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聚集诱导发光材料在光学诊疗中的研究进展
特邀报告 | 更新时间：2021-03-19
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聚集诱导发光材料在光学诊疗中的研究进展
- Recent Advances of Aggregation-induced Emission Materials in Phototheranostics
- 发光学报 2021年 42卷 第3期 (2021)
- 作者机构：深圳大学 材料学院， AIE研究中心,广东,深圳,518060;香港科技大学 化学系， 国家人体组织功能重建工程技术研究中心香港分中心,香港,中国,999077
- 作者简介：
- 基金信息：国家自然科学基金(51903163;21801169);中国博士后科学基金(2019M653036);广东省杰出青年基金(2020B1515020011);深圳市自然科学基金(JCYJ20190808153415062)
- DOI：10.37188/CJL.20210029 中图分类号： O482.31
纸质出版日期：2021-03-01，
收稿日期：2021-01-16，
修回日期：2021-02-02，
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引用本文
张志军, 康苗苗, 王媛玮, 等. 聚集诱导发光材料在光学诊疗中的研究进展[J]. 发光学报, 2021, 42(3):361-378.
Zhi-jun ZHANG, Miao-miao KANG, Yuan-wei WANG, et al. Recent Advances of Aggregation-induced Emission Materials in Phototheranostics[J]. Chinese Journal of Luminescence, 2021, 42(3):361-378.
张志军, 康苗苗, 王媛玮, 等. 聚集诱导发光材料在光学诊疗中的研究进展[J]. 发光学报, 2021, 42(3):361-378. DOI： 10.37188/CJL.20210029.
Zhi-jun ZHANG, Miao-miao KANG, Yuan-wei WANG, et al. Recent Advances of Aggregation-induced Emission Materials in Phototheranostics[J]. Chinese Journal of Luminescence, 2021, 42(3):361-378. DOI： 10.37188/CJL.20210029.
聚集诱导发光材料在光学诊疗中的研究进展
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"data": "光学诊疗是一种利用光激活的激发态能量转化效应实现疾病诊断和同时原位治疗的新型诊疗模式，它具有时空选择性高、毒副作用低、疗效好和可控性强等优点，在疾病诊疗中展现了巨大的应用潜力。近些年，得益于其生物安全性好、光物理性质可调、易于合成和功能化修饰、出色的荧光和光敏性能、以及可便于构筑多模态诊疗试剂等优势，聚集诱导发光材料在光学诊疗领域取得了重大突破进展。基于此，本文从如何通过精准分子设计以及调控分子在聚集态下的运动构筑高效的聚集诱导发光光诊疗体系出发，从荧光成像指导的光动力治疗、光声成像指导的光热治疗和多模态成像指导的协同治疗三个方面总结了聚集诱导发光材料在光学诊疗领域的最新研究进展，并对其未来的发展方向与前景进行了展望。"
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"data": "诊疗一体化是将疾病诊断和治疗手段有机同步地结合起来、在诊断的同时实现疾病治疗的一种新方法"
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"data": "。诊疗一体化的实施将药物靶向递送、示踪、疾病治疗和疗效反馈等多种功能有效地整合为一体，实现了多模态影像诊断以及影像指导的联合治疗，从而极大地提高了疾病治疗的精准性和有效性"
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"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。随着光学技术和纳米技术的迅速发展，光学诊疗(Phototheranostics)逐渐发展成为诊疗一体化领域中的一个重要分支"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "4",
"type": "bibr",
"rid": "R4",
"data": [
{
"name": "text",
"data": "4"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。与传统的诊疗方法相比，光学诊疗是一种利用光(特别是近红外光)激活的激发态能量转化效应实现疾病诊断和实时原位治疗的新型诊疗模式，它具备时空选择性高、毒副作用低、创伤小、疗效好和可控性强等优点，已成为国际纳米生物医药领域的研究热点之一，也是向医疗精准化和个体化方向发展的有效途径"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "5",
"type": "bibr",
"rid": "R5",
"data": [
{
"name": "text",
"data": "5"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "6",
"type": "bibr",
"rid": "R6",
"data": [
{
"name": "text",
"data": "6"
}
]
}
}
],
"rid": [
"R5",
"R6"
],
"text": "5-6",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "迄今为止，多种有机和无机材料包括金纳米棒、纳米碳管、量子点、磁性纳米粒子、氧化石墨烯、有机聚合物和小分子等已被开发用于光学诊疗的研究"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "7",
"type": "bibr",
"rid": "R7",
"data": [
{
"name": "text",
"data": "7"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。其中，有机小分子材料具有确定且易于修饰的化学结构、良好的重现性和优异的生物相容性，有望发展成为一类极具临床转化前景的光诊疗剂"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "8",
"type": "bibr",
"rid": "R8",
"data": [
{
"name": "text",
"data": "8"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。此外，在用于构建光学诊疗体系的多种成像手段中，荧光成像(Fluorescence imaging，FLI)具有灵敏度高、操作简便且能对细胞和活体进行无损实时跟踪等诸多优势，已成为疾病研究、医疗实践和临床实验中一个不可或缺的工具"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "9",
"type": "bibr",
"rid": "R9",
"data": [
{
"name": "text",
"data": "9"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "10",
"type": "bibr",
"rid": "R10",
"data": [
{
"name": "text",
"data": "10"
}
]
}
}
],
"rid": [
"R9",
"R10"
],
"text": "9-10",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。然而，传统的有机荧光染料在稀溶液中强烈发光，而在高浓度或聚集态下易发生严重的分子间π-π堆积导致荧光减弱甚至完全消失，这一现象即为“聚集导致荧光猝灭(Aggregation-caused quenching，ACQ)”"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "11",
"type": "bibr",
"rid": "R11",
"data": [
{
"name": "text",
"data": "11"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。ACQ效应极大地限制了染料分子在生物诊断中的使用浓度，从而显著降低了检测体系的灵敏度以及成像的光稳定性。事实上，即便在生物成像中使用较低浓度的荧光染料也仍然难以消除ACQ效应，因为染料分子的大π共轭结构赋予了其极强的疏水性，从而使得其在机体内水环境下易于聚集。此外，传统荧光染料的斯托克斯位移较小(一般"
},
{
"name": "text",
"data": "<"
},
{
"name": "text",
"data": "50 nm)，激发和发射光谱之间存在严重串扰，导致成像信噪比低，进一步限制了其在生物成像中的应用。特别地，类似于大多数传统荧光分子遭受的ACQ问题，目前临床应用的有机小分子光敏剂(如卟啉类)在使用过程中随着浓度增加或包裹于纳米载体时，其光化学效率或光敏性能也会急剧下降，这归因于聚集态下分子间形成的强π-π作用促进了激发态能量通过其他非辐射途径耗散"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "12",
"type": "bibr",
"rid": "R12",
"data": [
{
"name": "text",
"data": "12"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。以上特点是传统平面型有机荧光染料和光敏剂分子的固有性质，难以改善。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "2001年，唐本忠院士课题组基于观察到的1-甲基-1，2，3，4，5-五苯基噻咯(HPS)在乙腈中不发光、但在含大量不良溶剂(水)的乙腈溶液中发出很强绿色荧光的现象，首次提出了“聚集诱导发光(Aggregation-induced emission，AIE)”概念，并开发了一系列具有AIE性质的有机荧光小分子"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "13",
"type": "bibr",
"rid": "R13",
"data": [
{
"name": "text",
"data": "13"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "14",
"type": "bibr",
"rid": "R14",
"data": [
{
"name": "text",
"data": "14"
}
]
}
}
],
"rid": [
"R13",
"R14"
],
"text": "13-14",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。与传统有机荧光染料不同，这类特殊的化合物具有独特的螺旋桨式分子构型，分子内存在大量的转子和/或振子，在溶液中由于活跃的分子内运动，激发态能量以热耗散的形式散失，分子不发光或只发射微弱的荧光；而在聚集状态下由于分子内运动受限(Restriction of intramolecular motion，RIM)，非辐射跃迁被抑制实现荧光显著增强"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "15",
"type": "bibr",
"rid": "R15",
"data": [
{
"name": "text",
"data": "15"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。AIE分子这种“越聚集越亮”的性质有效克服了传统荧光分子ACQ效应的局限，在使用过程中无需控制浓度，也不必担心将其负载入纳米载体后发生聚集荧光猝灭现象，反而在该状态下可以发出更强的荧光，大大提高了荧光探针的检测灵敏度和成像光稳定性，拓展了有机小分子荧光材料的应用范围"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "16",
"type": "bibr",
"rid": "R16",
"data": [
{
"name": "text",
"data": "16"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "17",
"type": "bibr",
"rid": "R17",
"data": [
{
"name": "text",
"data": "17"
}
]
}
}
],
"rid": [
"R16",
"R17"
],
"text": "16-17",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。除此之外，AIE分子还具有发光波长易于调节、斯托克斯位移大、发光效率高且能够对研究目标实现“点亮”检测等特点，在疾病诊断方面具有极大的优势"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "18",
"type": "bibr",
"rid": "R18",
"data": [
{
"name": "text",
"data": "18"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "20",
"type": "bibr",
"rid": "R20",
"data": [
{
"name": "text",
"data": "20"
}
]
}
}
],
"rid": [
"R18",
"R19",
"R20"
],
"text": "18-20",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。同时通过发挥其结构可调、功能基团可修饰的优点，AIE材料在聚集状态下除了具有高效的发光效率之外，还被证明具有卓越的活性氧(Reactive oxygen species，ROS)产生能力，在光动力治疗(Photodynamic therapy，PDT)领域具有广阔的应用前景"
},
{
"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": "。根据Jablonski能级图"
},
{
"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": "("
},
{
"name": "xref",
"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": ")，其优异活性氧产生能力主要可以从以下两点来阐述：一、在聚集状态下，AIE材料通过热耗散衰变能量的非辐射渠道被禁阻，使得激发态能量只能通过辐射衰变和系间窜越(Intersystem crossing，ISC)途径来消耗。前者能够促进发光效率的极大提升，后者有利于活性氧的产生。二、根据“聚集导致系间窜越(Aggregation-induced intersystem crossing，AI-ISC)”理论"
},
{
"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": "，相比单分子状态而言，聚集状态下分子的单线态(S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": ")和三线态间(T"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": ")的能量匹配更好，单线态到三线态的能极差(Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": ")更小，有利于激子能量由单线态向三线态转移，促进系间窜越速率，进而提升活性氧的产生效率。"
}
]
},
{
"name": "fig",
"data": {
"id": "F1",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图1"
}
],
"title": [
{
"name": "text",
"data": "Jablonski能级图以及不同光物理过程在高效光诊疗剂开发中发挥的指导作用"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "22",
"type": "bibr",
"rid": "R22",
"data": [
{
"name": "text",
"data": "22"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.1"
}
],
"title": [
{
"name": "text",
"data": "Schematic illustration of Jablonski diagram and its important role in guiding the design of high-performance phototheranostic agents"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "22",
"type": "bibr",
"rid": "R22",
"data": [
{
"name": "text",
"data": "22"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
}
]
}
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},
{
"name": "p",
"data": [
{
"name": "text",
"data": "除了利用分子内运动受限理论用以开发高效的AIE光敏剂之外，最近有研究表明，通过主动促进AIE分子在纳米聚集体中的运动，AIE材料还能够被开发成为具有优良光热转换效率的光热转换剂，实现高效的光热治疗(Photothermal therapy，PTT)"
},
{
"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": "。在特定波长的激发光照射下，AIE分子吸收光能并将其转化为热能，使附近的组织发生热弹性膨胀，由此形成的宽带超声波发射还可用于光声成像(Photoacoustic imaging，PAI)，便于实现光声成像指导的光热治疗"
},
{
"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": "。另外，AIE分子产生的热量还可被热成像系统捕获用于光热成像(Photothermal imaging，PTI)，实现对光热治疗过程的实时监测"
},
{
"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": "。AIE分子结构中含有大量能够运动的基团，使其拥有内在的独特优势成为平衡能量耗散的绝佳模板。通过合理的结构设计，使AIE分子在聚集状态下的运动仅受到部分限制，进而调控辐射衰变和非辐射衰变之间的平衡以最大化地利用激发态能量，还可将AIE分子开发成为多功能光诊疗剂，实现多模态成像指导的协同治疗。AIE材料在光学诊疗领域展现出优异的“聚集增强诊疗(Aggregation-enhanced theranostics, AET)”特征"
},
{
"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": "，具有传统材料很难拥有的单分子多功能性，可以用来简化材料设计，提高制备的可重复性"
},
{
"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": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "基于此，本文综述了AIE材料在光学诊疗中的最新研究进展，从荧光成像指导的光动力治疗、光声成像指导的光热治疗和多模态成像指导的协同治疗三个方面进行了系统概括和总结，并对其未来的发展方向与前景进行了展望。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2 荧光成像指导的光动力治疗"
}
],
"level": "1",
"id": "s2"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "光动力治疗是利用光和光敏剂共同作用以实现疾病治疗的一种新方法"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "30",
"type": "bibr",
"rid": "R30",
"data": [
{
"name": "text",
"data": "30"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。通过使用特定波长的光照射病变部位，使聚集在病灶部位的光敏剂活化，生成具有细胞毒性的活性氧，从而氧化破坏组织、细胞或微生物中的各种生物大分子，产生毒性作用或引起机体的其他生物反应，使病变细胞或微生物发生不可逆的损伤，最终导致其死亡，达到疾病治疗的目的"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "31",
"type": "bibr",
"rid": "R31",
"data": [
{
"name": "text",
"data": "31"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "33",
"type": "bibr",
"rid": "R33",
"data": [
{
"name": "text",
"data": "33"
}
]
}
}
],
"rid": [
"R31",
"R32",
"R33"
],
"text": "31-33",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。相比于传统的治疗手段，光动力治疗具有非侵入性、可控性、高时空精度和低毒副作用等优势，在多种疾病的治疗方面表现出巨大的优势和应用前景"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "34",
"type": "bibr",
"rid": "R34",
"data": [
{
"name": "text",
"data": "34"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "35",
"type": "bibr",
"rid": "R35",
"data": [
{
"name": "text",
"data": "35"
}
]
}
}
],
"rid": [
"R34",
"R35"
],
"text": "34-35",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "作为光动力治疗的核心，光敏剂在光动力治疗中的作用至关重要，其性能的好坏直接影响光动力治疗的效果。具有AIE性质的光敏剂分子除了具有生物相容性好、光学性质优异、光稳定性好等优势，还表现出优良的光敏性能"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "16",
"type": "bibr",
"rid": "R16",
"data": [
{
"name": "text",
"data": "16"
}
]
}
},
{
"name": "text",
"data": ","
},
{
"name": "xref",
"data": {
"text": "28",
"type": "bibr",
"rid": "R28",
"data": [
{
"name": "text",
"data": "28"
}
]
}
},
{
"name": "text",
"data": ","
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
}
]
}
}
],
"rid": [
"R36",
"R37"
],
"text": "36-37",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。近年来，研究者通过不同的策略设计出了结构各异的基于AIE分子的光诊疗体系用于荧光成像指导的光动力治疗"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
]
}
},
{
"name": "text",
"data": ","
},
{
"name": "xref",
"data": {
"text": "38",
"type": "bibr",
"rid": "R38",
"data": [
{
"name": "text",
"data": "38"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.1 D-A策略"
}
],
"level": "2",
"id": "s2a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "一般而言，当光敏剂分子吸收光子能量后，会由基态(S"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "0"
}
]
},
{
"name": "text",
"data": ")跃迁到激发单线态，处于激发单线态的分子，可以通过非辐射跃迁释放热量或辐射跃迁发射荧光两条途径返回基态。当Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "足够小时，激发单线态的光敏剂分子可以快速通过ISC途径跃迁至较长寿命的激发三线态。随后，处于三线态的光敏剂与底物或者周围氧分子之间发生电子转移或能量转移，产生Ⅰ型活性氧(自由基类)或Ⅱ型活性氧(单线态氧，"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "O"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": ")，进而发挥光动力治疗作用"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "39",
"type": "bibr",
"rid": "R39",
"data": [
{
"name": "text",
"data": "39"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "42",
"type": "bibr",
"rid": "R42",
"data": [
{
"name": "text",
"data": "42"
}
]
}
}
],
"rid": [
"R39",
"R40",
"R41",
"R42"
],
"text": "39-42",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。因此，提高系间窜越效率、增加三线态产率是设计高效光敏剂的常用策略"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
]
}
},
{
"name": "text",
"data": ","
},
{
"name": "xref",
"data": {
"text": "43",
"type": "bibr",
"rid": "R43",
"data": [
{
"name": "text",
"data": "43"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。依据系间窜越速率公式"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "44",
"type": "bibr",
"rid": "R44",
"data": [
{
"name": "text",
"data": "44"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，降低Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "可以显著提高系间窜越速率。将AIE分子设计成具有典型电子给体(D)-电子受体(A)结构实现最高占据分子轨道(HOMO)和最低未占分子轨道(LUMO)之间的有效分离是降低Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "、增加系间窜越速率的一个简便有效的策略"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
]
}
},
{
"name": "text",
"data": ","
},
{
"name": "xref",
"data": {
"text": "44",
"type": "bibr",
"rid": "R44",
"data": [
{
"name": "text",
"data": "44"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "Liu等于2014年报道了第一例D-A构型的AIE光敏剂用于荧光成像指导的光动力治疗"
},
{
"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，强D-A构型的引入，还有利于AIE光敏剂吸收和发射波长的红移，便于生物体内的诊疗应用。例如，Liu课题组报道了一个具有近红外发射的光敏剂分子TPETCAQ用于近红外荧光成像指导的光动力治疗"
},
{
"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": "。如"
},
{
"name": "xref",
"data": {
"text": "图2(a)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(a)"
}
]
}
},
{
"name": "text",
"data": "所示，他们通过在AIE分子TPEDC1的电子给体和受体之间引入苯环得到AIE分子TPEDC2，苯环的引入使得TPEDC2分子的共轭延长，HOMO和LUMO进一步分离，其中LUMO主要分布于双氰基乙烯基(DC)受体上，导致Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "从0.350 eV下降到0.230 eV，提高了其单线态氧产率；随后，在TPEDC2分子的受体部分进一步引入DC基团得到目标分子TPETCAQ。由于TCAQ部分特殊的芳香结构和较强的吸电子效应，TPETCAQ分子的LUMO主要限域在TCAQ部分，HOMO和LUMO出现明显分离，导致Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "进一步降低为0.067 eV，使得单线态氧产率进一步提高("
},
{
"name": "xref",
"data": {
"text": "图2(b)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(b)"
}
]
}
},
{
"name": "text",
"data": ")。此外，强的D-A效应促使TPETCAQ的发射波长红移至近红外光区(发射峰约为820 nm)，为该分子用于近红外荧光成像指导的光动力治疗提供了保障。最近的研究表明，在AIE骨架上引入多个电子给体或电子受体能够进一步提高其光敏性能，而且引入更多的电子受体比引入更多的电子给体更加有利于Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "的降低"
},
{
"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": "。如"
},
{
"name": "xref",
"data": {
"text": "图2(c)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(c)"
}
]
}
},
{
"name": "text",
"data": "所示，Tang等设计了4个含有不同数量电子给体和电子受体的AIE分子TBT、BTB、TBTBT和BTBTB。实验结果表明，含有更多电子受体的BTB和BTBTB分子具有更强的光敏效率("
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "Φ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "o"
}
]
},
{
"name": "text",
"data": "为8.7%和10.8%)，明显高于含有更多电子给体的TBT和TBTBT("
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "Φ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "o"
}
]
},
{
"name": "text",
"data": "为5.6%和7.0%)("
},
{
"name": "xref",
"data": {
"text": "图2(d)",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2(d)"
}
]
}
},
{
"name": "text",
"data": ")。"
}
]
},
{
"name": "fig",
"data": {
"id": "F2",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图2"
}
],
"title": [
{
"name": "text",
"data": "(a)具有高活性氧产率的近红外AIE光敏剂TPETCAQ的分子结构和设计示意图；(b)TPEDC1、TPEDC2和TPETCAQ的HOMO-LUMO能级的分子轨道振幅图和Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "inlineformula",
"data": [
{
"name": "math",
"data": {
"math": ""
}
}
]
},
{
"name": "text",
"data": "；(c)含有不同数目电子给体和电子受体的TBT、BTB、TBTBT和BTBTB的分子结构；(d)TBT、BTB、TBTBT和BTBTB的荧光量子产率和光敏效率"
},
{
"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": "。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.2"
}
],
"title": [
{
"name": "text",
"data": "(a)Design scheme and molecular structure of NIR AIE-active photosensitizer TPETCAQ. (b)Molecular orbital amplitude plots of HOMO and LUMO energy levels and Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": " of TPEDC1, TPEDC2 and TPETCAQ"
},
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"text": "46",
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},
{
"name": "text",
"data": ". (c)Molecular structures of TBT, BTB, TBTBT and BTBTB possessing different amount of electron donor and electron acceptor. (d)Quantum yields("
},
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"data": [
{
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"data": "Φ"
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"data": "f"
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]
},
{
"name": "text",
"data": ") and photosensitization efficiencies("
},
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"data": [
{
"name": "text",
"data": "Φ"
}
]
},
{
"name": "sub",
"data": [
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"data": "o"
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{
"name": "text",
"data": ") of TBT, BTB, TBTBT and BTBTB"
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"name": "sup",
"data": [
{
"name": "text",
"data": "["
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"name": "xref",
"data": {
"text": "47",
"type": "bibr",
"rid": "R47",
"data": [
{
"name": "text",
"data": "47"
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{
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"data": "．"
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"data": "依据D-A策略，目前已有一系列不同激发和发射波长(涵盖紫外可见到近红外区域)的D-A构型AIE光敏剂被相继开发并用于荧光成像指导的光动力治疗"
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"text": "16",
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"data": [
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"data": "16"
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"data": ","
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"data": {
"text": "21",
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"data": "21"
}
]
}
},
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"data": ","
},
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"data": {
"text": "28",
"type": "bibr",
"rid": "R28",
"data": [
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"data": "28"
}
]
}
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"data": ","
},
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"data": [
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"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
}
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}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
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}
}
],
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"R37"
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"text": "36-37",
"type": "bibr"
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},
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]
},
{
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"data": "。如Tang等通过引入正电性的基团作为电子受体设计合成D-A构型的AIE分子TPE-IQ-2O，在癌细胞负电性的线粒体膜和正电性TPE-IQ-2O之间静电相互作用的驱动下，成功实现癌细胞线粒体靶向成像和癌细胞选择性光动力杀伤"
},
{
"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": "。此外，该课题组还报道了一类自报告型AIE光诊疗剂TPE-4EP"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "＋"
}
]
},
{
"name": "text",
"data": "，在光动力诱导癌细胞死亡后，TPE-4EP"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "＋"
}
]
},
{
"name": "text",
"data": "可以从线粒体转移到细胞核，指示治疗终点，有助于提高治疗的精准性，避免过度治疗"
},
{
"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": "。随后，该课题组又报道了一系列可用于线粒体靶向的双光子成像引导的光动力治疗的AIE诊疗剂"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
}
]
}
},
{
"name": "text",
"data": ","
},
{
"name": "xref",
"data": {
"text": "50",
"type": "bibr",
"rid": "R50",
"data": [
{
"name": "text",
"data": "50"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。此外，研究者们还设计出了靶向细胞膜、脂滴、内质网等细胞器的AIE光诊疗剂，通过在光照条件下产生ROS诱导细胞凋亡或坏死，实现癌细胞的高效光动力杀伤"
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"name": "text",
"data": "["
},
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"data": {
"data": [
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"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
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"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
}
]
}
}
],
"rid": [
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"R37"
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"type": "bibr"
}
},
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"name": "text",
"data": ","
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "51",
"type": "bibr",
"rid": "R51",
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"data": "51"
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"data": "-"
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"data": {
"text": "52",
"type": "bibr",
"rid": "R52",
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"data": "52"
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}
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"type": "bibr"
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"data": "]"
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]
},
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"name": "text",
"data": "。最近，Tang等还开发了一系列D-A构型的I型AIE光敏剂，用于I型活性氧介导的肿瘤光动力治疗"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "53",
"type": "bibr",
"rid": "R53",
"data": [
{
"name": "text",
"data": "53"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。由于I型活性氧的产生对于氧气的依赖性较小，该策略能够有效克服基于Ⅱ型活性氧的传统光动力治疗所面临的肿瘤内部乏氧问题，提高光动力治疗的效果。除了癌症治疗，AIE光敏剂在病原菌的检测和杀伤领域也有广泛的应用"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "54",
"type": "bibr",
"rid": "R54",
"data": [
{
"name": "text",
"data": "54"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，如Tang等通过调控分子D-A效应，设计合成了一系列吸收和发射波长逐渐红移、活性氧产生逐渐增强的AIE光敏剂，并将其成功应用于革兰氏阳性菌的检测和光动力抗菌以及大鼠皮肤伤口革兰氏阳性菌感染的治疗，收到了良好效果"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "55",
"type": "bibr",
"rid": "R55",
"data": [
{
"name": "text",
"data": "55"
}
]
}
},
{
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"data": "]"
}
]
},
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"name": "text",
"data": "。"
}
]
}
]
},
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"title": [
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"data": "2.2 聚合策略"
}
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}
},
{
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"data": [
{
"name": "text",
"data": "除了D-A策略，Liu等报道了另外一种能够降低Δ"
},
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"data": [
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"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
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"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "来提高单线态氧产生效率的新方法，即聚合增强光敏策略"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "56",
"type": "bibr",
"rid": "R56",
"data": [
{
"name": "text",
"data": "56"
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]
}
},
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]
},
{
"name": "text",
"data": "。如"
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"name": "xref",
"data": {
"text": "图3(a)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(a)"
}
]
}
},
{
"name": "text",
"data": "所示，基于AIE分子SM1、SM2、SM3和非AIE分子SM4，他们制备了4种相对应的共轭聚合物光敏剂CP1-CP4。与相应小分子光敏剂相比，共轭聚合物具有更高的单线态氧产生效率，如共轭聚合物CP1的单线态氧产率提高了5.07倍，是光动力治疗中最常用的光敏剂之一Ce6(Chlorin e6)的3.71倍。密度泛函理论模拟结果表明，随着聚合度的增加，光敏剂激发单线态和三线态之间的能量匹配更好，能极差逐渐减小，系间窜越途径增多且速率提高，单线态氧产率由此得以提高("
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"data": {
"text": "图3(b)、(c)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(b)、(c)"
}
]
}
},
{
"name": "text",
"data": ")。此外，与对应小分子相比，所制备的这4种共轭聚合物的摩尔吸光系数均有所提升，且部分聚合物的最大吸收波长也发生红移，这使得共轭聚合物光敏剂的吸光能力也增强，进一步促进了单线态氧的产生。基于CP1较高的单线态氧产率和深红/近红外荧光发射("
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "Φ"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "f"
}
]
},
{
"name": "text",
"data": " 为6.2%)，研究者们利用两亲性聚合物DSPE-PEG作为包覆基质，进一步制备了具有优异的水溶液分散性的纳米颗粒CP1 NPs，并通过细胞水平和小鼠体内水平实验验证了CP1 NPs在肿瘤荧光成像引导的光动力治疗中的效果。实验结果表明，与其相应的小分子光敏剂SM1和商用光敏剂Ce6相比，共轭聚合物CP1表现出更加优异的光动力治疗效果。更重要的是，CP1 NPs可以在短时间内(静脉注射3 d后)通过肠道排出体外，表现出良好的生物相容性。"
}
]
},
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"data": {
"id": "F3",
"caption": [
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"lang": "zh",
"label": [
{
"name": "text",
"data": "图3"
}
],
"title": [
{
"name": "text",
"data": "(a)小分子SM1、SM2、SM3、SM4和相对应的共轭聚合物CP1、CP2、CP3、CP4的分子结构；(b)小分子光敏剂和共轭聚合物光敏剂不同的光敏作用过程；(c)不同模型化合物的理论计算能级图和可能的ISC跃迁渠道"
},
{
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"data": [
{
"name": "text",
"data": "["
},
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"data": {
"text": "56",
"type": "bibr",
"rid": "R56",
"data": [
{
"name": "text",
"data": "56"
}
]
}
},
{
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"data": "]"
}
]
},
{
"name": "text",
"data": "；(d)小分子光敏剂TPEDC以及共轭聚合物光敏剂PTPEDC1和PTPEDC2的分子结构；(e)TPEDC、PTPEDC1、PTPEDC2的吸收和发射光谱；(f)Ce6和TPEDC、PTPEDC1、PTPEDC2纳米颗粒的活性氧产生情况；(g)TPEDC、PTPEDC1和PTPEDC2纳米颗粒在水溶液中的双光子吸收截面；(h)PTPEDC2纳米颗粒在斑马鱼肝脏肿瘤双光子成像和双光子光动力治疗中的应用"
},
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"data": [
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"data": "["
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"data": {
"text": "60",
"type": "bibr",
"rid": "R60",
"data": [
{
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"data": "60"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.3"
}
],
"title": [
{
"name": "text",
"data": "(a)Molecular structures of small molecular SM1, SM2, SM3, SM4 and conjugated polymer CP1, CP2, CP3, CP4. (b)Different photosensitization processes of small-molecule photosensitizer and conjugated polymer photosensitizer. (c)Calculated energy levels and possible ISC channels of different model compounds"
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"data": "["
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"data": [
{
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"data": "56"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": ". (d)Chemical structures of TPEDC, PTPEDC1 and PTPEDC2. (e)Normalized absorption and photoluminescence(PL) spectra of AIE PS dots in aqueous media. (f)ROS generation measurement of PS dots in aqueous media. (g)Two-photon absorption cross-section(2PACS) spectra of PS dots in aqueous solution. (h)Two-photon(2PF) imaging and two-photon excited photodynamic therapy(2PE-PDT) of PTPEDC2 dots in zebrafish liver tumor model"
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"data": "["
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"data": {
"text": "60",
"type": "bibr",
"rid": "R60",
"data": [
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"data": "60"
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"data": [
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"data": "近年来，为实现深层组织中肿瘤的光动力治疗，研究者将目光转向了双光子光动力治疗。与单光子激发的光动力治疗不同，双光子光动力是一种利用近红外光来激发光敏剂产生活性氧的方法"
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"data": "["
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"data": {
"text": "57",
"type": "bibr",
"rid": "R57",
"data": [
{
"name": "text",
"data": "57"
}
]
}
},
{
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"data": "]"
}
]
},
{
"name": "text",
"data": "。双光子光敏剂的引入将激发光波长从可见光区红移到了近红外区，能够克服光源在生物组织中穿透深度低的问题，为深层组织肿瘤治疗提供了可能。另外，基于光敏剂的非线性双光子吸收特性，双光子激发可以对分布在肿瘤组织中的光敏剂实现三维层面上的精准激活，实现高效可控精准的光动力治疗"
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"data": "["
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"data": {
"text": "58",
"type": "bibr",
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"data": [
{
"name": "text",
"data": "58"
}
]
}
},
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"data": {
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"type": "bibr",
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"data": "59"
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]
}
}
],
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{
"name": "text",
"data": "。活性氧产生效率和双光子吸收截面是决定双光子光敏性能的两个主要因素。D-A策略虽然可以降低Δ"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "E"
}
]
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "S-T"
}
]
},
{
"name": "text",
"data": "，提高系间窜越速率，增强AIE光敏剂的光敏化效应，但这种策略会使得分子共轭受限，不利于提高分子的双光子吸收能力。2019年，Liu等通过聚合策略实现了AIE光敏剂双光子吸收能力和活性氧产生效率的同时增强"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "60",
"type": "bibr",
"rid": "R60",
"data": [
{
"name": "text",
"data": "60"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。如"
},
{
"name": "xref",
"data": {
"text": "图3(d)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(d)"
}
]
}
},
{
"name": "text",
"data": "所示，在小分子AIE光敏剂TPEDC的基础上，通过聚合得到具有AIE性质的聚合物光敏剂PTPEDC1和PTPEDC2。它们的吸收和发射行为如"
},
{
"name": "xref",
"data": {
"text": "图3(e)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(e)"
}
]
}
},
{
"name": "text",
"data": "所示。随后，利用两亲性基质DSPE-PEG将它们分别包覆成为具有良好生物相容性的纳米颗粒AIE dots。与小分子TPEDC相比，PTPEDC1和PTPEDC2 dots在双光子激发下都表现出更高的活性氧产生能力。其中，PTPEDC2 dots的活性氧产率提高了5.48倍，是光敏剂Ce6的6.37倍("
},
{
"name": "xref",
"data": {
"text": "图3(f)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(f)"
}
]
}
},
{
"name": "text",
"data": ")。同时，PTPEDC2 dots的双光子吸收截面(7.36×10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "5"
}
]
},
{
"name": "text",
"data": " GM)是TPEDC dots(1.13×10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "5"
}
]
},
{
"name": "text",
"data": " GM)的6.51倍("
},
{
"name": "xref",
"data": {
"text": "图3(g)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(g)"
}
]
}
},
{
"name": "text",
"data": ")。以上结果表明，聚合策略除了可以增加系间窜越速率、提高活性氧产生效率，还能进一步改善分子共轭，提高双光子吸收截面。得益于其较大的双光子吸收截面和活性氧产生效率，PTPEDC2 dots在癌细胞的双光子光动力杀伤方面表现优异，同时在斑马鱼肿瘤模型中能够通过血液循环在肝脏肿瘤中富集，对肿瘤表现出明显的双光子光动力治疗效果("
},
{
"name": "xref",
"data": {
"text": "图3(h)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(h)"
}
]
}
},
{
"name": "text",
"data": ")。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.3 纳米策略"
}
],
"level": "2",
"id": "s2c"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "激发态光敏剂分子的能量可以通过多通道发生耗散，通过纳米策略实现空间限域，抑制热耗散的非辐射跃迁，促使激发态能量通过辐射跃迁和系间窜越途径耗散，从而成为提高AIE光敏剂荧光量子产率和活性氧产生效率的重要途径"
},
{
"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": "。目前，两亲性聚合物、硅基体、介孔材料、二维材料、蛋白质和多糖等已作为载体被广泛应用于AIE分子的负载"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "61",
"type": "bibr",
"rid": "R61",
"data": [
{
"name": "text",
"data": "61"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "67",
"type": "bibr",
"rid": "R67",
"data": [
{
"name": "text",
"data": "67"
}
]
}
}
],
"rid": [
"R61",
"R62",
"R63",
"R64",
"R65",
"R66",
"R67"
],
"text": "61-67",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。载体材料包裹或与基体材料的复合不仅实现了AIE分子性能的提升，同时赋予了诊疗体系优异的生物相容性和水溶液中的分散性，是推动AIE光敏剂更广泛地应用于生物医学领域的有效方法"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "68",
"type": "bibr",
"rid": "R68",
"data": [
{
"name": "text",
"data": "68"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。基体材料的种类及其与AIE分子间的相互作用是影响限域作用发挥的重要因素。例如，硅氧网状结构包裹的BTPEAQ分子表现出12.1%的量子产率，而被DSPE-PEG两亲性聚合物包裹的纳米粒子量子产率只有3.9%。但同时，致密的硅氧网状结构也近乎完全抑制了其活性氧的释放"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "69",
"type": "bibr",
"rid": "R69",
"data": [
{
"name": "text",
"data": "69"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。2018年，Tang课题组通过优化荧光纳米粒子中的限域微环境开发出了同时具有高效荧光量子产率和活性氧产生效率的AIE dots"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "70",
"type": "bibr",
"rid": "R70",
"data": [
{
"name": "text",
"data": "70"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。他们利用碗烯的特殊骨架以及与AIE分子间的相互作用，强烈限制分子内旋转，抑制激发态能量的非辐射衰减，实现荧光量子产率和活性氧产生效率的同步增强。如"
},
{
"name": "xref",
"data": {
"text": "图4(a)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(a)"
}
]
}
},
{
"name": "text",
"data": "所示，分别用碗烯和线性脂肪族聚合物DSPE-PEG封装TPP-TPA分子形成纳米粒子Cor-AIE dots 和DSPE-AIE dots。得益于碗烯更加封闭和更加刚性的分子结构，以及与TPP-TPA间强烈的偶极-偶极相互作用，TPP-TPA结构中苯环的自由转动被极大限制，非辐射跃迁因此受限，Cor-AIE纳米点的荧光发射和活性氧产生能力均得到增强("
},
{
"name": "xref",
"data": {
"text": "图4(b)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(b)"
}
]
}
},
{
"name": "text",
"data": ")。具有刚性限域微环境的Cor-AIE dots的荧光量子产率高达26.8%，而具有柔性限域微环境的DSPE-AIE dots的量子产率仅有6.7%，并且Cor-AIE dots活性氧的产生能力是DSPE-AIE dots的5.4倍("
},
{
"name": "xref",
"data": {
"text": "图4(c)、(d)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(c)、(d)"
}
]
}
},
{
"name": "text",
"data": ")。在腹膜转移瘤模型中，Cor-AIE dots表现出更加优异的近红外荧光成像指导的肿瘤切除效果，小于1 mm的微小肿瘤能够被有效切除("
},
{
"name": "xref",
"data": {
"text": "图4(e)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(e)"
}
]
}
},
{
"name": "text",
"data": ")。同时，发挥其高效的活性氧产生能力，Cor-AIE dots能够更加有效地抑制腹膜转移瘤的生长，大大提高小鼠的生存率和中位生存时间("
},
{
"name": "xref",
"data": {
"text": "图4(f)",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4(f)"
}
]
}
},
{
"name": "text",
"data": ")。因此，通过空间限域策略构筑AIE纳米颗粒对提升荧光量子产率和活性氧产生效率具有重要意义。"
}
]
},
{
"name": "fig",
"data": {
"id": "F4",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图4"
}
],
"title": [
{
"name": "text",
"data": "(a)纳米沉淀法制备Cor-AIE dots和 DSPE-AIE dots示意图；(b)具有柔性限域微环境的DSPE-AIE dots和刚性限域微环境的Cor-AIE dots的光物理过程示意图；(c)Cor-AIE dots和 DSPE-AIE dots的荧光发射光谱；(d)Cor-AIE dots和 DSPE-AIE dots活性氧产生情况；(e)荧光成像指导下的肿瘤切除和非荧光成像指导的直接切除所得到的肿瘤的荧光图(左)、生物发光图(中)及直径统计柱状图(右)；(f)小鼠活体肿瘤时间依赖的生物发光成像"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "70",
"type": "bibr",
"rid": "R70",
"data": [
{
"name": "text",
"data": "70"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.4"
}
],
"title": [
{
"name": "text",
"data": "(a)Scheme for the preparation of Cor-AIE dots and DSPE-AIE dots using nanoprecipitation method. (b)Jablonski diagram showing the nonradiative, radiative and intersystem crossing(ISC) processes for AIEgens in flexible(DSPE-AIE dots) and rigid(Cor-AIE dots) matrixes. (c)PL spectra of Cor-AIE dots and DSPE-AIE dots. (d)ROS generation measurement of Cor-AIE dots and DSPE-AIE dots in aqueous media. (e)Fluorescence image(left), bioluminescence(middle) and histogram of nodule diameters(right) extracted from unguided and Cor-AIE dots fluorescence guided groups. (f)Time-dependent bioluminescence imaging of the peritoneal carcinomatosis-bearing mice in “Saline，” “DSPE-AIE dots＋L，” and “Cor-AIE dots＋L ” groups"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "70",
"type": "bibr",
"rid": "R70",
"data": [
{
"name": "text",
"data": "70"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "．"
}
]
}
],
"subcaption": [],
"note": [],
"graphics": [
{
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"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3 光声成像指导的光热治疗"
}
],
"level": "1",
"id": "s3"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "光热治疗是指通过外部光源照射具有光热转换效应的材料、将光能转化为热能来治疗包括癌症在内的各种疾病的一种新型疗法"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "71",
"type": "bibr",
"rid": "R71",
"data": [
{
"name": "text",
"data": "71"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "72",
"type": "bibr",
"rid": "R72",
"data": [
{
"name": "text",
"data": "72"
}
]
}
}
],
"rid": [
"R71",
"R72"
],
"text": "71-72",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。此外，高效的光热转换材料本身就具有优良的光声成像性能，便于实现光声成像指导的光热治疗。相比于荧光成像手段，光声成像技术结合了超声检查的优势，能够提供超越光学扩散距离限制的深层组织穿透能力，成像深度可达毫米甚至厘米级，并且具有较高的空间分辨率和对比度，在肿瘤诊断、脑血流动力学研究和血管结构可视化等生物医学领域已被成功应用"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "73",
"type": "bibr",
"rid": "R73",
"data": [
{
"name": "text",
"data": "73"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "74",
"type": "bibr",
"rid": "R74",
"data": [
{
"name": "text",
"data": "74"
}
]
}
}
],
"rid": [
"R73",
"R74"
],
"text": "73-74",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。目前，AIE分子在光声成像指导的光热治疗领域刚刚起步，所报道的例子为数不多。从设计策略上，这些分子可以分为两类。一、通过侧链工程延长侧链长度，使得分子在聚集态的排列更为疏松，有利于基团在聚集态的转动，从而有利于激发态能量更多地以热的形式释放出来。"
},
{
"name": "xref",
"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5"
}
]
}
},
{
"name": "text",
"data": "中NDTA分子体系(包括NDTA、2TPE-NDTA和2TPE-2NDTA)和"
},
{
"name": "xref",
"data": {
"text": "图6",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6"
}
]
}
},
{
"name": "text",
"data": "中NIR分子体系(包括NIRb14、NIRb10、NIRb6和NIR6)属于这一类设计策略。二、通过利用分子内化学键伸缩振动的自发、剧烈、不受外界因素限制等优势诱导光热转化。"
},
{
"name": "xref",
"data": {
"text": "图7",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7"
}
]
}
},
{
"name": "text",
"data": "中分子DCP-TPA和DCP-PTPA属于这一类设计策略。"
}
]
},
{
"name": "fig",
"data": {
"id": "F5",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图5"
}
],
"title": [
{
"name": "text",
"data": "(a)NDTA系列分子结构和聚集态下分子内运动诱导光热转化示意图；不同纳米粒子在808 nm激光照射下的红外热图片(b)和时间-温度变化曲线(c)；(d)2TPE-2NDTA纳米粒子在荷瘤小鼠体内的光声成像效果"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "76",
"type": "bibr",
"rid": "R76",
"data": [
{
"name": "text",
"data": "76"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.5"
}
],
"title": [
{
"name": "text",
"data": "(a)Molecular structures and schematic illustration showing active excited-state intramolecular motion in aggregation state. (b)IR thermal images of various NPs in aqueous solution(100 μmol/L) upon exposure to 808 nm(0.8 W/cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": ") laser irradiation for different times. (c)Corresponding temperature changes as a function of time. (d)Representative PA images of tumors from 2TPE-2NDTA-doped NP-administrated mice"
},
{
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"data": [
{
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"data": "["
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"data": {
"text": "76",
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"rid": "R76",
"data": [
{
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"data": "76"
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]
}
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]
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"title": [
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"name": "text",
"data": "(a)通过侧链工程策略调控分子结构增强聚集态下分子运动增强光热性能示意图；(b)NIR系列分子的纳米粒子在808 nm激光照射下的光热转化行为；(c)NIRb14纳米粒子在荷瘤小鼠体内的光声成像效果；(d)NIRb14纳米粒子在荷瘤小鼠体内的光热效果"
},
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"data": [
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"data": {
"text": "77",
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"data": "77"
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"data": "。"
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]
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"label": [
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"data": "Fig.6"
}
],
"title": [
{
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"data": "(a)Molecular design "
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"data": [
{
"name": "text",
"data": "via"
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]
},
{
"name": "text",
"data": " side-chain engineering strategy for enhanced molecular motion and photothermal conversion performance in aggregation state. (b)Comparison of the photothermal conversion behavior of the NIR molecules-loaded NPs(100 μmol/L) in PBS solution under 808 nm(0.8 W/cm"
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{
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"data": [
{
"name": "text",
"data": "2"
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},
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"name": "text",
"data": ") laser irradiation. (c)Representative PA images at tumor sites from mice intravenously injected with NIRb14-PAE/PEG(660 μmol/L) for different time. (d)IR thermal images of 4T1 tumor-bearing mice under 808 nm laser irradiation(0.8 W/cm"
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"data": [
{
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{
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"data": ") for various time"
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"data": [
{
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"data": "["
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"data": {
"text": "77",
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"rid": "R77",
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"data": "77"
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"data": "．"
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"label": [
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"data": "图7"
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"title": [
{
"name": "text",
"data": "(a)DCP-TPA和DCP-PTPA的分子结构及其激发态运动模型示意图；(b)DCP-TPA和DCP-PTPA分子在不同波数下的重组能，及其键长、键角、二面角对总重组能的贡献；(c)DCP-TPA和DCP-PTPA纳米粒子在660 nm激光照射下的红外热图片和光热稳定性；(d)两种纳米粒子在不同浓度下的光声图像及光声信号强度-分子浓度之间的线性关系"
},
{
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"data": [
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"data": "["
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"name": "xref",
"data": {
"text": "79",
"type": "bibr",
"rid": "R79",
"data": [
{
"name": "text",
"data": "79"
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"data": "]"
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]
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{
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"data": "。"
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"label": [
{
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"data": "Fig.7"
}
],
"title": [
{
"name": "text",
"data": "(a)Molecular structures of DCP-TPA and DCP-PTPA and schematic illustration of their motion models in the excited state. (b)Calculated reorganization energy of DCP-TPA and DCP-PTPA at different wavenumbers and the contribution to the total reorganization energy from the bond length, bond angle and dihedral angle. (c)IR thermal images of DCP-TPA and DCP-PTPA NPs(100 μmol/L) upon 660 nm laser irradiation(0.45 W/cm"
},
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"data": [
{
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"data": "2"
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]
},
{
"name": "text",
"data": ") and the cycles of heating-cooling process indicating the photothermal conversion stability of the two NPs. (d)PA images of the two NPs at various molecular concentrations and plot of PA intensity against molecular concentration of two NPs"
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"data": [
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"data": "["
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"data": {
"text": "79",
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"rid": "R79",
"data": [
{
"name": "text",
"data": "79"
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]
}
},
{
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"data": "]"
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"data": "．"
}
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"title": [
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"data": "3.1 侧链工程策略"
}
],
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"id": "s3a"
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{
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"data": [
{
"name": "text",
"data": "AIE分子通常具有强的疏水性，通过生物相容性两亲性基质将其包裹成纳米颗粒是增加其水溶性、满足其在机体水环境中应用的最常用策略"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "73",
"type": "bibr",
"rid": "R73",
"data": [
{
"name": "text",
"data": "73"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。此外，纳米制剂还拥有长的血液循环能力以及肿瘤靶向富集等优势，增强AIE分子在生物体内的诊疗效果"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "75",
"type": "bibr",
"rid": "R75",
"data": [
{
"name": "text",
"data": "75"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。根据Jablonski能级图，荧光发射和光热效应的光物理过程是彼此竞争的，当AIE分子在纳米聚集态下的堆集过于紧密时，其分子内运动由于缺乏运动空间在很大程度上受到抑制，虽然荧光亮度会得到显著提升，但其产热能力大大降低。基于此，Tang等提出了一种新的分子设计理念，利用固态下分子运动促进非辐射跃迁产热来构建高效光热材料"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "76",
"type": "bibr",
"rid": "R76",
"data": [
{
"name": "text",
"data": "76"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。该分子设计理念是对AIE概念的一次逆向思维，与力图抑制AIE分子运动来打开辐射跃迁途径而发出荧光不同，该研究则致力于最大程度地实现固态或纳米聚集态下的分子运动来增强非辐射跃迁，从而将光能转化为热能。如"
},
{
"name": "xref",
"data": {
"text": "图5(a)",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5(a)"
}
]
}
},
{
"name": "text",
"data": "所示，该工作以四苯乙烯(TPE)作为转子单元，以带长烷基链的萘二酰亚胺作为电子受体，构建了NDTA、2TPE-NDTA和2TPE-2NDTA 3个分子。具有大π-共轭结构的强吸电子能力的受体与TPE相连时，能使分子具有长波长的吸收、高的摩尔吸光系数和强的分子内扭曲电荷转移效应(TICT)。长烷基分叉型侧链的引入可以使处于聚集态下的分子彼此之间产生疏松的空间，以促进TPE基团的自由转动。转子和长烷基链同时引入的2TPE-NDTA和2TPE-2NDTA分子被证实可以在聚集体以及固体状态下实现活跃的分子运动以及高效的非辐射跃迁。如"
},
{
"name": "xref",
"data": {
"text": "图5(b)、(c)",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5(b)、(c)"
}
]
}
},
{
"name": "text",
"data": "所示，在808 nm激光照射5 min后，2TPE-NDTA和2TPE-2NDTA纳米粒子的温度分别升高到69.6 ℃和81.4 ℃。光热转化效率测试表明，与文献所报道的明星半导体分子SPNs相比，2TPE-NDTA纳米粒子(43.0%)和2TPE-2NDTA纳米粒子(54.9%)都表现出比SPNs(27.5%)更高的光热转换效率。进一步的光声信号测试结果表明，与商业化的亚甲基蓝和已知的明星半导体高分子SPNs对比，2TPE-NDTA和2TPE-2NDTA纳米粒子均表现出更强的光声信号，并且展现出优异的光学稳定性。最后，将2TPE-2NDTA纳米粒子用于小鼠活体近红外光声成像，得到了良好的成像效果(5(d))。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "同年，Tang课题组进一步利用侧链工程策略调控有机分子在聚集时的分子运动，提高聚集态下分子激发态TICT性质增强非辐射跃迁，进而提高光热转化效率"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "77",
"type": "bibr",
"rid": "R77",
"data": [
{
"name": "text",
"data": "77"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。在该工作中，研究者选用苯并双噻二唑为强电子受体，噻吩为电子给体，三苯胺既作为电子给体又作为分子转子，支化长烷基链位于噻吩单元上，设计并合成了一系列窄带隙的D-A型共轭小分子NIR6、NIRb6、NIRb10和NIRb14("
},
{
"name": "xref",
"data": {
"text": "图6(a)",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6(a)"
}
]
}
},
{
"name": "text",
"data": ")。支化长烷基链的存在对聚集态分子运动和TICT性质的调节起到了至关重要的作用。在溶液态下，长烷基链有助于分子扭曲，更有利于TICT态的形成。在聚集态下，烷基链的支化作用可以有效减弱分子间强相互作用，给分子内旋转提供空间，有利于TICT态的形成，从而增强了非辐射跃迁和光热转化效率。值得注意的是，支化烷基链的支化点最好位于第二个碳。如果位于第一个碳，位阻过大，则容易发射荧光；如果没有支化，则不能有效阻止分子间相互作用，达不到光热效率增强的目的。从光热性能测试结果("
},
{
"name": "xref",
"data": {
"text": "图6(b)",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6(b)"
}
]
}
},
{
"name": "text",
"data": ")可以看出，相对于直型烷基链分子NIR6，分叉型烷基链分子NIRb6、NIRb10和NIRb14具有更好的光热转化性能，而具有最长烷基链的NIRb14(含2-癸基十四烷基团)具有最好的光热效果，其光热转化效率(31.2%)显著高于GNR(20.7%)，且具有良好的热稳定性。在得到性质优良的光热转化剂NIRb14后，通过pH响应两亲性聚合物(PAE-"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "b"
}
]
},
{
"name": "text",
"data": "-PCL)将其包裹成纳米颗粒(NIRb14-PAE/PEG NPs)。该纳米粒子在血液环境中(pH＝7.4)带负电荷，可以增强血液循环时间；当通过被动靶向运输到肿瘤部位时(pH＝6.5)，外层PAE被质子化而带正电荷，从而增强了纳米粒子在肿瘤部位的富集，达到提高治疗效果的目的。随后，作者将NIRb14-PAE/PEG纳米粒子用于小鼠肿瘤的光声成像指导的光热治疗("
},
{
"name": "xref",
"data": {
"text": "图6(c)、(d)",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6(c)、(d)"
}
]
}
},
{
"name": "text",
"data": ")。结果表明，与对照组(PEG-"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "b"
}
]
},
{
"name": "text",
"data": "-PCL包裹纳米粒子)相比，NIRb14-PAE/PEG纳米粒子在小鼠肿瘤部位富集明显增强，产生了更强的光声信号并诱导肿瘤产生更高的温度，且对肿瘤生长有明显的抑制作用。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3.2 化学键伸缩振动策略"
}
],
"level": "2",
"id": "s3b"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "虽然通过增强转子在聚集态下的转动能力能够获得有效的光热响应，但这种方法受到分子间堆积及分子间空腔等控制因子的影响，材料设计和合成过程比较繁琐。分子内键的伸缩振动是一种高频的分子运动，通常在沿着键轴很短的距离(0.01 nm)进行"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "78",
"type": "bibr",
"rid": "R78",
"data": [
{
"name": "text",
"data": "78"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。这种分子运动是自发的、有力的，非常有利于光热转化。基于此，Tang等利用化学键伸缩振动自发、剧烈、不受外界因素限制等优势，进一步提出了分子内键伸缩振动诱导光热转化的新概念"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "79",
"type": "bibr",
"rid": "R79",
"data": [
{
"name": "text",
"data": "79"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。如"
},
{
"name": "xref",
"data": {
"text": "图7(a)",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7(a)"
}
]
}
},
{
"name": "text",
"data": "所示，研究者设计合成了两个D-A型共轭小分子DCP-TPA和DCP-PTPA，其中芳香胺作为电子给体单元，吡嗪作子受体单元。另外，吡嗪还作为键伸缩振动器，促进激发态下的分子内运动。理论研究表明("
},
{
"name": "xref",
"data": {
"text": "图7(b)",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7(b)"
}
]
}
},
{
"name": "text",
"data": ")，DCP-TPA中吡嗪单元内C—N键的伸缩振动对分子激发态能量的耗散起绝对作用。相比而言，DCP-PTPA中由于更多苯环的引入，分子运动能力增强，但分子内键伸缩振动依然主导分子激发态行为。由于键的伸缩振动发生剧烈且距离小，利用分子内键伸缩振动能够在不受外界因素限制下以最简便和有效的方式获得光热转化。随后，作者将DCP-TPA和DCP-PTPA分子制备成具有良好水溶性的纳米颗粒。在660 nm激光的连续照射下，两种纳米粒子溶液的温度都迅速升高("
},
{
"name": "xref",
"data": {
"text": "图7(c)",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7(c)"
}
]
}
},
{
"name": "text",
"data": ")，光热转化效率高达52%和59%。此外，两种纳米粒子的光热稳定性实验结果表明，两种纳米粒子的温度在加热-冷却五次循环后没有明显变化，显示出了优异的稳定性。同时，得益于高的光热转化效率，这两种材料能够将产生的热转化为比先前报道的高性能半导体聚合物和商业化材料亚甲基蓝更强的光声信号("
},
{
"name": "xref",
"data": {
"text": "图7(d)",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7(d)"
}
]
}
},
{
"name": "text",
"data": ")。鉴于光声成像深度深且空间分辨率高等优势，这两种材料能够实现对活体小鼠肿瘤快速和高信噪比(信噪比高达6.9倍)的光声成像。此外，这类材料还表现出体内生物毒性小以及代谢快等优势，为后期的进一步应用研究打下了良好的基础。该研究为利用分子内化学键的运动来捕获光热和设计光声造影剂提供了一种全新的策略。"
}
]
}
]
}
]
},
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"data": [
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"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "4 多模态成像指导的协同治疗"
}
],
"level": "1",
"id": "s4"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "虽然AIE材料在荧光成像指导的光动力治疗和光声成像指导的光热治疗中展现出巨大潜力，然而在实际临床应用中，仅通过单一模态的光学成像或单一模态的光学治疗仍然很难达到最佳的疾病诊疗效果"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "80",
"type": "bibr",
"rid": "R80",
"data": [
{
"name": "text",
"data": "80"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "81",
"type": "bibr",
"rid": "R81",
"data": [
{
"name": "text",
"data": "81"
}
]
}
}
],
"rid": [
"R80",
"R81"
],
"text": "80-81",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。例如，荧光成像技术虽然具有高的灵敏度，但其穿透深度和空间分辨力却欠佳；光声成像技术虽能够提供足够的穿透深度和高空间分辨能力，但其灵敏度却不高；而单独的光动力治疗或光热治疗其效率往往受制于疾病组织的氧气浓度和热休克效应。基于此，开发多功能光学诊疗体系，同时进行多模态成像和协同治疗是至关重要的。目前构建多模态光学诊疗系统最常用的策略是将具有单个功能的多种成分组合到一个纳米平台，然而这种多合一(All-in-one)的方法不可避免地会受到成分复杂、重复性低和药代动力学不明确的限制，难以进行临床转化"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "82",
"type": "bibr",
"rid": "R82",
"data": [
{
"name": "text",
"data": "82"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。因此，设计集多种功能于一体的智能分子用以构建可靠的光学诊疗系统用于临床疾病的诊疗意义重大"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "83",
"type": "bibr",
"rid": "R83",
"data": [
{
"name": "text",
"data": "83"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "87",
"type": "bibr",
"rid": "R87",
"data": [
{
"name": "text",
"data": "87"
}
]
}
}
],
"rid": [
"R83",
"R84",
"R85",
"R86",
"R87"
],
"text": "83-87",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。与传统的诊疗分子相比，AIE分子拥有独特的结构优势：其结构中具有大量自由运动的基团。活跃的分子运动能够使激发态能量通过非辐射衰变以热耗散的方式消散，而限制分子运动可以使吸收的能量流向伴随荧光发射的辐射能量耗散途径以及通过系间窜越到三线态最终以产生活性氧的形式散失。结构扭曲且在聚集态呈现非晶态的AIE分子在聚集态下将自然地呈现出杂乱无章的疏松排列方式，此时AIE分子的运动仅受部分限制，辐射和非辐射能量耗散得以平衡，激发态能量将得到最大化利用以充分实现其多功能性。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "基于此，Tang等开发了一系列具有多模态诊疗性能的全能型AIE分子"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "88",
"type": "bibr",
"rid": "R88",
"data": [
{
"name": "text",
"data": "88"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "91",
"type": "bibr",
"rid": "R91",
"data": [
{
"name": "text",
"data": "91"
}
]
}
}
],
"rid": [
"R88",
"R89",
"R90",
"R91"
],
"text": "88-91",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，并且通过不断调节分子的D-A强度，实现了荧光发射从近红外一区到二区(NIR-Ⅱ，1 000～1 700 nm)的移动"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "92",
"type": "bibr",
"rid": "R92",
"data": [
{
"name": "text",
"data": "92"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "，显著提高了体内诊疗效果。例如，他们以1，3-双(二氰基亚甲基)茚满作为电子受体、噻吩作为电子给体、三苯胺作为电子给体以及分子转子，设计合成了3个化合物(TI，TSI和TSSI)"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "89",
"type": "bibr",
"rid": "R89",
"data": [
{
"name": "text",
"data": "89"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。三苯胺基元高度扭曲的构象能够延长聚集态下分子间的距离，实现相对松散的分子间堆积，有助于保留部分分子内转动，从而有利于提高分子在纳米颗粒内聚集态下的产热能力。同时，三苯胺基元赋予这些化合物螺旋桨式的扭曲结构，有效阻止分子间π-π堆积进而抑制分子在纳米聚集体中的荧光猝灭，确保这些化合物具有AIE性质。另一方面，两个丙二腈修饰的茚满作为电子受体不仅具有强的吸电子能力，而且碳氮键伸缩振动能够保证这些AIE分子在纳米聚集态下的产热性能。噻吩的引入除了增强分子D-A强度、红移吸收和发射波长以及提高活性氧产生能力外，还扩大了三苯胺基元与受体之间的空间距离，增强转子在纳米颗粒内的转动能力。随后，他们将具有最强D-A效应和最强分子内运动能力的TSSI分子用DSPE-PEG载体包裹成纳米颗粒，实验结果表明该纳米颗粒具有明亮的近红外二区荧光发射、较高的活性氧产率以及优异的光热转换效率，实现了不同通道能量耗散之间的完美平衡。体内研究进一步证实了具有出色生物相容性和高通用性的全能型TSSI纳米粒子在小鼠肿瘤近红外二区荧光-光声-光热三模式成像引导的光动力-光热协同治疗中表现优异。值得一提的是，由于高效的光动力-光热协同治疗效应，在体内治疗过程中仅需一次注射和一次光照，就实现了对实体肿瘤的彻底消除。"
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"label": [
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"data": "图8"
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"title": [
{
"name": "text",
"data": "(a)全能型AIE分子结构、纳米制备和多模态光学诊疗应用示意图；(b)TSSI纳米粒子在荷瘤小鼠体内的近红外二区荧光成像和光声成像效果；(c)TSSI纳米粒子在荷瘤小鼠体内的光热效果；(d)TSSI纳米粒子的体外活性氧产生能力；(e)TSSI纳米粒子的体内光动力-光热协同治疗效果"
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"label": [
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],
"title": [
{
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"data": "(a)Schematic illustration of molecular structures, nanofabrication and versatile phototheranostic application. (b)NIR-Ⅱ FL images(upper row) and PA images of tumor tissues(lower row) at different monitoring times after administration of TSSI NPs. (c)IR thermal images of tumor-bearing mice during continuous 660 nm laser irradiation on tumor site at 12 h postinjection of TSSI NPs. (d)ROS generation of TSSI NPs(1 μmol/L) upon 660 nm laser irradiation. (e)Synergistic PDT-PTT tumoricidal effect of TSSI NPs on 4T1 tumor-bearing mice"
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"data": "5 结论与展望"
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{
"name": "p",
"data": [
{
"name": "text",
"data": "得益于高选择性、低毒副作用和优异的治疗效果，光学诊疗在生物医学和临床应用中展现了巨大潜力。有机小分子材料由于结构精确可控、生物相容性好以及易于功能化修饰等优点有望成为推动光学诊疗试剂向临床转化的最佳选择。传统的结构平面化的ACQ类有机小分子，由于存在高浓度或聚集态下荧光效率和活性氧产率降低的问题，无法满足在生物体水环境中的应用。相反地，AIE分子结构中含有大量能够运动的基团，并呈现螺旋桨式的分子构象，其荧光和活性氧产生效率呈现聚集增强的现象，极大地拓宽了有机小分子在光学诊疗领域的应用范围。同时，依据Jablonski能级图，通过精准分子设计以及调控分子在聚集态下的运动还可以实现热耗散、辐射衰变和系间窜越3个能量耗散通道间的调节与平衡，以实现光诊疗效果的最佳化。基于此，本文系统总结了通过分子结构设计以及聚集行为调控增强AIE材料的光学诊疗效果的策略，并从荧光成像指导的光动力治疗、光声成像指导的光热治疗和荧光-光声-光热成像指导的光动力-光热协同治疗三个方面综述了AIE材料在光学诊疗中的最新研究进展。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "尽管AIE材料在光学诊疗领域已取得了突破性进展，然而面向临床应用，目前仍存在一些亟待解决的问题与挑战。一方面，目前开发的AIE光诊疗剂的激发波长大多处在可见光区域，考虑到生物体内的应用，迫切需要开发具有近红外吸收或多光子吸收特性的AIE分子，以增大激发光的组织穿透深度，实现深层组织疾病的诊疗。另一方面，基于单个AIE分子的多模态诊疗目前尚处于起步阶段，需要开发更多的体系来探究这类材料的构-效关系，建立一套行之有效的理论来指导材料的设计、合成。此外，由于光学治疗能够有效地刺激机体产生大量的免疫原性抗原，将光学治疗与免疫治疗联用有望进一步提高疾病治疗效果。另外，作为一类新型材料，AIE 材料的生物安全性和体内清除问题尚缺乏系统的研究，相关工作需要进一步深入。综上所述，我们坚信，在多学科多领域科学家的不懈坚持和努力下，AIE材料在光学诊疗乃至整个生物医学领域必将得到快速发展与优化升级，具有光学诊疗特性的AIE材料也必将在临床实践中得以推广应用。"
}
]
}
]
}
],
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"text": [
{
"name": "text",
"data": "Supported by National Natural Science Foundation of China (51903163, 21801169); China Postdoctoral Science Foundation (2015054); Natural Science Foundation for Distinguished Young Scholars of Guangdong Province (2020B1515020011); Science and Technology Foundation of Shenzhen City (JCYJ20190808153415062)"
}
]
}
],
"history": {
"received": "2021-01-16",
"revised": "2021-02-02",
"ppub": "2021-03-01",
"opub": "2021-10-22"
},
"copyright": {
"data": [],
"year": "2021"
}
},
"appendix": [],
"type": "research-article",
"ethics": [],
"supplementary": [],
"journalTitle": "发光学报",
"issue": "03",
"volume": "42",
"originalSource": []
}
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