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探索通过电化学剥离制备的石墨烯量子点的表面态和激基复合物主导的聚集诱导电化学发光。

Exploring Surface State and Exciplex Dominated Aggregation Induced Electrochemiluminescence of Graphene Quantum Dots Prepared via Electrochemical Exfoliation.

作者信息

Zhang Congyang, Cai Zhenzhong, Chu Kenneth, Shiu Wai-Tung, Hu Ping, Liu Lijia, Zhang Qiao, Ding Zhifeng

机构信息

Department of Chemistry, Western University, London, ON N6A 5B7, Canada.

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, 215123, China.

出版信息

Chemphyschem. 2025 Apr 1;26(7):e202401074. doi: 10.1002/cphc.202401074. Epub 2025 Feb 20.

Abstract

Graphene quantum dots (GQDs) have emerged as promising materials for electrochemiluminescence (ECL) applications due to their unique optical and electronic properties. In this study, GQDs were synthesized via electrochemical exfoliation of graphite in a constant current density mode, enabling scalable production with controlled size and surface functionalization. GQDs-4 and GQDs-20, synthesized at applied current densities of 4 mA/cm and 20 mA/cm to the graphite electrode, respectively, were investigated on roles of surface states and exciplex dominated aggregation-induced emission (AIE) in their ECL performance. GQDs-4 obtained an absolute ECL quantum efficiency of 0.0012 %±0.0002 %. GQDs-20, with a smaller particle size, achieved an absolute ECL quantum efficiency of 0.028±0.002 %, demonstrating high efficiency in converting electrons into photons. While GQDs-4 exhibited minor intensity in PL and ECL, they displayed a similar emission spectrum to GQDs-20 in the ECL process. This finding highlights the significant role of surface states and AIE in influencing the emission properties of GQDs, independent from core-state transitions. These results provide critical insights into the mechanisms governing GQD-based ECL and offer pathways for optimizing these materials for use in biosensing, optoelectronics, and imaging applications. Keywords: Electrochemiluminescence, Graphene Quantum Dots, Exciplex, Surface States, Multi-color Emission.

摘要

由于其独特的光学和电子特性,石墨烯量子点(GQDs)已成为电化学发光(ECL)应用中很有前景的材料。在本研究中,通过在恒流密度模式下对石墨进行电化学剥离来合成GQDs,从而实现具有可控尺寸和表面功能化的可扩展生产。分别在施加电流密度为4 mA/cm和20 mA/cm的条件下合成到石墨电极上的GQDs-4和GQDs-20,被研究了表面态和激基复合物主导的聚集诱导发光(AIE)在其ECL性能中的作用。GQDs-4获得的绝对ECL量子效率为0.0012%±0.0002%。粒径较小的GQDs-20实现了0.028±0.002%的绝对ECL量子效率,证明了在将电子转化为光子方面具有高效率。虽然GQDs-4在PL和ECL中表现出较小的强度,但它们在ECL过程中显示出与GQDs-20相似的发射光谱。这一发现突出了表面态和AIE在影响GQDs发射特性方面的重要作用,与核心态跃迁无关。这些结果为基于GQD的ECL的调控机制提供了关键见解,并为优化这些材料用于生物传感、光电子和成像应用提供了途径。关键词:电化学发光;石墨烯量子点;激基复合物;表面态;多色发射

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/248e/11963972/55a822d136f9/CPHC-26-e202401074-g002.jpg

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