共晶诱导增强的电化学发光9,10-二苯基蒽-苝微晶构建高效尿酸传感器

doi:10.7503/cjcu20200294

高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (9): 1989.doi: 10.7503/cjcu20200294

共晶诱导增强的电化学发光9,10-二苯基蒽-苝微晶构建高效尿酸传感器

廖妮, 张捷源, 黄梓阳, 赵晏汐, 柴雅琴, 袁若, 卓颖()

发光分析与分子传感教育部重点实验室(西南大学), 西南大学化学化工学院, 重庆 400715

收稿日期:2020-05-26 出版日期:2020-09-10 发布日期:2020-09-02
通讯作者: 卓颖 E-mail:yingzhuo@swu.edu.cn
基金资助:
国家自然科学基金(21675130);重庆市英才计划青年拔尖人才项目(CQYC201905067)

Construction of High Efficiency Uric Acid Sensor Based on the co-Crystal Enhanced Electrochemiluminescence from 9,10-Diphenylanthracene-perylene Microcrystals

LIAO Ni, ZHANG Jieyuan, HUANG Ziyang, ZHAO Yanxi, CHAI Yaqin, YUAN Ruo, ZHUO Ying()

Key Laboratory of Luminescence Analysis and Molecular Sensing(Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China

Received:2020-05-26 Online:2020-09-10 Published:2020-09-02
Contact: ZHUO Ying E-mail:yingzhuo@swu.edu.cn
Supported by:
Supported by the National Natural Science Foundation of China(21675130);the Chongqing Talents Touth Top?notch Personnel Support Program, China(CQYC201905067)

摘要/Abstract

摘要：

采用表面活性剂辅助自组装方法, 制得非共平面分子9,10-二苯基蒽(DPA)与平面型分子苝(Pe)形成的具有共晶诱导增强效应的电化学发光(ECL)新材料. DPA的引入不仅可以有效降低Pe分子因π-π作用聚集引起的聚集诱导猝灭(ACQ)效应, 导致Pe分子的ECL发射从二聚体或多聚体激发态(¹Pe^2*)转变为单体激发态(¹Pe^*); 还发挥了供体分子的作用, 为受体分子Pe提供了有效的能量传递, 进一步增强了ECL响应. 将该共晶发光材料修饰到玻碳电极表面构建了新型ECL尿酸传感器, 其对尿酸检测的线性范围为0.01 μmol/L~ 5.0 mmol/L, 检出限为4.0 nmol/L, 具有良好的选择性和稳定性.

关键词: 共晶诱导增强电化学发光, 9,10-二苯基蒽, 苝, 尿酸, 传感器

Abstract:

A new luminophore with co-crystal enhanced electrochemiluminescence(ECL) was obtained by the surfactant assisted self-assembly of the non-coplanar molecule 9,10-diphenylanthracene(DPA) and planar molecule perylene(Pe). The introduction of DPA in the co-crystals can not only reduce the aggregation-caused quenching(ACQ) effect of perylene, making the ECL emission of Pe molecule from the dimer or multimer excited state(¹Pe^2*) to the monomer excited state(¹Pe^*), but also plays a role as a donor molecule, providing effective energy transfer to the acceptor molecule of Pe, which further enhances the ECL response. The electrochemical sensor for uric acid based on DPA-Pe microcrystals has an extremely wide linear of 0.01 μmol/L—5.0 mmol/L and a detection limit of 4.0 nmol/L. In addition, the sensor has a nice stability and selectivity for uric acid detection.

Key words: co-Crystal enhanced electrochemiluminescence, 9,10-Diphenylanthracene, Perylene, Uric acid, Sensor

中图分类号:

O657

TrendMD:

廖妮, 张捷源, 黄梓阳, 赵晏汐, 柴雅琴, 袁若, 卓颖. 共晶诱导增强的电化学发光9,10-二苯基蒽-苝微晶构建高效尿酸传感器. 高等学校化学学报, 2020, 41(9): 1989.

LIAO Ni, ZHANG Jieyuan, HUANG Ziyang, ZHAO Yanxi, CHAI Yaqin, YUAN Ruo, ZHUO Ying. Construction of High Efficiency Uric Acid Sensor Based on the co-Crystal Enhanced Electrochemiluminescence from 9,10-Diphenylanthracene-perylene Microcrystals. Chem. J. Chinese Universities, 2020, 41(9): 1989.

图/表 6

Scheme 1 Preparation process of DPA-Pe MCs

Fig.1 SEM image(A) and XRD patterns(B) of DPA?Pe MCs(a), the standard PDF cards of Pe(b) and DPA(c) crystals

Fig.2 ECL intensity of different MCs modified GCE in blank solution(A) and cyclic voltammograms of different MCs modified GCE in 0.1 mol/L PBS containing 0.7 mol/L [bmim][BF4] as supporting electrolyte(B)a. Bare GCE; b. Pe MCs/GCE; c. DPA MCs/GCE; d. DPA-Pe MCs/GCE.

Fig.3 UV?Vis absorption spectra of Pe MCs(a) and ECL spectra of DPA MCs(b) in an aqueous solution(A); normalized FL emission spectra of the Pe molecule in THF(a), Pe MCs(b) and DPA?Pe MCs(c) in an aqueous solution(B); FL emission spectra of Pe MCs(b) and DPA?Pe MCs(c) in an aqueous solution(C); the maximum ECL emission peak of Pe MCs(D) and DPA?Pe MCs(E) via a 3D surface image; two?dimensional ECL emission peaks of DPA?Pe MCs(a) and Pe MCs(b)(F); the possible ECL mechanism of DPA?Pe MCs(G)

Fig.4 Molecular structures of Pe(A), DPA(B) and DPA/Pe in different perspectives(C, D) and RDG analysis for DPA/Pe(E)(A―D) The geometry optimization of DPA/Pe was carried out at the M062X-D3 level with TZVP basis sets by ORCA package.

Fig.5 ECL responses of the UA sensor for different concentrations of UA(A), selective(B, C) and its stability(D)(A) UA concentration/(μmol·L-1), a―g: 0.01, 0.2, 10, 200, 1000, 2000, 5000. Inset of (A): the calibration curve for UA.(B) a. K+; b. Ca2+; c. CO32-; d. Cl-; e. SO42-; f. Mg2+; g. UA. (C) a. L?Cys; b. L?His; c. urea; d. glucose; e. vitamin C; f. UA.

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共晶诱导增强的电化学发光9,10-二苯基蒽-苝微晶构建高效尿酸传感器

Construction of High Efficiency Uric Acid Sensor Based on the co-Crystal Enhanced Electrochemiluminescence from 9,10-Diphenylanthracene-perylene Microcrystals

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