氧化石墨烯铽配合物电致化学发光体合成及四环素的灵敏检测  

Synthesis of Graphene Oxide Terbium Complex Electrochemiluminescence Material and Sensitive Detection of Tetracycline

作　　者：杨延梅[1] 冉雨晴 王存 YANG Yanmei;RAN Yuqing;WANG Cun*(Hehai College,Chongqing Jiaotong University,Chongqing 400074,China;College of Biological and Chemical Engineering,Chongqing University of Education,Chongqing 400067,China)

机构地区：[1]重庆交通大学河海学院,重庆400074 [2]重庆第二师范学院生物与化学工程学院,重庆400067

出　　处：《高等学校化学学报》2025年第3期34-43,共10页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金青年项目(批准号:22204010);重庆市自然科学基金(批准号:CSTB2022NSCQ-MSX0967);重庆市博士后研究项目(批准号:2022CQBSHTB3005);重庆市教委科技研究项目(批准号:KJQN202201631)资助。

摘　　要：在镧系配合物的制备过程中引入导电性好、比表面积高的氧化石墨烯,合成了一种导电性好的氧化石墨烯铽配合物(GO-Tb-COP)电致化学发光(ECL)阴极发光体.相对于传统配合物(如Tb-COP),GO-Tb-COP具有更高的ECL强度、更强的导电性和更大的比表面积,其原因是GO增加了GO-Tb-COP的导电性和比表面积,进而加速内部电荷传输,提高其自身的电化学活性,最终实现强的ECL发光信号.以环境污染物四环素(TC)为信号猝灭靶分子,GO-Tb-COP为ECL发光体,立方体二氧化铈(CeO_(2))为共反应促进剂和信号稳定剂,过硫酸根离子(S_(2)O_(8)^(2-))为共反应试剂,构建了用于TC检测的三元ECL传感器,其检出限低至0.44 pmol/L(S/N=3).此外,该传感器具有高的选择性、良好的稳定性和重现性,可用于实际样品TC的检测.通过增强配合物的导电性和比表面积提高镧系配合物ECL性能的策略,为合成高效镧系配合物ECL发光体提供了新的机遇.Graphene oxide with good electrical conductivity and high specific surface area was introduced into the preparation of lanthanide complexes,and a well-conductive graphene terbium complex(GO-Tb-COP)electrochemiluminescence(ECL)cathodoluminescent was synthesized.GO-Tb-COP has higher ECL intensity,stronger conductivity,and larger specific surface area than traditional complexes(such as Tb-COP)because GO increases the conductivity and specific surface area of GO-Tb-COP,which further accelerates its internal charge transport,improves its electrochemical activity,and ultimately achieves strong ECL emission signals.A ternary ECL sensor for sensitive detection of tetracycline(TC)was constructed with TC as signal quenching target molecule,GO-Tb-COP as ECL emitter,cubic ceria dioxide(CeO_(2))as co-reaction promoter and signal stabilizer,and persulfate ion(S_(2)O_(8)^(2-))as co-reaction reagent,and the detection limit of the sensor was as low as 0.44 pmol/L(S/N=3).In addition,the sensor has high selectivity,good stability and reproducibility,and has been successfully applied to the detection of TC in real samples.In conclusion,the strategy of improving the ECL performance of lanthanide complexes by enhancing the conductivity and specific surface area of the complexes provides new opportunities for the synthesis of high-efficiency lanthanide complex ECL emitter.

关 键 词：氧化石墨烯 镧系配合物 电致化学发光 四环素 传感器 

分 类 号：O657[理学—分析化学]