Temperature-gradient method for gaining insights into the luminescence origin and formation mechanism of carbon dots  

利用温度梯度法探究碳点的发光起源和形成机制

作　　者：Yan-Ting Yang Yue-Xing Zhang You Cheng Xin-Ru Xu Jing Han Zi-Xin Chen Hang-Xing Wang 杨艳婷;张跃兴;程有;许鑫茹;韩晶;陈子欣;汪航行(College of Chemistry and Chemical Engineering,Key Laboratory for the Synthesis and Application of Organic Functional Molecules(MOE),Hubei University,Wuhan 430062,China;Shandong Universities Engineering Research Center of Integrated Circuits Functional Materials and Expanded Applications,Dezhou University,Dezhou 253023,China)

机构地区：[1]College of Chemistry and Chemical Engineering,Key Laboratory for the Synthesis and Application of Organic Functional Molecules(MOE),Hubei University,Wuhan 430062,China [2]Shandong Universities Engineering Research Center of Integrated Circuits Functional Materials and Expanded Applications,Dezhou University,Dezhou 253023,China

出　　处：《Science China Materials》2024年第10期3096-3105,共10页中国科学（材料科学）（英文版）

基　　金：supported by the National Natural Science Foundation of China(21875060 and 22076042).

摘　　要：Carbon dots(CDs)are a fascinating new class of fluorescent nanomaterials,yet the understanding of the fluorescent origin of CDs still lags well behind their applications.The key challenges for unveiling the fluorescent mechanism of CDs relate to the insufficient basis for structural evaluation.This work presents a temperature-gradient route to control the bottom-up approach of CDs,enabling the precise structural characterization of intermediates and the establishment of definite structure-property relationships,akin to the domino reaction synthesis of complex natural products from small organic molecules.Taking the binary components citric acid and meta-dimethylaminophenol generated CDs as a case study,their emissive mechanism,particularly the unique excitation-dependent fluorescence behavior,is reasonably explained and supported by structural evaluation through retrosynthetic analysis.The formation process of CDs is investigated using a combination of spectroscopic,thermal,and theoretical calculation techniques,demonstrating the significant potential of the temperature-gradient route in the exploration structure-property relationships and guiding the rational design of advanced CD applications.碳点(CDs)是一种新型荧光纳米材料,但人们对于CDs的荧光来源的理解相对滞后于其广泛的应用.揭示CDs发光机理的关键在于对其结构进行精确评估.本文利用温度梯度策略控制自下而上法CDs的形成过程,通过对反应中间体进行精确的结构表征,建立明确的化学结构-荧光性质关系,类似于利用多米诺反应将小有机分子转化成复杂的天然产物.本文以二元组分柠檬酸和间二甲氨基苯酚生成的红色荧光CDs为例,通过逆合成分析,结合光谱表征和热力学计算,对该CDs的双波长发射的荧光来源,尤其是独特的激发波长依赖性的荧光发射特性进行了充分地阐述.该研究表明,温度梯度策略在探索CDs的结构-性能关系方面潜力巨大,十分有利于指导特定功能CDs的合理设计.

关 键 词：carbon dots temperature gradient domino effect fluorescent origin solid-state emission 

分 类 号：TQ127.11[化学工程—无机化工] TB383.1[一般工业技术—材料科学与工程]