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生物基碳点制备及其在LED器件上的应用
特邀报告 | 更新时间：2021-09-03
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生物基碳点制备及其在LED器件上的应用 增强出版
- Preparation and Application of Bio-based Carbon Dots for LED Chips
- 发光学报 2021年 42卷 第8期 (2021)
- 作者机构：云南师范大学 可再生能源材料先进技术与制备教育部重点实验室,云南,昆明,650500;云南师范大学 化学化工学院,云南,昆明,650500;云南民族大学 化学与环境学院,云南,昆明,650500
- 作者简介：
- 基金信息：国家自然科学基金(U1802257);国家自然科学基金-云南联合基金(U1702254);云南省高校科技创新团队支持计划资助项目
- DOI：10.37188/CJL.20210159 中图分类号： O482.31
纸质出版日期：2021-08-01，
收稿日期：2021-04-30，
修回日期：2021-05-12，
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引用本文
王琴, 杨雯, 庄镜儒, 等. 生物基碳点制备及其在LED器件上的应用[J]. 发光学报, 2021, 42(8):1314-1322.
Qin WANG, Wen YANG, Jing-ru ZHUANG, et al. Preparation and Application of Bio-based Carbon Dots for LED Chips[J]. Chinese Journal of Luminescence, 2021, 42(8):1314-1322.
王琴, 杨雯, 庄镜儒, 等. 生物基碳点制备及其在LED器件上的应用[J]. 发光学报, 2021, 42(8):1314-1322. DOI： 10.37188/CJL.20210159.
Qin WANG, Wen YANG, Jing-ru ZHUANG, et al. Preparation and Application of Bio-based Carbon Dots for LED Chips[J]. Chinese Journal of Luminescence, 2021, 42(8):1314-1322. DOI： 10.37188/CJL.20210159.
生物基碳点制备及其在LED器件上的应用 增强出版
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"data": "，具有高发光性、良好的生物相容性、低毒性和低成本等特点，在光电子、储能、光伏、生物医学、农业等领域具有广阔的应用前景"
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"data": "。2004年，人们在制备单壁碳纳米管的副产物中发现了碳点"
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"data": "。Liu等在2007年报道了利用蜡烛燃烧的煤烟制备碳点，并发现其有彩色荧光效应，这标志着碳点的合成原料首次从无机材料扩展到了有机、生物质材料"
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"data": "。碳点的制备方法通常分为两大类:“自上而下”法和“自下而上”法"
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"data": "。“自上而下”法是采用石墨、石墨烯、碳纳米管和富勒烯等无机碳材料作为碳源，利用激光消融、电化学、电弧放电、化学氧化法等方法，获得碳点"
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"data": "。但该方法制备过程复杂，反应条件苛刻，通常涉及高温、高压，难以实现规模生产，其表面性质的改性、掺杂需要进一步处理，大多需要多步合成"
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"data": "。“自下而上”法通常以有机碳源为原料，采用水热、微波、热解等方法处理得到碳点，由于生物基材料本身富含氮、磷、硫等元素及各种含氧官能团，经过对原料的筛选，可一步合成目标掺杂的碳点，其过程简化，反应条件简单，易实现规模化生产，也对生物质的利用和废弃物处理提供了新的思路"
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"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": "16",
"type": "bibr",
"rid": "R16",
"data": [
{
"name": "text",
"data": "16"
}
]
}
}
],
"rid": [
"R14",
"R15",
"R16"
],
"text": "14-16",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。碳点最引人关注的是其光致发光特性"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "17",
"type": "bibr",
"rid": "R17",
"data": [
{
"name": "text",
"data": "17"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "18",
"type": "bibr",
"rid": "R18",
"data": [
{
"name": "text",
"data": "18"
}
]
}
}
],
"rid": [
"R17",
"R18"
],
"text": "17-18",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。虽然迄今碳点的光致发光机理尚未完全清楚，但大多认为碳点表现出的光致发光行为是由于碳原子以sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "杂化共轭π域和sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "杂化态组成，其中，C"
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"data": "C 键具有sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "杂化共轭π域，其π-π"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "*"
}
]
},
{
"name": "text",
"data": "跃迁能够捕获短波长光子，通常是在紫外光区(260~320 nm)表现出明显的光学特征吸收峰，还可延伸到可见光范围"
},
{
"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": "。通常认为碳点中的sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
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]
},
{
"name": "text",
"data": "共轭π域是荧光发射的固有中心，同时，碳点的 sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "共轭π域还有可能被 sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "杂化碳态(如C—OH,C—NH"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "等)包围。因此，除了sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "共轭π域电子-空穴对("
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "e"
}
]
},
{
"name": "text",
"data": "-"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "h"
}
]
},
{
"name": "text",
"data": ")的复合，碳点核心和表面态之间的非辐射电子跃迁也可促进碳点的荧光发射"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "20",
"type": "bibr",
"rid": "R20",
"data": [
{
"name": "text",
"data": "20"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
}
],
"rid": [
"R20",
"R21",
"R22",
"R23"
],
"text": "20-23",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "目前，荧光碳点主要为单峰发射"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "24",
"type": "bibr",
"rid": "R24",
"data": [
{
"name": "text",
"data": "24"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "25",
"type": "bibr",
"rid": "R25",
"data": [
{
"name": "text",
"data": "25"
}
]
}
}
],
"rid": [
"R24",
"R25"
],
"text": "24-25",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，且大多只在液体溶液中表现出良好的光致发光效应，当其以固体形式存在时，由于团聚引起的荧光猝灭，导致难以直接获得高效的荧光碳点粉体"
},
{
"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": "。目前主流方法是将碳点分散于无机介质或者高分子介质中，使其能以固态形式应用于LED器件中"
},
{
"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": [
"R27",
"R28"
],
"text": "27-28",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。本文采用生物质材料为碳源，采用一锅热解法制备出碳点和掺杂碳点，该类碳点具有双发射荧光和固态发光特性；探讨了其结构与发光行为间的关系。将所得碳点直接应用于LED器件，简化了器件制作工艺，为开发固态荧光材料提供了一种环保、简便的新思路。"
}
]
}
]
},
{
"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 荧光碳点的制备及表征"
}
],
"level": "2",
"id": "s2a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "主要试剂及原料:硼酸(分析纯，天津市风船化学试剂科技有限公司)；尿素(分析纯，天津市风船化学试剂科技有限公司)；乙醇(分析纯，国药集团化学试剂有限公司)；硫酸奎宁(分析纯，上海阿拉丁生化科技股份有限公司)；大麦苗(中国安徽);K"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "SiF"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "6"
}
]
},
{
"name": "text",
"data": "∶Mn"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "4+"
}
]
},
{
"name": "text",
"data": "(深圳英特美光电有限公司)。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "主要仪器:样品红外光谱、紫外-可见吸收光谱和光电子能谱(XPS)分别用傅里叶变换红外光谱仪(美国Thermo Fisher,IS10)、紫外-可见分光光度计(美国安捷伦，Agilent HP8453E)和 X 射线光电子能谱仪(美国赛默飞K-Alpha+)进行测试。样品的激发和发射光谱通过荧光分光光度计(美国瓦里安技术有限公司，Cary Eclipse FL 1011M003)进行测试。粉体量子产率通过附带积分球的荧光分光光度计(日本日立，F7000)进行测试。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "制备方法:本文采用一锅热解法制备大麦苗基碳点(RM-CDs)及其掺杂碳点，分别为硼掺杂大麦苗基碳点(RMB-CDs)、氮掺杂大麦苗基碳点(RMN-CDs)、硼氮双掺大麦苗基碳点(RMBN-CDs)，工艺流程如"
},
{
"name": "xref",
"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": "所示。具体实验方法如下:"
}
]
},
{
"name": "fig",
"data": {
"id": "F1",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图1"
}
],
"title": [
{
"name": "text",
"data": "生物基碳点一锅热解法制备流程示意图"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.1"
}
],
"title": [
{
"name": "text",
"data": "Process diagram of one-pot pyrolysis preparation method for bio-based carbon dots"
}
]
}
],
"subcaption": [],
"note": [],
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"data": [
{
"name": "text",
"data": "前处理:取一定质量的大麦苗，用蒸馏水洗净晒干后，用粉碎机粉碎成粉末，以备后续使用。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "一锅法制备碳点:以制备RMBN-CDs为例，称取0.60 g硼酸倒入50 mL烧杯中，加入25 mL蒸馏水，使其溶解；再加入0.60 g尿素和2.00 g预先制备的大麦苗粉末，超声10 min；倒于50 mL坩埚中，放入烘箱240 ℃热解15 min，冷却至室温后备用。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "碳点的后处理:取上述粉末转移至离心管中，按30 mL/0.20 g的比例用去离子水溶解，放入高速离心机中以11 000 r/min离心10 min。取上层清液，得到碳点原液。将碳点原液过滤、透析分离和冷冻干燥处理后，得到碳点粉体，经计算产率约为6%。"
}
]
}
]
},
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"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.2 LED器件制作及性能分析"
}
],
"level": "2",
"id": "s2b"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "对于单一碳点基LED器件制作，是先将碳点粉体均匀混合于环氧树脂AB胶中，再均匀涂敷在GaN蓝光LED芯片上，将其置于烘箱中固化，即得LED器件。对于白光LED器件制作，工艺与上述流程相似，不同之处在于碳点中加入了适量的K"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "SiF"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "6"
}
]
},
{
"name": "text",
"data": "∶Mn"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "4+"
}
]
},
{
"name": "text",
"data": "商用红粉。采用LED光谱测试仪(杭州虹谱光电科技有限公司，HSP6000)对LED器件性能进行测试。"
}
]
}
]
}
]
},
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"data": [
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"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3 结果与讨论"
}
],
"level": "1",
"id": "s3"
}
},
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"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3.1 荧光碳点的组成"
}
],
"level": "2",
"id": "s3a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "采用紫外-可见分光光度计和傅里叶变换红外光谱仪对RM-CDs、RMB-CDs、RMN-CDs和RMBN-CDs等4种碳点的吸收光谱和表面官能团进行了测试分析；采用XPS对RMBN-CDs进行了分析，结果如"
},
{
"name": "xref",
"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "所示。"
},
{
"name": "xref",
"data": {
"text": "图2(a)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(a)"
}
]
}
},
{
"name": "text",
"data": "为4种碳点的吸收光谱，由图可知，碳点在220 nm附近表现出明显的光学特征吸收峰，可归因于其C"
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"data": "C 键的p®"
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"name": "text",
"data": "跃迁，能捕获短波长光子"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
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},
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"name": "text",
"data": "]"
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"name": "text",
"data": "；在280 nm附近出现肩峰，可归因于表面官能团的n®"
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{
"name": "text",
"data": "跃迁"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "22",
"type": "bibr",
"rid": "R22",
"data": [
{
"name": "text",
"data": "22"
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]
},
{
"name": "text",
"data": "；值得注意的是，在更长波长400 nm附近也会有吸收峰，特别是硼掺杂和硼氮共掺的碳点表现尤为明显，预示其表面态极可能捕获激发态能量，实现特征发光"
},
{
"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": "。"
}
]
},
{
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"data": {
"id": "F2",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图2"
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],
"title": [
{
"name": "text",
"data": "(a)RM-CDs、RMB-CDs、RMN-CDs和RMBN-CDs水溶液的紫外-可见吸收光谱(插图为350~700 nm部分放大图像);(b)RM-CDs、RMB-CDs、RMN-CDs和RMBN-CDs的红外光谱；(c)RMBN-CDs的XPS全谱(各元素含量分析图);(d)RMBN-CDs C1s高分辨率光谱；(e)RMBN-CDs B1s高分辨率光谱；(f)RMBN-CDs N1s高分辨率光谱。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.2"
}
],
"title": [
{
"name": "text",
"data": "(a)Absorption spectra of RM-CDs, RMB-CDs, RMN-CDs and RMBN-CDs in distilled water, illustrated with a partially enlarged image at 350-700 nm. (b)FT-IR spectra of RM-CDs, RMB-CDs, RMN-CDs and RMBN-CDs. (c)Full-scan XPS spectra of RMBN-CDs. (d)High resolution XPS spectra of RMBN-CDs for C1s. (e)High resolution XPS spectra of RMBN-CDs for B1s. (f)High resolution XPS spectra of RMBN-CDs for N1s."
}
]
}
],
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"data": {
"text": "图2(b)",
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"data": "图2(b)"
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}
},
{
"name": "text",
"data": "为4种碳点的红外光谱图，由图可知，3 400 cm"
},
{
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"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "附近有明显的吸收带，可归因于—OH的拉伸，表明这类碳点富含—OH官能团，亲水性强；2 800 cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "及776 cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "附近表现出 N—H/C—H 的伸缩振动，但吸收带并不明显。1 600,1 400,1 050 cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "附近为化学键C"
},
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"data": "O、C—C/C"
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},
{
"name": "text",
"data": "C 和 C—O 的特征吸收，而2 024 cm"
},
{
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"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "附近的C≡C的特征吸收峰则不明显，表明这类碳点的碳核核心主要靠C≡C及C"
},
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"data": "C键组成。当有N掺杂时，1 600 cm"
},
{
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"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "处的吸收峰变宽，从图中可看出，RMN-CDs与RM-CDs峰形明显不同，这是由于RMN-CDs含有C—NH"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "后，峰型被拉宽。同理，RMBN-CDs的峰型也有适当变宽，而RMB-CDs与RM-CDs相似，表明它们在1 600 cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "处的峰更多的是由单纯C—C/C"
},
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"data": "C的吸收振动引起。说明N掺杂后，有更多的C—NH"
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{
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"data": "2"
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]
},
{
"name": "text",
"data": "存在。在RMB-CDs体系中，1 191 cm"
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{
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"data": "-1"
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]
},
{
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"data": "和670 cm"
},
{
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"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "处出现掺B之后的特征峰，可归因于C—B和B—O键伸缩振动。"
}
]
},
{
"name": "p",
"data": [
{
"name": "xref",
"data": {
"text": "图2(c)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(c)"
}
]
}
},
{
"name": "text",
"data": "为RMBN-CDs的全扫描 XPS 光谱及各元素含量分布图，可知C1s、O1s、B1s、N1s、P1s和S1s的原子百分比分别为 43.99%、31.43%、14.30%、9.71%、0.43%和0.12%。其中，如"
},
{
"name": "xref",
"data": {
"text": "图2(d)、(e)、(f)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(d)、(e)、(f)"
}
]
}
},
{
"name": "text",
"data": "所示，C1s高分辨率光谱在284.8,286.3,288.1 eV处有3个峰"
},
{
"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": "，分别表示C元素以C"
},
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"data": "C/C—C、C—O、C"
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},
{
"name": "text",
"data": "O组成；B1s高分辨率光谱在192.6 eV和193.6 eV处有两个响应峰，分别表示B元素以BCO"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "和B"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "O"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "形式存在"
},
{
"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": ";N1s高分辨率光谱显示N元素以N—C"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "(399.6 eV)和C—NH"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "(400.7 eV)形式存在"
},
{
"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": "。样品中还含有极少量的P和S，源于生物基材料大多含有P、S，但由于含量极少，在此不进行专门讨论。从"
},
{
"name": "xref",
"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "可看出，XPS的分析结果与红外光谱分析结果相吻合。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3.2 液体荧光碳点的光致发光性质分析"
}
],
"level": "2",
"id": "s3b"
}
},
{
"name": "p",
"data": [
{
"name": "xref",
"data": {
"text": "图3(a)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(a)"
}
]
}
},
{
"name": "text",
"data": "为RM-CDs、RMB-CDs、RMN-CDs和RMBN-CDs 4种碳点的水溶液照片，在紫外光照射下表现出明亮的蓝光发射，这表明样品对紫外光具有良好的吸收。"
},
{
"name": "xref",
"data": {
"text": "图3(b)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(b)"
}
]
}
},
{
"name": "text",
"data": "为4种碳点水溶液的激发光谱，可见样品在260~400 nm之间的紫外光区表现宽带激发。为此进一步研究了碳点在不同波长光激发下的发光性能，结果如"
},
{
"name": "xref",
"data": {
"text": "图3(c)~(f)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(c)~(f)"
}
]
}
},
{
"name": "text",
"data": "所示。从图中可以看出，当激发波长能量较高时，4种碳点都出现了双峰发射特征，其中掺硼的RMB-CDs和RMBN-CDs,350 nm附近的发射比其他两种更为明显。本文利用间接测定法"
},
{
"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": "，对4种碳点的液态荧光量子效率进行了测定，结果分别为RM-CDs:5%,RMB-CDs:11%,RMN-CDs:8%和RMBN-CDs:13%。从上面的数据可以看出，掺硼和硼氮共掺的碳点液体荧光量子效率会稍高一些。虽然碳点的光致发光机理目前并没有一个定论，但从电子能级的角度来看"
},
{
"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": "，在常温下，碳点中成键电子大多处于基态S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "0"
}
]
},
{
"name": "text",
"data": "，在最低振动能级。当受到光激发时，会吸收其特征频率相一致的光子，部分处于S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "0"
}
]
},
{
"name": "text",
"data": "基态的电子会跃迁到更高的电子激发态(S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "、S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": ")，这就产生了紫外-可见光谱的吸收峰，这时的电子具有较大动能。处于S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "中各振动能级的电子通过内转化、振动弛豫等非辐射跃迁方式到达S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "，最终受激发的电子将从S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "→S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "0"
}
]
},
{
"name": "text",
"data": "，这个过程可伴随着光子发射，产生荧光。生物基碳点通常也借鉴有机染料分子轨道模型来解释"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "29",
"type": "bibr",
"rid": "R29",
"data": [
{
"name": "text",
"data": "29"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，它以sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "杂化碳核为中心，被表面官能团包围。如前通过对样品的紫外-可见吸收光谱、傅里叶变换红外光谱及XPS全谱图(各元素含量分析图)分析可知，本文所制备的碳点富含C"
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"name": "text",
"data": "C，证明sp"
},
{
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"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "共轭π域为其荧光发射的固有中心，产生π-π跃迁。由于生物基碳点本身含有一定的N、O、S等元素，会在碳核外围形成表面官能团，经过掺杂后，表面官能团种类和数量更加丰富，由此产生另一类特征吸收，归因于表面官能团的n-π跃迁"
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{
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"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
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"name": "xref",
"data": {
"text": "30",
"type": "bibr",
"rid": "R30",
"data": [
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"data": "30"
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]
}
},
{
"name": "text",
"data": "-"
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"name": "xref",
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"text": "31",
"type": "bibr",
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"name": "text",
"data": "31"
}
]
}
}
],
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"text": "30-31",
"type": "bibr"
}
},
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}
]
},
{
"name": "text",
"data": "。本文所制备的碳点中，当硼元素引入后，从XPS中可知，多了一些B—C和B—O键，从物理学的角度来看，附着在碳点表面/边缘上新的官能团和杂原子诱导了新的表面/缺陷态进入碳点体系，从而调整碳点中的电子结构和响应的光电子跃迁通道"
},
{
"name": "sup",
"data": [
{
"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": [
{
"name": "text",
"data": "32"
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]
}
},
{
"name": "text",
"data": "-"
},
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"name": "xref",
"data": {
"text": "33",
"type": "bibr",
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{
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{
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}
]
},
{
"name": "text",
"data": "，表现出更优异的发光特性，因此产生了明显的双发射现象。"
}
]
},
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"caption": [
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"label": [
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"data": "图3"
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"title": [
{
"name": "text",
"data": "(a)碳点水溶液在自然光和紫外光下的照片，从左到右依次为RM-CDs、RMB-CDs、RMN-CDs和RMBN-CDs;(b)碳点水溶液的激发光谱(监测波长为440 nm);(c)~(f)碳点水溶液在不同波长光激发下的发射光谱。"
}
]
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],
"title": [
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"data": "(a)Pictures of CDs solution under natural light and UV light, from left to right, they are RM-CDs, RMB-CDs, RMN-CDs and RMBN-CDs. (b)Excitation spectra of the CDs solution(monitoring at 440 nm). (c)-(f)Emission spectra of CDs solution excited by different wavelength light."
}
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}
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"title": [
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"data": "3.3 固体荧光碳点的光致发光性质分析"
}
],
"level": "2",
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"data": [
{
"name": "text",
"data": "将RM-CDs、RMB-CDs、RMN-CDs和RMBN-CDs 4种碳点进行冷冻干燥后，RM-CDs和RMN-CDs粉体在紫外光和蓝光下没有明显的荧光发射，为此重点讨论RMB-CDs和RMBN-CDs粉体的发光性能。"
},
{
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"data": {
"text": "图4(a)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(a)"
}
]
}
},
{
"name": "text",
"data": "为RMB和RMBN粉体的激发光谱，这两种碳点表现出类似的激发光谱。样品最强激发带位于蓝光区，与其液体荧光光谱相比，出现了明显的红移，这可能是因为粉体发生了严重的π-π聚集现象，这种聚集过程引发了能级突变"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "34",
"type": "bibr",
"rid": "R34",
"data": [
{
"name": "text",
"data": "34"
}
]
}
},
{
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"data": "]"
}
]
},
{
"name": "text",
"data": "。样品在可见光下呈现淡黄色，这也意味着RMB-CDs和RMBN-CDs粉体对蓝光具有很强的吸收。该宽带激发可以与蓝光GaN芯片的发射完美匹配，这意味着RMB-CDs和RMBN-CDs在蓝光LED上具有潜在的应用。"
},
{
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"data": {
"text": "图4(b)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(b)"
}
]
}
},
{
"name": "text",
"data": "为RMB-CDs在不同激发波长下的发射光谱。随着激发波长的增加，样品的主发射峰位于500 nm左右，没有观察到发射峰位置的明显移动。样品在678 nm处也存在较弱的发射。与RMB发射光谱相比，RMBN粉体的主发射峰稍稍有点红移，位于506 nm左右("
},
{
"name": "xref",
"data": {
"text": "图4(c)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(c)"
}
]
}
},
{
"name": "text",
"data": ")。样品的发射峰并未随激发波长的变化而改变，但发光强度不同。当激发波长为440 nm时，样品的绿光发射强度最大。在蓝光照射下，RMB-CDs和RMBN-CDs粉体均能发射出明亮的绿光。由"
},
{
"name": "xref",
"data": {
"text": "图4(d)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(d)"
}
]
}
},
{
"name": "text",
"data": "可以看出，随着温度升高，RMB-CDs粉体和RMBN-CDs粉体的发射强度在缓慢下降。值得一提的是，经过硼、氮共同修饰后，RMBN-CDs粉体在240 ℃时的发射强度约为初始值的95%。这表明这两种荧光碳点粉体具有很好的热稳定性。此外，这两种碳点粉体量子效率分别为5%和7%，与文献报道结果相近"
},
{
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"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
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"name": "xref",
"data": {
"text": "35",
"type": "bibr",
"rid": "R35",
"data": [
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"name": "text",
"data": "35"
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]
}
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"data": "-"
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"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
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"data": "37"
}
]
}
}
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"R37"
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}
},
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}
]
},
{
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"data": "。"
}
]
},
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"label": [
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"title": [
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"name": "text",
"data": "(a)RMB-CDs粉体和RMBN-CDs粉体的激发光谱(监测波长500 nm)(插图为RMB-CDs粉体和RMBN-CDs粉体在自然光条件下的拍摄图);(b)RMB-CDs粉体在不同波长光激发下的发射光谱(插图为RMB-CDs粉体在365 nm光照下的拍摄图);(c)RMBN-CDs粉体在不同波长光激发下的发射光谱(插图为RMBN-CDs粉体在365 nm光照下的拍摄图);(d)RMB-CDs粉体和RMBN-CDs粉体在不同温度下的相对发射强度。"
}
]
},
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"label": [
{
"name": "text",
"data": "Fig.4"
}
],
"title": [
{
"name": "text",
"data": "(a)Excitation spectra of RMB-CDs powder and RMBN-CDs powder by monitoring at 500 nm(the illustration shows the pictures of RMB-CDs powder and RMBN-CDs powder under natural light conditions). (b)Emission spectra of RMB-CDs powder excited by different wavelength light(the illustration shows the image of RMB-CDs powder under 365 nm light). (c)Emission spectra of RMBN-CDs powder excited by different wavelength light(the illustration shows the image of RMBN-CDs powder under 365 nm light). (d)Temperature-dependent emission intensity of RMB-CDs powder and RMBN-CDs powder."
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"data": [
{
"name": "text",
"data": "通过对样品固态发光与液态发光性能的对比，可以看到4种样品只有两种样品有固态发光，且双发射现象也随之消失。目前，研究人员并没有就固态碳点发光给出一个确切的解释和方案，通常从液态到固态，碳点荧光猝灭有以下3种解释"
},
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"data": [
{
"name": "text",
"data": "["
},
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"data": {
"text": "26",
"type": "bibr",
"rid": "R26",
"data": [
{
"name": "text",
"data": "26"
}
]
}
},
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"data": "]"
}
]
},
{
"name": "text",
"data": ":(1)一些碳点的结构天生容易受到分子转动/振动的影响，这可能导致电子处在激发态的能量耗散，从而产生荧光猝灭效应。(2)当碳点聚集时，由于π-π的相互作用，使得能量在粒子间传递，这种能量共振转移在形成固体粉末聚集态时会尤为突出，导致有部分甚至全部激子以非辐射跃迁方式回到基态，从而影响固态碳点的荧光性质。(3)碳点(特别是生物基碳点)通常含有许多含氧官能团，氧具有较强的三重态猝灭能力。本文中的RMB-CDs和RMBN-CDs以固态粉末形式仍能发光，可能是由于杂原子硼改变了碳点的结构，丰富了碳点表面环境，使激发态回到基态的路径增多，当碳点聚集时，这类表面官能团捕获了一定的能量，以光子形式释放，避免全部激子都以非辐射跃迁回到基态，从而与液态相比，只产生了部分荧光猝灭，仍具有固态发光特性"
},
{
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"data": [
{
"name": "text",
"data": "["
},
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"name": "xref",
"data": {
"text": "7",
"type": "bibr",
"rid": "R7",
"data": [
{
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"data": "7"
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]
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"data": ","
},
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"data": {
"data": [
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"name": "xref",
"data": {
"text": "38",
"type": "bibr",
"rid": "R38",
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"data": {
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"title": [
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"data": "3.4 固体荧光碳点在LED器件上的应用"
}
],
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}
},
{
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"data": [
{
"name": "text",
"data": "鉴于RMB-CDs和RMBN-CDs粉体在蓝光激发下表现出优异的发光性能，初步将其应用于蓝光GaN芯片上。"
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{
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"data": {
"text": "图5(a)、(b)",
"type": "fig",
"rid": "F5",
"data": [
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"data": "图5(a)、(b)"
}
]
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},
{
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"data": "为利用RMB-CDs和RMBN-CDs粉体所制作的LED器件在不同电流驱动下的发光光谱。图中较强的蓝光发射为GaN芯片的发射峰，从500~750 nm的宽峰对应于碳点吸收芯片所产生的黄绿光发射。由于碳点在红光区域的发射较弱，导致两种发光器件的发光偏冷光(见"
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"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
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"data": "图5"
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{
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"data": "插图)。随着器件驱动电流的升高，器件的发射光谱形状并无明显变化，这也间接证明RMB-CDs和RMBN-CDs具有较好的热稳定性。对比"
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"data": {
"text": "图5(a)",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5(a)"
}
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}
},
{
"name": "text",
"data": "和"
},
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"data": {
"text": "图5(b)",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5(b)"
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}
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{
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"data": "，可发现RMBN-CDs粉体LED器件黄绿光成分比RMB-CDs粉体器件的黄绿光发射更为饱满，更有利于LED的发光性能。两种LED器件相关光电参数如"
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"data": {
"text": "表1",
"type": "table",
"rid": "T1",
"data": [
{
"name": "text",
"data": "表1"
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]
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},
{
"name": "text",
"data": "、"
},
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"data": {
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"type": "table",
"rid": "T2",
"data": [
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"data": "2"
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},
{
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"data": "所示。从表中可见，随着电流增大，器件的流明效率(LE)逐渐下降，但对应的光辐射功率(LF)则明显上升。对比两种器件的色坐标(CIE)可知，RMBN-CDs粉体LED具有更好的CIE坐标值("
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"data": "Tab.1"
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"title": [
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"data": "(a)~(b)RMB-CDs粉体和RMBN-CDs粉体LED器件在不同电流驱动下的发光光谱(插图为LED器件的点亮图);(c) RMB-CDs粉体和RMBN-CDs粉体分别与K"
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"data": "混合后制作的白光LED器件在20 mA电流驱动下的发光光谱；(d)上述白光LED器件色坐标图及点亮照片；(e)~(f)RMB-CDs粉体LED器件和RMBN-CDs粉体LED器件在不同电流驱动下的CIE坐标变化图。"
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"data": "(a)-(b)Luminescent spectra of LED devices based on RMB-CDs powder and RMBN-CDs powder under different currents, respectively(luminance photographs of that two LEDs). (c)Luminescent spectra of white LEDs by combining RMB-CDs powder or RMBN-CDs powder with K"
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"data": "SiF"
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"data": "∶Mn"
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"data": [
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{
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"data": " under the 20 mA current, respectively. (d)CIE coordinates and luminance photographs of that two white LEDs. (e)-(f)CIE coordinate change diagram of white LED devices made by RMB-CDs powder or RMBN-CDs powder under different current driving conditions, respectively."
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"name": "text",
"data": "为了进一步提高上述LED器件的红光发射强度，将商用K"
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"data": "2"
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"data": [
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"data": "4+"
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]
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"data": "红色荧光粉引入上述两种LED器件中，它们的电致发光光谱如"
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"data": {
"text": "图5(c)",
"type": "fig",
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"data": [
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"data": "图5(c)"
}
]
}
},
{
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"data": "所示。图中600~650 nm 之间的窄带红光发射起源于Mn"
},
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"data": [
{
"name": "text",
"data": "4+"
}
]
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{
"name": "text",
"data": "的"
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"data": [
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"data": "2"
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"data": "E"
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"data": "g"
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"data": "→"
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"data": "4"
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"data": "A"
},
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"data": [
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"data": "2g"
}
]
},
{
"name": "text",
"data": "能级跃迁。K"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "SiF"
},
{
"name": "sub",
"data": [
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"data": "6"
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]
},
{
"name": "text",
"data": "∶Mn"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "4+"
}
]
},
{
"name": "text",
"data": "的引入明显提高了器件的显色指数("
},
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"data": [
{
"name": "text",
"data": "Ra"
}
]
},
{
"name": "text",
"data": ":80.7,84.4)。在20 mA电流驱动下，两种器件表现出很强的白光发射，其CIE值分别为(0.267, 0.314)、(0.285,0.330)，上述两种白光LED的CIE色坐标值随着电流的增加而下降("
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"data": {
"text": "图5(e)、(f)",
"type": "fig",
"rid": "F5",
"data": [
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"data": "图5(e)、(f)"
}
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}
},
{
"name": "text",
"data": ")。"
}
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}
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"id": "s4"
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},
{
"name": "p",
"data": [
{
"name": "text",
"data": "本文以大麦苗为碳源，采用一锅热解法成功获得碳点，并对其硼、氮及混合掺杂体系进行研究，获得了RM-CDs、RMB-CDs、RMN-CDs和RMBN-CDs 4种碳点。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "该类型碳点在水溶液中表现出很强的紫外光区宽带吸收，其中，RMN-CDs和RMBN-CDs不同于其他两种碳点。4种荧光碳点水溶液在蓝光区和绿光区均表现出难得的双峰发射，其中RMN-CDs和RMBN-CDs的双峰发射现象更加明显，表明硼的掺杂丰富了表面官能团，赋予了碳点更多的表面陷阱，使激发态回到基态的途径变多，从而产生了双峰发射现象。值得注意的是，RMN-CDs和RMBN-CDs还表现出不常见的固态发光，在不同激发波长下，均出现506 nm左右的发射。利用这一特性，将RMN-CDs和RMBN-CDs粉体分别与商用K"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "SiF"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "6"
}
]
},
{
"name": "text",
"data": "∶Mn"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "4+"
}
]
},
{
"name": "text",
"data": "红色荧光粉制作出白光LED器件。在20 mA电流驱动下，两种固态白光LED器件的流明效率分别为15.1 lm/W和14.6 lm/W；显色指数高达80.7和84.4。这些研究结果为生物基碳点的制备及其在LED领域的应用提供了新思路。"
}
]
},
{
"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.20210159."
}
]
}
]
}
],
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"title": [
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"name": "text",
"data": "参考文献:"
}
],
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"articlemeta": {
"doi": "10.37188/CJL.20210159",
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[
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"dc": [
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"fundinggroup": [
{
"lang": "zh",
"text": [
{
"name": "text",
"data": "国家自然科学基金（U1802257）；国家自然科学基金-云南联合基金（U1702254）；云南省高校科技创新团队支持计划资助项目"
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"text": [
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"name": "text",
"data": "Supported by National Natural Science Foundation of China (U1802257); The Joint Funds of The National Natural Science Foundation of China-Yunnan Provinces (U1702254); The Program for Innovative Research Team (in Science and Technology) in University of Yunnan Province"
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]
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],
"history": {
"received": "2021-04-30",
"revised": "2021-05-12",
"ppub": "2021-08-01",
"opub": "2021-10-19"
},
"copyright": {
"data": [],
"year": "2021"
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},
"appendix": [],
"type": "research-article",
"ethics": [],
"supplementary": [],
"journalTitle": "发光学报",
"issue": "08",
"volume": "42",
"originalSource": []
}
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