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Crystalline(phthalic acid)-induced Luminescence of Carbon Dots for White-light-emitting Diode Devices
Synthesis and Properties of Materials | Updated：2022-04-20
|
Crystalline(phthalic acid)-induced Luminescence of Carbon Dots for White-light-emitting Diode Devices Enhanced Publication
- Chinese Journal of Luminescence Vol.43, Issue 4, (2022)
- 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：Key R & D Projects of Shanxi Province(201903D321111);National Natural Science Foundation of China(51502189);Shanxi Graduate Education Innovation Project(2020SY441)
- DOI：10.37188/CJL.20220003 CLC： O482.31
Published：01 April 2022，
Received：06 January 2022，
Revised：18 January 2022，
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Cite this article
Bo-rui LYU, Jun-chao CUI, Wen-jun XU, et al. Crystalline(phthalic acid)-induced Luminescence of Carbon Dots for White-light-emitting Diode Devices. [J]. Chinese Journal of Luminescence 43(4):528-535(2022)
Bo-rui LYU, Jun-chao CUI, Wen-jun XU, et al. Crystalline(phthalic acid)-induced Luminescence of Carbon Dots for White-light-emitting Diode Devices. [J]. Chinese Journal of Luminescence 43(4):528-535(2022) DOI： 10.37188/CJL.20220003.
Crystalline(phthalic acid)-induced Luminescence of Carbon Dots for White-light-emitting Diode Devices Enhanced Publication
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"name": "text",
"data": "。以丙酮代替N,N-二甲基甲酰胺(DMF)溶剂，上述C-dots又获得发射波长为594 nm的橙红色荧光，但FLQYs从8%显著提高到29%"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "14",
"type": "bibr",
"rid": "R14",
"data": [
{
"name": "text",
"data": "14"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Lu等利用NaOH/HCl溶液调节反应溶液的酸碱度，同样制备了硫脲掺杂的碳点，由最初的蓝色发光转变为610 nm的红色发光，FLQY=24%"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "18",
"type": "bibr",
"rid": "R18",
"data": [
{
"name": "text",
"data": "18"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。可见，硫脲作为S和N掺杂剂有利于实现长波长的荧光发射。然而，这些碳点溶液在固化成碳点粉末的过程中极易变质或发生严重的ACQ。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "目前，利用基质如高分子聚合物"
},
{
"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": "、硅酸盐"
},
{
"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": "、淀粉"
},
{
"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": "、MOFs"
},
{
"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": "和无机盐"
},
{
"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": "等分散碳点进而增加碳点之间的距离，以避免共振能量转移(RET)或π-π相互作用的发生"
},
{
"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": "。这样做看似解决了固态碳点聚集诱导猝灭(ACQ)问题，但也产生了新的问题：如二次处理制备固化C-dots基复合材料的难度增大"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "25",
"type": "bibr",
"rid": "R25",
"data": [
{
"name": "text",
"data": "25"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、光学性能不可控"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "26",
"type": "bibr",
"rid": "R26",
"data": [
{
"name": "text",
"data": "26"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、且加入过多的C-dots后仍会面临ACQ"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "27",
"type": "bibr",
"rid": "R27",
"data": [
{
"name": "text",
"data": "27"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。因此，开发一种简单和高度可控的方法来实现固态碳点材料的制备仍具挑战。本文提出了一种以邻苯二甲酸(PA)和硫脲(TU)为原料，在乙酸乙酯溶剂辅助下一步热解制备固态碳点材料的简易方法。制备的碳点呈橙红色，具有多峰发射和高固态荧光量子产率。结果表明，PA热解形成的晶态物分散并固定了碳点，从而抑制了碳点的聚集，减弱了荧光猝灭。并利用所制备碳点，开展了白光发光二极管(WLED)器件的应用研究。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"label": [
{
"name": "text",
"data": "2"
}
],
"title": [
{
"name": "text",
"data": "实验"
}
],
"level": "1",
"id": "s2"
}
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"label": [
{
"name": "text",
"data": "2.1"
}
],
"title": [
{
"name": "text",
"data": "样品制备"
}
],
"level": "2",
"id": "s2a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "邻苯二甲酸(≥99.5%,PA)和硫脲(≥99.0%,TU)由阿拉丁化学(中国)有限公司提供。乙酸乙酯等试剂购于天津丰川化学试剂技术有限公司。所有化学试剂、试剂和溶剂使用前未做进一步纯化操作。称取1.371 6 g PA和0.628 4 g TU至聚四氟乙烯反应釜内，向其加入10 mL乙酸乙酯溶液。将反应釜放入高温干燥箱内进行220 ℃恒温加热，反应3 h后待其冷却至室温。取出反应釜内合成的针状晶态材料至50 mL的烧杯中，加入30 mL去离子水进行超声，过滤去除未反应物，反复两次。最后在80 ℃烘箱中干燥4 h，得到样品。该样品被研磨成粉末，待使用。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"label": [
{
"name": "text",
"data": "2.2"
}
],
"title": [
{
"name": "text",
"data": "样品表征"
}
],
"level": "2",
"id": "s2b"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "透射电子显微镜(TEM)图像由JEOL/JEM-2100采集；扫描电子显微镜(SEM)图片由JEOL/JSM-7200F仪器在20 kV加速电压下拍摄记录；傅里叶红外(FTIR)光谱采集波段为500~4 000 cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "(Nicolet iS50, Thermo Fisher，美国);X射线光电子能谱(XPS)采用PHI-5000C ESCA系统，采用Al-Kα X射线辐射获得(PerkinElmer Inc.,USA)；吸收光谱由日本产日立U-3900紫外/可见分光光度计采集；使用FLS-1000荧光分光光度计记录荧光光谱、寿命和量子产率(爱丁堡仪器，英国)。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"label": [
{
"name": "text",
"data": "2.3"
}
],
"title": [
{
"name": "text",
"data": "基于C-dots的 LED封装"
}
],
"level": "2",
"id": "s2c"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "将C-dots粉末与OE-6550(道康宁)硅胶以1∶1的质量比混合，然后快速滴在波长395 nm的芯片上，固化后得到LED器件。同样，C-dots粉、黄绿粉SiAlON∶Eu"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2+"
}
]
},
{
"name": "text",
"data": "和蓝粉BaMgAl"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "10"
}
]
},
{
"name": "text",
"data": "O"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "17"
}
]
},
{
"name": "text",
"data": "∶Eu"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2+"
}
]
},
{
"name": "text",
"data": "按照一定的质量比与上述硅胶进行混合，涂在波长395 nm芯片上(三安光电)，在150 ℃下干燥1 h，得到WLED器件。"
}
]
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"label": [
{
"name": "text",
"data": "3"
}
],
"title": [
{
"name": "text",
"data": "结果与讨论"
}
],
"level": "1",
"id": "s3"
}
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"label": [
{
"name": "text",
"data": "3.1"
}
],
"title": [
{
"name": "text",
"data": "碳点制备及发光性质"
}
],
"level": "2",
"id": "s3a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "在碳点的热解法制备中，反应温度和时间是影响碳点发光效果的两个关键因素。"
},
{
"name": "xref",
"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": "为不同时间(3~12 h，间隔3 h)和不同温度(140~240 ℃，间隔20 ℃)时所制备碳点的照片。可以看出，除了140 ℃的弱红光外，碳点在紫外光照射下能发出耀眼的橙红光，发光亮度和颜色略微不同。"
},
{
"name": "xref",
"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "为不同时间所制备碳点的发射谱(Em)。显然，所有光谱均呈现了三个峰：586,632,690 nm。随着时间的增加，三个峰的位置没有发生变化。但峰强比值"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "632"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "586"
}
]
},
{
"name": "text",
"data": "、"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "690"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "586"
}
]
},
{
"name": "text",
"data": "和"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "690"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "632"
}
]
},
{
"name": "text",
"data": "逐渐增大，这意味着碳点长波长发光峰(632 nm和690 nm)占比增大，碳点发光颜色整体红移。然而从"
},
{
"name": "xref",
"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": "可以看出，随着时间的增加，碳点发光亮度似乎变弱了。"
}
]
},
{
"name": "fig",
"data": {
"id": "F1",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图1"
}
],
"title": [
{
"name": "text",
"data": "不同反应时间(3~12 h)和反应温度(140~240 ℃)下制备碳点的照片(日光和紫外光照射)"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig. 1"
}
],
"title": [
{
"name": "text",
"data": "Photos of the resultant CDs in different time and tempreatures(day and UV lights)"
}
]
}
],
"subcaption": [],
"note": [],
"graphics": [
{
"print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=26724435&type=",
"small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=26724430&type=",
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"name": "fig",
"data": {
"id": "F2",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图2"
}
],
"title": [
{
"name": "text",
"data": "不同反应时间(3~12 h)碳点的发射光谱"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig. 2"
}
],
"title": [
{
"name": "text",
"data": "Emission spectra of the CDs in time of 3-12 h"
}
]
}
],
"subcaption": [],
"note": [],
"graphics": [
{
"print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=26724440&type=",
"small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=26724445&type=",
"big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=26724442&type="
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},
{
"name": "p",
"data": [
{
"name": "xref",
"data": {
"text": "图3",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3"
}
]
}
},
{
"name": "text",
"data": "为不同温度下所制备碳点的发射光谱。同样，随着温度的升高碳点发射光谱中的三个峰并未发生位置的变化，然而随着温度达到200~240 ℃，比值"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "632"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "586"
}
]
},
{
"name": "text",
"data": "、"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "690"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "586"
}
]
},
{
"name": "text",
"data": "和"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "690"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "632"
}
]
},
{
"name": "text",
"data": "发生了变化："
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "690"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "586"
}
]
},
{
"name": "text",
"data": "几乎维持不变，"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "632"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "586"
}
]
},
{
"name": "text",
"data": "和"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "690"
}
]
},
{
"name": "text",
"data": "/"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "632"
}
]
},
{
"name": "text",
"data": "大幅增加，到达240 ℃时趋于稳定。综上，为了实现长波长区碳点的高效发光，在3 h、240 ℃所制备的碳点最为符合。"
},
{
"name": "xref",
"data": {
"text": "图4",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4"
}
]
}
},
{
"name": "text",
"data": "呈现了该条件下所制备碳点的紫外-可见光吸收光谱、激发和发射光谱。C-dots的吸收光谱(Abs)在270~600 nm处有多个非常宽且强的峰，产生原因包括sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "杂化区域的类石墨烯碎片的π-π"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "*"
}
]
},
{
"name": "text",
"data": "跃迁和类石墨烯碎片与邻苯二甲酸通过sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "杂化嵌在晶态基体中的跃迁，以及C—O/C—N/C—S和O—C"
},
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{
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"data": "O表面基团的n-π"
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{
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"data": [
{
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"data": "*"
}
]
},
{
"name": "text",
"data": "跃迁等。而激发谱(Ex)显示，与碳点关联的跃迁能级形成了激发，在大于400 nm区间的吸收并未对激发产生贡献。激发光谱(Ex)中出现了三个明显的峰，尽管与发射光谱(Em)间存在较大的斯托克斯位移("
},
{
"name": "text",
"data": ">"
},
{
"name": "text",
"data": "100 nm)，但与发射光谱中出现的三个峰形成对照，最终C-dots实现了17%的荧光量子产率。"
}
]
},
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"data": "不同反应温度(140~240 ℃)碳点的发射光谱"
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},
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"label": [
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"data": "Fig. 3"
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],
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"data": "Emission spectra of the CDs from 140 to 240 ℃"
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]
}
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"data": "240 ℃、3 h制备碳点的吸收和光致发光光谱。"
}
]
},
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"label": [
{
"name": "text",
"data": "Fig. 4"
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],
"title": [
{
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"data": "Absorption, Excitation and emission spectra of the CDs in 240 ℃, 3 h."
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]
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"data": "碳点的形貌结构"
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"level": "2",
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{
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"data": "如"
},
{
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"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5"
}
]
}
},
{
"name": "text",
"data": "所示，C-dots呈团簇状准球形，粒径不均匀，平均粒径为(4.48±0.07) nm(如"
},
{
"name": "xref",
"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5"
}
]
}
},
{
"name": "text",
"data": "右下角的插图所示)。"
},
{
"name": "xref",
"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5"
}
]
}
},
{
"name": "text",
"data": "右上角的HRTEM照片中C-dots的晶格条纹间距为0.21 nm，与石墨(010)面一致"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "28",
"type": "bibr",
"rid": "R28",
"data": [
{
"name": "text",
"data": "28"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，暗示了制备的C-dots的碳核中拥有多的类石墨结构。为了深入了解C-dots的结构，利用Jade 6.5对C-dots的XRD谱进行指标化，结果与标准PDF卡数据(No.PDF#45-1680)的邻苯二甲酰亚胺晶体结构高度吻合("
},
{
"name": "xref",
"data": {
"text": "图6",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6"
}
]
}
},
{
"name": "text",
"data": ")。受上述分析启发，C-dots复合材料由邻苯二甲酰亚胺晶态物作基质、石墨化的碳点嵌套其中组成，该晶态基质固定了C-dots之间的空间位置，有效阻止了ACQ的发生。"
}
]
},
{
"name": "fig",
"data": {
"id": "F5",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图5"
}
],
"title": [
{
"name": "text",
"data": "碳点的TEM、HRTEM(右上)和粒径统计直方图(右下)。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig. 5"
}
],
"title": [
{
"name": "text",
"data": "TEM image, HRTEM image(the inset in the top right corner), the statistical histogram of particle sizes(the inset in the lower right corner) of C-dots."
}
]
}
],
"subcaption": [],
"note": [],
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],
"title": [
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"name": "text",
"data": "碳点的XRD图"
}
]
},
{
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"label": [
{
"name": "text",
"data": "Fig. 6"
}
],
"title": [
{
"name": "text",
"data": "XRD pattern of C-dots powder"
}
]
}
],
"subcaption": [],
"note": [],
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},
{
"name": "p",
"data": [
{
"name": "text",
"data": "通过XPS测试能够进一步确定C-dots粉体的组成和表面基团。如"
},
{
"name": "xref",
"data": {
"text": "图7",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7"
}
]
}
},
{
"name": "text",
"data": "所示，C-dots粉体的XPS信号主要表现为O、N、C和S元素，其含量依次为15.33%、5.78%、78.48%和0.4%。部分元素详细的图谱分解结果如"
},
{
"name": "xref",
"data": {
"text": "图8",
"type": "fig",
"rid": "F8",
"data": [
{
"name": "text",
"data": "图8"
}
]
}
},
{
"name": "text",
"data": "~"
},
{
"name": "xref",
"data": {
"text": "10",
"type": "fig",
"rid": "F10",
"data": [
{
"name": "text",
"data": "10"
}
]
}
},
{
"name": "text",
"data": "所示，C 1s光谱拟合后在284.7,285.7,288.8 eV处出现信号，对应为C—C/C"
},
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"data": "C、C—N/C—O/C—S和—COOH键或基团。N 1s谱在398.9,399.7,400.1 eV拟合出3个峰，分别归属于吡啶N、吡咯N和石墨N。石墨N的出现为碳纳米点的生成提供了有力佐证，这与"
},
{
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"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
{
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"data": "图5"
}
]
}
},
{
"name": "text",
"data": "中的HRTEM结果一致。S 2p谱应该包含两个以162.9 eV和164.1 eV为中心的峰，分别代表C—S—C共价键的2p"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "3/2"
}
]
},
{
"name": "text",
"data": "和2p"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "1/2"
}
]
},
{
"name": "text",
"data": "，这在大多数S掺杂文献中都出现过"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "14",
"type": "bibr",
"rid": "R14",
"data": [
{
"name": "text",
"data": "14"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "15",
"type": "bibr",
"rid": "R15",
"data": [
{
"name": "text",
"data": "15"
}
]
}
}
],
"rid": [
"R14",
"R15"
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"text": "14-15",
"type": "bibr"
}
},
{
"name": "text",
"data": ","
},
{
"name": "xref",
"data": {
"text": "17",
"type": "bibr",
"rid": "R17",
"data": [
{
"name": "text",
"data": "17"
}
]
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "。而168.28 eV处出现的C-SO"
},
{
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"data": [
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"data": [
{
"name": "text",
"data": "x"
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},
{
"name": "text",
"data": "("
},
{
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"data": [
{
"name": "text",
"data": "x"
}
]
},
{
"name": "text",
"data": "=2,3,4)峰证实了硫元素通过氧化作用形成的表面态，这为分析碳点的发光机理提供了更多的可能性。以上表明，在乙酸乙酯溶剂的辅助下，PA和TU的脱水缩合反应形成了碳点，碳点的碳核经由碳核表面的官能团与邻苯二甲酰亚胺晶态物键合形成该碳点复合材料，这使得C-dots在不同溶剂、pH值和温度条件下能够保持稳定。"
}
]
},
{
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{
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"name": "text",
"data": "碳点的XPS图"
}
]
},
{
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"label": [
{
"name": "text",
"data": "Fig. 7"
}
],
"title": [
{
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"data": "XPS spectrum of C-dots powder"
}
]
}
],
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"data": "碳点的C 1s元素分解图谱"
}
]
},
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"label": [
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}
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],
"title": [
{
"name": "text",
"data": "碳点的N 1s 元素分解图谱"
}
]
},
{
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"label": [
{
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"data": "Fig. 9"
}
],
"title": [
{
"name": "text",
"data": "High-resolution spectra of N 1s in C-dots"
}
]
}
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"subcaption": [],
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"data": "图10"
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"title": [
{
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"data": "碳点的S 2p 元素分解图谱"
}
]
},
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"label": [
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"data": "Fig. 10"
}
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"title": [
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"data": "High-resolution spectra of S 2p in C-dots"
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"data": [
{
"name": "text",
"data": "如"
},
{
"name": "xref",
"data": {
"text": "图11",
"type": "fig",
"rid": "F11",
"data": [
{
"name": "text",
"data": "图11"
}
]
}
},
{
"name": "text",
"data": "所示，我们进一步采用时间相关单光子计数(TCSPC)技术，通过探测C-dots在发射波长"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "λ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "em"
}
]
},
{
"name": "text",
"data": "=586,631,690 nm处的荧光寿命，来了解C-dots荧光的起源。基于非线性最小二乘分析，C-dots对应的荧光衰减曲线可用指数函数"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I"
}
]
},
{
"name": "text",
"data": "("
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "t"
}
]
},
{
"name": "text",
"data": ")拟合"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "29",
"type": "bibr",
"rid": "R29",
"data": [
{
"name": "text",
"data": "29"
}
]
}
},
{
"name": "text",
"data": "-"
},
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"data": {
"text": "30",
"type": "bibr",
"rid": "R30",
"data": [
{
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"data": "30"
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]
}
}
],
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"R30"
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"text": "29-30",
"type": "bibr"
}
},
{
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}
]
},
{
"name": "text",
"data": "，公式如下："
},
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{
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"data": "为衰减时间常数，"
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"data": "表示"
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"data": "的贡献指数。C-dots的平均寿命("
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"data": [
{
"name": "text",
"data": "τ"
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]
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"data": "avg"
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"name": "text",
"data": ")由如下公式计算："
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"data": "(2)"
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"data": "结果得到585 nm的发射由3个寿命值组成，分别是"
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"data": "τ"
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"data": "1"
}
]
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{
"name": "text",
"data": "=0.59 ns (38.83%),"
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"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
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"name": "text",
"data": "2"
}
]
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{
"name": "text",
"data": "=2.39 ns (45.71%),"
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"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
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"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "=9.37 ns (15.46%);632 nm的发射对应的值为"
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"name": "italic",
"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "=0.62 ns (44.26%),"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "=2.35 ns (40.79%),"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "=8.40 ns (14.96%);690 nm发射对应的值为"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "=0.72 ns (44.34%),"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "=2.77 ns (46.04%),"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "=10.59 ns (9.61%)。可以看出，在不同的发射波长下，均拟合出"
},
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"data": "τ"
}
]
},
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"name": "sub",
"data": [
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"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "、"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "τ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "两个短寿命和"
},
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"data": [
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"name": "text",
"data": "τ"
}
]
},
{
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"data": [
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"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "的长寿命。一般来说，寿命的三指数行为意味着C-dots材料有多个发射位点，其特征是表面态(长寿命)和碳核态(短寿命)的复合"
},
{
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"data": [
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"data": "["
},
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"data": {
"data": [
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"name": "xref",
"data": {
"text": "30",
"type": "bibr",
"rid": "R30",
"data": [
{
"name": "text",
"data": "30"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "31",
"type": "bibr",
"rid": "R31",
"data": [
{
"name": "text",
"data": "31"
}
]
}
}
],
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"text": "30-31",
"type": "bibr"
}
},
{
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"data": "]"
}
]
},
{
"name": "text",
"data": "。根据TEM、XRD和XPS的分析结果，碳核态应分别来自碳点本身和由PA晶态物包裹形成的核壳结构，两者主导了C-dots的发射。表面态"
},
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]
},
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"data": "占据了较少的比例，但却可能是影响发光颜色的主要因素。最终，3个波长的发射对应的平均寿命依次为2.77,2.49,2.61 ns，这意味着表面态和碳核态对不同发射并无分工，而是共同决定了3个波长的发射。"
}
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"data": "三个发射波长下碳点的寿命曲线"
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"label": [
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"data": "Fig. 11"
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"data": "Fluorescence decay curves of C-dots at "
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"data": "=585, 632, 690 nm"
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"title": [
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"data": "基于碳点的LED器件"
}
],
"level": "2",
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"data": [
{
"name": "text",
"data": "利用固态发光碳点纳米材料取代传统荧光粉以封装LED电致发光器件是碳点材料的应用之一。在制作LED器件之前，C-dots晶态材料需在玛瑙研钵中耐心研磨数小时。"
},
{
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"data": {
"text": "图12",
"type": "fig",
"rid": "F12",
"data": [
{
"name": "text",
"data": "图12"
}
]
}
},
{
"name": "text",
"data": "为使用所制备碳点粉末与硅胶混合后滴在商用芯片上获得的LED器件(见插图)，在电流为20 mA时采集相应的发射光谱。显然，这与单一的C-dots晶态材料的发射光谱一致，说明碳点材料在硅胶中发光的稳定性，更使得C-dots纳米材料适合作为一个良好的橙色光发光荧光材料。如"
},
{
"name": "xref",
"data": {
"text": "图13",
"type": "fig",
"rid": "F13",
"data": [
{
"name": "text",
"data": "图13"
}
]
}
},
{
"name": "text",
"data": "所示，该LED器件在电流为20 mA时的色度坐标为(0.54,0.33)，对应的显色指数(CRI)为55，相关色温(CCT)约为1 700 K。此外，由于C-dots荧光粉的多峰发射特性，特别适合制备高CRI的WLED器件。"
},
{
"name": "xref",
"data": {
"text": "图14",
"type": "fig",
"rid": "F14",
"data": [
{
"name": "text",
"data": "图14"
}
]
}
},
{
"name": "text",
"data": "的插图是在硅胶中按照一定质量比例混合黄绿色SiAlON∶Eu"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2+"
}
]
},
{
"name": "text",
"data": "和蓝色BaMgAl"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "10"
}
]
},
{
"name": "text",
"data": "O"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "17"
}
]
},
{
"name": "text",
"data": "∶Eu"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2+"
}
]
},
{
"name": "text",
"data": "商用荧光粉，和前文所制备橙红色发光C-dots粉体材料，滴在发射波长为395 nm的UV LED芯片上制备的WLED器件。其在20 mA电流下发射的电致发光光谱主要表现为4个峰，其中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15",
"type": "fig",
"rid": "F15",
"data": [
{
"name": "text",
"data": "图15"
}
]
}
},
{
"name": "text",
"data": "显示了该WLED对应的色度坐标为(0.43,0.40),CRI接近82,CCT为3 118 K。与其他使用碳点材料作为荧光粉制备的LED器件相比"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
},
{
"name": "text",
"data": ","
},
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"name": "blockXref",
"data": {
"data": [
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"name": "xref",
"data": {
"text": "32",
"type": "bibr",
"rid": "R32",
"data": [
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"data": "32"
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}
},
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"data": "-"
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"data": {
"text": "33",
"type": "bibr",
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{
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"data": "，该WLED器件具有优异的暖白光发光性能。综上，上述所制备橙红色发光碳点材料在封装照明设备上具有很大的应用潜力。"
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"label": [
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"data": "结论"
}
],
"level": "1",
"id": "s4"
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},
{
"name": "p",
"data": [
{
"name": "text",
"data": "综上所述，在DMF溶剂的辅助下，通过硫氮元素共掺杂的方法一锅热解简单合成了结晶诱导的荧光C-dots材料。通过调节反应温度和时间，碳点材料均能发出明亮的橙红色荧光，然而通过发射光谱分析，在3 h、240 ℃获得的碳点发光效果更佳。所制备碳点晶态材料具有多峰发射特性，这应该是由于包裹在碳点单体(或碳点团簇)外的邻苯二甲酸晶态物有效隔离了碳点，从而高效地防止了碳点荧光猝灭的发生。由于C-dots具有良好的固态光学性能，将其用于封装LED。所封装WLED通过测试，获得了显色指数接近82，相关色温为3 118 K等优异的光度学参数，这些结果为该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：http://cjl.lightpublishing.cn/thesisDetails#10.37188/CJL.20220003."
}
]
}
]
}
],
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"reflist": {
"title": [
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"data": "参考文献："
}
],
"data": [
{
"id": "R1",
"label": "[1]",
"citation": [
{
"lang": "en",
"text": [
{
"name": "text",
"data": "YANG H Y"
},
{
"name": "text",
"data": ", "
},
{
"name": "text",
"data": "LIU Y L"
},
{
"name": "text",
"data": ", "
},
{
"name": "text",
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"response": [],
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"articlemeta": {
"doi": "10.37188/CJL.20220003",
"clc": [
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"data": "O482.31"
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"dc": [
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"text": [
{
"name": "text",
"data": "山西省重点研发计划（201903D321111）；国家自然科学基金（51502189）；山西省研究生教育创新项目（2020SY441）资助"
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"data": "Supported by Key R & D Projects of Shanxi Province (201903D321111); National Natural Science Foundation of China (51502189); Shanxi Graduate Education Innovation Project (2020SY441)"
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],
"history": {
"received": "2022-01-06",
"revised": "2022-01-18",
"ppub": "2022-04-01",
"opub": "2022-04-20"
},
"copyright": {
"data": [],
"year": "2022"
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},
"appendix": [],
"type": "research-article",
"ethics": [],
"supplementary": [],
"journalTitle": "发光学报",
"issue": "4",
"volume": "43",
"originalSource": []
}
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