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Crystalline Phase-tuned Multicolor Luminescence of Carbon Dots for White-light-emitting Diode Devices
Synthesis and Properties of Materials | Updated：2023-03-13
|
Crystalline Phase-tuned Multicolor Luminescence of Carbon Dots for White-light-emitting Diode Devices
- Chinese Journal of Luminescence Vol.44, Issue 2, (2023)
- Affiliations：School of Applied Science， Taiyuan University of Science and Technology,Taiyuan,China,030024;Shanxi Quantum Digital Technology Co. LTD,Taiyuan,China,030021
- Author bio：
- Funds：Fundamental Research Program of Shanxi Province(202103021224268);Key R & D Projects of Shanxi Province(201903D321111);Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(2021L298);National Natural Science Foundation of China(51502189)
- DOI：10.37188/CJL.20220316 CLC： O482.31;TN312.8
Published：05 February 2023，
Received：31 August 2022，
Revised：17 September 2022，
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Cite this article
张学文,苗润泽,许凤利等.晶相对碳点多色发光的调制及其在白光发光二极管器件中的应用[J].发光学报,2023,44(02):298-306.
ZHANG Xuewen,MIAO Runze,XU Fengli,et al.Crystalline Phase-tuned Multicolor Luminescence of Carbon Dots for White-light-emitting Diode Devices[J].Chinese Journal of Luminescence,2023,44(02):298-306.
张学文,苗润泽,许凤利等.晶相对碳点多色发光的调制及其在白光发光二极管器件中的应用[J].发光学报,2023,44(02):298-306. DOI： 10.37188/CJL.20220316.
ZHANG Xuewen,MIAO Runze,XU Fengli,et al.Crystalline Phase-tuned Multicolor Luminescence of Carbon Dots for White-light-emitting Diode Devices[J].Chinese Journal of Luminescence,2023,44(02):298-306. DOI： 10.37188/CJL.20220316.
Crystalline Phase-tuned Multicolor Luminescence of Carbon Dots for White-light-emitting Diode Devices
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"data": "，呈现出非晶特性。到目前，对碳点发光机理的研究尚未清晰，并且多数碳点为液态发光，当溶液干燥形成固态粉末时，由于出现聚集诱导猝灭（AIQ）效应，固态碳点的荧光强度会大幅衰减甚至猝灭"
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"data": "，这严重阻碍了碳点在LED、光电显示和照明等领域的推广应用。通常，小分子合成的碳点会因为高度脱水碳化导致碳点内部大共轭区域的形成，这为共振能量转移（RET）"
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"data": "或π-π相互作用"
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"data": "的发生提供了可能，固态时两种作用的加剧是碳点发生猝灭的原因"
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"data": "。为了解决这一问题，改变碳点结构、增大碳点之间距离和调控前驱体表面官能团"
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"data": "成为可选途径。其中，在制备固态碳点的过程中加入其他基质，例如高分子聚合物"
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"text": "10",
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{
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"data": "、淀粉"
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},
{
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"data": "、MOF"
},
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"data": [
{
"name": "text",
"data": "["
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"data": {
"text": "12",
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"data": [
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"data": "12"
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]
}
},
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}
]
},
{
"name": "text",
"data": "、硅酸盐"
},
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"data": [
{
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"data": "["
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"data": {
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},
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"data": "等对碳点进行分散包覆。这从根本上增大碳点之间的距离，从而有效抑制了固态碳点的猝灭。例如，Liu等使用柠檬酸和高分子聚合物b-PEI水热法制备出荧光量子产率（PLQYs）高达26%的绿色固态荧光碳点"
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]
},
{
"name": "text",
"data": "；Zhou等选择表面带负电荷的碳点，利用静电相互作用加入Ba"
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"data": [
{
"name": "text",
"data": "4"
}
]
},
{
"name": "text",
"data": "在碳点碳核周围生长形成复合物，同样制备了固态碳点，PLQYs由初始的15%提高到27%，且增强了光稳定性"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "15",
"type": "bibr",
"rid": "R15",
"data": [
{
"name": "text",
"data": "15"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。可见，通过不同种类基质分散包覆碳点的方法，能够有效减弱聚集诱导猝灭效应的发生，提高固态碳点的发光效率。然而，基质中低碳点加载量和基质对碳点有限的荧光发光调控作用"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "16",
"type": "bibr",
"rid": "R16",
"data": [
{
"name": "text",
"data": "16"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "18",
"type": "bibr",
"rid": "R18",
"data": [
{
"name": "text",
"data": "18"
}
]
}
}
],
"rid": [
"R16",
"R17",
"R18"
],
"text": "16-18",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，成为基质包覆碳点制备固态碳点的瓶颈。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "最近，部分研究说明了晶态基质对碳点发光的调控作用，这主要是硼酸和尿素作为前驱体的结果。Ding等使用柠檬酸和硼酸制备碳点复合物，其中刚性晶体B"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "O"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "作为发光中心，有效地稳定了碳点的能级，提高了复合物的PLQYs"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "19",
"type": "bibr",
"rid": "R19",
"data": [
{
"name": "text",
"data": "19"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。同样，硼酸作为基质通过结晶固定三重态，并通过与不同的有机前驱体反应形成了多色磷光碳点"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "20",
"type": "bibr",
"rid": "R20",
"data": [
{
"name": "text",
"data": "20"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。更有甚者，碳点基硼酸固态复合物通过研磨改变其从高能异质态到更低能的结晶态，这使得碳点在硼酸基质中趋于均匀分布，获得了超强（QY=48%）的室温磷光发射"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Wang等通过控制尿素含量，微波法合成三聚氰胺晶体，原位嵌套碳点成固态发光材料"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "22",
"type": "bibr",
"rid": "R22",
"data": [
{
"name": "text",
"data": "22"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。该过程不仅调控碳点的发光从黄色荧光变为红色的室温磷光，而且显著提高了PLQYs。可以看出，结晶体作为基质分散碳点的同时，对碳点的发光颜色和光效也进行了调控，这可能是由于晶体的结晶过程改变了碳点的碳核尺寸及表面态结构。这不仅实现了对碳点的分散，从而消除聚集诱导猝灭效应的发生，更是对碳点发光调控的有效途径之一。受此启发，本文提出了以邻苯二甲酸和领苯二胺为原料，在不同溶剂辅助下一步热解制备晶态多色荧光碳点的简便方法。通过光谱和形貌结构分析，研究晶体结构变化对固态碳点发光的影响，并利用所制备的固态碳点作为荧光粉，开展白光发光二极管（WLED）器件的应用研究。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2 实 验"
}
],
"level": "1",
"id": "s2"
}
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.1 试剂与原料"
}
],
"level": "2",
"id": "s2a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "所需化学药品和溶剂，包括邻苯二甲酸（≥99.5%，PA）、领苯二胺（≥98%，o-PD）由阿拉丁化学（中国）有限公司购买，无水乙醇、N-N二甲基甲酰胺（DMF）由天津光复科技发展有限公司购买。实验室用水均为去离子水。所有化学药品和溶剂使用前未做进一步纯化。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.2 样品制备"
}
],
"level": "2",
"id": "s2b"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "利用邻苯二甲酸和邻苯二胺通过微波法合成晶态CDs的步骤是：称取0.377 2 g邻苯二甲酸和0.122 8 g邻苯二胺到圆底烧瓶中，分散在20 mL去离子水中，超声5 min后，置于微波反应仪中以800 W的功率加热3 min。反应结束后，待冷却到室温，以10 000 r/min的速度离心，并在80 ℃对沉淀物进行12 h干燥处理，之后通过研磨过程得到蓝色发光的固态碳点（B-CDs）。将溶剂改为10 mL的N-N二甲基甲酰胺（DMF），重复上述步骤，待冷却到室温，转移到装有乙醇的离心管中，同样以10 000 r/min的速度离心，烘干，研磨得到绿色发光的碳点粉末（G-CDs）。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.3 样品表征"
}
],
"level": "2",
"id": "s2c"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "形貌测试采用JEM-2100型号的透射电子显微镜（TEM）；傅里叶红外光谱（FTIR）是由美国ThermoFisher公司生产的型号为Nicolet iS50在500~4 000 cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "波段采集；X射线光电子能谱采用美国PeakinElmer公司PHI5000C型仪器，利用Al-Kα X射线源辐照获得；吸收谱采用北京普析通用仪器有限责任公司TU-1901型紫外/可见分光光度计采集；光致发光谱、荧光寿命采用英国爱丁堡仪器FLS-1000型荧光分光光度计获得。"
}
]
}
]
}
]
},
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{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3 结果与讨论"
}
],
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"id": "s3"
}
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3.1 晶态碳点的形貌结构"
}
],
"level": "2",
"id": "s3a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "透射电子显微镜（TEM）能够直观地分析碳点纳米颗粒的形貌。如"
},
{
"name": "xref",
"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": "所示，B-CDs和G-CDs均为类球形结构，平均粒径分别为（3.57±0.06） nm和（3.51±0.06） nm，因此二者的尺寸相差无几。然而，B-CDs的晶格条纹间距为0.25 nm，这对应石墨烯结构的（100）晶面。而G-CDs晶格条纹间距为0.27 nm，除了可能对应石墨烯结构（020）的晶面"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "说明二者均具有类石墨结构之外"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "24",
"type": "bibr",
"rid": "R24",
"data": [
{
"name": "text",
"data": "24"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，增大的条纹间距可能是因为G-CDs碳核中更多的氮掺杂所致"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "25",
"type": "bibr",
"rid": "R25",
"data": [
{
"name": "text",
"data": "25"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "26",
"type": "bibr",
"rid": "R26",
"data": [
{
"name": "text",
"data": "26"
}
]
}
}
],
"rid": [
"R25",
"R26"
],
"text": "25-26",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。为了进一步了解碳点的结构形态，利用X光衍射光谱分析了碳点的晶态结构。如"
},
{
"name": "xref",
"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "所示，B-CDs和G-CDs有着明显的结晶峰，这不同于多数碳点的结构，且G-CDs有着更佳的结晶特性；其图谱呈现出不同于B-CDs的峰型和数量，说明二者具有不同的晶态结构。遗憾的是，目前尚不能确定二者的具体晶体结构对称性，这与已有的邻苯二甲酸结晶的结果不同"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "27",
"type": "bibr",
"rid": "R27",
"data": [
{
"name": "text",
"data": "27"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "28",
"type": "bibr",
"rid": "R28",
"data": [
{
"name": "text",
"data": "28"
}
]
}
}
],
"rid": [
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"R28"
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"text": "27-28",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。因此，可以初步认为本研究中获得的多色荧光固态纳米材料是由具有石墨化结构碳核的碳点和晶态基质包覆而成，晶态基质不仅分散了碳点，有效防止了碳点荧光猝灭的发生，晶态结构的变化可能也与固态碳点发光颜色改变存在关联。"
}
]
},
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"label": [
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"title": [
{
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"data": "B-CDs（a）和G-CDs（b）的TEM、HRTEM（右上）和粒径统计直方图（右下）。"
}
]
},
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"label": [
{
"name": "text",
"data": "Fig.1"
}
],
"title": [
{
"name": "text",
"data": "TEM images， HRTEM images（the inset in the top right corner）， the statistical histogram of particle sizes（the inset in the lower right corner） of B-CDs（a） and G-CDs（b）."
}
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}
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"title": [
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"data": "B-CDs和G-CDs的X光衍射（XRD）谱"
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"label": [
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"data": "Fig.2"
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"title": [
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"data": "XRD patterns of B-CDs and G-CDs"
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"data": [
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"data": "两种碳点的X射线光电子能谱（XPS）分析能够进一步确定碳点的元素含量和表面基团。如"
},
{
"name": "xref",
"data": {
"text": "图3",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3"
}
]
}
},
{
"name": "text",
"data": "所示，两种固态碳点均由C、O和N元素组成。B-CDs中三种元素的含量依次为72.88%、18.83%、8.29%。G-CDs中三种元素的含量依次为76.58%、12.65%、10.77%。显然，G-CDs中C和N元素明显增多，说明G-CDs形成过程中脱水缩合反应的加剧和氮掺杂的增多。三种元素详细的图谱分解结果呈现在"
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{
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"data": {
"text": "图4",
"type": "fig",
"rid": "F4",
"data": [
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"name": "text",
"data": "图4"
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"data": "中。可以看出，C 1s元素的光谱拟合后在284.62，285.27，288.51 eV处出现信号，对应为C—C/C=C、C—N/C—O和COOH基团。相较于B-CDs, G-CDs中C—C/C=C的增多和COOH基团的减少，均体现了通过脱水缩合反应加剧了碳化程度。N 1s元素的光谱在398.8 eV和400.44 eV处拟合出两个峰，分别属于吡啶氮和石墨氮。石墨氮的出现说明碳点的碳核中存在石墨结构，这与"
},
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"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": "中HRTEM的结果吻合。然而，在G-CDs中氮含量增多的前提下，G-CDs中石墨氮含量减少，吡啶氮却大幅增多，这说明G-CDs是通过碳核表面的吡啶氮基团和晶态基质成键形成，吡啶氮成为碳点的碳核和外部晶态基质在界面处结合成G-CDs的关键基团。O 1s元素的光谱可以拟合为两个峰：531.5 eV和 532.7 eV，分别对应于C=O和C—O基团。相较于B-CDs，G-CDs中两类基团几乎没有变化。"
}
]
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"lang": "zh",
"label": [
{
"name": "text",
"data": "图3"
}
],
"title": [
{
"name": "text",
"data": "B-CDs和G-CDs的光电子能谱"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.3"
}
],
"title": [
{
"name": "text",
"data": "XPS spectra of B-CDs and G-CDs"
}
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"label": [
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"data": "图4"
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],
"title": [
{
"name": "text",
"data": "B-CDs和G-CDs中C 1s（（a）、（d））、N 1s（（b）、（e）） 和O 1s（（c）、（f））元素的分解图谱。"
}
]
},
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"label": [
{
"name": "text",
"data": "Fig.4"
}
],
"title": [
{
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"data": "C 1s（（a）， （d））， N 1s（（b）， （e）） and O 1s（（c）， （f）） high-resolution spectra of B-CDs and G-CDs."
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"data": [
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"data": "与XPS相同，傅里叶红外光谱（FTIR）分析能够全面清晰地理解碳点中各基团的情况。如"
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}
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"data": "所示，B-CDs在3 478 cm"
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"data": "-1"
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{
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"data": "和3 064 cm"
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]
},
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"data": "处出现的 吸收峰分别是O—H和N—H的伸缩振动。在 2 639~ 2 876 cm"
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"data": "-1"
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]
},
{
"name": "text",
"data": "范围内的吸收峰归因于C—H的伸缩振动。而G-CDs中这些位置处只有微弱的信号，这体现了G-CDs中通过C—H/O—H/N—H官能团进行反应的加剧。在1 600~1 800 cm"
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"data": "-1"
}
]
},
{
"name": "text",
"data": "范围内主要是COOH官能团的吸收峰。COOH官能团在两色荧光碳点对应红外光谱中的不同，反映了前驱体邻苯二甲酸在生成两色荧光碳点过程中的作用并非一致，这也为其在形成B-CDs和G-CDs时生长成不同的晶体结构提供了佐证。1 586 cm"
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"data": [
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"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "处为芳香烃苯环结构中C=C的吸收峰，这同样说明了固态碳点中存在着类苯环骨架结构。接着，在G-CDs的光谱中，1 561 cm"
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"data": [
{
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"data": "-1"
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]
},
{
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"data": "和1 382 cm"
},
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"data": [
{
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"data": "-1"
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]
},
{
"name": "text",
"data": "处出现了更为明显的C=N基团振动峰，结合XPS中氮元素的能谱分析，这应该是吡啶氮增多所致。此外，在600~1 200 cm"
},
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"data": [
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"data": "-1"
}
]
},
{
"name": "text",
"data": "波数范围内B-CDs和G-CDs均存在C=C/C=N、C—O、C—N、C—O—C以及类苯环基团等的吸收峰。综上所述，两种发光颜色不同的固态碳点的形成是由于在不同溶剂的作用下，PA和o-PD脱水缩合形成碳点的同时在其外围生长晶态基质；然而DMF溶剂作用下碳核表面出现更多的吡啶氮结构基团，这导致晶态基质相结构不尽相同，通过晶态结构的变化实现了固态碳点的发光调控，最终导致了固态碳点不同性能的荧光发射。"
}
]
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"data": "图5"
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"data": "B-CDs和G-CDs的傅里叶红外光谱"
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]
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"label": [
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"data": "Fig.5"
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],
"title": [
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]
}
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"data": "3.2 晶态碳点的荧光特性"
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"text": "图6",
"type": "fig",
"rid": "F6",
"data": [
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"data": "图6"
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}
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"data": "展示了B-CDs和G-CDs的紫外-可见吸收（Abs）、激发（Ex）和发射（Em）光谱。"
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"data": {
"text": "图6",
"type": "fig",
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"data": [
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"data": "图6"
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}
},
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"data": "（a）中，B-CDs在300~400 nm波长区间存在强吸收，这是由于碳核边缘的C=O/C=N键的n-π跃迁"
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"data": "["
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"data": {
"text": "29",
"type": "bibr",
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"data": "29"
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"text": "30",
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"data": "30"
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]
}
}
],
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},
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"data": "。420~530 nm区间的吸收可能来自外层的晶态基质。而G-CDs 中两个区间的吸收加强，尤其是400~500 nm区间的吸收，使得二者几乎连接为一个强吸收区间（"
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"data": "（b））。激发谱（"
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]
},
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"data": "=470 nm）呈现了和吸收谱一致的变化，除在约350 nm处出现了强激发外，相较于B-CDs, G-CDs的最佳激发（"
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]
},
{
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"data": "=510 nm）红移至约450 nm处，这应该是晶态基质结构的变化所导致。因此，在吡啶环中C=N键和晶态基质结构变化的共同作用下，B-CDs实现蓝色发光，波长为475 nm；而G-CDs获得绿色发光，波长为511 nm。"
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"title": [
{
"name": "text",
"data": "B-CDs（a）和G-CDs（b）碳点的吸收、激发和发射光谱。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.6"
}
],
"title": [
{
"name": "text",
"data": "UV-Vis， excitation and emission spectra of B-CDs（a） and G-CDs（b）."
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]
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"data": "为了深入理解所制备晶态碳点的发光机制，采用时间相关单光子计数（TCSPC）技术，收集了二者的荧光寿命数据。"
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"text": "图7",
"type": "fig",
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"data": "给出了B-CDs（"
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"data": "=475 nm）和G-CDs（"
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"data": "=511 nm）的PL衰减曲线。"
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]
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"label": [
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"data": "Fig.7"
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],
"title": [
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"data": "Fluorescence attenuation curves of B-CDs and G-CDs"
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]
}
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"data": "基于非线性最小二乘法分析，B-CDs和G-CDs对应的荧光衰减曲线可用指数函数"
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"data": [
{
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"data": "I"
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]
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{
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"data": "（t）拟合"
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"data": [
{
"name": "text",
"data": "["
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"data": {
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"data": {
"text": "31",
"type": "bibr",
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"data": {
"text": "32",
"type": "bibr",
"rid": "R32",
"data": [
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"data": "32"
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}
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"data": "，公式如下："
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"data": "其中"
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"data": "为衰减时间常数，"
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"data": "的贡献指数。碳点的平均寿命（"
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"data": "利用两个函数拟合和计算的结果记录在"
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"data": "中。可以看出，B-CDs和G-CDs的荧光寿命曲线均符合双指数拟合规律，其中长寿命的"
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"data": "（1～2 ns）属于sp"
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"data": "3"
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]
},
{
"name": "text",
"data": "/sp"
},
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"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "结构共存的“碳核态”"
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"data": [
{
"name": "text",
"data": "["
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"data": [
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"data": {
"text": "32",
"type": "bibr",
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"data": "32"
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"data": "。晶态碳点的发光由二者复合决定，最终两条曲线拟合后得到碳点的平均寿命依次为6.0 ns和9.5 ns。具体地，B-CDs的发光寿命中"
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"data": "占88.4%，这意味着该晶态碳点的发光由碳核态主导。而G-CDs中"
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"data": "仅30.7%，且由B-CDs的1.9 ns变为5.3 ns。尽管"
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]
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"data": "的值没有明显变化，但其所占分数比例从B-CDs的11.6%提高到69.3%。结合上文分析，G-CDs的"
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"data": "2"
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]
},
{
"name": "text",
"data": "发光寿命应该源自于晶态基质结构变化所导致的碳点碳核边缘吡啶类基团的大量出现，这些处于碳点边缘和外围晶态基质界面的新生基团成为G-CDs荧光发光的主要源头。"
}
]
},
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{
"lang": "zh",
"label": [
{
"name": "text",
"data": "表1"
}
],
"title": [
{
"name": "text",
"data": "碳点的荧光衰减曲线拟合指数"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Tab.1"
}
],
"title": [
{
"name": "text",
"data": "Fitting index of fluorescence attenuation curve of B-CDs and G-CDs"
}
]
}
],
"note": [],
"table": [
{
"head": [
[
{
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"data": "样品"
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"data": [
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"data": [
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"data": "1"
}
]
},
{
"name": "text",
"data": "/%"
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]
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{
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"data": "A"
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},
{
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"data": [
{
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"data": "2"
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},
{
"name": "text",
"data": "/%"
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]
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"style": "border-top:solid;border-bottom:solid;",
"data": [
{
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"data": [
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{
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"data": "Ave"
}
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]
}
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]
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"data": "B‑CDs"
}
]
},
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"data": [
{
"name": "text",
"data": "5.3"
}
]
},
{
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"data": [
{
"name": "text",
"data": "88.4"
}
]
},
{
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"data": [
{
"name": "text",
"data": "9.2"
}
]
},
{
"align": "center",
"data": [
{
"name": "text",
"data": "11.6"
}
]
},
{
"align": "center",
"data": [
{
"name": "text",
"data": "6.0"
}
]
},
{
"align": "center",
"data": [
{
"name": "text",
"data": "1.144"
}
]
}
],
[
{
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"style": "border-bottom:solid;",
"data": [
{
"name": "text",
"data": "G‑CDs"
}
]
},
{
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"data": [
{
"name": "text",
"data": "1.9"
}
]
},
{
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"style": "border-bottom:solid;",
"data": [
{
"name": "text",
"data": "30.7"
}
]
},
{
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"data": [
{
"name": "text",
"data": "10.1"
}
]
},
{
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"style": "border-bottom:solid;",
"data": [
{
"name": "text",
"data": "69.3"
}
]
},
{
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"data": [
{
"name": "text",
"data": "9.5"
}
]
},
{
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"style": "border-bottom:solid;",
"data": [
{
"name": "text",
"data": "1.168"
}
]
}
]
],
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"data": "3.3 晶态碳点在WLED器件中的应用"
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"data": [
{
"name": "text",
"data": "纳米发光碳点材料制备简单、颜色丰富且光学性能稳定等优势成为其替代传统荧光粉用以封装LED器件的源动力"
},
{
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"data": [
{
"name": "text",
"data": "["
},
{
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"data": {
"data": [
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"name": "xref",
"data": {
"text": "34",
"type": "bibr",
"rid": "R34",
"data": [
{
"name": "text",
"data": "34"
}
]
}
},
{
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"data": "-"
},
{
"name": "xref",
"data": {
"text": "35",
"type": "bibr",
"rid": "R35",
"data": [
{
"name": "text",
"data": "35"
}
]
}
}
],
"rid": [
"R34",
"R35"
],
"text": "34-35",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。对于WLED器件产业，高光效、高显色指数、低色温（小于4 500 K）成为其作为照明产品的新需求。本文所制备晶态碳点作为荧光粉，在制作LED器件之前在玛瑙质研钵中细心研磨了数小时，直至其非常细腻。多次尝试之后，利用蓝色光B-CDs粉末和商用黄色荧光粉（（Sr,Ba）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "SiO"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "4"
}
]
},
{
"name": "text",
"data": "∶Eu"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2+"
}
]
},
{
"name": "text",
"data": "，主峰550~560 nm）、红色荧光粉（CaAlSiN"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "∶Eu"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2+"
}
]
},
{
"name": "text",
"data": "，主峰620~630 nm）按照质量比4∶2∶1进行混合，365 nm芯片作为激发光源封装后获得了如"
},
{
"name": "xref",
"data": {
"text": "图8",
"type": "fig",
"rid": "F8",
"data": [
{
"name": "text",
"data": "图8"
}
]
}
},
{
"name": "text",
"data": "所示的WLED器件。在电流为20 mA时采集相应的发射光谱如"
},
{
"name": "xref",
"data": {
"text": "图8",
"type": "fig",
"rid": "F8",
"data": [
{
"name": "text",
"data": "图8"
}
]
}
},
{
"name": "text",
"data": "（a）所示。可以看出，蓝色区域的峰强度远低于其他峰，这赋予了该器件在防蓝光光电产业领域的潜在应用价值。"
},
{
"name": "xref",
"data": {
"text": "图8",
"type": "fig",
"rid": "F8",
"data": [
{
"name": "text",
"data": "图8"
}
]
}
},
{
"name": "text",
"data": "（b）中，该WLED对应的色度坐标为（0.37,0.36），光效为8.04 lm/W，其相关色温（CCT）为4 061 K,说明该WLED器件为暖白光，显色指数（CRI）为88.4，说明其能够作为白光照明光源使用。"
}
]
},
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"caption": [
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"lang": "zh",
"label": [
{
"name": "text",
"data": "图8"
}
],
"title": [
{
"name": "text",
"data": "B-CDs和商用黄、红荧光粉混合封装的WLED器件的电致发光谱（a）及其色度图（b）。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.8"
}
],
"title": [
{
"name": "text",
"data": "Emission spectrum（a） and chromaticity diagram（b） of the WLED which was fabricated by mixing B-CDs powder with commercial yellow and red phosphors"
}
]
}
],
"subcaption": [],
"note": [],
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"data": [
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"data": "对于制备的绿色光碳点，它与同样的商用红色荧光粉按照质量比5∶1进行混合后，滴涂在蓝色光芯片（445~450 nm）上并进行烘干，获得的WLED器件如"
},
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"data": {
"text": "图9",
"type": "fig",
"rid": "F9",
"data": [
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"data": "图9"
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]
}
},
{
"name": "text",
"data": "（a）中插图所示。相较于"
},
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"text": "图8",
"type": "fig",
"rid": "F8",
"data": [
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}
},
{
"name": "text",
"data": "中的WLED器件，这里的WLED器件的发射光谱更为丰富，尤其是蓝绿光区。如"
},
{
"name": "xref",
"data": {
"text": "图9",
"type": "fig",
"rid": "F9",
"data": [
{
"name": "text",
"data": "图9"
}
]
}
},
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"name": "text",
"data": "（b）所示，该WLED器件在电流为20 mA时的色度坐标为（0.36,0.34），光效提高为12.7 lm/W，对应的显色指数（CRI）为85，相关色温（CCT）为4 478 K，这些光度学参数同样说明该WLED器件能够作为暖白光照明光源使用。尽管与其他使用碳点材料作为荧光粉制备的LED器件相比，这里分别使用两色光碳点封装的WLED器件具有优异的暖白光发光性能，且较高的显色指数也赋予了其在照明领域潜在的应用价值。但是，由于B-CDs的发射光谱和G-CDs的吸收谱存在较大的交叠（"
},
{
"name": "xref",
"data": {
"text": "图6",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6"
}
]
}
},
{
"name": "text",
"data": "），容易发生蓝光到绿光的“重吸收和重发射”"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
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"name": "blockXref",
"data": {
"data": [
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"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
}
]
}
},
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"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
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]
}
}
],
"rid": [
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"R37"
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"text": "36-37",
"type": "bibr"
}
},
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"data": "]"
}
]
},
{
"name": "text",
"data": "，因此两种色光的碳点无法作为两个基色共同封装在同一个WLED器件中。综上，本文所制备的蓝光和绿光晶态碳点能够作为荧光粉封装WLED器件，并且获得了优异的光度学参数，说明这些材料在LED、显示以及照明等光电设备上具有良好的应用前景。"
}
]
},
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"data": {
"id": "F9",
"caption": [
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"lang": "zh",
"label": [
{
"name": "text",
"data": "图9"
}
],
"title": [
{
"name": "text",
"data": "G-CDs和商用红色荧光粉混合封装的WLED器件的电致发光谱（a）及其色度图（b）"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.9"
}
],
"title": [
{
"name": "text",
"data": "Emission spectrum（a） and chromaticity diagram（b） of the WLED which was fabricated by mixing G-CDs powder with commercial red phosphors"
}
]
}
],
"subcaption": [],
"note": [],
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"data": "4 结 论"
}
],
"level": "1",
"id": "s4"
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},
{
"name": "p",
"data": [
{
"name": "text",
"data": "综上所述，在不同溶剂的辅助下，通过微波热解法一步合成了晶态基质包覆碳点且发光颜色不同的固态荧光材料。分析表明，外围包覆的晶态基质能够有效稳定地分散碳点，有效减少“聚集诱导猝灭效应”的发生。并且，溶剂作用致使静态基质结构的变化所导致的在基质和碳核界面处吡啶氮类基团的显著增多成为晶态碳点发光颜色改变的诱因。发现晶态结构相变对碳点荧光的影响为获得稳定发光的固态碳点材料提供了一种思路。所制备碳点发光性能优异，适合用于LED器件封装的应用开发。两种晶态碳点与商用荧光粉混合后获得的WLED器件，通过测试均获得了优异的光度学参数，其中的暖白光性能和高显色指数为这些材料在光电器件领域的应用奠定了基础。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "本文专家审稿意见及作者回复内容的下载地址："
},
{
"name": "extlink",
"data": {
"text": [
{
"name": "text",
"data": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/"
}
],
"href": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/"
}
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "CJL.20220316."
}
]
}
]
}
],
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"title": "Surface ligand dynamics-guided preparation of quantum dots-cellulose composites for light-emitting diodes"
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"response": [],
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"citeme": [
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"data": [
{
"name": "text",
"data": "张学文,苗润泽,许凤利等.晶相对碳点多色发光的调制及其在白光发光二极管器件中的应用[J].发光学报,2023,44(02):298-306."
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"text": "张学文,苗润泽,许凤利等.晶相对碳点多色发光的调制及其在白光发光二极管器件中的应用[J].发光学报,2023,44(02):298-306."
},
{
"data": [
{
"name": "text",
"data": "ZHANG Xuewen,MIAO Runze,XU Fengli,et al.Crystalline Phase-tuned Multicolor Luminescence of Carbon Dots for White-light-emitting Diode Devices[J].Chinese Journal of Luminescence,2023,44(02):298-306."
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"text": "ZHANG Xuewen,MIAO Runze,XU Fengli,et al.Crystalline Phase-tuned Multicolor Luminescence of Carbon Dots for White-light-emitting Diode Devices[J].Chinese Journal of Luminescence,2023,44(02):298-306."
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"fundinggroup": [
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"text": [
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"data": "山西省基础研究计划 （202103021224268）； 山西省重点研发计划 （201903D321111）； 山西省高等学校科技创新项目（2021L298）； 国家自然科学基金（51502189）"
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"data": "Supported by Fundamental Research Program of Shanxi Province（202103021224268）； Key R & D Projects of Shanxi Province（201903D321111）； Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi（2021L298）； National Natural Science Foundation of China（51502189）"
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"history": {
"received": "2022-08-31",
"revised": "2022-09-17",
"ppub": "2023-02-05",
"opub": "2023-03-13"
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"type": "research-article",
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"supplementary": [],
"journalTitle": "发光学报",
"issue": "2",
"volume": "44",
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}
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