N vacancy and self-enhancement induced high anodic electrochemiluminescence of 3D g-C3N4 for sensitive staphylococcus aureus analysis

Yuxuan Wang; Xinya Jiang; Weiwei Cao; Haijun Wang; Ruo Yuan

doi:10.1016/j.talanta.2024.126144

N vacancy and self-enhancement induced high anodic electrochemiluminescence of 3D g-C₃N₄ for sensitive staphylococcus aureus analysis

Talanta. 2024 Apr 23:275:126144. doi: 10.1016/j.talanta.2024.126144. Online ahead of print.

Authors

Yuxuan Wang¹, Xinya Jiang², Weiwei Cao³, Haijun Wang⁴, Ruo Yuan⁵

Affiliations

¹ Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing, 400715, China. Electronic address: 1324315084@qq.com.
² Chongqing Key Laboratory of Inorganic Special Functional Materials, College of Chemistry and Chemical Engineering, Yangtze Normal University, Fuling, Chongqing, 408100, China. Electronic address: 1023496341@qq.com.
³ Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing, 400715, China. Electronic address: 2635392203@qq.com.
⁴ Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing, 400715, China. Electronic address: hjwang@swu.edu.cn.
⁵ Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing, 400715, China. Electronic address: yuanruo@swu.edu.cn.

PMID: 38663062
DOI: 10.1016/j.talanta.2024.126144

Abstract

Here, 3D g-C₃N₄ with dense N vacancy in its 3D porous interconnected open-framework was synthesized, and the co-reactive 3-(dibutylamino)propylamine (DBAPA) was further covalently coupled onto the surface, resulting in a strong self-enhanced anodic electrochemiluminescence (ECL). Through introduction of high-density N vacancy, for the obtained 3D g-C₃N₄-NV, the band gap was broadened and the electrical conductivity was enhanced, realizing an obvious ECL improvement. Moreover, after the covalent binding of co-reactive DBAPA, the obtained 3D g-C₃N₄-NV-DBAPA exhibited a more intensive self-enhanced ECL signal due to the higher co-reaction efficiency originated from shorter electron transfer distance and lower energy loss. Based on the high initial signal of the proposed 3D g-C₃N₄-NV-DBAPA, a sensitive ECL biosensor with signal "on-off" was fabricated in assistance with multiple horizontal ordered hybridization chain reaction (HO-HCR). Through orderly fixing the reacted DNA chains on the Y-shape DNA structure on the electrode could effectively decrease diffusion process and improve the reaction efficiency of HCR process, resulting in the formation of numerous long horizontal double-strand DNA that could immobilize abundant ferrocene-doxorubicin (Fc-Dox) with ECL quenching effect. Meanwhile, compared to the traditional vertical HCR, the HO-HCR could make the quench reagent closer to the ECL emitter on the electrode surface and obtain a more effective quenching effect to enhance the sensing sensitivity. As a result, the proposed ECL biosensor archived the sensitive measurement of staphylococcus aureus with a detection limit of 10.3 aM.

Keywords: 3D g-C(3)N(4); HO-HCR; N vacancy; Self-enhanced anodic ECL; staphylococcus aureus.