From Carbon Dots to Carbonized Polymer Dots: Development and Challenges Enhanced Publication

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "从碳点到碳化聚合物点：发展和挑战" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "From Carbon Dots to Carbonized Polymer Dots: Development and Challenges" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "孟", "givenname": "维雪", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "MENG", "givenname": "Wei-xue", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "first-author" ], "bio": [ { "lang": "zh", "text": [ "孟维雪(1995-)，女，河南周口人，硕士研究生，2018年于河南农业大学获得学士学位，主要从事碳基材料的合成及其电催化应用的研究。E-mail: 18738153540@163.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207656&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207663&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207670&type=" } ], "data": [ [ { "name": "text", "data": "孟维雪" }, { "name": "text", "data": "(1995-)，女，河南周口人，硕士研究生，2018年于河南农业大学获得学士学位，主要从事碳基材料的合成及其电催化应用的研究。E-mail: " }, { "name": "text", "data": "18738153540@163.com" } ] ] } ], "email": "18738153540@163.com", "deceased": false }, { "name": [ { "lang": "zh", "surname": "杨", "givenname": "柏", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "YANG", "givenname": "Bai", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff2", "text": "2" } ], "role": [], "deceased": false }, { "name": [ { "lang": "zh", "surname": "卢", "givenname": "思宇", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "LU", "givenname": "Si-yu", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor1", "lang": "en", "text": "E-mail: sylu2013@zzu.edu.cn", "data": [ { "name": "text", "data": "E-mail: sylu2013@zzu.edu.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "卢思宇(1986-)，男，河南开封人，博士，教授，博士研究生导师，2016年于吉林大学获得博士学位，主要从事碳点的设计制备及其杂化体系在发光和能源领域的机理与应用的研究。E-mail: sylu2013@zzu.edu.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207680&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207687&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207694&type=" } ], "data": [ [ { "name": "text", "data": "卢思宇" }, { "name": "text", "data": "(1986-)，男，河南开封人，博士，教授，博士研究生导师，2016年于吉林大学获得博士学位，主要从事碳点的设计制备及其杂化体系在发光和能源领域的机理与应用的研究。E-mail: " }, { "name": "text", "data": "sylu2013@zzu.edu.cn" } ] ] } ], "email": "sylu2013@zzu.edu.cn", "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "label": "1", "text": "郑州大学　化学学院(绿色催化中心)，河南 　 郑州 　 450001", "data": [ { "name": "text", "data": "郑州大学　化学学院(绿色催化中心)，河南 　 郑州 　 450001" } ] }, { "lang": "en", "label": "1", "text": "College of Chemistry(Green Catalysis Center), Zhengzhou University, Zhengzhou 450001, China", "data": [ { "name": "text", "data": "College of Chemistry(Green Catalysis Center), Zhengzhou University, Zhengzhou 450001, China" } ] } ] }, { "id": "aff2", "intro": [ { "lang": "zh", "label": "2", "text": "吉林大学化学学院　超分子结构与材料国家重点实验室，吉林 　 长春 　 130012", "data": [ { "name": "text", "data": "吉林大学化学学院　超分子结构与材料国家重点实验室，吉林 　 长春 　 130012" } ] }, { "lang": "en", "label": "2", "text": "State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, China", "data": [ { "name": "text", "data": "State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, China" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "碳点(CDs)由于其出色的光学性能、高生物相容性和低毒性，因此在许多领域都具有潜在应用。对其光致发光(PL)机制的认识已得到广泛研究，对于指导可调节PL发射的CDs的合成和推广应用具有重要意义。但是，PL发射的内在机理尚不清楚，并且由于颗粒结构的差异，尚未找到统一的机理。本综述根据对结构和性能特征的分析，总结了一种新的CDs分类，称为碳化聚合物点(CPDs)。概述了与结构差异有关的三种PL机制:内部因素主导发射(包括共轭效应、表面状态和协同效应)、外部因素主导发射(包括分子态和环境效应)以及交联-发射增强。除此之外，还简要介绍了CDs的光学应用。最后，讨论了PL机制的研究前景，并指出了未来工作中存在的挑战和方向。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Carbon dots(CDs) may be useful in many fields due to its excellent optical properties, high biocompatibility and low toxicity. The knowledge of its photoluminescence(PL) mechanism has been extensively studied, which is of great significance for guiding the synthesis and popularization of CDs with adjustable PL emission. However, the internal mechanism of PL emission is still unclear, and due to the difference in particle structure, a unified mechanism has not yet been found. This review summarizes a new CDs classification based on the analysis of structural and performance characteristics, called carbonized polymer dots(CPDs). Three PL mechanisms related to structural differences are summarized: internal factors dominate emission(including conjugation effects, surface state and synergistic effects), external factors dominate emission(including molecular state and environmental effects), and cross-linking-emissions. The optical application of CDs is also briefly introduced. Finally, the prospects for research into PL mechanisms are discussed, noting the remaining challenges and directions for future work." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "碳点" } ], [ { "name": "text", "data": "光致发光机制" } ], [ { "name": "text", "data": "表面态" } ], [ { "name": "text", "data": "分子态" } ], [ { "name": "text", "data": "交联增强发射" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "carbon dots" } ], [ { "name": "text", "data": "photoluminescence mechanisms" } ], [ { "name": "text", "data": "surface state" } ], [ { "name": "text", "data": "molecular state" } ], [ { "name": "text", "data": "crosslink-enhanced emission" } ] ] } ], "highlights": [], "body": [ { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "1　引言" } ], "level": "1", "id": "s1" } }, { "name": "p", "data": [ { "name": "text", "data": "2004年，科学家在碳纳米管制备中偶然发现了荧光碳点(CDs)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。作为新型的零维碳纳米材料，CDs不仅具有类似于传统量子点的发光性能与小尺寸特性，而且还具有水溶性好、生物毒性低和导电性好的优势" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "2", "type": "bibr", "rid": "R2", "data": [ { "name": "text", "data": "2" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "4", "type": "bibr", "rid": "R4", "data": [ { "name": "text", "data": "4" } ] } } ], "rid": [ "R2", "R3", "R4" ], "text": "2-4", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，CDs在生命科学、环境分析及能源催化等领域受到极大关注。之前科学家一直认为CDs是无机材料，并称之为碳量子点(CQDs)。但是，对于利用多官能团小分子和聚合物为前驱体、通过自下而上方法(水热、溶剂热或微波等)制备的CDs，并不仅仅是无机材料，其兼具聚合物和量子点的优势。我们将这种经缩聚、消去和芳构化形成的CDs命名为碳化聚合物点(CPDs)。CPDs的性质更加丰富，尤其是它的荧光与光电化学性质等已成为研究热点。然而结构也更为复杂，人们对其结构、性质的理解和研究仍然处于萌芽阶段，还存在许多争议。目前，CPDs领域人们亟待解决的科学问题主要包括:(1)发光中心及多色CPDs的可控制备；(2)发光峰宽度的调控及CPDs的纯化；(3)CPDs的稳定性；(4)CPDs具体结构等。针对上述科学问题开展深入系列研究，无论是对深入理解碳纳米结构的基础科学问题，还是对推进它们在生物医学、光电及催化能源等领域的广泛应用都至关重要。本综述主要阐述CDs的制备、分类、发光机理、应用以及未来的发展和挑战。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　碳点的合成方法、分类与表征" } ], "level": "1", "id": "s2" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1　合成方法" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "随着CDs领域的发展，过去数年中出现了多种制备方法。但是总的来说，CDs的合成方法主要包括两类" }, { "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": "。一是自上而下的碳源裂解法，如吉林大学杨柏教授课题组、上海大学吴明红教授课题组、北京理工大学曲良体教授课题组、苏州大学康振辉课题组和南京大学朱俊杰课题组等分别采用的水热法/溶剂热裂解还原型氧化石墨烯、电化学裂解石墨烯和浓硫酸/浓硝酸裂解碳纤维等制备性能优异的石墨烯量子点；二是自下而上的小分子/聚合物碳化法，该类方法选用糖类、柠檬酸和胺类小分子作为起始碳源，通过煅烧、水热、微波、超声、等离子体等途径进行处理，同时利用反应温度或时间来控制小分子的碳化程度，从而制备系列的CDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "7", "type": "bibr", "rid": "R7", "data": [ { "name": "text", "data": "7" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "8", "type": "bibr", "rid": "R8", "data": [ { "name": "text", "data": "8" } ] } } ], "rid": [ "R7", "R8" ], "text": "7-8", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。其中自下而上合成方法由于简单易操作、产率高，在目前CDs制备领域中占据主导地位。如吉林大学杨柏教授课题组采用柠檬酸、乙二胺一步水热法制备CDs，荧光量子产率可高达80%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。为了阐明CPDs荧光的真正来源，必须使用有效的分离程序来消除杂质并降低样品本身的复杂性，这些杂质本身可以作为荧光源或引起CPDs的荧光猝灭。纯化方法包括凝胶电泳、透析、柱色谱法和尺寸排阻色谱法(" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": ")。在柱色谱法中，CPDs根据极性分离；而在尺寸排阻色谱法中，分离是基于分子量的。硅胶柱色谱法因其成本低廉而被广泛使用。对于不同类型的CPDs，分离和纯化的方法也不同。碳化程度低的聚合物点(PDs)具有许多聚合物结构，可以通过常用的聚合物分离方法(例如尺寸排阻色谱法)进行纯化，而CQDs的碳化程度高且聚合物链很少。CQDs之间的差异主要体现在大小上，它更适合于通过离心进行区分。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "CDs的提纯。(a)通过超速离心获得的不同极性的CDs及其发射曲线" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)CPDs合成和纯化步骤示意图" }, { "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": ";(c)使用SEC获得大小不同的CPDs" }, { "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": ";(d)使用色谱柱色谱分离具有不同发射波长的CPDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "Purification of CDs. (a)CDs of different polarities obtained by ultracentrifugation and their emission curves" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Schematic diagram of the synthesis and purification steps of CPDs" }, { "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": ". (c)Use SEC to obtain CPDs of different sizes" }, { "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": ". (d)Use column chromatography to separate CPDs with different emission wavelengths" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207702&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207716&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207708&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　碳点的分类" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "CDs是一个广义术语，用于广泛表征尺寸小于10 nm的零维碳纳米材料" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。许多CDs在紫外线激发下都具有强烈的荧光特性。CDs的结构通常由sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "/sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "杂化碳核组成" }, { "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": "，表面通常是基于氧/氮的表面官能团和丰富的聚合物链，这使得CDs的水分散性非常好。由于多种多样的合成方法(自上而下和自下而上)以及广泛的原材料(石墨，小分子，聚合物，甚至天然材料等)，各种不同类型的CDs迅速被合成。当前，在科学文献中，对CDs的命名各不相同，主要集中在碳点、碳纳米颗粒、石墨烯量子点、碳量子点、碳纳米点、聚合物点、碳化聚合物点等" }, { "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": "。尽管关于CDs的分类和命名存在广泛的争论，但在很多综述和研究文章中，越来越清楚地将CDs划分为石墨烯量子点(GQDs)、碳量子点(CQDs)、碳纳米点(CNDs)和碳化聚合物点(CPDs)(" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "中的四张图是CPDs几种可能的碳核结构，分别为有序聚合物框架、类石墨结构、聚合物-石墨结构和共轭的网状结构。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "CDs的分类示意图" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "]" } ] } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "Schematic diagram of the classification of CDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "]" } ] } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207722&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207736&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207729&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "GQDs在边缘上具有一层或几层石墨烯以及相连的化学基团，它们是各向异性的，其横向尺寸大于其高度" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。CQDs几乎总是准球形或球形" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } } ], "rid": [ "R21", "R22", "R23" ], "text": "21-23", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，具有一定的晶格结构，但是内核中石墨结构的层数多于GQDs，值得注意的是，很多具有多层石墨内核结构并具有明显晶格结构的CDs也不一定是CQDs;PDs是由单体或线性聚合物制备的交联聚合物或聚集的聚合物链。CNDs具有较高的碳化度，表面具有一些化学基团，但通常不表现出明显的晶格结构和聚合物特征，其光致发光主要来自石墨碳核内的缺陷/表面态和亚畴态，而没有粒径的量子限制效应。CPDs具有聚合物/碳杂化结构，其在表面和碳核上包含丰富的官能团/聚合物链。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "CPDs是近些年新提出的一种CDs，从严格意义上讲，通过水热途径获得的大多数CDs都可以归类为CPDs。CPDs显示出聚合物/碳杂化结构，这是CPDs的主要特性，与传统的自上而下裂解所得CDs不同" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。CPDs不仅具有传统CDs的突出光学特性，而且还继承了聚合物的特性" }, { "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": "，这主要归因于聚合物/碳杂化结构和特殊的光致发光机理。CPDs也表现出许多独特的特性，例如高的氧/氮含量、优异的水溶性和出色的光致发光量子产率等。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "我们认为，CPDs通常应通过高聚物簇或者胶束的碳化来获得，因此碳化程度可作为评估CPDs中聚合物/碳杂化结构的重要参数，其对CPDs的性能具有重要影响" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } } ], "rid": [ "R26", "R27", "R28" ], "text": "26-28", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，也可以通过用聚合物或有机分子对CQDs进行后装饰来制备CPDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "29", "type": "bibr", "rid": "R29", "data": [ { "name": "text", "data": "29" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } } ], "rid": [ "R29", "R30" ], "text": "29-30", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。通过后期修饰制备的CPDs具有完整的CQDs核心结构并且在壳核和聚合物壳之间具有清晰的边界；相反，通过自下而上碳化的方法制备的CPDs通常不存在核壳之间的明确边界。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "CPDs的碳核与CQDs的核结构相似。碳核分别显示本征态发射，或由聚合物框架包围的微小碳簇组成的准结晶碳核结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，或部分脱水的交联和紧密编织的聚合物结构核，可形成有序结构且可保持稳定作为完全碳化的碳骨架" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } } ], "rid": [ "R32", "R33" ], "text": "32-33", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。作为碳核中的微小碳簇不仅可以是共轭π结构，而且可以是三角形或菱形等其他结构，并且共轭π结构也可以是平面或弯曲的，例如富勒烯片段或富勒烯结构等。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "虽然CDs的分类很多，但是这几种分类之间并不是独立的，而都是相互关联的。GQDs和CQDs都具有石墨的基本层状结构，CQDs的剥落程度决定了最终产品是各向异性的GQDs(几层厚度)还是CQDs(多层厚度);GQDs如果未适当稳定化，可能会发生快速聚集和结构转变，最终转变为无定形CPDs；同样，CQDs可以视为CPDs的一种极端类型，其中内部聚合物网络在类石墨片中高度有序；而PDs则被视为是CPDs的前体，碳化程度增加时PDs会逐渐向CPDs转变" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "目前人们对CDs的认识并不是很深入，在表征和定义CDs上也存在很多困难，完全分离的较为纯净的CDs可以通过高分辨透射电镜(HR-TEM)、选区电子衍射(SAED)、X射线衍射(XRD)、原子力显微镜(AFM)、拉曼(Raman)等表征手段对其结构性质进行表征。根据其定义，碳核既可以是单晶多层石墨碳(002平面的层间距为0.34 nm;001平面的层间距为0.21 nm)，也可以由无定形碳组成。粉末XRD会在布拉格角(2" }, { "name": "italic", "data": [ { "name": "text", "data": "θ" } ] }, { "name": "text", "data": ")22°左右出现特征峰，对于与CDs不同晶面，考虑到石墨(002平面)的层间间距为0.34 nm,2~5 nm大小的碳核中将由约6~14层单层石墨烯组成，这种层的数量可以通过使用AFM测量高度轮廓来定量获得。拉曼光谱法是一种无损的通用技术，已成为识别石墨烯基材料性质的基准。D带(1 360 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": ")表征缺陷或非晶性质，G带(1 580 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": ")表征sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "石墨碳的平面内振动，对于结晶多层石墨碳核，通常不应观察到D带。考虑到由于官能团的连接而产生的边缘缺陷，观察到强度较低的D带(与G带相比)并不奇怪。另一方面，对于非晶碳核，既没有观察到层间间隔也没有观察到晶格条纹。此外，对于无定形核心结构，在XRD中会在布拉格角(2" }, { "name": "italic", "data": [ { "name": "text", "data": "θ" } ] }, { "name": "text", "data": ")处出现宽峰，而在拉曼光谱中会发现缺陷带较宽。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "通过上述表征将很难区分不同类型的CDs，因为它们可能都包含相似的碳核。但是，可以通过热重分析(TGA)识别CDs表面的荧光团或者聚合物链，有机荧光团和聚合物链相对更易挥发，熔化温度比石墨核低得多，在其熔化温度下，CDs表面的荧光团和聚合物链将首先被破坏(不会干扰核)，样品的总质量会开始损失，总能量也开始变化，CDs的荧光团和表面聚合物链的破坏将大大降低光致发光效率。而随着温度继续升高，当所有的荧光团和聚合物链部分被破坏时，其余的光致发光应仅源自碳核结构，在稍后的阶段，碳核才会被逐渐破坏。另一方面，对于聚集的分子荧光团，应观察到荧光完全猝灭的现象。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "我们希望以上讨论将为自下而上合成的CDs的鉴定和表征及其相关的光致发光性质提供一些指导。特别值得注意的是，是否为GQDs或者CQDs并不是由存不存在晶格而决定，而是在于是否存在量子尺寸效应，有时存在的晶格并不一定对应的就是石墨的晶格常数，也有可能是聚合物纳米晶。此外，值得注意的是充分的纯化和表征对于CDs未来的发展至关重要。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3　碳点的发光机理" } ], "level": "1", "id": "s3" } }, { "name": "p", "data": [ { "name": "text", "data": "CDs由于其出色的光学性能、高生物相容性和低毒性，在许多领域(如生物成像、发光二极管、传感和信息加密)都发挥着重要的作用。随着其应用领域的蓬勃发展，了解其光致发光(PL)机理，从而可控制备具有特殊价值的CDs显得尤为重要。但是，目前CDs PL发射机理依然模糊，并且由于CDs原料的广泛性和合成步骤的不可控性，尚未找到统一的机理。目前的研究中，CDs的PL发射机理主要分为三类:内部因素主导发射(包括共轭效应、表面态和协同效应)、外部因素主导发射(包括分子态和溶剂效应)以及交联-增强发射(CEE)(" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": ")。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "CDs的PL机制" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "]" } ] } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "PL mechanism of CDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "]" } ] } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207743&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207759&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207751&type=" } ] } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1　内部因素主导发射" } ], "level": "2", "id": "s3a" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1.1　共轭效应" } ], "level": "3", "id": "s3a1" } }, { "name": "p", "data": [ { "name": "text", "data": "量子限制效应或尺寸效应是一种广为接受的PL机理，其中“尺寸”是指sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "(石墨烯)结构域(有效共轭长度)，而不是实际粒径" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "34", "type": "bibr", "rid": "R34", "data": [ { "name": "text", "data": "34" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。随着“尺寸”减小到纳米级，费米能级附近的准连续电子能级转换为离散能级。对于CDs，较大的“尺寸”会减小带隙，并相应增加PL发射波长。CDs内部石墨烯结构域的增加会导致更多的离域和更均匀的能量分配，进而减小最高占据分子轨道(HOMO)与最低未占据分子轨道(LUMO)之间的能隙。该模型适用于解释具有晶格结构或高度石墨化程度的PL。几个研究小组已经研究了CDs的颗粒尺寸依赖性PL。Li等使用石墨电极在碱性条件下电解乙醇水溶液以获得四种不同粒径的CDs(" }, { "name": "xref", "data": { "text": "图4(a)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(a)" } ] } }, { "name": "text", "data": ")" }, { "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": "。他们证实PL特性随颗粒大小而变化:小尺寸的CDs(1.2 nm)位于UV区(~350 nm)；中尺寸的CDs(1.5~3 nm)位于可见区域(400~700 nm)；大尺寸的CDs(3.8 nm)位于近红外区域(~800 nm)。这种粒度依赖性与量子限制效应一致。Kim等得出同样的结论，CDs的吸收光谱受粒径控制。理论计算证实了量子限制效应。Chen等使用高斯和随时间变化的密度泛函理论(DFT)计算出了不同直径的原始锯齿形CDs的发射波长" }, { "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": "。直径为0.46~2.31 nm的CDs在从深紫外线到近红外线的范围内发出。最小的CDs(苯，~0.5 nm)在235.2 nm波长处发射，而2.31 nm的CDs在999.5 nm处发射。随着CDs直径从0.89 nm增加到1.80 nm，发射范围遍及整个可见区域(400~770 nm)。发射波长随颗粒尺寸增加的红移可以解释为由于π电子离域而引起的带隙减小，即量子限制效应。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "内部因素影响。(a)使用色谱柱色谱分离具有不同发射波长的CPDs" }, { "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": ";(b)蓝色(左边)、绿色(中间)和红色(右边)CDs的TEM表征" }, { "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": ";(c)CDs的发射波长和掺杂原子的电负性具有相似的变化趋势" }, { "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": ";(d)具有不同氧化程度的CDs可调PL模型" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(e)通过调整表面状态来控制CDs的发射激发依赖性和独立性示意图" }, { "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": ";(f)F,N-CDs的合成" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "Influence of internal factors. (a)Use column chromatography to separate CPDs with different emission wavelengths" }, { "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": ". (b)TEM characterization of blue(left), green(middle) and red(right) CDs" }, { "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": ". (c)Emission wavelength of CDs and the electronegativity of dopant atoms have similar changing trends" }, { "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": ". (d)Models of adjustable PL for CDs with different oxidation levels" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (e)A schematic diagram of controlling the emission excitation dependence and independence of CDs by adjusting the surface state" }, { "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": ". (f)Synthesis of F,N-CDs" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207767&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207785&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207775&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "但是，在许多情况下都违反了这种依赖性。Miao等通过柠檬酸(CA)和尿素可控热裂解合成具有多色发射的CDs,CDs的平均粒径为(3.96±0.54),(4.12±0.68),(4.34±0.49)nm(" }, { "name": "xref", "data": { "text": "图4(b)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(b)" } ] } }, { "name": "text", "data": ")" }, { "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": "。X射线衍射和拉曼光谱分析表明，石墨化程度与增加的CDs尺寸趋势不符，因此发射波长的红移归因于石墨化程度的增加或有效共轭长度的增加，而不是尺寸的增大。Tang等还观察到了通过微波辅助水热法制备的CDs中颗粒大小无关的PL，并将其归因于自钝化层的存在，该自钝化层导致CDs的石墨烯结构域无法反映其实际尺寸" }, { "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": "。Ding等通过对苯二胺和尿素的混合物进行水热处理，合成了4个具有不同颜色的CDs，平均粒径约为2.6 nm的4个样品具有蓝色、绿色、黄色和红色荧光。这种变化在此归因于表面氧化程度" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "尽管共轭效应通常很好地解释了CDs尺寸与PL之间的关系，但存在一些与CDs尺寸无关的PL的反例，我们将其归为以下原因。首先，“尺寸”不是实际的物理粒度，而是反映sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "域或有效共轭长度，这对于包含嵌入sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "碳基质中的孤立的sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "簇(石墨烯碳核)的CDs而言非常重要。其次，除了尺寸效应外，其他效应可能会主导发射并影响PL。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1.2　表面态" } ], "level": "3", "id": "s3a2" } }, { "name": "p", "data": [ { "name": "text", "data": "附着状态对PL也可能存在影响，因为这种“表面态”说明了不存在共轭效应的情况。本质上，表面态模型解释了与电子能级的变化相对应的发光部位的变化。表面态一般包括两类，即表面构型" }, { "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": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } } ], "rid": [ "R30", "R31" ], "text": "30-31", "type": "bibr" } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "42", "type": "bibr", "rid": "R42", "data": [ { "name": "text", "data": "42" } ] } } ], "rid": [ "R38", "R39", "R40", "R41", "R42" ], "text": "38-42", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "和掺杂原子" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "51", "type": "bibr", "rid": "R51", "data": [ { "name": "text", "data": "51" } ] } } ], "rid": [ "R43", "R44", "R45", "R46", "R47", "R48", "R49", "R50", "R51" ], "text": "43-51", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。表面构型可以理解为是宽泛的表面结构类型，例如聚合物，官能团(不同程度的氧化)、缺陷和边缘状态很重要，后者涉及杂原子如氮、氟、硫、磷或硒对PL的影响。许多研究表明，控制表面状态以调整CDs的能量结构会影响其发光度。表面构型的改变可能会改变CDs的电子能级或发光位置，甚至可能诱发先前非发光CDs的发射" }, { "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": "。表面构型可以通过氧化还原反应、氨基修饰和分子修饰来调节。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "电化学方法可通过调节电极电势和电流密度来精确控制CDs的合成。Bao等通过电化学蚀刻碳纤维同时调节电极电位来制备CDs，较高的电位导致CDs较小" }, { "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": "。在较高电位下合成的CDs的发射发生红移，抵消了共轭效应。进一步的工作表明，较高的电势会增加表面氧化，并相应增加发射波长，这可能是由于更高的氧化程度会增加表面缺陷密度并导致更多的激子被俘获，其激子复合产生红移辐射。因此，具有高表面氧化度的CDs呈现绿色PL。Liu等研究了在碱性条件下使用烛灰作为碳源，通过水热合成的CDs的pH响应" }, { "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": "。当在碱性条件下溶解时，所得CDs发出荧光，而在酸性条件下PL猝灭。这种现象归因于在酸性条件下形成氢键，这防止了源自羟基的发射。CDs上的羟基涂层增强了PL,PL是由辐射复合产生的:当羟基或羧基嵌入CDs表面时，电子和空穴在激发光照射下辐射重组，从而导致PL。吸电子基团(例如羧基)吸收部分辐射信号，从而削弱PL，而供电子基团羟基则促进PL。Zheng等使用硼氢化钠将表面羰基和环氧部分还原为羟基，并证实给电子表面基团可增强PL" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "42", "type": "bibr", "rid": "R42", "data": [ { "name": "text", "data": "42" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "氨基修饰或氨基钝化可用于调整CDs的表面状态。Li等推测CDs的PL激发依赖性受表面胺化程度的影响(" }, { "name": "xref", "data": { "text": "图4(e)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(e)" } ] } }, { "name": "text", "data": ")" }, { "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": "。如果所有表面状态都被氨基钝化，则发射会通过sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "碳的辐射跃迁的单一模式发生，而与激发波长无关。当表面态不那么钝化时，诸如C—O、C" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207793&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207806&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207799&type=" } } } ] }, { "name": "text", "data": "O和O" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207811&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207826&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207817&type=" } } } ] }, { "name": "text", "data": "C—OH之类的官能团会产生许多不同的能级，然后荧光发射取决于激发能。含有氨基的有机分子也被用来修饰CDs表面以控制其PL。表面功能化赋予CDs新的能级，使其表现出非常窄的光谱宽度的长波长PL。理论计算还确定了表面氨基官能化的作用。Kundelev等对氨基官能化CDs的吸收和PL进行了全面的量子化学DFT研究，将光学中心描述为分子状，其中1个、2个或3个氨基与多环芳烃分子的外环相连，并且光学中心之间的光学特性不同" }, { "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": "。他们发现氨基表面基团不仅引起红移，而且还保留了CDs固有的高PL强度。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "氮(N)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "47", "type": "bibr", "rid": "R47", "data": [ { "name": "text", "data": "47" } ] } } ], "rid": [ "R43", "R44", "R45", "R46", "R47" ], "text": "43-47", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、氟(F)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "44", "type": "bibr", "rid": "R44", "data": [ { "name": "text", "data": "44" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "45", "type": "bibr", "rid": "R45", "data": [ { "name": "text", "data": "45" } ] } } ], "rid": [ "R44", "R45" ], "text": "44-45", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、硫(S)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "47", "type": "bibr", "rid": "R47", "data": [ { "name": "text", "data": "47" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、磷(P)" }, { "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": "和一些重原子" }, { "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": "的杂原子掺杂是改变CDs的电子结构广泛使用的手段。通常考虑的是掺杂原子而不是表面构型，但是由于这两种方法都在本质上发生变化，因此可以将电子结构掺杂视为一种表面状态技术" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "49", "type": "bibr", "rid": "R49", "data": [ { "name": "text", "data": "49" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "51", "type": "bibr", "rid": "R51", "data": [ { "name": "text", "data": "51" } ] } } ], "rid": [ "R49", "R50", "R51" ], "text": "49-51", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。N和S是常见的掺杂物，前者的原子半径与碳相似，而后者的电负性相似。Dong等研究了它们对CDs的量子产率(QYs)和激发依赖性的影响，将它们归类为具有低QYs值、激发依赖性发射和宽UV-Vis吸收带的O掺杂“O-CDs”" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。N掺杂的“N-CDs”具有更高的QYs值、相似的激发依赖性和宽光谱；以及N-S掺杂的“N,S-CDs”具有高QYs值和不依赖激发的发射。各种O-CDs的表面态(“O态”)是激发依赖性和宽吸收带的原因。氮掺杂引入了一种新型的表面态(“N态”)，其作用于电子以产生高辐射复合产率。S原子的进一步添加似乎消除了O态并增强了N态，并具有更强的激发无关PL发射。Song等提出了一种通过S掺杂增强N掺杂的类似机制" }, { "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": "。氟是最具负电性的元素，也是一种有效的掺杂剂。Jiang等用聚乙烯亚胺和左氧氟沙星的微波辅助热分解法合成了具有压力触发的聚集诱导发射(AIE)的F-N共掺杂CDs，这是由于在压力下—NH" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "和C—F表面基团之间的氢键缩短而引起的(" }, { "name": "xref", "data": { "text": "图4(f)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(f)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "44", "type": "bibr", "rid": "R44", "data": [ { "name": "text", "data": "44" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "45", "type": "bibr", "rid": "R45", "data": [ { "name": "text", "data": "45" } ] } } ], "rid": [ "R44", "R45" ], "text": "44-45", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Jiang等进一步证明了F掺杂的主要功能是形成氢键(F具有高电负性)" }, { "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": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "关于重元素掺杂，Yang等提出了一种基于电子给体和受体的与电负性有关的理论(" }, { "name": "xref", "data": { "text": "图4(c)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(c)" } ] } }, { "name": "text", "data": ")" }, { "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": "。他们发现，将S或Se掺杂到CDs中会使其PL光谱发生红移，而N掺杂则具有相反的偏移，重元素掺杂CDs的QYs值取决于杂原子的电负性。这归因于诸如N的电子受体促进电子转移(增加QYs)，以及诸如S和Se的电子供体减少电子转移(将QYs降低到N-CDs以下)。还发现，O-CDs中大量的含氧基团会导致局部电子-空穴对的非辐射偶联，从而抑制了辐射跃迁，因此考虑到高电负性氧的掺杂导致QYs值非常低。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "总之，表面修饰和杂原子的引入提供了对CDs的电子结构和能级的控制，并具有广泛适用的潜在PL机制。但是，由于表面状态主要取决于碳核，因此必须考虑其与碳核的相互作用，了解它们的共同作用(协同效应)对于理解CDs的 PL发射是必不可少的。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1.3　协同效应" } ], "level": "3", "id": "s3a3" } }, { "name": "p", "data": [ { "name": "text", "data": "一些研究表明，碳核和表面状态都与CDs的 PL有关。Yu等用微波方法制备了6种类型的具有不同C和N含量的CDs，发现可变的发射和激发与不同的CDs结构有关" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "52", "type": "bibr", "rid": "R52", "data": [ { "name": "text", "data": "52" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。5个以305,355,410,445,500 nm为中心的CDs发射带分别对应于本征C(4.1 eV)、石墨N(3.5 eV)、吡啶N(3.0 eV)、氨基N(2.8 eV)和C" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207834&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207848&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207843&type=" } } } ] }, { "name": "text", "data": "O(2.5 eV)的电子跃迁，这些能量转移过程是由碳核与表面态之间的协同作用引起的。由内部因素决定的发射取决于碳核中的共轭效应，尤其是具有石墨烯结构的CDs的PL通常以碳核为主。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "表面官能团经常与共轭作用协同作用以产生CDs的 PL。Liu等使用氧化的碳化纤维在硝酸中制成CDs，然后用氢氧化钠和硼氢化钠处理" }, { "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": "。他们的研究表明，能隙是由电子系统和羰基的耦合决定的，而QYs取决于羰基。总体而言，官能团和π电子系统在CDs的PL上具有协同作用。如前所述，石墨化会影响CDs的发射，但Miao等提出表面—COOH基团的浓度是影响PL的另一个因素" }, { "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": "。石墨化的加剧和—COOH量的增加导致了发射红移。Bao等通过硝酸中碳纤维的氧化合成荧光CDs，然后通过透析将反应产物分为3组，分子量分别为" }, { "name": "text", "data": "<" }, { "name": "text", "data": "3,3~10,10~30 ku的CDs" }, { "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": "。反应时间的增加导致通过表面氧化相关的PL使最大发射峰发生红移，CDs的直径为3组(分别约为2.7,3.3,4.1 nm)，与红移的程度相对应。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "从根本上说，内部因素占主导地位的发射涉及碳核和表面状态所产生的影响的整合和相互作用。从碳核的共轭长度的角度来看，共轭效应解释了CDs尺寸对发光的影响。表面状态的影响更为普遍，并解释了由发射位点或电子能级的变化引起的不同发光。考虑它们的协同作用也许可以更全面地解释CDs的PL，但是某些现象仍无法由内部因素主导的发射来解释。例如，某些PL独立于碳核而发生，并且外部环境也作用于CDs的PL，因此需要其他PL机制。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2　外部因素主导发射" } ], "level": "2", "id": "s3b" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2.1　分子态" } ], "level": "3", "id": "s3b1" } }, { "name": "p", "data": [ { "name": "text", "data": "由于最初的CDs溶液可能包含许多杂质，因此使用透析袋进行透析纯化对于CDs的合成至关重要，根据CDs的尺寸将CDs与杂质分离。在透析袋的内部和外部都观察到了类似的PL，这表明PL源于渗入透析袋的小分子。发光的CDs部位可能是独立于碳核而存在的分子状态，并且被物理化学吸附在CDs的表面。因此，分子态可能是CDs发光的重要因素。大多数分子态是通过自下而上的途径产生的，因为小分子会自发反应以制造荧光团分子。在这里，基于共轭和非共轭的小分子，可以通过自下而上的途径产生分子态的机理进行介绍，这些小分子可以分别视为表面态和共轭效应的特殊情况。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "由CA进行自下而上合成CDs的过程中可能会生成小分子荧光团。本质上，分子态是由原材料通过有机反应形成的。CA是许多非共轭分子系统的关键单体。根据分子态理论" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "55", "type": "bibr", "rid": "R55", "data": [ { "name": "text", "data": "55" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "58", "type": "bibr", "rid": "R58", "data": [ { "name": "text", "data": "58" } ] } } ], "rid": [ "R55", "R56", "R57", "R58" ], "text": "55-58", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ",CA在低温下脱水并与其他小分子缩合形成荧光团，然后随着温度的升高聚合并碳化成碳核(石墨烯或无定形结构)。最终，附着在碳核表面上的荧光团形成CDs主体，这是造成大多数发射的原因。Song等通过从CA和乙二胺(EDA)制备CDs来研究分子态作为荧光来源(" }, { "name": "xref", "data": { "text": "图5(f)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(f)" } ] } }, { "name": "text", "data": ")" }, { "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": "。通过小分子有机合成反应，他们构建了咪唑并［1,2-a］吡啶-7-羧酸(IPCA)，并进行了一系列表征，包括PL和吸收光谱、PL寿命测量、红外光谱、质谱、核磁共振波谱分析，证实CDs包含分子IPCA。在140 ℃下由CA和EDA合成该分子态。在较高的温度下，会发生更强的聚合反应和碳化反应，生成的碳核具有弱的、依赖于激发的发光，并且荧光团分子也可能在其他反应系统中发生" }, { "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": "。除基于CA的CDs系列外，苯二胺最近还被用作CDs的制备前体，并且在某些情况下偶尔会发现分子荧光团的存在。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "外部因素影响。(a)PL行为的动力学方面的说明" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)溶剂分子和CDs之间的氢键对发光的影响" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(c)CDs的两个发光位置:核心(带Ⅰ)和表面(带Ⅱ)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "64", "type": "bibr", "rid": "R64", "data": [ { "name": "text", "data": "64" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(d)~(e)由共轭小分子通过自下而上途径合成的红色发射CDs示意图" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "67", "type": "bibr", "rid": "R67", "data": [ { "name": "text", "data": "67" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "68", "type": "bibr", "rid": "R68", "data": [ { "name": "text", "data": "68" } ] } } ], "rid": [ "R67", "R68" ], "text": "67-68", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(f)不同温度下CDs形成的图形说明" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.5" } ], "title": [ { "name": "text", "data": "Influence of external factors. (a)Description of the dynamics of PL behavior" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Effect of hydrogen bonds between solvent molecules and CDs on luminescence" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)Two luminescence positions of CDs: core(band Ⅰ) and surface(band Ⅱ)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "64", "type": "bibr", "rid": "R64", "data": [ { "name": "text", "data": "64" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (d)-(e)Schematic diagram of red emitting CDs synthesized by conjugated small molecules through a bottom-up approach" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "67", "type": "bibr", "rid": "R67", "data": [ { "name": "text", "data": "67" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "68", "type": "bibr", "rid": "R68", "data": [ { "name": "text", "data": "68" } ] } } ], "rid": [ "R67", "R68" ], "text": "67-68", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (f)Graphic illustration of CDs formed at different temperatures" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207857&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207871&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207864&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "与确定荧光团化学结构且其发光中心可以独立于CDs的非共轭分子系统不同，共轭小分子并不严格显示分子发光，并且对于某些该类分子，适用了共轭效应的原理。然而，从分子或合成的角度考虑分子态可以解释CDs的发光中心。在Zhang等的最新报告中，将对苯二胺添加到5种不同的反应溶剂(二甲基甲酰胺、乙醇、二氯甲烷、二甲基亚砜、乙酸乙酯和丙酮)中(" }, { "name": "xref", "data": { "text": "图5(b)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(b)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，多色CDs溶液是在水热/溶剂热条件下获得的，发射光谱从蓝色到红色。在这种情况下，具有红色发射的样本显示出单指数衰减，并且寿命为9.4 ns，这与所检测的波长无关。此外，进行了多次结构测量，并确认红色发射源于由含氮有机荧光团组成的分子态。然后，各种理论模型证实了分子态和溶剂之间的氢键效应是CDs光谱移动的主要机理。这些事实与分子态转变的特征非常吻合。在自下而上的途径中，无论是确定荧光团的化学结构还是推测形成CDs的方式，都是对分子态的研究。但是，由于CDs以难以表征的混合物形式形成，因此确定其组成是一项常见的研究挑战，并且代表了对分子态使用的重大限制。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2.2　溶剂影响" } ], "level": "3", "id": "s3b2" } }, { "name": "p", "data": [ { "name": "text", "data": "溶剂对于CDs的制备和表征至关重要，既影响合成又影响颗粒溶解。不同的溶剂会产生不同的CDs结构，并具有不同的光学特性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "2", "type": "bibr", "rid": "R2", "data": [ { "name": "text", "data": "2" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "47", "type": "bibr", "rid": "R47", "data": [ { "name": "text", "data": "47" } ] } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } } ], "rid": [ "R59", "R60" ], "text": "59-60", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。当颗粒溶解时，溶剂也会影响发射，强调了理解CDs和溶剂分子之间相互作用的重要性。溶剂极性、pH值和其他属性的差异会影响这些相互作用，从而导致其他类似颗粒的PL行为不同。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "溶剂弛豫是一种溶剂效应" }, { "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": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } } ], "rid": [ "R61", "R62", "R63" ], "text": "61-63", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Khan等用时间分辨的发射来揭示依赖于激发的PL，这违反了Kasha-Vavilov规则，该规则指出在荧光发射之前，被激发的分子通常返回到第一个激发单重态的最低振动能级，从而导致与激发无关的发射(" }, { "name": "xref", "data": { "text": "图5(a)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(a)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Khan等考虑到吸收后(10" }, { "name": "sup", "data": [ { "name": "text", "data": "-15" } ] }, { "name": "text", "data": " s)，依次发生了两个非辐射过程(振动和溶剂松弛)，然后是辐射PL(10" }, { "name": "sup", "data": [ { "name": "text", "data": "-9" } ] }, { "name": "text", "data": " s)。振动弛豫的时间尺度平均为10" }, { "name": "sup", "data": [ { "name": "text", "data": "-12" } ] }, { "name": "text", "data": " s，而后期的溶剂弛豫则由溶剂决定" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Arshad等通过在375 nm激发下记录分散在不同溶剂中的CDs的发射光谱发现通过用水代替乙酸乙酯来增加溶剂的极性，使发射峰红移了~0.26 eV" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。进一步的研究归因于极性更强的溶剂能够更好地稳定激发态，而对基态几乎没有影响，从而使发射红移。诸如氢键和CDs的内部渗透之类的溶剂相互作用也影响CDs的光学性能。Zhang等发现含氮荧光团中的氨基与溶剂分子形成氢键，同时充当电子受体和供体，氢键在质子中的作用比非质子溶剂大" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。这种相互作用促进了内部转换，增加了光谱偏移，缩短了PL寿命并降低了QYs值。溶剂分子也可能进入CDs的内部，从而影响其光学性能。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "依赖温度的PL使CDs具有作为温度探测器的潜在应用。Yu等通过将P" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O" }, { "name": "sub", "data": [ { "name": "text", "data": "5" } ] }, { "name": "text", "data": "添加到冰醋酸和H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O的混合物中制备CDs(" }, { "name": "xref", "data": { "text": "图5(c)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(c)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "64", "type": "bibr", "rid": "R64", "data": [ { "name": "text", "data": "64" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。他们的理论模型表明，PL谱由两个高斯函数很好地拟合:一个对应于核心(带Ⅰ)，另一个对应于表面态(带Ⅱ)，符合内部因素主导的发射机制。实验证明PL强度随温度升高而降低，紧随Arrhenius关系。Wang等提出聚集是造成PL温度依赖性的原因" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "65", "type": "bibr", "rid": "R65", "data": [ { "name": "text", "data": "65" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。他们通过在谷胱甘肽存在下对葡萄糖进行水热处理来制造CDs，并发现PL强度随温度升高而降低。外部温度的变化不会影响CDs的UV-Vis光谱，但会改变粒径，从80 ℃的(4.4±0.2) nm到室温下的(2.6±0.2) nm。因此，加热可能使CDs聚集，导致PL猝灭。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "外部压力可能会压缩CDs并改变其辐射路径。压力的大幅度增加甚至可能改变CDs的结构，例如CDs的sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "结构部分转化为sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "结构，使PL光谱不可逆转地蓝移" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。外部条件的变化可能会影响CDs与周围环境的相互作用，从而改变发射位置和电子能级。环境还可能影响CDs的聚集甚至改变CDs的结构，从而对PL机制产生重要影响。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.3　交联增强发射(CEE)" } ], "level": "2", "id": "s3c" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.3.1　CEE基本原理" } ], "level": "3", "id": "s3c1" } }, { "name": "p", "data": [ { "name": "text", "data": "CEE对CDs发光的影响可根据两个主要方面进行总结:固定化和产生新的能级" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } } ], "rid": [ "R69", "R70" ], "text": "69-70", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Jablonski图描述了发光的本质:基态电子经历吸收和内部转换，或者通过直接返回基态发射PL，或者在系统间交叉后通过返回基态发射磷光。被激发的电子还可以经历非辐射衰变，返回基态而不发光。辐射跃迁和非辐射衰变共存并相互竞争。固定可以大大减少振动和旋转，从而抑制非辐射衰减并促进发光。另外，在交联和聚集之后，官能团之间距离的变化导致新的重叠和耦合电子云的形成，能级的重新排列刺激了沿着辐射路径的选择。在CEE理论被提出前，有关CDs发光机理的争论很多，这从变化的辐射跃迁角度为PL解析提供了最可能的解释。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.3.2　共价键CEE" } ], "level": "3", "id": "s3c2" } }, { "name": "p", "data": [ { "name": "text", "data": "作为强相互作用，共价键可以减少系统中的振动和旋转，从而增加PL甚至改变辐射路径。聚乙烯亚胺是CDs合成中的关键材料，Zhu等在带有CEE的CDs的第一个演示中使用了它，使用支化的聚乙烯亚胺(PEI)合成了四种类型的CDs" }, { "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": ":CD1具有四氯化碳交联；CD2由PEI水热法制得；通过将PEI连接到CDs来制备CD3和CD4，前者是无定形CDs，后者是CDs(" }, { "name": "xref", "data": { "text": "图6(a)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(a)" } ] } }, { "name": "text", "data": ")。将CD1暴露在紫外线下20 min会使稳态PL降低至38%，并使PL寿命增加30%，这可以用CEE解释:当不进行UV辐照时，交联的CD1结构会限制非辐射跃迁，但部分辐照破坏结构并增加非辐射跃迁(而辐射跃迁减少)。随后使用飞秒瞬态吸收光谱法对这4个CDs的研究表明，它们都具有相同的PL中心。与裸PEI相比，由于CEE,CD1和CD2中辐射过程的比例增加。与原始CDs相比，具有PEI表面连接的CDs也显示出增强的发射，因为CEE增强了碳核(在CD3中)或由CDs的多层晶格(在CD4中)引起中和的非辐射过程的天线效应。紫外线可以破坏交联结构，某些离子物种也可以破坏交联结构。Tong等由聚氨酯合成了CDs，并使用亲水性封端剂进行了改性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "71", "type": "bibr", "rid": "R71", "data": [ { "name": "text", "data": "71" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。最初的CDs的PL通过与Fe" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "反应猝灭，但随后通过添加螯合剂(乙二胺四乙酸)进行恢复。作者建议将CEE作为PL的起源，当Fe" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "离子与CDs结合时，它将被猝灭。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "自交联发射。(a)裸PEI和PD 1~4的CEE插图" }, { "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": ";(b)使用CCl" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "交联支链PEI" }, { "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": ";(c)描述通过“自下而上”路线制备CPDs的HTCP反应过程示意图" }, { "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": ";(d)乙二胺(EDA)与偶联剂通过两条合成途径反应形成CDs1和CDs3,EDA与三碳烯酸反应形成CDs2" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "72", "type": "bibr", "rid": "R72", "data": [ { "name": "text", "data": "72" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "Self-crosslinking emission. (a)CEE illustrations of bare PEI and PD 1-4" }, { "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": ". (b)Cross-linked branched PEI with CC" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207878&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207891&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207883&type=" } } } ] }, { "name": "text", "data": ". (c)Schematic diagram describing the HTCP reaction process for preparing CPDs through the “bottom-up” route" }, { "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": ". (d)Ethylenediamine(EDA) reacts with the coupling agent through two synthetic pathways to form CDs1 and CDs3, and EDA reacts with trimethylene acid to form CDs2" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "72", "type": "bibr", "rid": "R72", "data": [ { "name": "text", "data": "72" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207898&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207908&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207903&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.3.3　非共价键CEE" } ], "level": "3", "id": "s3c3" } }, { "name": "p", "data": [ { "name": "text", "data": "非共价相互作用比共价键具有更广泛的作用，因此作用范围更广。氢键键合可导致非共价CEE。Vallan等研究了其对3种CDs发光的介导:在140 ℃下分别使用EDA和CA或三羧酸通过微波合成了CDs1和CDs2;CDs3在室温下使用CA、EDA和偶联剂合成(" }, { "name": "xref", "data": { "text": "图6(d)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(d)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "72", "type": "bibr", "rid": "R72", "data": [ { "name": "text", "data": "72" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。与CD2相比，CD1和CD3具有很高的QYs值。结构表征鉴定出CDs1和CDs3中的相似结构，不同于CDs2的结构，这表明底物中的羟基会影响CDs的合成和发光。随后的实验发现，PL强度在酸性环境中会减弱，表明发光受到氢键或静电力的影响。此外，理论计算表明，对于一条小的聚合链，分子内和分子间氢键对CDs发射的影响是不同的。对于分子内相互作用，对非辐射跃迁的抑制非常小，以至于大多数电子非辐射地返回基态，并且发射发生红移。分子间的相互作用形成了一个相对刚性的网络，该网络极大地促进了辐射跃迁并减少了红移(发射波长约为650 nm)。Tao等认为交联结构可以包裹荧光团，以防止非辐射跃迁" }, { "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": "。聚丙烯酸和EDA用于水热制备具有高QYs值的CDs。实验表明，CDs的PL中心包含有—C" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207912&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207924&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207916&type=" } } } ] }, { "name": "text", "data": "O和—N" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207928&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207941&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207933&type=" } } } ] }, { "name": "text", "data": "O基团的荧光团。PL光谱的温度依赖性表明，荧光团振动和旋转的活化是影响PL强度的主要因素。此外，CDs的溶解导致荧光团被聚合物链包围和保护，聚合物链中的许多羧基使发光发生红移。识别出的CEE固定并保护了发光中心，并且还影响了发射波长。" } ] } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4　 碳点的应用" } ], "level": "1", "id": "s4" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4.1　生物成像" } ], "level": "2", "id": "s4a" } }, { "name": "p", "data": [ { "name": "text", "data": "强大的发光性、低毒性和令人惊讶的穿透力(红色发射成像)使CDs在生物成像上有很好的应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "74", "type": "bibr", "rid": "R74", "data": [ { "name": "text", "data": "74" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "75", "type": "bibr", "rid": "R75", "data": [ { "name": "text", "data": "75" } ] } } ], "rid": [ "R74", "R75" ], "text": "74-75", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。癌细胞的准确检测和定位已引起很多研究关注。近年来，大尺寸CDs悬剂注射液已被临床认可" }, { "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": "，因为 CDs可以从体内快速排出，毒性低同时产生可靠的光信号。另外，CDs已经用作光动力疗法和光热疗法的光声对比剂" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "78", "type": "bibr", "rid": "R78", "data": [ { "name": "text", "data": "78" } ] } } ], "rid": [ "R77", "R78" ], "text": "77-78", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。与无机量子点相比，CDs具有低毒性、低副作用且适合于生物系统" }, { "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": "。其次，高稳定性和明亮的荧光有望在实验中获得更好结果，并且仅需要少量的CDs即可生成所需的光信号" }, { "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": "。此外，某些CDs具有多光子发射，与低阶成像相比，高阶多光子发射上转换荧光具有穿透深度增加、自发荧光减少和分辨率提高的优点。此外，具有NIR发射特性的CDs也有望成为对深部组织样本成像的候选者。Lin等报道了一种用于制备高效红色发射CDs(R-CDs)的简便方法(" }, { "name": "xref", "data": { "text": "图7(b)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(b)" } ] } }, { "name": "text", "data": ")" }, { "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": "。发现R-CDs可以单光子和双光子模式特别点亮富含RNA的核仁，并且与其他经典的亚细胞染料具有出色的复染相容性。核糖核酸酶消化试验支持R-CDs在核仁中的定位，并且进一步证实了较强的发射是由于积累过程引起的。另外，证实R-CDs容易与异硫氰酸荧光素缀合，然后将其带入活细胞。Sun小组以D-葡萄糖和L-天冬氨酸为起始原料，通过直接的热解途径合成了具有针对脑癌神经胶质瘤靶向功能的CDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "83", "type": "bibr", "rid": "R83", "data": [ { "name": "text", "data": "83" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。所制备的CDs不仅具有出色的生物相容性和可调谐的全色发射，而且还具有在不借助任何额外靶向分子的情况下靶向C6胶质瘤细胞的显着能力。体内荧光图像显示尾静脉注射15 min后CDs的高对比度生物分布。在神经胶质瘤部位检测到的荧光信号比正常大脑中的荧光信号强得多，表明它们能够自由穿透血脑屏障并精确靶向神经胶质瘤组织。Yang的小组报告了水热合成高效红色发射氮掺杂CDs的方法，其最佳发射波长约为630 nm(" }, { "name": "xref", "data": { "text": "图7(a)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(a)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "84", "type": "bibr", "rid": "R84", "data": [ { "name": "text", "data": "84" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，所制备的CDs在体外和体内均可成功用作生物成像的荧光探针。更重要的是，生物分布结果表明，大多数CDs及其代谢物不仅通过尿液排泄，而且通过肝胆系统迅速排泄。此外，这些CDs可以轻松穿越血脑屏障，这可以通过实时跟踪为某些脑部疾病的诊断提供有价值的策略。此外，使用CDs作为荧光成像剂也可以实现小鼠胃和血液循环过程的活体近红外荧光成像。最近，由于荧光成像有一些比较依赖于荧光发射波长，而且采用一些可见光对CDs进行照射，可能会对细胞有一定的损伤，所以近些年开发出了光声成像、多模式成像" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "85", "type": "bibr", "rid": "R85", "data": [ { "name": "text", "data": "85" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "和双光子荧光成像。光声成像是由光能转化为热能，之后转化为信号图像的一个机理；多模式成像是将不同成像模式结合到一起，进行生物医学成像的原理；双光子成像是一种利用双光子复合探测恢复待测物体空间信息的一种新型成像技术。" } ] }, { "name": "fig", "data": { "id": "F7", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图7" } ], "title": [ { "name": "text", "data": "(a)在高温高压下，在HNO" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "存在下具有共轭芳族苯骨架的CDs可能的形成机理以及在生物成像中的应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "84", "type": "bibr", "rid": "R84", "data": [ { "name": "text", "data": "84" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)R-CDs的制备和表征以及在生物成像中的应用" }, { "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": ";(c)CDs在电致发光LEDs中的应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "93", "type": "bibr", "rid": "R93", "data": [ { "name": "text", "data": "93" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(d)多色带隙荧光CDs的LEDs应用" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.7" } ], "title": [ { "name": "text", "data": "(a)Possible formation mechanism of CDs with a conjugated aromatic benzene skeleton in the presence of HNO" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " and their application in bioimaging at high temperature and high pressure" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "84", "type": "bibr", "rid": "R84", "data": [ { "name": "text", "data": "84" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Preparation and characterization of R-CDs and their application in bioimaging" }, { "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": ". (c)Application of CDs in electroluminescent LEDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "93", "type": "bibr", "rid": "R93", "data": [ { "name": "text", "data": "93" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (d)Application of multicolor band gap fluorescent CDs in LEDs" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207946&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207958&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207952&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4.2　发光二极管" } ], "level": "2", "id": "s4b" } }, { "name": "p", "data": [ { "name": "text", "data": "CDs由于具有可调、稳定的PL和环境兼容性，逐渐开始取代昂贵的稀土基磷光体和有毒金属半导体量子点" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "67", "type": "bibr", "rid": "R67", "data": [ { "name": "text", "data": "67" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "86", "type": "bibr", "rid": "R86", "data": [ { "name": "text", "data": "86" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。多色CDs和固态CDs的大规模制备为多色 LEDs的制备铺平了道路，特别是半峰宽较宽的CDs，使其成为制造白光LEDs(WLEDs)的理想选择" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "87", "type": "bibr", "rid": "R87", "data": [ { "name": "text", "data": "87" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } } ], "rid": [ "R87", "R88", "R89" ], "text": "87-89", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。预期寿命长，功耗低，响应时间快，体积小，已成为社会可持续发展的重要节能技术。因此，人们做出了一些努力来实现CDs在LEDs中的巨大应用潜力" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "90", "type": "bibr", "rid": "R90", "data": [ { "name": "text", "data": "90" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。可以根据发光的原因将设备分类为光致发光或电致发光。光致发光LEDs使用CDs复合材料作为荧光粉，而电致发光LEDs是通过直接电激发产生的" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "91", "type": "bibr", "rid": "R91", "data": [ { "name": "text", "data": "91" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。光致发光和电致发光是目前制备CDs基LEDs最常用的手段，光致发光LEDs作为目前最常用的手段，具有操作简单的特点，即将CDs直接与聚合物介质混合，涂覆在相应发光的芯片上，即可实现对应波长的发光。但是，基于光致发光LEDs对CDs的工业化价值不大，并且随着芯片温度的升高，CDs的稳定性会下降。相对于光致发光LEDs，电致发光LEDs是目前科学家致力开发的领域，因其实用价值更大，但是限制其发展的因素依然很多，如器件构筑困难、外量子效率难以提高等。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "将发光CDs嵌入到诸如环氧树脂溶液或聚二甲基硅氧烷的固体基质中，可以产生光致发光的多色LEDs" }, { "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": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，也可以通过将CDs与互补色混合来获得白光LEDs。显色指数极高，因此发出的光非常接近纯白光。Yang的小组获得了一系列发光的蓝移CDs/PVA复合荧光粉" }, { "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": "。然后，还可以通过涂覆CDs/PVA复合材料来获得几乎全色和白色的基于磷光体的LEDs。这些荧光粉LEDs的发射光谱分别显示(0.21,0.11)、(0.31,0.41)、(0.41,0.48)、(0.48,0.35)和(0.29,0.30)的CIE颜色坐标，而白色LEDs则显示白光显色指数(CRI)为83。此外，基于黄绿色、橙红色和白色的荧光粉LEDs的亮度分别达到近5 000,10 000,5 000 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2[" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。该小组制备了抗自猝灭性固态荧光聚合物CDs(SSFPCDs)，通过调节CDs与淀粉的比例，获得了可调谐的固态荧光粉，例如SSFPCDs-淀粉与蓝色(b-CDs)的淀粉复合物、绿色(g-CDs)和黄色(y-CDs)粉末，这些具有不同发射率的荧光粉可用作LEDs应用中的荧光粉" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "88", "type": "bibr", "rid": "R88", "data": [ { "name": "text", "data": "88" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。制作了具有各种颜色发射的固态LEDs，其CIE色坐标分别为(0.59,0.41)、(0.43,0.48)、(0.30,0.49)和(0.26,0.33)。通过组合b-PCDs粉末和SSFPCDs粉末，还获得了CIE坐标接近(0.31,0.31)的白色照明固态LEDs，从而实现了具有相同化学结构的SSFPCDs的全波长发射LEDs，成功制备了QYs为53%的红色发光CDs。首次实现了基于紫外(UV)泵浦的CQDs荧光粉的暖白色发光二极管(WLEDs)，其显色指数达到97。这项工作为探索低成本、环保的封装提供了新途径。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "电致发光LEDs还可以实现多色发光和混合白光" }, { "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": "。通常，CDs宽的半峰宽会导致不纯的发射颜色，从而限制了它们在LEDs中的应用。Fan的小组制备了多色窄带宽发射CDs，其QYs为54%~72%(" }, { "name": "xref", "data": { "text": "图7(c)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(c)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "93", "type": "bibr", "rid": "R93", "data": [ { "name": "text", "data": "93" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。然后，基于这些CDs的多色LEDs显示出良好的稳定性，高色纯度和高性能，最大亮度为1 882~4 762 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，电流效率为1.22~5.11 cd·A" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "。同一小组通过简单地控制CA和二氨基萘的融合和碳化合成了多色荧光CDs，并实现了基于CDs的具有稳定的从蓝色到红色的发射颜色的单色电致发光LEDs的示例，该CDs直接用作没有空穴传输层的有源发射层(" }, { "name": "xref", "data": { "text": "图7(d)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(d)" } ] } }, { "name": "text", "data": ")" }, { "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": "。LEDs显示非常稳定且与电压无关的发射颜色。蓝色LEDs的" }, { "name": "italic", "data": [ { "name": "text", "data": "L" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "max" } ] }, { "name": "text", "data": "达到136 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "。此外，还通过使用混合了聚(N-乙烯基咔唑)的CDs作为发光层来制造CIE色坐标为(0.30,0.33)的WLEDs，最大亮度和电流效率达到约2 050 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "和1.1 cd·A" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4.3　传感" } ], "level": "2", "id": "s4c" } }, { "name": "p", "data": [ { "name": "text", "data": "CDs的传感应用包括pH传感" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "94", "type": "bibr", "rid": "R94", "data": [ { "name": "text", "data": "94" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "95", "type": "bibr", "rid": "R95", "data": [ { "name": "text", "data": "95" } ] } } ], "rid": [ "R94", "R95" ], "text": "94-95", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、金属离子检测和物质监测" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "96", "type": "bibr", "rid": "R96", "data": [ { "name": "text", "data": "96" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Wang等报道了使用新型的无标记CDs进行细胞内比例荧光pH传感(" }, { "name": "xref", "data": { "text": "图8(a)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(a)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "97", "type": "bibr", "rid": "R97", "data": [ { "name": "text", "data": "97" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，合成了在单波长激发下在475 nm和545 nm处显示双发射带的CDs。结果表明，在两次发射时合成的CDs的荧光强度同时对pH敏感。强度比(" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "475 nm" } ] }, { "name": "text", "data": "/" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207964&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207972&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207967&type=" } } } ] }, { "name": "text", "data": ")与缓冲溶液中5.2~8.8的pH值呈线性关系，具有作为细胞内pH传感的比例探针的功能。它还显示CDs在pH测量中显示出极好的可逆性和光稳定性。利用这种纳米探针，成功地将两种发射比率(" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "475 nm" } ] }, { "name": "text", "data": "/" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "545 nm" } ] }, { "name": "text", "data": ")用于细胞内pH的定量荧光成像技术在HeLa细胞中的应用。Yang课题组合成的CDs在低pH值下显示出较高的QYs(61.12%)及在强酸和强碱下的强度变化，可以很好地作为pH检测剂" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "98", "type": "bibr", "rid": "R98", "data": [ { "name": "text", "data": "98" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。当添加额外的NaOH时，发射峰会红移，发射峰可移至487 nm。由于Fe" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "与CDs的酚羟基之间特殊的配位相互作用，CDs的荧光被Fe" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "猝灭。同一小组通过简单的自组装方法制备了双发射量子点(QDs)/聚合物碳点(PCDs)组装的复合纳米颗粒" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "99", "type": "bibr", "rid": "R99", "data": [ { "name": "text", "data": "99" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，该复合材料对Hg" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "具有很高的灵敏度和选择性。随着Hg" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "浓度的增加，复合材料的发光颜色从粉红色变为紫色，最后变为蓝色。发光光谱法检测Hg" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "的检出限为10 nmol/L，肉眼观察为100 nmol/L。通过一步热解从葡萄糖酸锌合成了Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "钝化的CDs。受Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "和EDTA之间的络合反应的启发，基于CDs的去钝化和再钝化，构建了可逆的“关闭”荧光纳米传感器，用于检测EDTA和Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "，检出限低至3.2×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-7" } ] }, { "name": "text", "data": " mol/L和5.1×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-7" } ] }, { "name": "text", "data": " mol/L。所提出的基于CDs的纳米传感器已被进一步用于自来水中的EDTA和Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "监测，回收率极高(" }, { "name": "xref", "data": { "text": "图8(b)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(b)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "100", "type": "bibr", "rid": "R100", "data": [ { "name": "text", "data": "100" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F8", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图8" } ], "title": [ { "name": "text", "data": "(a)无标记CDs的制备及其在细胞内pH传感中的应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "97", "type": "bibr", "rid": "R97", "data": [ { "name": "text", "data": "97" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "钝化的CDs对EDTA和Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "的检测" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "100", "type": "bibr", "rid": "R100", "data": [ { "name": "text", "data": "100" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(c)基于CDs的油墨照片及其潜在应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "105", "type": "bibr", "rid": "R105", "data": [ { "name": "text", "data": "105" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(d)使用基于CDs的长期RTP/TADF的时间分辨的信息安全" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "113", "type": "bibr", "rid": "R113", "data": [ { "name": "text", "data": "113" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.8" } ], "title": [ { "name": "text", "data": "(a)Preparation of unlabeled CDs and their application in intracellular pH sensing" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "97", "type": "bibr", "rid": "R97", "data": [ { "name": "text", "data": "97" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Detection of EDTA and Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": " by Zn" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": " passivated CDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "100", "type": "bibr", "rid": "R100", "data": [ { "name": "text", "data": "100" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)Ink photos based on CDs and their potential applications" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "105", "type": "bibr", "rid": "R105", "data": [ { "name": "text", "data": "105" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (d)Time-resolved information security using long-term RTP/TADF based on CDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "113", "type": "bibr", "rid": "R113", "data": [ { "name": "text", "data": "113" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207977&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207990&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207983&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4.4　信息加密" } ], "level": "2", "id": "s4d" } }, { "name": "p", "data": [ { "name": "text", "data": "发光安全油墨的制造和设计策略在防伪应用中起着重要作用，其主要挑战在于制造具有高稳定性、高发光强度、低成本和在油墨介质中具有良好分散性的发光纳米材料。当前常用的发光材料集中在无机量子点和稀土元素掺杂的纳米材料上。CDs由于其独特的抗漂白能力、出色发光强度、低成本和低毒性而逐渐成为新一代的安全防伪油墨" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "101", "type": "bibr", "rid": "R101", "data": [ { "name": "text", "data": "101" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "103", "type": "bibr", "rid": "R103", "data": [ { "name": "text", "data": "103" } ] } } ], "rid": [ "R101", "R102", "R103" ], "text": "101-103", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。另外，CDs的表面富含亲水性官能团，例如羟基、羧基等，这种丰富的表面官能团使CDs具有良好的滤纸粘附性，因此可以通过喷墨印刷获得各种精细的图案(" }, { "name": "xref", "data": { "text": "图8(c)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(c)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "104", "type": "bibr", "rid": "R104", "data": [ { "name": "text", "data": "104" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "105", "type": "bibr", "rid": "R105", "data": [ { "name": "text", "data": "105" } ] } } ], "rid": [ "R104", "R105" ], "text": "104-105", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。通常，这些图案不能在日光下显示，需要特定的光源来照射以显示特定的图像。借助于CDs的荧光特性，它可以用作荧光防伪油墨。在CDs发展的早期，其防伪应用大多体现在CDs的荧光性质上，但是随着科技的发展，人们逐渐意识到荧光已经不能满足大家的需求。因此，基于磷光的防伪应用逐渐被开发，可以通过卤素原子掺杂、包覆等实现CDs的长余辉发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "106", "type": "bibr", "rid": "R106", "data": [ { "name": "text", "data": "106" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。利用激发依赖性的优点，可以将各种彩色光源用于照射和成像" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "107", "type": "bibr", "rid": "R107", "data": [ { "name": "text", "data": "107" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。最初，将CDs嵌入到各种基质(例如聚乙烯醇、滤纸和结晶Mn框架)中，以获得用于防伪的基于CDs的室温磷光(RTP)材料" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "108", "type": "bibr", "rid": "R108", "data": [ { "name": "text", "data": "108" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "110", "type": "bibr", "rid": "R110", "data": [ { "name": "text", "data": "110" } ] } } ], "rid": [ "R108", "R109", "R110" ], "text": "108-110", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Li等报道了一种通用方法来制备硼酸基质复合的多色RTP CDs，以进行防伪技术和信息加密，在复合材料中引入B可以减少单重态和三重态之间的能隙" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "111", "type": "bibr", "rid": "R111", "data": [ { "name": "text", "data": "111" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "；为了促进S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "之间的ISC，形成的玻璃态可以保护CDs的激发三重态免受非辐射失活。然而，通过附加基质的这种物理固定复合物中可逆相互作用的不稳定性限制了它们的实际应用。为了解决上述问题，Yang等设计了由聚丙烯酸和乙二胺制备的无金属 RTP CDs，并成功应用于防伪" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "112", "type": "bibr", "rid": "R112", "data": [ { "name": "text", "data": "112" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，从RTP和热活化延迟荧光的氧化也可以控制CDs在防伪和多层信息安全中的应用(" }, { "name": "xref", "data": { "text": "图8(d)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(d)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "113", "type": "bibr", "rid": "R113", "data": [ { "name": "text", "data": "113" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "5　结论与展望" } ], "level": "1", "id": "s5" } }, { "name": "p", "data": [ { "name": "text", "data": "自2004年首次报道以来，作为一种优异的荧光碳纳米材料，CDs得到了广泛的研究。十多年来，通过各种合成方法合成了大量的CDs，这些CDs在结构和性能特性上存在很大差异。本篇综述根据CDs的结构和性能特点，提出了CDs的新分类，包括GQDs、CQDs、CNDs和CPDs，这将有助于为CDs的本质提供启发。特别是，它揭示了CPDs作为一种新型CDs正在出现，具有独特的聚合物/碳杂化结构和性能。此外，根据先前的报道对CPDs形成过程的成核机理进行了讨论和分析。CDs结构的多样性导致模型的3个一般分类:内部因素主导发射、外部因素主导发射和CEE。尽管在理解CDs PL机制方面取得了巨大进展，但仍然存在重大挑战和研究空白。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(1)CDs的可控制备是要解决的关键问题。根据核-壳结构理论，通过调节碳化程度和聚合度以及CDs的表面，可以精确合成具有特定结构的CDs。这一挑战的重点是对反应过程的监控和对反应机理的解释。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(2)聚合物参数的确定以及合成后CDs的理化性质表征是CDs研究领域的主线。这些过程简述如下:通过实验和理论计算，表征了CDs的形态和大小、化学结构、元素组成、表面基团和其他性能，并建立了结构模型。结合上述特性，将研究结构-活性关系，这对于控制合成和PL机理尤为重要。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(3)为了确定发光中心和发光机理，光物理特性对于充分揭示更准确的PL机制至关重要。迄今为止，飞秒瞬态吸收、稳态瞬态PL测量，原位PL和高压下的吸收测量等广泛用于辅助机理分析。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(4)与荧光相比，磷光和上转换发光的研究较少，这对于扩大CDs在防伪和近红外(甚至是近红外区域Ⅱ)成像中的应用尤为重要。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(5)CDs的发光机理研究已经开展了大量工作，但是，涉及CDs的自组装以2D/3D形态存在的工作很少，在组装材料的荧光机理研究中几乎是空白。宏观粒子行为是奇妙的，值得进一步研究。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "在新近发展的手性和人体科学领域，将进一步研究CDs更广泛的应用。只有从结构的角度来看，才能精确地操纵CDs的制备，从而达到澄清PL机制和扩大CDs应用范围的双重目标。尽管上述艰苦的工作仍然长期存在，但如今CDs领域已经取得了巨大的进步，CDs的未来代表了基础研究和实际应用的良好愿景。" } ] }, { "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.20210155." } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献:" } ], "data": [ { "id": "R1", "label": "[1]", "citation": [ { "lang": "en", "text": [ { "name": "text", "data": "XU X Y" }, { "name": "text", "data": ", " }, { "name": "text", 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