Solid-state Luminescent Carbon Dots Resistant to Aggregation-induced Fluorescence Quenching: Preparation, Photophysical Properties and Applications Enhanced Publication

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "抗聚集诱导荧光猝灭的固态发光碳纳米点：制备、光物理性质及应用" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "Solid-state Luminescent Carbon Dots Resistant to Aggregation-induced Fluorescence Quenching: Preparation, Photophysical Properties and Applications" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "曲", "givenname": "彦霏", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "QU", "givenname": "Yan-fei", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" }, { "rid": "aff2", "text": "2" } ], "role": [ "first-author" ], "bio": [ { "lang": "zh", "text": [ "曲彦霏(1996-)，男，吉林白山人，硕士研究生，2018年于吉林大学获得学士学位，主要从事固态发光碳纳米点材料及应用方面的研究。E-mail: 846523613@qq.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207655&type=", "small": 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"graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207676&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207683&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207693&type=" } ], "data": [ [ { "name": "text", "data": "李迪" }, { "name": "text", "data": "(1984-)，女，辽宁营口人，博士，副教授，2012年于吉林大学获得博士学位，主要从事碳纳米点发光特性及应用方面的研究。E-mail:" }, { "name": "text", "data": "dili@jlu.edu.cn" } ] ] } ], "email": "dili@jlu.edu.cn", "deceased": false }, { "name": [ { "lang": "zh", "surname": "曲", "givenname": "松楠", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "QU", "givenname": "Song-nan", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff4", "text": "4" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor2", "lang": "en", "text": "artqusongnan@163.com", "data": [ { "name": "text", "data": "artqusongnan@163.com" } ] } ], "bio": [ { "lang": "zh", "text": [ "曲松楠(1981-)，男，吉林长春人，博士，教授，博士研究生导师，2009年于吉林大学获得博士学位，主要从事碳基发光材料及应用方面的研究。E-mail: artqusongnan@163.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207701&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207707&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207718&type=" } ], "data": [ [ { "name": "text", "data": "曲松楠" }, { "name": "text", "data": "(1981-)，男，吉林长春人，博士，教授，博士研究生导师，2009年于吉林大学获得博士学位，主要从事碳基发光材料及应用方面的研究。E-mail: " }, { "name": "text", "data": "artqusongnan@163.com" } ] ] } ], "email": "artqusongnan@163.com", "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "label": "1", "text": "中国科学院长春光学精密机械与物理研究所　发光学及应用国家重点实验室，吉林 　 长春 　 130033", "data": [ { "name": "text", "data": "中国科学院长春光学精密机械与物理研究所　发光学及应用国家重点实验室，吉林 　 长春 　 130033" } ] }, { "lang": "en", "label": "1", "text": "State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, China", "data": [ { "name": "text", "data": "State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, China" } ] } ] }, { "id": "aff2", "intro": [ { "lang": "zh", "label": "2", "text": "中国科学院大学，北京 　 100049", "data": [ { "name": "text", "data": "中国科学院大学，北京 　 100049" } ] }, { "lang": "en", "label": "2", "text": "University of Chinese Academy of Sciences, Beijing 100049, China", "data": [ { "name": "text", "data": "University of Chinese Academy of Sciences, Beijing 100049, China" } ] } ] }, { "id": "aff3", "intro": [ { "lang": "zh", "label": "3", "text": "吉林大学材料学与工程学院　汽车材料教育部重点实验室，吉林 　 长春 　 130012", "data": [ { "name": "text", "data": "吉林大学材料学与工程学院　汽车材料教育部重点实验室，吉林 　 长春 　 130012" } ] }, { "lang": "en", "label": "3", "text": "Key Laboratory of Automobile Materials, College of Materials Science and Engineering, Jilin University, Changchun 130012, China", "data": [ { "name": "text", "data": "Key Laboratory of Automobile Materials, College of Materials Science and Engineering, Jilin University, Changchun 130012, China" } ] } ] }, { "id": "aff4", "intro": [ { "lang": "zh", "label": "4", "text": "澳门大学应用物理与材料研究所　教育部联合重点实验室，中国 　 澳门 　 999078", "data": [ { "name": "text", "data": "澳门大学应用物理与材料研究所　教育部联合重点实验室，中国 　 澳门 　 999078" } ] }, { "lang": "en", "label": "4", "text": "Joint Key Laboratory of the Ministry of Education, Institute of Applied Physics and Materials Engineering, University of Macau, Macau 999078, China", "data": [ { "name": "text", "data": "Joint Key Laboratory of the Ministry of Education, Institute of Applied Physics and Materials Engineering, University of Macau, Macau 999078, China" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "碳点由于其低毒性、易制备、良好的光稳定性及可调的发光等特性有望成为一类理想的新型固态发光材料。然而，由于聚集诱导荧光猝灭(ACQ)效应的存在，使得碳点在固态发光领域的发展受到了限制，因此制备具有抗ACQ效应的固态发光碳点是碳点研究领域的一个重要方向。本文根据固态发光碳点研究的最新进展，从碳核、表面态调控、超分子及聚合物交联增强发光方面分类总结了具有抗ACQ效应固态发光碳点的制备方法及光物理性质，探讨了其实现固态发光的物理机制。此外，还介绍了该类碳点在固态发光领域的应用进展，并对固态发光碳点的发展现状和所面临的问题进行了讨论。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Because of their low toxicity, easy preparation, good photostability and color-tunable photoluminescence, carbon dots are expected to be a new kind of ideal solid-state photoluminescent materials. However, due to the aggregation-induced fluorescence quenching(ACQ) effect, the development of carbon dots in the field of solid-state photoluminescence is limited. Preparing solid-state emissive carbon dots featuring anti-ACQ ability is an important topic in the field of carbon dot research. On basis of the latest progress in the study of solid-state emissive carbon dots, this review summarizes the synthesis and photophysical properties of these carbon dots with anti-ACQ ability in terms of core/surface state controlling and supramolecular/polymer crosslink-enhanced emission, and discusses the physical mechanisms for the occurrence of the solid-state emission. Moreover, the application progress of these carbon dots in the field of solid-state photoluminescence is introduced, and the current situation and problems they faced are discussed." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "碳点" } ], [ { "name": "text", "data": "聚集诱导荧光猝灭" } ], [ { "name": "text", "data": "固态发光" } ], [ { "name": "text", "data": "发光二极管" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "carbon dots" } ], [ { "name": "text", "data": "aggregation-induced fluorescence quenching" } ], [ { "name": "text", "data": "solid-state luminescence" } ], [ { "name": "text", "data": "light emitting diode" } ] ] } ], "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": "自2004年Xu等" }, { "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": "首次发现带有荧光特性的碳纳米粒子以来，碳纳米点(碳点，CDs)就由于其低毒性、易制备、良好的光稳定性及可调的发光等特性受到了广泛的关注，在能源、催化、光电器件、生物医疗和信息加密等多个领域都有很好的应用前景。碳点通常被认为是粒径在10 nm以下，由具有类石墨烯堆积结构的碳核和表面的官能团(例如羟基、羰基、羧基和胺基等)组成。碳点的合成主要分为自上而下法和自下而上法。前者主要是利用物理方法对石墨、碳纳米管等材料进行刻蚀；而后者主要是用化学方法利用小分子化合物前体进行化学反应得到碳点，通常采用的方式有微波加热法、水热法、溶剂热法等" }, { "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": "5", "type": "bibr", "rid": "R5", "data": [ { "name": "text", "data": "5" } ] } } ], "rid": [ "R2", "R3", "R4", "R5" ], "text": "2-5", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。自下而上法是目前常用的碳点合成方法，相较于自上而下法，其表面具有更丰富的官能团，且可以通过控制前体化合物、溶剂、反应温度、时间、反应体系酸碱度等方式使生成的碳点结构发生变化，从而影响其物理化学性质。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "目前常用的发光材料有稀土材料、有机材料、无机半导体材料等。然而，稀土材料存在储量有限；有机发光材料制备复杂、光稳定性较差；高品质的半导体发光材料制备工艺较为苛刻；无机半导体量子点材料通常含有重金属元素(镉、铅)，存在潜在毒性问题。碳点原料来源广泛，制备方法简单，成本低，具有良好的生物相容性和环境相容性，有潜力开发为稳定、高效的新型发光材料。近些年随着研究的深入，碳点在溶液相中的荧光发射已经覆盖从紫外到整个可见光波段，乃至近红外波段" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "7", "type": "bibr", "rid": "R7", "data": [ { "name": "text", "data": "7" } ] } } ], "rid": [ "R6", "R7" ], "text": "6-7", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，且有很多发光连续可调的碳点的相关报道" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "8", "type": "bibr", "rid": "R8", "data": [ { "name": "text", "data": "8" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } } ], "rid": [ "R8", "R9", "R10" ], "text": "8-10", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，各波段发光的荧光量子效率(PLQY)也在不断提高(蓝光-绿光PLQY" }, { "name": "text", "data": ">" }, { "name": "text", "data": "90%；红光PLQY" }, { "name": "text", "data": ">" }, { "name": "text", "data": "60%；近红外PLQY" }, { "name": "text", "data": ">" }, { "name": "text", "data": "40%)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "12", "type": "bibr", "rid": "R12", "data": [ { "name": "text", "data": "12" } ] } } ], "rid": [ "R10", "R11", "R12" ], "text": "10-12", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。但是多数碳点在聚集态由于粒子间相互作用会产生能量转移、表面电子跃迁和碳核间π-π相互作用等非辐射跃迁方式，使得本身在溶液相中具有荧光特性的碳点在聚集态时发生荧光猝灭，这种现象被称为聚集诱导荧光猝灭效应(ACQ)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } } ], "rid": [ "R13", "R14" ], "text": "13-14", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。由于ACQ效应的存在，使得具有固态发光特性的碳点的研究相对缓慢，限制了碳点体系在固态发光方向的应用。目前常用的抑制ACQ效应的方法是将碳点分散至聚合物、无机盐、金属有机框架(MOF)材料等固态基质中" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "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" } ] } } ], "rid": [ "R15", "R16", "R17", "R18" ], "text": "15-18", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。例如，Qu课题组将碳点分别分散在淀粉、Ba" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "SO" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "、NaSiO" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "等基质中获得绿光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=515 nm)的碳点@淀粉、碳点@Ba" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "SO" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "复合荧光粉以及发光覆盖蓝光-红光区(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=448~638 nm)的系列碳点@NaSiO" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "复合荧光粉" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } } ], "rid": [ "R19", "R20", "R21" ], "text": "19-21", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";Wang等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "将碳点分散在Zn-MOF材料中获得了发光覆盖整个可见区的白光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=400~700 nm)的碳点@MOF复合物；Bhunia等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "将碳点掺杂入聚二甲基硅氧烷(PDMS)中制得了绿光(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=525 nm)、黄光(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=560 nm)和橙光(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=585 nm)发射的碳点@PDMS复合物。但是，这种方法存在碳点可能分布不均、重复性差、稳定性差、负载率低等问题。同时当碳点分散浓度小时，由于发光中心数量有限而降低了荧光发射强度；而当碳点浓度增大时，碳点粒子间距离减小，ACQ效应重新出现，会导致碳点的PLQY降低甚至完全猝灭。故而合成自身具有抗ACQ效应的固态发光碳点引起了研究者的广泛关注，并得到了快速发展。目前，研究人员通过改变碳点的组成、结构、表面性质或粒子间作用方式，可以获得发射波段从蓝光逐渐红移至绿光、黄光乃至于红光波段的一系列固态发光碳点。本综述立足于抗聚集诱导荧光猝灭的固态发光碳点，总结其制备方法及光物理性质，探究其发光机制和抗ACQ机理，并简述该类碳点在固态发光领域的应用进展。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　抗聚集诱导荧光猝灭碳纳米点的制备方法及光物理性质" } ], "level": "1", "id": "s2" } }, { "name": "p", "data": [ { "name": "text", "data": "碳点的结构和发光机理尚不清晰，目前广泛接受的研究结果表明碳点的发光主要来源于碳核发光和表面态发光；此外，调控碳点纳米粒子之间的组装、相互作用方式同样可以调控其发光特性。在研究碳点发光特性的同时，如何克服ACQ效应是制备固态荧光碳点要解决的另一个主要问题。已有的研究结果表明，碳点ACQ效应的产生主要是由于粒子在一定的距离内产生的能量传递或电子非辐射跃迁，为了抑制这两种物理过程，科研人员提出了多种解决方式，本文将碳点实现抗ACQ效应的手段归类为碳核调控、表面态调控、超分子交联增强和聚合物交联增强4个方面(" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": ")，并分别讨论其制备方法、光物理性质和聚集态发光机制。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "碳点的抗ACQ效应" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "Anti-ACQ effect of carbon dots" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207725&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207737&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207732&type=" } ] } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1　碳核调控" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "在碳核作为荧光发射主导的碳点中，sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "杂化域的存在直接与碳点的荧光特性相关联，但与此同时，大量sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "杂化域的存在也使得碳点在聚集态粒子间的π-π相互作用更强，电子非辐射跃迁导致碳点聚集态荧光猝灭。将大尺寸的sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "杂化域进行“分割”可以减弱/抑制π-π相互作用，从而阻止非辐射跃迁的产生。Li等" }, { "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": "用邻苯二甲酸氢钾、叠氮化钠和偏硼酸钾为原料，甲醛为溶剂进行微波加热反应得到了碳核为类金刚石结构固态发光碳点，其吸收峰位为232 nm和270 nm，两个吸收峰分别源自于碳核内C" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207744&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207762&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207752&type=" } } } ] }, { "name": "text", "data": "C键和芳香环的π-π" }, { "name": "sup", "data": [ { "name": "text", "data": "*" } ] }, { "name": "text", "data": "能级跃迁。其溶液态和固态的荧光发射峰位都在~413 nm，通过XPS和拉曼光谱表征证明了碳点中存在大量sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "结构，极大地削弱了π-π相互作用的影响，抑制ACQ效应。其固态的PLQY可以达到67.7%，相较于溶液相中的73%降低很少。Yoo等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "以柠檬酸尿素为原料，通过调控尿素与柠檬酸的质量比，经微波加热法分别合成了固态下的绿光发射碳点(u-CDs," }, { "name": "italic", "data": [ { "name": "text", "data": "m" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "柠檬酸" } ] }, { "name": "text", "data": "∶" }, { "name": "italic", "data": [ { "name": "text", "data": "m" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "尿素" } ] }, { "name": "text", "data": " =1∶8)和固态荧光猝灭碳点(c-CDs," }, { "name": "italic", "data": [ { "name": "text", "data": "m" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "柠檬酸" } ] }, { "name": "text", "data": "∶" }, { "name": "italic", "data": [ { "name": "text", "data": "m" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "尿素" } ] }, { "name": "text", "data": " =8∶1)。在固态下，u-CDs发射峰位于530 nm,PLQY为1.3%。当原料中尿素比例较大时，所合成的碳点碳核内sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "/sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "的比值较低，碳核结晶度较低，碳点内含氧和含氮基团的增加能够抑制sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "结构的生长，进而抑制ACQ效应。与此同时，通过减少反应时间的方式同样可以降低碳核内sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "/sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "的比值，使得原料中尿素比例较低时(" }, { "name": "italic", "data": [ { "name": "text", "data": "m" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "柠檬酸" } ] }, { "name": "text", "data": "∶" }, { "name": "italic", "data": [ { "name": "text", "data": "m" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "尿素" } ] }, { "name": "text", "data": " =8∶1)所合成的碳点实现固态荧光，进一步证明了sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "结构与ACQ效应的关联性。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "当碳点的发光来源于碳核时，碳核的共轭尺寸决定了吸收/发射峰位，一般情况下，随着碳核尺寸增大，碳点的吸收/发射峰位红移。在粒子尺寸分布较宽的碳点体系中，聚集态时不同粒径、不同发光带隙的粒子之间易发生能量转移，导致荧光猝灭，因此，合成尺寸均一的碳点有利于抑制ACQ效应。Zhou等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "以柠檬酸、尿素和氯化钙为原料，在水溶液中进行真空梯度加热反应，在140 ℃的条件下合成了具有450 nm蓝光发射的分子荧光团，当反应温度逐步升高到250 ℃时，分子荧光团碳化形成碳点，其发射波长红移至520 nm。其在溶液和固态时的PLQY为72%和65%。随着核磁共振碳谱sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "碳特征区间(1.427×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": "~1.252×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": ")特征峰的出现以及酰胺基和羰基特征峰(1.568×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": ",1.625×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": ")的减弱，对应于发射光谱中520 nm处发射强度增加而450 nm处发射强度的减弱，证明了绿光碳点的发光来源于碳核sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "结构。在真空膨化和原位烧结过程中，碳核生长受到限制，所制备的碳点粒径小而均一，避免了聚集态中碳点间的能量传递，抑制了ACQ效应。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "在碳点结构中引入杂原子，利用杂原子本身不同的电子排布方式对碳点的电子结构和能带进行调控是另一种抑制ACQ效应的有效策略。Niu等" }, { "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": "以苯三酚和硼酸为原料通过直接加热法制备了硼掺杂的红色荧光碳点，该碳点具有很宽的吸收和发射峰，强度最大的发射峰位于620 nm处。该碳点的发光中心实际上是分布于碳点中以硼为中心的结构，当硼掺杂含量从0.39%增加到4.71%时，其PLQY也对应地由5.63%增加到18.2%；但当碳点中硼含量继续增加时，其PLQY由于ACQ效应反而降低。Choi等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "以柠檬酸、乙二胺、硼酸为原料微波加热合成硼氮共掺杂碳点(BN-CDs)；作为对比，在相同条件下以柠檬酸和乙二胺为原料合成了氮掺杂碳点(N-CDs)。在水溶液中，350 nm激发下BN-CDs和N-CDs的发射峰都位于~450 nm,PLQY分别为80.8%和40.2%。在聚集态下，BN-CDs粉末PLQY为67.6%,N-CDs粉末PLQY仅为1%。N-CDs的吸收光谱在420 nm具有肩峰并伴有长波长区拖尾，同时发射峰位具有激发波长依赖特性。与N-CDs不同，BN-CDs在420 nm以后的长波长区无吸收，且荧光发射峰位不具有激发波长依赖性。由于N-CDs和BN-CDs具有几乎相同的尺寸分布，因此，N-CDs长波长区吸收和激发波长依赖特性来源于表面态。如" }, { "name": "xref", "data": { "text": "图2(a)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(a)" } ] } }, { "name": "text", "data": "，结构、组成、光谱分析以及理论计算证明了硼原子掺杂有利于BN-CDs碳核中石墨化结构的形成，使表面态更均一、表面缺陷更少，因此，BN-CDs比N-CDs具有更好的发光性能。Shen等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "29", "type": "bibr", "rid": "R29", "data": [ { "name": "text", "data": "29" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "以硼酸和乙二胺为原料通过水热反应制备了硼掺杂碳点。在水溶液中，碳点具有激发波长依赖的发光，最大发射波长为430 nm(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ex" } ] }, { "name": "text", "data": "= 340 nm),PLQY为22%。在固态下发光不猝灭，PLQY为18%。硼原子本身缺电子的特性可以抑制碳点表面电子给体和受体相互作用引起的分子间电荷转移；同时，碳点表面B—OH形成的氢键和表面负电荷(Zeta电位-25 mV)的斥力，可以有效地阻止发光中心的聚集。上述因素使碳点克服了ACQ效应，实现固态发光。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "(a)N-CD和BN-CD结构示意图" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)形成碳点和纯羟基表面态示意图" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(c)CD(上)和ox-CD(下)处于分散和聚集状态示意图，右侧的框显示了聚集态CD可能的能带结构和猝灭过程以及聚集态ox-CD的重组过程" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "(a)Structure of N-CD and BN-CD" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Schematic strategy proposed to form CDs and pure hydroxy surface states" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)CDs(up) and ox-CDs(down) in dispersed and aggregated states, frames on the right show possible band-energy structures and quenching processes of CDs in the aggregated state and recombination processes of ox-CDs in the aggregated state" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207770&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207783&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207777&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　表面态调控" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "由于碳点具有丰富的表面官能团或荧光分子，碳点表面物理化学特性聚集态中纳米粒子间的表面相互作用是影响其固态发光的重要因素。例如，相邻纳米粒子间表面能级的空间交叠可以引起新的表面态吸收和表面电子的非辐射跃迁" }, { "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": "，造成荧光猝灭。因此，通过调控碳点表面官能团性质及聚集态碳点相互作用等表面态调控方法，可以抑制ACQ效应。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "通过表面官能团的合理选择和后处理，获得表面化学环境均一的碳点可以抑制碳点聚集引起的新的表面态吸收及无辐射跃迁，提高碳点固态PLQY。Li等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "用聚乙烯醇(PVA)作为唯一原料，用氢氧化钠加速碳化和聚合反应，采用水热法制备了表面仅含有羟基的在固态下为黄绿色荧光发射的碳点。420 nm激发下发射峰位于540 nm且具有激发波长依赖性。反应流程如" }, { "name": "xref", "data": { "text": "图2(b)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(b)" } ] } }, { "name": "text", "data": ",PVA长链分子规则交联形成片状结构，片状结构之间再进一步相互反应形成相互交叉的环形碳点产物，由于其表面态所含官能团仅有羟基，避免了表面态之间不同基团形成电子给体受体，同时其独特的环形结构也相互支撑，增加了碳点之间的距离，两种因素共同使得其具有抗猝灭特性。Zhou等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "用柠檬酸和氨水通过微波加热制得在溶液中具有蓝光发射且固态荧光猝灭的碳点(CDs)，将该碳点用双氧水进行处理，得到了溶液中具有蓝光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=435 nm,PL QY 17%)的碳点(ox-CDs)。ox-CDs固态下具有无激发波长依赖的发光特性，发射峰位在525 nm和450 nm激发下PLQY为25%。双氧水处理没有明显改变碳点的尺寸，而是使碳点的表面发生氧化:使表面电荷分布更均匀(给电子官能团(N—H)减少，吸电子官能团(C" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207791&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207804&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207797&type=" } } } ] }, { "name": "text", "data": "O/COO,Pyridinic N)增加，同时获得宽带隙的表面能级结构。碳点吸收光谱的变化可以证明这个结论。CDs溶液中，表面态吸收峰位于长波长区(450 nm肩峰及长波长拖尾)，在聚集态下，相邻碳点表面态能级的空间交叠形成窄带隙，进而在长波长区形成宽吸收和无辐射跃迁通道，造成固态荧光猝灭。氧化处理后，ox-CDs表面带隙展宽，溶液吸收光谱中氧化官能团吸收峰(300 nm前短波长区)明显增强，450 nm以后的吸收明显减弱，聚集态下，相邻碳点表面能级交叠形成宽的吸收带隙，激发态电子通过辐射跃迁去活，实现ox-CDs固态发光(" }, { "name": "xref", "data": { "text": "图2(c)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(c)" } ] } }, { "name": "text", "data": ")。Tao等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "以柠檬酸三钠和二硫脲为原料用水热法合成了碳点，在溶液相中发射峰位为440 nm(激发波长350 nm),PLQY为7.6%；在固态下发射峰位为495 nm(激发波长420 nm),PLQY为29.2%。碳点在溶液中非浓度依赖的激发和发射光谱以及单指数衰减的荧光寿命证明了其单一的发光中心。在固态下，碳点激发和发射峰位明显红移，且荧光寿命呈双指数衰减，表明聚集态中表面官能团相互作用可能引起碳点组装，表面态交叠形成新的发光中心；同时，通过与表面无Na" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "的碳点对比，Na" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "修饰可以在碳点表面形成大量的羧酸钠官能团，抑制π-π堆积从而有利于碳点的固态发光。Zhao等" }, { "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": "利用氯化铝、柠檬酸和尿素通过微波加热反应制得了PLQY高达72.7%的固态绿色发射碳点(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=550 nm)，铝离子由于与酰胺具有较强的配位能力而在碳点表面形成交联聚合物，其空间位阻效应有效地阻止了碳点聚集导致的ACQ效应。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "通常情况下，荧光分子相互靠近会产生ACQ效应，而与之相反，Tang等" }, { "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": "于2001年报道了在稀溶液中没有荧光发射、而在聚集态具有荧光特性的有机分子。这类分子一般具有可旋转的单键，聚集态下使分子内运动(例如振动和转动)受限，降低分子内运动造成的无辐射跃迁，表现出荧光增强的现象，这种荧光特性被称之为聚集诱导发光(AIE)。Yang等" }, { "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": "根据AIE分子的结构特性制备了具有AIE特性的碳点。如" }, { "name": "xref", "data": { "text": "图3(a)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(a)" } ] } }, { "name": "text", "data": "，三聚氰胺与二硫代水杨酸在乙酸中经溶剂热反应生成表面具有可旋转的二硫单键的碳点。当分散在溶液中时，碳点展现出来自碳核的蓝光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ex" } ] }, { "name": "text", "data": "=315 nm," }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=467 nm)，由于表面对称的杂环结构可围绕二硫键旋转消耗了吸收的光能，使得表面态发光猝灭。在聚集态下，碳点形成J-聚集体，其碳核的蓝光由于π-π堆积而猝灭；同时表面二硫键的分子内旋转受到抑制，碳点展现出来自表面态的红光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ex" } ] }, { "name": "text", "data": "=559 nm," }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=621 nm)。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "(a)碳点的核和表面的发光原理和推测的结构(发光边缘的颜色表示其荧光的颜色)" }, { "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": "；不同浓度下碳点的荧光光谱(b)和CIE坐标(c)" }, { "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": " ;(d)聚合物碳点示意图及其具有发光颜色一致性的固态发光机理" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "(a)Fluorescence principle and proposed structure of CD's core and surface(the colors of glowing edges represent the color of their fluorescence)" }, { "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": ". Fluorescence spectra(b) and CIE color coordinates(c) of the CDs at different concentrations" }, { "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": " . (d)Schematic illustration of polymer carbon dot and its mechanism for solid-state luminescence with the emission color consistency" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207813&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207825&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207818&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.3　超分子交联增强固态发光" } ], "level": "2", "id": "s2c" } }, { "name": "p", "data": [ { "name": "text", "data": "碳点丰富的表面官能团可以实现多种超分子相互作用，包括氢键、静电相互作用等。在聚集态碳点中，纳米粒子之间的超分子相互作用可以影响纳米粒子的堆积结构及聚集体的能级和电子分布，进而调控碳点的固态发光性能。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "Meng等" }, { "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": "通过碳酸胍和磷酸二氢钾在二氯甲烷中溶剂热反应制备了在水溶液中具有蓝光发射的碳点。该碳点溶液的荧光发射具有浓度依赖特性，如" }, { "name": "xref", "data": { "text": "图3(b)~(c)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(b)~(c)" } ] } }, { "name": "text", "data": "，从稀溶液到固态，碳点的发光峰位从450 nm红移到550 nm,PLQY从21.9%降低到11%。碳点的固体粉末具有极宽的发射峰，覆盖整个可见区(400~750 nm，半峰宽200 nm)，呈暖白光发射(色坐标:0.48,0.43)。红外和核磁共振氢谱证明碳点表面的羰基和氨基在聚集过程中形成氢键，进而诱导碳点形成大尺寸的固态聚集体并产生暖白光发射。Feng等" }, { "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": "以对氨基水杨酸和柠檬酸为原料进行水热反应，通过调控反应溶液的pH分别合成了溶液中具有蓝光(pH=2.1)和黄绿光(pH=1.0)发射的碳点。在固态下，两种碳点发光红移，分别具有黄光和橙红光发射，PLQY分别为1.04%和0.42%。作者推测在固态下，碳点通过超分子相互作用(氢键、静电相互作用及部分π-π相互作用)形成密堆积结构，诱发原本在溶液中由于振动或转动能量损耗而猝灭的窄带隙发光团在聚集态下发光，从而实现超分子交联增强的窄带隙固态发光。Meng等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "39", "type": "bibr", "rid": "R39", "data": [ { "name": "text", "data": "39" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "以对苯二乙腈和对苯二甲醛为原料，用溶剂热法通过控制反应条件合成了聚集态下具有蓝光(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=474 nm)、绿光(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=530 nm)和红光(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=630 nm)发射的碳量子环，其PLQY分别为38%、46%和30%。随着碳化程度的提高，碳量子环尺寸增大，其发光峰位从蓝光红移至红光区。带状π-共轭片层边缘—CN基团间的斥力诱导环状结构的形成，进而有效抑制了聚集态下π-π相互作用，实现高效固态发光。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.4　聚合物交联增强固态发光" } ], "level": "2", "id": "s2d" } }, { "name": "p", "data": [ { "name": "text", "data": "Yang课题组" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "40", "type": "bibr", "rid": "R40", "data": [ { "name": "text", "data": "40" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "44", "type": "bibr", "rid": "R44", "data": [ { "name": "text", "data": "44" } ] } } ], "rid": [ "R40", "R41", "R42", "R43", "R44" ], "text": "40-44", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "制备了系列聚合物碳点并提出了聚合物交联增强发射实现碳点固态发光的方法。在碳点制备过程中，原料通过脱水缩合、交联及碳化过程形成聚合物网络结构，这些聚合物骨架可以作为一种“基质”分散碳点内部及表面的发光中心(碳核内的sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "结构、表面的官能团或分子态生色团)，从而避免ACQ效应，实现高效固态发光。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "Kwak等" }, { "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": "将柠檬酸和二亚乙基三胺(DETA)溶解在水中低温(70 ℃)加热形成了具有交联聚合物骨架结构的碳点。如" }, { "name": "xref", "data": { "text": "图3(d)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(d)" } ] } }, { "name": "text", "data": "，该碳点具有单一的分子态荧光发射中心，其溶液和固态的发射峰位一致，均为434 nm,PLQY分别为68.2%和62.7%，其单一的发光中心分散于形成碳点骨架的聚合物网络结构中，既避免了ACQ效应，又抑制了聚集态中不同发光中心的共振能量转移带来的固态发射红移。Shao等" }, { "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": "用马来酸和乙二胺通过微波加热经脱水缩合、交联、聚合及部分碳化形成具有聚合物网络结构的碳点。该碳点具有浓度依赖的发光特性，稀溶液发射波长为460 nm,PLQY为18.9%，随着浓度的增大溶液发射波长逐渐红移，PLQY逐渐降低，在固态下具有红光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=625 nm),PLQY为8.5%。该碳点的发光并非来自于π-π共轭结构，而是一些非共轭的特殊官能团，固态下，聚合物网络结构阻止发光中心的聚集，同时非共轭的发光团避免了π-π，进而抑制了ACQ效应。Liu等" }, { "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": "以柠檬酸和支链聚乙烯亚胺(b-PEI)为原料通过水热反应制得了固态下绿光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=510 nm)的碳点，450 nm激发下PLQY为26%。b-PEI作为氮源和表面钝化剂的同时，聚集态下其骨架和支链结构可以分离并固定发光中心，抑制表面电子跃迁和共轭内核的π-π相互作用。Chen等" }, { "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": "首先以PVA作为碳源。EDA作为氮源，通过水热法合成了固态下具有绿光发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "em" } ] }, { "name": "text", "data": "=525 nm)的碳点，PLQY为35%；并用不同含氮化合物作为氮源制备了具有不同发光特性的氮掺杂固态发光碳点，碳点氮含量的不同使得其发射波长不同，而表面的PVA长链结构阻止了发光中心的直接接触，从而抑制了ACQ效应。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "综上所述，碳点的发光主要来源于碳核和表面态的共同作用，碳核的石墨化结构和表面基团不同导致的能级结构不同使得碳点具有不同的光学性质" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "49", "type": "bibr", "rid": "R49", "data": [ { "name": "text", "data": "49" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。而与之相对应，固态发光碳点抑制ACQ效应的手段也包括对碳点碳核和表面态结构的调控，通过控制碳核sp" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "结构的尺寸与比例、调节表面态能级和减少表面缺陷态等方式实现碳点的固态发光。此外，通过超分子相互作用和聚合物交联分隔碳点或碳点内部发光中心也可以达到抗ACQ效应的目的。" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "总结了上文介绍的固态发光碳点的合成原料、固态下的光物理性质和抑制ACQ效应的机理。多种多样的抗ACQ效应策略也可以为今后合成固态发光碳点所借鉴，从而使得固态发光碳点领域的成果更加丰富多样。" } ] }, { "name": "table", "data": { "id": "T1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表1" } ], "title": [ { "name": "text", "data": "固态发光碳点原料、固态时的光学性质和抑制ACQ效应机理" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab.1" } ], "title": [ { "name": "text", "data": "Raw materials, optical properties in solid state and mechanisms of anti-ACQ effect of solid-state emissive carbon dots" } ] } ], "note": [], "table": [ { "head": [ [ { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "反应物" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "发光峰位/nm　(固态)　" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "荧光量子效率/%(固态)" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "抑制荧光猝灭机理　" } ] } ] ], "body": [ [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "邻苯二甲酸氢钾/叠氮化钠/偏硼酸钾" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "413" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { 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"name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "硼酸/乙二胺" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "430" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "18" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "硼掺杂抑制电荷转移" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "29", "type": "bibr", "rid": "R29", "data": [ { "name": "text", "data": "29" } ] } }, { "name": "text", "data": "]" } ] } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "PVA" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "540" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "—" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "表面态单一及独特支撑结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } }, { "name": "text", "data": "]" } ] } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "柠檬酸/氨水" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "525" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "25" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "氧化表面结构改变表面能级" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", 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"data": "3　固态发光碳点的应用" } ], "level": "1", "id": "s3" } }, { "name": "p", "data": [ { "name": "text", "data": "碳点在克服了ACQ效应后拓宽了其在固态发光领域的应用范围，包括照明、光通讯及信息加密等。而相较于通过基质掺杂获得的固态荧光碳点体系，具有自身抗猝灭特性的固态荧光碳点性质更加稳定，发光更加均匀，排除了掺杂比例因素的影响，可重复性更强。以下将对已报道的该类碳点的应用进行总结。" } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1　固态发光器件" } ], "level": "2", "id": "s3a" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1.1　发光二极管" } ], "level": "3", "id": "s3a1" } }, { "name": "p", "data": [ { "name": "text", "data": "作为新型发光材料，固态发光碳点可以作为转光层应用于光致发光器件。将碳点覆盖至不同发光的LED芯片上制得各色的LED器件不止需要碳点具备合适的激发及发射波长，还要求碳点具有良好的光稳定性和热稳定性。所制得的LED器件性能通常通过相关色温(CCT)、色度图(CIE)、显色指数(RA)和发光效率来衡量。目前碳点作为转光层制备LED器件一方面可以与其他的发光材料混合，配合碳点本身发光和LED芯片的激发光制得具有较高显色指数的白光LED(WLED)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "50", "type": "bibr", "rid": "R50", "data": [ { "name": "text", "data": "50" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "51", "type": "bibr", "rid": "R51", "data": [ { "name": "text", "data": "51" } ] } } ], "rid": [ "R50", "R51" ], "text": "50-51", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "；另一方面可以利用其发光可调性质，覆盖在LED芯片上制得多种颜色的LED发光器件" }, { "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": "。Zhu等" }, { "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": "将颜色梯度变化的固态荧光碳点(" }, { "name": "xref", "data": { "text": "图4(a)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(a)" } ] } }, { "name": "text", "data": ")作为转光层涂敷在460 nm芯片上制备了从冷白至暖白的一系列LED发光器件(" }, { "name": "xref", "data": { "text": "图4(b)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(b)" } ] } }, { "name": "text", "data": "),CIE坐标由(0.285,0.286)变化为(0.453,0.412)(" }, { "name": "xref", "data": { "text": "图4(c)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(c)" } ] } }, { "name": "text", "data": ")，色温从9 579 K变化至2 752 K，发光效率19~51 lm·W" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，在连续工作40 h后其发光仍几乎没有变化，碳点荧光粉在器件中具有良好的稳定性。Kwak等" }, { "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": "以柠檬酸和DETA为原料，用加热法和溶剂热法合成了荧光非浓度依赖的碳点(PCD)，在溶液相和固态时PCD的发射峰为434 nm，溶液相中PLQY为68.2%，固态时为62.7%，且发光不具有激发波长依赖性。由于PCD具有抗ACQ特性，将其掺杂入PVA中覆盖于LED发光芯片表面时，随着在PVA中掺杂的PCD比例增大，如" }, { "name": "xref", "data": { "text": "图4(d)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(d)" } ] } }, { "name": "text", "data": "，所制得的LED亮度也会增加，其中PCD的CIE坐标由(0.166,0.121)变化至(0.260,0.354)，发光效率随碳点掺杂量的增加从3.11 lm·W" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "增加至12.78 lm·W" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "。Meng等" }, { "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": "制备的碳点由于在固态时具有良好的白光发光特性，故而可将其直接覆盖在紫外LED芯片上获得白光LED器件。" }, { "name": "xref", "data": { "text": "图4(e)、(f)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(e)、(f)" } ] } }, { "name": "text", "data": "分别展示了器件的实物图和发光谱图，其CIE坐标位于(0.42,0.38)，色温为3 032 K，属于暖白光，显色指数91。" }, { "name": "xref", "data": { "text": "图4(g)、(h)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(g)、(h)" } ] } }, { "name": "text", "data": "分别为用商用LED和碳点LED照射水果的照片，相较于商用LED(CRI约为85)，碳点LED更能真实地反映出水果的实际颜色，且当施加电流从20 mA增加至120 mA时，碳点LED的CCT和CRI数值变化很小，表现出良好的稳定性。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "(a)基于CD的6个WLED发射光谱；(b)具有可调CCT(从冷白光到暖白光)的6个WLED照片；(c)6个WLED的CIE色度图" }, { "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": ";(d)具有不同PCD负载量的LED照片(左)和CIE色度图(右)" }, { "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": ";(e)基于碳点的暖光WLED照片；(f)碳点LED荧光光谱；在商用暖白光LED(g)和基于碳点的暖白光LED(h)照射下的水果颜色照片" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "(a)Emission spectra of the CD-based six WLEDs. (b)Photographs of six WLEDs with adjustable CCTs(from cold white to warm white light). (c)CIE chromaticity diagram of the six WLEDs presented in (a)" }, { "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": ". (d)Photographs(left) and color gamut(right) of LED fabricated using PCD with different loading fractions" }, { "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": ". (e)Photograph of the warm WLED using CDs as phosphor. (f)Emission spectrum of the LED. Fruit colors under the commercial warm WLED lamp(g) and under the CD-based warm WLED lamp(h)" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207844&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207856&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207849&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "电致发光二极管经过快速的发展目前正逐步代替液晶显示器并可用作照明或者背光源。碳点可作为发光层应用于电致发光器件" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "54", "type": "bibr", "rid": "R54", "data": [ { "name": "text", "data": "54" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "56", "type": "bibr", "rid": "R56", "data": [ { "name": "text", "data": "56" } ] } } ], "rid": [ "R54", "R55", "R56" ], "text": "54-56", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。由于ACQ效应，通常将碳点掺杂在主体材料中制备发光层，以非掺杂碳点作为发光层的电致发光器件性能较差" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "57", "type": "bibr", "rid": "R57", "data": [ { "name": "text", "data": "57" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } } ], "rid": [ "R57", "R58", "R59" ], "text": "57-59", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如" }, { "name": "xref", "data": { "text": "图5(c)~(h)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(c)~(h)" } ] } }, { "name": "text", "data": ",Yuan等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "以柠檬酸和不同二氨基萘为原料，通过控制反应时间和原料结构合成了系列蓝光-红光(430~604 nm)发射碳点(MCBF-CQDs)，其溶液PLQY随着波长增大由75%降低至12%。以聚(3,4-乙撑二氧吩噻)∶聚苯乙烯磺酸盐(PEDOT∶PSS)为空穴注入层、MCBF-CQDs为发光层、1,3,5-三(N-苯基苯并咪唑-2-基)苯(TPBI)为电子传输层(ETL)构筑器件，实现了非掺杂碳点的电致发光(EL)，发射峰位为455~628 nm，与相应碳点薄膜的发光峰位一致。器件最大亮度为136 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "(蓝光碳点器件)。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "(a)小信号频率响应和数据传输测量示意图；(b)使用蓝色激光二极管(峰值为442 nm)和ox-CDs荧光粉产生的白光光谱，插图:将ox-CD掺入环氧树脂并产生白光(右)的照片" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(c)器件结构包括ITO/PEDOT∶PSS(阳极)、MCBF-CQDs(发射层)、TPBi(ETL)和Ca/Al(阴极)；蓝光发射碳点(d)、绿光发射碳点(e)、黄光发射碳点(f)、橙光发射碳点(g)和红光发射碳点(h)薄膜的归一化PL光谱和相应的EL光谱，(d)~(h)插图中的照片显示了单色LED的蓝光、绿光、黄光、橙光和红光发射的特写视图" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.5" } ], "title": [ { "name": "text", "data": "(a)Schematic diagram of the small-signal frequency-response and data transmission measurements. (b)Spectrum of the white light generated using blue laser diode(spike at 442 nm) and ox-CDs phosphor. Inset: photograph of plate that dope ox-CDs into the epoxy resin(left), and generated white light(right)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)Device structure comprising ITO/PEDOT∶PSS (anode), MCBF-CQDs(active emission layer), TPBi(ETL), and Ca/Al(cathode). The normalized PL spectra and the corresponding output EL spectra of the thin films of blue luminescent carbon dots(d), green luminescent carbon dots(e), yellow luminescent carbon dots(f), orange luminescent carbon dots(g), and red luminescent carbon dots(h). The photographs in the insets of (d)-(h) display the close-up view of the surface emission from blue, green, yellow, orange, and red emission of monochrome LEDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207863&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207877&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207869&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1.2　可见光通讯" } ], "level": "3", "id": "s3a2" } }, { "name": "p", "data": [ { "name": "text", "data": "可见光通讯(VLC)是快速无线数据通讯领域新兴的一项技术。目前快速无线数据通讯领域常用的宽带射频(RF)和微波通信技术的发展受到带宽和频谱拥塞效应的限制，而VLC具有不受限制的通信频谱，且能源效率更高，安全性更强，具有很好的发展潜力" }, { "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": "62", "type": "bibr", "rid": "R62", "data": [ { "name": "text", "data": "62" } ] } } ], "rid": [ "R61", "R62" ], "text": "61-62", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。目前常用在VLC中的白光LED(WLED)主要使用稀土材料，其长荧光寿命使得其制得的WLED带宽被限制在几个MHz内，碳点的荧光寿命较短，可用于制备适合VLC使用的WLED，实现高调制带宽和高数据传输速率。Zhou等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "用" }, { "name": "xref", "data": { "text": "图5(a)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(a)" } ] } }, { "name": "text", "data": "所示装置对固态绿光发射碳点ox-CDs进行了信号频率响应测试。低功率450 nm蓝色激光二极管(34.5 mA)发射的蓝光经发射镜准直后激发ox-CDs产生如" }, { "name": "xref", "data": { "text": "图5(b)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(b)" } ] } }, { "name": "text", "data": "所示蓝绿混合的白光，白光经滤光片滤去蓝光后由接收镜汇聚，其光信号由雪崩式光电二极管(APD)转换为电信号收集。测得所得白光CIE坐标为(0.34,0.37)，色温为5 240 K。滤光片前后白光和绿光的带宽分别为285 MHz和120 MHz，传输速率435 Mbps。基于该碳点制得的VLC其光电转换的数据传输误码率(BER)在350 Mbps下只有3.6×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "，在425 Mbps仅有3.3×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "，远低于无错误操作所需的前向纠错阈值(FEC)。Liu等" }, { "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": "用所制得的绿光发射碳点进行信号频率响应测试，得到传输带宽为55 MHz，最大传输速率为181 Mbps，证明了固态荧光碳点在VLC领域的应用前景。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2　信息加密" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "信息加密技术要求物质在不同的环境条件下表现出不同的特性，该特性变化应易于被观察，如形态变化、颜色变化、发光性质变化等，同时要兼具稳定性保证信息在传递过程中不会丢失。碳点的发光特性随物理、化学环境(温度、湿度、pH、极性等)、激发波长等因素而变化，可在外界条件变化的情况下表现出不同的发光特性；其中，具有磷光和延迟荧光发射的碳点可在照射后保持长余辉特性，在信息加密领域具有很好的应用潜力。Yang等" }, { "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": "制备的具有AIE效应的固态发光碳点在分散态下用365 nm紫外光激发为蓝色荧光。254 nm紫外激发无荧光，而由于其疏水性，碳点在水中聚集，该状态下254 nm激发显红色荧光。基于这种发光特征可设计如" }, { "name": "xref", "data": { "text": "图6(b)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(b)" } ] } }, { "name": "text", "data": "的信息双重加密方式。首先准备“SCAUSCNU”样式的滤纸字母串，使用碳点处理字母“SC”、“US”和“NU”，待碳点干燥后再分别将三组字母中的“C”、“S”和“U”用蜡密封；将该字母串置于365 nm紫外光照射下只会呈现无意义的字符串，而在254 nm紫外光照下字符串干燥时同样无法观察到信息，只有将字符串经过水处理后用254 nm紫外光照射才能得到正确的“SUN”密码。除了在不同条件下具有不同荧光特性的碳点，具有磷光长余辉特性的碳点同样是很好的制作信息加密的材料。Tao等" }, { "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": "分别利用乙二胺和乙醇胺与聚丙烯酸水热反应制得了两种室温下具有不同波长固态磷光发射的碳点PCD" }, { "name": "sub", "data": [ { "name": "text", "data": "SI-1" } ] }, { "name": "text", "data": "和PCD" }, { "name": "sub", "data": [ { "name": "text", "data": "SI-2" } ] }, { "name": "text", "data": "，利用两种碳点进行了如" }, { "name": "xref", "data": { "text": "图6(a)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(a)" } ] } }, { "name": "text", "data": "的信息加密应用展示。在365 nm紫外照射下两种碳点与其他荧光物质(荧光涂料和其他固态荧光碳点)共同显示蝴蝶和“Just Love U”图案，而当关闭紫外灯后则会展示变化的蝴蝶图案和“JLU”图案。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "(a)图形安全和信息加密照片" }, { "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": ";(b)将HMP用作双重加密徽章" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "(a)Photographs of graphic security and information encryption" }, { "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": ". (b)HMP utilized as a dual-encryption badge" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207882&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207897&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21207889&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "指纹作为刑事案件中重要的证据和线索，其检测和提取对于案件的取证和侦破都起着极为重要的作用。指纹显影要求所用的荧光物质在各种表面都可以均匀分散，且能够准确反映出指纹的各种细节。碳点由于其在固态一般呈粉末状、毒性低易制取、且一般可被紫外光激发等优点在指纹显影和采集领域具有应用潜力" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "64", "type": "bibr", "rid": "R64", "data": [ { "name": "text", "data": "64" } ] } } ], "rid": [ "R63", "R64" ], "text": "63-64", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Niu等" }, { "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": "制备的红光碳点可由紫外光激发，分别将该碳点撒在具有指纹的玻璃、金属箔和塑料表面对指纹进行显影，可以清晰地显示出指纹的交叉、岛、分叉、核心、疤痕等细节；并且在紫外光照射1 h后其荧光发射仍不会衰减，证明其具有很好的稳定性，展示了其在指纹显影领域的应用潜力。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4　总结与展望" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "本文针对碳点聚集态荧光猝灭现象，总结了具有抗ACQ效应固态发光碳点的制备方法、光物理性质及其在固态发光领域的应用，并探讨了碳点实现固态发光的物理机制。已有的研究进展通过碳核、表面态调控，超分子、聚合物交联增强等方法实现了碳点从蓝光至红光区的高效固态发光，证明了固态发光碳点在发光器件、信息加密等领域的应用潜力。目前，抗ACQ效应的固态发光碳点研究仍处于起步阶段，为成为理想的固态发光材料，该类碳点在研究中仍有很多问题有待解决:(1)碳点的结构和内在发光机理仍需要深入探索，了解其结构与发光性质的内在联系，得出普适性的碳点发光机理以实现碳点的可控合成；(2)对导致碳点产生ACQ现象的结构特点和物理机制仍需要更深入明确的认识，以此为基础探索更多抗ACQ效应方法，丰富固态发光碳点材料体系并调控其发光性质；(3)与稀土、量子点等固态发光材料相比，碳点的物理化学性质仍需要进一步优化，通过将碳点与手性光学" }, { "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": "、聚集诱导发光等领域相结合，将碳点的物理化学性质进一步优化，丰富碳点的发光特性，以期获得具有实际应用价值的高性能碳点固态发光材料，突破碳点在现有应用(例如高品质光致/电致发光器件)中的不足，使其在医学、催化和能源等方向具有更大的应用空间。" } ] }, { "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.20210174." } ] } ] } ], "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", "data": "RAY R" }, { "name": "text", "data": ", " }, { "name": "text", "data": "GU Y L" }, { "name": "text", "data": ", " }, { "name": "text", "data": "et al" }, { "name": "text", "data": ". 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