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碳点的羧基和羰基与铝共配位组装形成发射增强的聚集体,用于灵敏传感和高效去除。

Carboxyl and carbonyl groups of carbon dots co-coordinated assembly with Al to emission-enhanced aggregates for sensitive sensing and efficient removal.

作者信息

Qin Ziyi, Xu Jinju, Cao Yuanxin, Liao Chunhui, Shi Shuyun

机构信息

College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, Hunan, China.

Natural Product Research Laboratory, Guangxi Baise High-tech Development Zone, Baise 533612, Guangxi, China.

出版信息

Spectrochim Acta A Mol Biomol Spectrosc. 2025 Apr 5;330:125688. doi: 10.1016/j.saa.2024.125688. Epub 2024 Dec 30.

Abstract

It is very challenging to prepare carbon dots (CDs) with aggregation-induced emission (AIE) property for simultaneous sensitive sensing and efficient removal. Herein, blue-emission CDs were facilely prepared by one-step solvothermal treatment of vine tea. Optical characterizations demonstrated that AIE phenomenon of CDs came from the restricted intramolecular motion. Through selected chemical modifications for structure-property relationship analysis, carboxyl and carbonyl groups on CDs were demonstrated as co-coordination active sites to bind with Al for turn-on sensing process. Fluorescence enhancement of CDs by Al chelation could be attributed to synergistic mechanism of AIE and chelation-enhanced fluorescence. Thus, the prepared CDs has been used as a selective, sensitive, and effective fluorescent probe for fast Al sensing (response time, 5 min; linear range, 0.5-30.0 μM; limit of detection, 0.31 μM). More interestingly, high binding affinity between CDs and Al made them assembly into large aggregates via flocculation for Al removal (removal efficiency, 97.5 %) with extraordinary adsorption behavior (adsorption capacity, 1316 mg/g). Furthermore, the proposed CDs were successfully applied in detecting Al in real wastewater samples with acceptable recoveries (98.7-103.0 %) and superior precision (relative standard deviations, less than 3.82 %), and removing Al in spiked samples with satisfactory results. The work thus gives a demonstration of the potential fabrication of CDs with AIE property, and a better understanding of sensing and removal mechanisms for more rational design of CDs with application values.

摘要

制备具有聚集诱导发光(AIE)特性的碳点(CDs)以实现同时灵敏传感和高效去除是一项极具挑战性的任务。在此,通过对藤茶进行一步溶剂热法轻松制备了蓝色发光的CDs。光学表征表明,CDs的AIE现象源于分子内运动受限。通过进行选定的化学修饰以分析结构-性质关系,证实CDs上的羧基和羰基作为与铝结合的协同配位活性位点,用于开启传感过程。铝螯合导致CDs荧光增强可归因于AIE和螯合增强荧光的协同机制。因此,所制备的CDs已被用作一种选择性、灵敏且有效的荧光探针,用于快速检测铝(响应时间为5分钟;线性范围为0.5 - 30.0 μM;检测限为0.31 μM)。更有趣的是,CDs与铝之间的高结合亲和力使它们通过絮凝作用组装成大聚集体以去除铝(去除效率为97.5%),具有非凡的吸附行为(吸附容量为1316 mg/g)。此外,所提出的CDs成功应用于实际废水样品中铝的检测,回收率可接受(98.7 - 103.0%)且精密度优异(相对标准偏差小于3.82%),并在加标样品中去除铝,结果令人满意。这项工作因此展示了具有AIE特性的CDs的潜在制备方法,并更好地理解了传感和去除机制,以便更合理地设计具有应用价值的CDs。

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