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负载碳点的分子筛发光材料
特邀报告 | 更新时间：2021-09-03
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负载碳点的分子筛发光材料 增强出版
- Photoluminescent Composite Materials by Embedding Carbon Dots in Zeolites
- 发光学报 2021年 42卷 第8期 (2021)
- 作者机构：吉林大学化学学院 无机合成与制备化学国家重点实验室,吉林,长春,130012
- 作者简介：
- 基金信息：国家自然科学基金(21621001);高等学校学科创新引智计划(B17020)
- DOI：10.37188/CJL.20210196 中图分类号： O482.31
纸质出版日期：2021-08-01，
收稿日期：2021-05-21，
修回日期：2021-06-05，
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引用本文
李莉, 于晓微, 张洪月, 等. 负载碳点的分子筛发光材料[J]. 发光学报, 2021, 42(8):1114-1124.
Li LI, Xiao-wei YU, Hong-yue ZHANG, et al. Photoluminescent Composite Materials by Embedding Carbon Dots in Zeolites[J]. Chinese Journal of Luminescence, 2021, 42(8):1114-1124.
李莉, 于晓微, 张洪月, 等. 负载碳点的分子筛发光材料[J]. 发光学报, 2021, 42(8):1114-1124. DOI： 10.37188/CJL.20210196.
Li LI, Xiao-wei YU, Hong-yue ZHANG, et al. Photoluminescent Composite Materials by Embedding Carbon Dots in Zeolites[J]. Chinese Journal of Luminescence, 2021, 42(8):1114-1124. DOI： 10.37188/CJL.20210196.
负载碳点的分子筛发光材料 增强出版
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"text": "吉林大学化学学院 无机合成与制备化学国家重点实验室，吉林 长春 130012",
"data": [
{
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"data": "吉林大学化学学院 无机合成与制备化学国家重点实验室，吉林 长春 130012"
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"data": "碳点具有优异的发光特性和广泛的应用，将碳点限域于具有纳米孔道结构的分子筛材料中，可开发出一类新型的碳点@分子筛复合材料。本文聚焦于具有独特发光性能的负载碳点的分子筛复合材料，综述了这类材料最新的研究进展，重点介绍了碳点@分子筛复合材料的制备方法、长余辉发光调控策略及主体分子筛基质对客体碳点的作用等，并对未来光致发光碳点@分子筛复合材料的发展前景进行了展望。"
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[
{
"name": "text",
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{
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[
{
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{
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{
"name": "text",
"data": "碳点(CDs)是一类具有荧光性质的碳颗粒，其尺寸一般不大于10 nm。碳点自2004年被首次报道以来，引起了广泛的关注"
},
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"data": "["
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"name": "text",
"data": "。相比于金属量子点材料，碳点材料毒性很低，对环境友好，具有良好的生物相容性；耐光漂白，发光性质稳定，荧光量子产率高；易被化学修饰，可用于设计合成多功能发光材料"
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"data": "4"
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"R3",
"R4"
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"type": "bibr"
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"name": "text",
"data": "。这些独特的特点使得碳点广泛应用于太阳能电池"
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"data": [
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"name": "text",
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}
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"rid": [
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"R7"
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"type": "bibr"
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"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、发光二极管"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "8",
"type": "bibr",
"rid": "R8",
"data": [
{
"name": "text",
"data": "8"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "9",
"type": "bibr",
"rid": "R9",
"data": [
{
"name": "text",
"data": "9"
}
]
}
}
],
"rid": [
"R8",
"R9"
],
"text": "8-9",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、超级电容器"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "10",
"type": "bibr",
"rid": "R10",
"data": [
{
"name": "text",
"data": "10"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "11",
"type": "bibr",
"rid": "R11",
"data": [
{
"name": "text",
"data": "11"
}
]
}
}
],
"rid": [
"R10",
"R11"
],
"text": "10-11",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、光催化降解有机物"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
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"name": "xref",
"data": {
"text": "12",
"type": "bibr",
"rid": "R12",
"data": [
{
"name": "text",
"data": "12"
}
]
}
},
{
"name": "text",
"data": "-"
},
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"data": {
"text": "13",
"type": "bibr",
"rid": "R13",
"data": [
{
"name": "text",
"data": "13"
}
]
}
}
],
"rid": [
"R12",
"R13"
],
"text": "12-13",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、检测各类重金属阳离子和各类阴离子"
},
{
"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": "18",
"type": "bibr",
"rid": "R18",
"data": [
{
"name": "text",
"data": "18"
}
]
}
}
],
"rid": [
"R14",
"R15",
"R16",
"R17",
"R18"
],
"text": "14-18",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、细胞标记"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "19",
"type": "bibr",
"rid": "R19",
"data": [
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]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、生物成像"
},
{
"name": "sup",
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"data": "["
},
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"data": {
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"type": "bibr",
"rid": "R20",
"data": [
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"name": "text",
"data": "20"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、荧光墨水"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
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"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "等领域。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "从结构上来看，碳点主要可以分为石墨烯量子点、碳纳米点和聚合物点。石墨烯量子点具有单层或多层石墨烯结构"
},
{
"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": "，其边缘链接不同的化学基团"
},
{
"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": "。碳纳米点可以有明显的晶格结构也可以是无晶格结构，其表面的官能团对碳点的荧光性质和溶解性起着至关重要的作用；同时，表面的氮、硫和其他元素基团能优化碳点的电子结构，使得发光效率和性能都大幅提高"
},
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"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
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"name": "blockXref",
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"data": [
{
"name": "xref",
"data": {
"text": "24",
"type": "bibr",
"rid": "R24",
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{
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"data": "24"
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}
},
{
"name": "text",
"data": "-"
},
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"name": "xref",
"data": {
"text": "25",
"type": "bibr",
"rid": "R25",
"data": [
{
"name": "text",
"data": "25"
}
]
}
}
],
"rid": [
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"R25"
],
"text": "24-25",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。聚合物点通常是指高分子通过交联和碳化形成的具有荧光性质的聚集体，一般不具有明显的碳的晶格结构"
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"name": "text",
"data": "27"
}
]
}
}
],
"rid": [
"R26",
"R27"
],
"text": "26-27",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。由于前驱体以及制备方法的多样性，碳点的发光机理也众说纷纭，目前主要的说法有以下几种"
},
{
"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": ":(1)带隙发射和量子限制效应；(2)表面态发射；(3)分子荧光团和碳核中心发射；(4)多环芳烃型分子发射；(5)溶剂化弛豫效应或溶剂变色偏移；(6)自陷激子发射；(7)表面偶极子发射中心；(8)聚集发射中心。碳点表面具有丰富的官能基团，给其化学修饰和嫁接提供了广阔的空间。嫁接后的碳点荧光发光性能通常可以得到保持，并且避免了固态碳点聚集诱导发光猝灭的影响，为其在复合材料方面的拓展提供了广阔的空间。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "近年来，沸石分子筛材料作为优异的载体材料备受关注。分子筛骨架上的硅铝原子或吸附的阳离子可以被一系列具有潜在发射能力的杂原子(例如稀土金属、过渡金属等)替换，从而制备出一系列具有光学性质的材料"
},
{
"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": "。此外，由于沸石分子筛丰富的孔道结构和容纳客体分子的能力，可以有效地吸附、封装或限域一系列发光分子(如金属簇、量子点、碳点等)，并可通过沸石分子筛的空间限域效应及主客体间相互作用等增强复合材料的发光性能和稳定性"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "30",
"type": "bibr",
"rid": "R30",
"data": [
{
"name": "text",
"data": "30"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "32",
"type": "bibr",
"rid": "R32",
"data": [
{
"name": "text",
"data": "32"
}
]
}
}
],
"rid": [
"R30",
"R31",
"R32"
],
"text": "30-32",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。特别是，主客体组装不仅保留了发光客体和沸石分子筛主体的独特性质，也将赋予复合材料新的发光性质"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "33",
"type": "bibr",
"rid": "R33",
"data": [
{
"name": "text",
"data": "33"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "34",
"type": "bibr",
"rid": "R34",
"data": [
{
"name": "text",
"data": "34"
}
]
}
}
],
"rid": [
"R33",
"R34"
],
"text": "33-34",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。本文从碳点@分子筛复合材料的制备方法、发光调控及主体分子筛基质对客体碳点的作用等方面综述了负载碳点分子筛发光材料的最新研究进展，并对该材料未来的发展前景进行了展望。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2 碳点@分子筛复合材料的制备"
}
],
"level": "1",
"id": "s2"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "近年来，具有独特发光性能的负载碳点的分子筛复合材料相继被开发出来，其制备方法主要有三种，即热解分子筛中有机模板剂法"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "35",
"type": "bibr",
"rid": "R35",
"data": [
{
"name": "text",
"data": "35"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "、原位水热/溶剂热合成法"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "和无溶剂合成法"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.1 热解法"
}
],
"level": "2",
"id": "s2a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "利用热解法制备碳点@分子筛复合材料，通常需要先合成分子筛材料，然后在高温下将分子筛中的模板剂或有机物热解成碳点，并限域在分子筛晶体内部。该方法制备的复合材料的荧光性质可以通过改变煅烧时间、煅烧气氛以及煅烧温度来进行调控。2008年，Giannelis课题组"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "38",
"type": "bibr",
"rid": "R38",
"data": [
{
"name": "text",
"data": "38"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "首次在沸石分子筛中制备出碳点。他们首先通过离子交换向NaY(FAU拓扑结构)沸石分子筛孔道中引入2,4-二氨基苯酚的氯化物，通过煅烧氧化在分子筛孔道中得到碳点。该工作不仅提出了一个制备碳点的有效方法，更使得碳点在具有规则孔道的无机骨架载体中得到了很好的分散。2010 年，Chen课题组"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "39",
"type": "bibr",
"rid": "R39",
"data": [
{
"name": "text",
"data": "39"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "以环己胺为模板剂，在水热条件下合成一种CHA结构类型的磷酸铝镁分子筛MAPO-44，通过煅烧分子筛得到负载碳点的复合材料，其发光随着煅烧时间的不同可以从蓝紫色变化到橙红色("
},
{
"name": "xref",
"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": ")。实验结果证明，热解条件不同导致了分子筛中有机模板的碳化程度不同，碳的含量直接对复合材料的发光特性产生影响，决定了其发光波长。氧化热解的时间越长所对应样品的荧光发射波长越短，即延长热处理时间可以使样品的发射波长发生蓝移。"
}
]
},
{
"name": "fig",
"data": {
"id": "F1",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图1"
}
],
"title": [
{
"name": "text",
"data": "(a)不同煅烧时间的CDs@MAPO-44的荧光照片及光谱"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "39",
"type": "bibr",
"rid": "R39",
"data": [
{
"name": "text",
"data": "39"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": ";(b)发光机制示意图"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "40",
"type": "bibr",
"rid": "R40",
"data": [
{
"name": "text",
"data": "40"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.1"
}
],
"title": [
{
"name": "text",
"data": "(a)PL emission spectra and photographs of CDs@MAPO-44 samples under UV irradiation"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "39",
"type": "bibr",
"rid": "R39",
"data": [
{
"name": "text",
"data": "39"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": ". (b) Schematic representation of the formation of photoluminescent CDs@MAPO-44 samples"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "40",
"type": "bibr",
"rid": "R40",
"data": [
{
"name": "text",
"data": "40"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "."
}
]
}
],
"subcaption": [],
"note": [],
"graphics": [
{
"print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207705&type=",
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},
{
"name": "p",
"data": [
{
"name": "text",
"data": "Garcia课题组"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "41",
"type": "bibr",
"rid": "R41",
"data": [
{
"name": "text",
"data": "41"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "通过煅烧纯硅分子筛ITQ-29(LTA结构类型)合成了具有较高量子产率的碳点复合材料。Li课题组在热解法制备碳点方面做了深入的工作"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "42",
"type": "bibr",
"rid": "R42",
"data": [
{
"name": "text",
"data": "42"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "44",
"type": "bibr",
"rid": "R44",
"data": [
{
"name": "text",
"data": "44"
}
]
}
}
],
"rid": [
"R42",
"R43",
"R44"
],
"text": "42-44",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，例如通过煅烧分子筛JU-92(JNT结构类型)合成的碳点复合材料具有较高的量子产率(11%)"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "45",
"type": "bibr",
"rid": "R45",
"data": [
{
"name": "text",
"data": "45"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。此外，她们还通过煅烧含不同有机模板剂的CHA和LEV拓扑结构的磷酸铝分子筛，制备了一系列具有绿色室温磷光(RTP)性质的碳点复合材料"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "46",
"type": "bibr",
"rid": "R46",
"data": [
{
"name": "text",
"data": "46"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。热解法制备碳点@分子筛复合材料比较简单，但需要分子筛基质具有高的热稳定性。此外，该方法适合一些小孔分子筛材料，大孔和超大孔分子筛材料在热解时往往会导致包含的有机物全部脱出，而不形成碳点。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "Ruan课题组"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "47",
"type": "bibr",
"rid": "R47",
"data": [
{
"name": "text",
"data": "47"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "采用二丙胺原位热解法在SAPO-46分子筛(AFS结构类型)中制备出尺寸均匀的碳点。使用该复合材料作为饱和吸收剂，提高了脉冲光纤激光器的稳定性。分子筛的纳米孔道可以很好地保护限域的碳点，并防止单一碳点的聚合；同时2个光纤连接器通过碳点连接形成相互兼容的饱和吸收剂，可以保证脉冲光纤激光器在高泵功率下高效稳定地工作。此外，他们通过在LTA分子筛纳米孔道中对正丙胺进行原位热解，制备了大小约2 nm的均匀碳点，所合成的复合材料具有宽频带的非线性光学饱和吸收特性，可作为饱和吸收剂用于超快脉冲光纤激光器的制备"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "48",
"type": "bibr",
"rid": "R48",
"data": [
{
"name": "text",
"data": "48"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.2 原位合成法"
}
],
"level": "2",
"id": "s2b"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "Yu和Li课题组"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "49",
"type": "bibr",
"rid": "R49",
"data": [
{
"name": "text",
"data": "49"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "在原位合成碳点@分子筛复合材料方面进行了深入系统的研究，提出了碳点限域于分子筛(CDs-in-zeolite)的合成策略，即在水热或溶剂热体系中，控制分子筛的晶化条件，使由有机模板剂或其他有机物种形成的碳点随分子筛的晶化嵌入到分子筛晶体中，形成复合材料("
},
{
"name": "xref",
"data": {
"text": "图2(a)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(a)"
}
]
}
},
{
"name": "text",
"data": ")。该方法形成的碳点通常限域在分子筛基质的间断空间中，通过分子筛基质的限域作用以及碳点与基质间的氢键相互作用等，易制备具有长余辉性质的复合材料。例如，在水热/溶剂热体系中，将碳点原位嵌入AlPO-5(AFI结构类型)分子筛晶体中制备出具有350 ms超长寿命的热延迟荧光(TADF)材料，在室温空气条件下即可展现出高达52.14%的荧光量子效率。独特的TADF现象是由于分子筛限域空间可抑制非辐射过程和阻碍氧猝灭来有效地稳定碳点的三重态，实现了反隙间窜越而导致("
},
{
"name": "xref",
"data": {
"text": "图2(b)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(b)"
}
]
}
},
{
"name": "text",
"data": ")。分子筛基质可以有效阻隔空气中的氧气，避免三重激发态遇分子氧发生猝灭，使得材料的延迟荧光现象在空气环境下得以展现。值得注意的是，将骨架刻蚀之后得到的碳点溶液或母液中的碳点均没有这种TADF现象，表明了分子筛骨架在稳定碳点三重态、实现TADF中的关键作用。"
},
{
"name": "xref",
"data": {
"text": "图2(c)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(c)"
}
]
}
},
{
"name": "text",
"data": "展示了材料在防伪方面的潜在应用，显示出其在光电应用方面的巨大潜力。在此基础上，她们利用原位合成法，通过调变分子筛的结构类型、骨架组成和碳源(如有机模板剂)种类等制备了一系列具有不同余辉颜色、寿命以及量子效率的碳点基复合材料。对于碳点@分子筛复合材料，其原位合成法的难点在于控制分子筛的晶化速度，使其与碳点的生成速度相匹配，从而使碳点随分子筛晶体的生长包裹在分子筛基质中。在这种条件下，负载进入分子筛基质中的碳点量很难控制。"
}
]
},
{
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"data": {
"id": "F2",
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"lang": "zh",
"label": [
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"data": "图2"
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"title": [
{
"name": "text",
"data": "(a)CDs@AlPO-5分子筛复合材料合成过程示意图；(b)TADF发光机制示意图；(c)在双模式防伪的应用示例"
},
{
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"text": "49",
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"data": "49"
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"data": "。"
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"label": [
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"data": "Fig.2"
}
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"title": [
{
"name": "text",
"data": "(a)Proposed "
},
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"data": "in situ"
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{
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"data": " formation process of photoluminescent CDs@AlPO-5 composite. (b)-(c)TADF mechanism of CDs@zeolite composites and dual-responsive security protection application"
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"data": [
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"data": "["
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"data": {
"text": "49",
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"data": [
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"data": "49"
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"title": [
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"data": "2.3 无溶剂合成法"
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{
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"data": [
{
"name": "text",
"data": "为进一步提高碳点复合材料的发光效率和长余辉寿命，Yu和Li课题组对原位水热/溶剂热合成方法进行改进，提出了无溶剂合成法和额外引入优质碳源的策略"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。该方法不使用溶剂，而是将分子筛固体原料和碳点前驱体在室温下简单研磨，然后加热晶化。该合成方法有效地避免了碳点留存在极性较高的溶剂(例如水溶剂)中而不是进入分子筛基质中的问题，并增强了碳点和基质间的相互作用，同时降低了合成过程中溶剂对环境的污染。此外，在碳源的选取上，该方法区别于常规分子筛合成中将有机模板剂作为碳源，在合成中添加了更丰富且高效的碳源，如氨基酸和乙二胺，将其与分子筛合成原料进行充分研磨，随后经过220 ℃、24 h的高温晶化制得碳点@分子筛复合材料("
},
{
"name": "xref",
"data": {
"text": "图3(a)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(a)"
}
]
}
},
{
"name": "text",
"data": ")。该方法能够最大限度地将碳点限域在分子筛晶体中，实现了高的碳点负载量(1.7%)，为常规水热/溶剂热方法制备材料的3倍左右。制备的碳点@分子筛复合材料具有独特的发光特性，在室温空气条件下展示出热致延迟荧光和室温磷光双发射，总量子产率90.7%，余辉寿命可达1.7 s和2.1 s。对碳点和分子筛的晶化过程研究发现，该体系下反应3 h时分子筛晶化完全，此时观测到碳点为交联的高分子状；随后在3~24 h反应过程中，碳点的碳核结构逐渐从无序到有序，同时主客体间的氢键作用逐渐增强。碳点有序的晶格结构降低了价健的振动和转动，结合强的主客体氢键相互作用的约束，促使复合材料实现高效的长余辉发射("
},
{
"name": "xref",
"data": {
"text": "图3(b)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(b)"
}
]
}
},
{
"name": "text",
"data": ")。鉴于该复合材料独特的长余辉发光特性，作者首次将其应用于交变LED领域，利用长余辉在交流电频闪时有适当的弥补作用，降低了交流电带来的频闪对人眼的伤害("
},
{
"name": "xref",
"data": {
"text": "图3(c)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(c)"
}
]
}
},
{
"name": "text",
"data": ")。值得注意的是，尽管无溶剂合成法有独特的优点，但相比前两种制备方法，该方法的应用目前不多，并且无溶剂条件下，生成的分子筛易出现杂相。"
}
]
},
{
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"id": "F3",
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"lang": "zh",
"label": [
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"title": [
{
"name": "text",
"data": "(a)无溶剂合成法和外引优质碳源的策略制备CDs@AlPO-5分子筛；(b)合成体系中碳点和分子筛晶体的形成过程；(c)交变LED领域的应用示例"
},
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"text": "37",
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"data": "37"
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},
{
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"data": "。"
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]
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"label": [
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"data": "Fig.3"
}
],
"title": [
{
"name": "text",
"data": "(a)Schematic representation of confinement synthesis of CDs in AlPO-5 zeolite. (b)CDs@AlPO-5 formed with varying crystallization time and proposed crystallization curve of the CDs@AlPO-5 composite. (c)Luminescence intensity variations of the labeled LED devices driven in AC periodic cycles and photographs of LED device"
},
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"data": "["
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"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
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"data": {
"title": [
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"name": "text",
"data": "3 CDs@分子筛复合材料的长余辉发光调控"
}
],
"level": "1",
"id": "s3"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "目前报道的碳点长余辉材料主要分为室温磷光材料和延迟荧光材料。磷光材料是基于三重激发态的发光，制备长寿命室温磷光材料的关键是通过增强系间窜越过程来有效活化三重态激子，同时抑制非辐射跃迁过程。热致延迟荧光材料因其可以通过反系间窜越过程有效利用三重态激子，使得内量子效率在理论上可以达到100%。由于材料的单重态-三重态能级差(Δ"
},
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"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "ST"
}
]
},
{
"name": "text",
"data": ")小，在环境热下，电子能够从T"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "态经过反系间窜跃过程返回S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "态而发光，从而完成延迟荧光过程。虽然两种材料的发光过程有所差别，但对三重激发态的高效利用是开发长寿命、高量子效率的室温磷光材料和延迟荧光材料的关键。分子筛的纳米空间限域作用可以有效地稳定碳点三重激发态，这为合成具有不同长余辉发光性能(室温磷光与热致延迟荧光)的碳点@分子筛复合材料提供了可能。然而，实现对长余辉的有效调控的研究还相对匮乏，下面介绍几种碳点@分子筛复合材料的长余辉调控策略。"
}
]
},
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"title": [
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"name": "text",
"data": "3.1 能量传递"
}
],
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}
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{
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"data": [
{
"name": "text",
"data": "由于激发态的非辐射衰减比例较大、激发态与基态之间的能量差较小等原因，具有红色发光室温磷光(RTP)的碳点(CDs)材料很少被报道。Yu和Li课题组报道了一种碳点-基质能量转移(CMET)策略，以此来调节复合材料的室温磷光(RTP)性质"
},
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"data": [
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"name": "text",
"data": "["
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"name": "xref",
"data": {
"text": "50",
"type": "bibr",
"rid": "R50",
"data": [
{
"name": "text",
"data": "50"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。在制备的复合材料中，分子筛基质能稳定碳点的三重态，并可以作为有效的能量受体，允许碳点到掺杂原子Mn的能量传递，从而产生红色室温磷光发射，但其磷光寿命较短(1.814 ms)"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "51",
"type": "bibr",
"rid": "R51",
"data": [
{
"name": "text",
"data": "51"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。在此基础上，为实现高效率的红色室温磷光发射，她们详细研究了CMET策略的两个关键因素:一个是碳源，它影响所制备碳点的三重态能级，从而影响其与能量受体的光谱重叠积分("
},
{
"name": "xref",
"data": {
"text": "图4(a)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(a)"
}
]
}
},
{
"name": "text",
"data": ")；二是锰原子在晶体骨架中的配位情况，这决定了晶体的场分裂，从而影响了受体的发射光谱("
},
{
"name": "xref",
"data": {
"text": "图4(b)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(b)"
}
]
}
},
{
"name": "text",
"data": ")。通过将预先设计的有机前体所制备的碳点嵌入具有六配位锰的目标骨架中，利用主客体的能量传递，制备了一种具有红色室温磷光的复合材料CDs@MnAPO-CJ50("
},
{
"name": "xref",
"data": {
"text": "图4(c)、(d)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(c)、(d)"
}
]
}
},
{
"name": "text",
"data": ")，与传统的有机和贵金属配合物材料相比，这种复合材料具有很高的稳定性，在防伪和发光方面具有潜在的应用价值。此外，还通过改变锰的配位数(四配位锰)和不同的碳前驱体，制备了一种具有黄绿色余辉的 CDs@MnAPO-tren复合材料。"
}
]
},
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"caption": [
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"label": [
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"data": "图4"
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"title": [
{
"name": "text",
"data": "碳点@锰开放骨架复合材料的设计示意图。(a)在水热条件下可能的碳点形成过程；(b)开放骨架中不同配位状态锰的发光；(c)碳点和含六配位Mn"
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"data": [
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"data": "2+"
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]
},
{
"name": "text",
"data": "的开放骨架MnAPO-50基质之间的能量传递；(d)含锰磷酸铝开放骨架MnAPO-CJ50的化学结构，其中蓝线标出的是与Mn"
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"data": "2+"
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]
},
{
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"data": "配位的有机模板剂"
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"data": "["
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"data": {
"text": "51",
"type": "bibr",
"rid": "R51",
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"data": "51"
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{
"name": "text",
"data": "。"
}
]
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"label": [
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],
"title": [
{
"name": "text",
"data": "Schematic representation of the design principle for CDs@Mn-framework composites. (a)Possible formation mechanism for CDs under hydrothermal conditions. (b)Different coordination geometries for Mn"
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{
"name": "text",
"data": "2+"
}
]
},
{
"name": "text",
"data": " ions in inorganic open frameworks with different emissions(shown in red and green-yellow). (c)Proposed CMET process between CDs and MnAPO-CJ50 matrix with octahedral Mn"
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"data": "2+"
}
]
},
{
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"data": " centers. (d)Chemical structure of Mn-containing aluminophosphate MnAPO-CJ50. The blue line highlights the organic template, which chelates with Mn"
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"data": "除了利用碳点-基质之间的能量传递调控余辉发射外，还可以在合成体系中引入两种碳点，利用不同碳点之间的能量转移来调控复合材料的余辉发射"
},
{
"name": "sup",
"data": [
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"name": "text",
"data": "["
},
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"data": {
"text": "52",
"type": "bibr",
"rid": "R52",
"data": [
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"data": "52"
}
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{
"name": "text",
"data": "。例如，通过在分子筛基质中引入蓝色碳点和绿色碳点，并改变绿色碳点前驱体的掺杂比例，改变其聚集碳化程度，使得蓝色碳点到绿色碳点之间的能量传递效率发生变化，从而将复合材料的TADF的颜色从蓝紫色调变到青色、浅绿色和橄榄绿。应用该方法制备的碳点@分子筛复合材料在室温空气条件下即可展现出最高荧光量子效率为42%、延迟荧光寿命860 ms的热活化延迟荧光，在防伪方面展示了潜在的应用。"
}
]
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"data": "3.2 激发态调控"
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"data": "到目前为止，杂原子掺杂、主客体复合、氢键聚集等策略都被开发用于实现碳点的超长室温磷光发光。但碳点基热致延迟荧光材料由于难以控制足够小的单线态-三线态能级差(Δ"
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]
},
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"data": "ST"
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]
},
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"name": "text",
"data": ")，实现激发态自由翻转，而鲜有报道。基于不同有机模板剂可以制备同一分子筛材料的特点，Yu和Li课题组通过调变不同的有机模板剂，开发了两种在室温空气环境下具有不同长余辉发射的碳点@分子筛复合材料"
},
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"data": "["
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"data": {
"text": "53",
"type": "bibr",
"rid": "R53",
"data": [
{
"name": "text",
"data": "53"
}
]
}
},
{
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"data": "]"
}
]
},
{
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"data": "。以(4-(2-氨基乙基)吗啉为模板剂制备的CDs@SBT-1展现出寿命长达574 ms的室温磷光发光行为，而以4,7,10-三氧-1,13-十三烷二胺为模板剂的CDs@SBT-2展现出寿命长达153 ms的热致延迟荧光发光行为。研究发现，不同的有机模板剂改变了原位生成的碳点的结构与组成，进而影响其发光能态，这两种复合材料具有不同的单线态-三线态能级差(Δ"
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]
},
{
"name": "text",
"data": ")，分别为0.36 eV及0.18 eV。因分子筛基质材料的稳定作用，碳点的三重激发态得以很好地保护，电子在室温下因由不同的Δ"
},
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"data": "E"
}
]
},
{
"name": "sub",
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"data": "ST"
}
]
},
{
"name": "text",
"data": "而呈现不同的电子跃迁过程。Δ"
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"data": "E"
}
]
},
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]
},
{
"name": "text",
"data": "较大的CDs@SBT-1主要呈现三重态的磷光发光；Δ"
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"data": [
{
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"data": "E"
}
]
},
{
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"data": "ST"
}
]
},
{
"name": "text",
"data": "较小的CDs@SBT-2中电子在室温热能活化下可以实现反系间窜跃过程，复合材料展现出热致延迟荧光发光现象("
},
{
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"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
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"data": "图5"
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},
{
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"data": ")。"
}
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"data": "(a)CDs@SBT-1和CDs@SBT-2的RTP/TADF机制；(b)安全防伪方面的应用示例"
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{
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"data": {
"text": "53",
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]
},
{
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"label": [
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],
"title": [
{
"name": "text",
"data": "(a)Proposed RTP/TADF mechanism of CDs@SBT-1 and CDs@SBT-2.(b)Application of CDs@SBT-1 and CDs@SBT-2 in security protection"
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{
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"data": [
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"text": "53",
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},
{
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"data": [
{
"name": "text",
"data": "寿命编码的光学多路复用可以有效地避免光谱重叠和背景干扰，被广泛应用于多个领域。实现寿命编码的光学多路复用的一个关键因素在于实现材料的发光寿命在宽范围内可调。目前，用于寿命编码的光学多路复用的材料大多含有毒性强、成本高且不可再生的稀土或重金属离子。此外，这些材料的寿命域局限在微秒。瞬态成像过程难以用相机捕捉，需要昂贵的时间分辨扫描系统，因此限制了寿命编码的光多路复用的应用。低毒性、低成本的碳点基室温磷光材料很容易实现秒级别的余辉发射，是裸眼可视的光多路复用的理想材料。"
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"data": [
{
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"data": "Yu和Li课题组通过调节碳点前驱体、沸石基质(拓扑结构和硅铝比)、晶化时间和温度，采用无溶剂合成法，设计了9种具有不同的室温磷光寿命的碳点@分子筛复合材料，其磷光寿命0.38~2.1 s"
},
{
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"data": [
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"data": "["
},
{
"name": "xref",
"data": {
"text": "54",
"type": "bibr",
"rid": "R54",
"data": [
{
"name": "text",
"data": "54"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "("
},
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"data": {
"text": "图6(a)、(b)",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6(a)、(b)"
}
]
}
},
{
"name": "text",
"data": ")。一般来说，最低单线态和最低三线态之间的带隙值越小，以及能促进S态和T态之间自旋轨道耦合的C"
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"data": "N键越多，越有利于产生一个较大的系间窜跃速率和较长的磷光寿命。此外，对碳点有效的固定，如将碳点限域在主体基质中，或构筑一个可以作为基质来自稳定三重态激子的致密碳核，会有效地抑制非辐射跃迁过程，降低非辐射跃迁速率，从而延长磷光寿命。在该工作中，受各种反应因素的影响，碳点的带隙值、碳点表面官能团的含量、碳核的结构以及碳点和沸石基质之间的相互作用可以调变，因此导致了可调的系间窜跃速率以及非辐射跃迁速率，这是实现碳点@分子筛复合材料磷光寿命设计的关键。鉴于这一系列材料具有宽范围内可调的长磷光寿命，将其应用于裸眼可视的寿命编码的光学多路复用，实现了人物加密("
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"text": "图6(c)、(d)",
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"data": ")。"
}
]
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"title": [
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"data": "(a)碳点和分子筛的前驱体；(b)碳点和碳点@分子筛复合材料制备示意图；(c)9种碳点@分子筛复合材料的伪彩处理磷光图像；(d)光多路复用应用"
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"data": {
"text": "54",
"type": "bibr",
"rid": "R54",
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"data": "54"
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},
{
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"data": "。"
}
]
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"label": [
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"title": [
{
"name": "text",
"data": "(a)Molecular formula diagrams of CDs and zeolite precursors. (b)Schematic diagrams of preparation process of CDs and CDs@zeolite composites. (c)Pseudo-color-mapped phosphorescence images of nine kinds of CDs@zeolite composites with various RTP lifetimes. (d)Optical multiplexing application"
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"data": "["
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"data": {
"text": "54",
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"rid": "R54",
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{
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"data": "54"
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"data": [
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"data": "碳点@分子筛复合材料的发光性质不仅与客体碳点本身的结构、含有的官能团以及能级有关，与作为主体基质的分子筛也密切相关。"
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]
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"data": "4.1 限域作用"
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"data": [
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"name": "text",
"data": "分子筛多孔材料在碳点生长过程中的一个重要作用是限域作用。作为一类具有规则有序孔道的基质材料，分子筛纳米空间为碳点的生长提供了理想的刚性微环境，避免碳点聚集诱导的荧光猝灭效应，促进其在固态设备中的应用。同时也限制了碳点尺寸的增长，从而产生尺寸大小较均一的碳点，特别是利用热解法制备的碳点@分子筛复合材料中碳点的尺寸可以小于2 nm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
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"name": "xref",
"data": {
"text": "46",
"type": "bibr",
"rid": "R46",
"data": [
{
"name": "text",
"data": "46"
}
]
}
},
{
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"data": "]"
}
]
},
{
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"data": "。但在原位合成的复合材料中，碳点通常会打破分子筛孔道限域生长在中断的缺陷位，形成碳点的尺寸为2~3 nm"
},
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"data": [
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"data": "["
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"data": {
"text": "50",
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"data": "50"
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}
},
{
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"data": "-"
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"data": [
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"data": "近期，Yu和Li课题组讨论了分子筛基质对碳点@分子筛复合材料磷光寿命的影响"
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{
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"data": [
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"data": "["
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"data": {
"text": "47",
"type": "bibr",
"rid": "R47",
"data": [
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"data": "47"
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}
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{
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"data": "]"
}
]
},
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"data": "。结果表明，以SAPO-20分子筛(SOD拓扑结构)为基质的复合材料的磷光寿命要远远低于以AlPO-5分子筛(AFI拓扑结构)为基质的复合材料的磷光寿命，并且在SAPO-20体系中，具有较大的Si/Al比的复合材料的磷光寿命也较长。进一步的研究发现，无论是分子筛拓扑结构还是Si/Al比主要影响的是碳点非辐射跃迁的速率，进而影响磷光寿命。由此可见，只有能够为碳点提供良好的限域环境的分子筛才能使碳点与分子筛之间具有较强的主-客体相互作用，进而有效地抑制碳点三重态激子的非辐射衰减，提高余辉寿命。"
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"data": "分子筛多孔材料的另一个重要作用是稳定客体碳点。具有惰性化学组成的分子筛作为基质会阻止氧气、温度、酸碱、机械破坏等导致的碳点光猝灭，稳定碳点的发光。此外，研究者还发现分子筛骨架可与碳点形成氢键甚至共价键，这类价键会限制碳点的振动和转动从而大大地减少非辐射跃迁，产生长寿命、高量子产率的长余辉发射。例如，CDs@MnAPO-CJ50复合材料在14种常见溶剂中储存10 d后，其发光强度和寿命不会发生猝灭，表明该材料具有很好的耐溶剂稳定性。此外，碳点@AlPO-5复合材料在365 nm紫外灯下连续辐射8 h，或在150 ℃中加热30 min后，其发光强度和寿命均能得到维持，说明该复合材料具有很好的耐光照和耐热稳定性。"
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"data": [
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"data": "基于碳点的主客体复合体系易于发生能量的传递过程，有效的能量传递可以发生在碳点和金属离子、碳点和碳点之间。分子筛材料中的紧密空间使给体和受体之间距离足够小，以便形成有效的能量转移途径。此外，分子筛骨架可以引入多种杂原子(除Si, Al, P外的原子)，杂原子作为能量受体可接受碳点的能量，发射出由杂原子类型、配位状态和不同晶体场调控下的不同光致发光颜色的荧光。因此，一个良好的主客体能量传递体系可以促进碳点在发光、光催化等方面具有前所未有的性能和潜力。"
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{
"name": "text",
"data": "作为一类新型的发光纳米材料，碳点@分子筛复合材料因其独特的发光性质，特别是长余辉发光引起了人们极大的关注。分子筛和碳点的多样性和可调控性，为大量新型的具有不同发光特性的碳点@分子筛复合材料的合成提供了可能，这类材料在生物成像、传感等方面的创新应用也将进一步得以开拓。同时，我们也认识到，目前该领域的研究还存在一些问题，如对复合材料发光的机理、激子的跃迁弛豫过程认识不够深入；长波长发射的复合材料仍难以合成；复合材料的应用比较单一，多用于防伪，需要向光催化、检测传感、光电材料等领域做更进一步的深入探索等。在今后的研究中，通过预先设计与筛选主客体材料、优化复合材料的合成方法、借助更先进的表征技术与理论计算，有望在复合材料的发光调控、机理研究和应用拓展上得以创新。"
}
]
},
{
"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.20210196."
}
]
}
]
}
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"ppub": "2021-08-01",
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"year": "2021"
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"journalTitle": "发光学报",
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}
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