obtained after the silica xerogel being grounded and dried at 150 ℃ for 8 h. The luminescent micropowder was blended in epoxy resin at concentrations of 6.0wt%, 9.0wt%, 12.0wt%, 15.0wt%, 18.0wt% and 21.0wt%, and the resultant mixtures were coated on 395 nm-emitting InGaN chips as the down-conversion luminescent materials in light-emitting diodes (LEDs). The LED prepared from poxy resin blended with 12wt% cationic iridium(Ⅲ) complex doped SiO₂ micropowder exhibited the best luminescent performances, with the maximum efficiency of 51.9 lm/W at 40.0 mA forward current and 5 V reverse voltage, the corresponding CIE color coordinate was (0.42, 0.42).

Key words: cationic iridium(III) complex, light-emitting diode, down-conversion luminescent materials, Sol-Gel

中图分类号:

O614

孟国云, 陈泽宇, 刘永, 魏丽莹, 汪正良, 唐怀军. 阳离子铱(III)配合物掺杂的SiO₂微粉的制备及在发光二极管中的应用[J]. 无机材料学报, 2015, 30(11): 1195-1200.

MENG Guo-Yun, CHEN Ze-Yu, LIU Yong, WEI Li-Ying, WANG Zheng-Liang, TANG Huai-Jun. Cationic Iridium(Ⅲ) Complex Doped in SiO₂ Micropowder: Preparation and Application in Light-emitting Diodes[J]. Journal of Inorganic Materials, 2015, 30(11): 1195-1200.

图/表 7

图1 阳离子铱(III)配合物的化学结构式

Fig. 1 Chemical structural formula of the cationic iridium(III) complex

图2 (a)阳离子铱(III)配合物掺杂的SiO2干凝胶, (b)紫外光下的阳离子铱(III)配合物掺杂的SiO2微粉和(c、d)阳离子铱(III)配合物掺杂的SiO2微粉的SEM照片

Fig. 2 (a) Cationic iridium(III) complex doped in SiO2 xerogel and (b) in SiO2 micropowder under UV light, and (c, d) SEM images of cationic iridium(III) complex doped in SiO2 micropowder

图3 阳离子铱(III)配合物掺杂的SiO2微粉的TG和DTA曲线

Fig. 3 TG and DTA curves of the cationic iridium(III) complex doped in SiO2 micropowder

图4 在CH2Cl2溶液中(1.0×10-5 mol/L) 阳离子铱(III)配合物, 掺杂在SiO2微粉中阳离子铱(III)配合物和纯的粉末状阳离子铱(III)配合物的归一化激发光谱(Ex)和发射光谱(Em)

Fig. 4 Normalized excitation (Ex) and emission (Em) spectra of the cationic iridium (III) complex in CH2Cl2 solution (1.0×10-5 mol/L), doped in SiO2 micropowder and pure cationic iridium (III) complex powder λEx = 395 nm, λEm = 580 nm

图5 在环氧树脂中掺入不同浓度阳离子铱(III)配合物掺杂的SiO2微粉制备的LEDs的归一化发射光谱

Fig. 5 Normalized emission spectra of the LEDs prepared from epoxy resin blended with different concentrations of cationic iridium(Ⅲ) complex doped SiO2 micropowder at 20 mA forward current and 5 V reverse voltage

表1 掺入不同浓度铱(III)配合物掺杂的SiO2微粉制备的LEDs的发光效果

Table 1 Performances of LEDs prepared from iridium(Ⅲ) complex doped SiO2 micropowder with different blending concentrations

Blending concentration/wt%	Forward current/mA	Luminous flux/lm	η_{p, max}/(lm·W^-1)	λ_max/nm	CIE/(x, y)
6.0	20.0	0.57	8.2	576	(0.43, 0.45)
9.0	20.0	0.84	12.0	577	(0.44, 0.46)
12.0	20.0	1.93	32.2	577	(0.47, 0.49)
12.0	40.0	7.26	51.9	579	(0.42, 0.42)
12.0	60.0	4.97	23.6	582	(0.39, 0.37)
15.0	20.0	0.75	10.8	578	(0.48, 0.49)
18.0	20.0	0.73	10.4	578	(0.49, 0.49)
21.0	20.0	0.59	8.4	578	(0.48, 0.49)

图6 在环氧树脂中掺入12wt%阳离子铱(III)配合物掺杂的SiO2微粉制备的LED在不同正向电流强度下的归一化发射光谱(5 V反向电压下)

Fig. 6 Normalized emission spectra at different forward current of the LED prepared from epoxy resin blended with 12wt% cationic iridium(Ⅲ) complex doped SiO2 micropowder (at 5 V reverse voltage)

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阳离子铱(III)配合物掺杂的SiO₂微粉的制备及在发光二极管中的应用

Cationic Iridium(Ⅲ) Complex Doped in SiO₂ Micropowder: Preparation and Application in Light-emitting Diodes

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