A Novel Surface‐tethered Analysis Method for Mercury (II) ion Detection via Self‐assembly of Individual Electrochemiluminescence Signal Units

Abstract

A novel analysis strategy based on the analyte‐induced surface‐tethered (AIST) of electrochemiluminescence (ECL) signal nanoparticles was first proposed for detection of Mercury (II) ion (Hg2+). In this work, luminol@Au‐cysteamine‐thymine (luminol@Au‐Cys‐T) multifunctional nanoarchitecture was designed as ECL signal units in the experimental process. Through a specific T‐Hg2+‐T coordination, luminol@Au‐Cys‐T composites were gravitationally self‐assembled to the electrode surface, which was coated with tris (2‐aminoethyl) amine functionalized graphene oxide@perylene‐3,4,9,10‐tetracarboxylic acid‐thymine (GO@PTCA‐TAEA‐T) complex film. This simple strategy of AIST of signal molecules could amplify the response signal and vastly enhance the sensitivity. Under the optimum condition, the linear relationship of Hg2+ concentration variation from 0.005 nM to 5 nM with a limit of detection (LOD) down to 0.002 nM (S/N=3), which also offered an alternative analytical approach with excellent performance of stability and selectivity. The regression equation was y=−414.52+2305.02 lgC(Hg2+) (pM). This Hg2+ ECL sensor had a good application prospects for the analysis of real samples.

Electrochemiluminescence Systems for Metal‐Ion Detection: A Systematic Review

“…Luminol's electrochemical reaction was generally reported to occur in alkaline solutions (Table 2). In the early 1980s, luminol was Co(II) [56] luminol@Au-Cys-T on GO@PTCA-TAEA-T 9.9 Hg(II) [58] γ-PGA-G-luminol 8.6 Hg(II) [59] ABEI/H 2 O 2 8 Hg(II) [60] poly(aniline-luminol)/ graphene oxide/chitosan 7.4 Hg(II) [61] luminol@Au-Cys-T and CdS QDs-Cys 9.9 Hg(II) [62] CdS QDs-luminol/H 2 O 2 7.8 Pb(II) [63] luminol/rGO-PdAu-GOx 8 Pb(II) [64] Au@luminol functionalized DNA2 probe 7.5 Cd(II) [65] Luminol/DO 11 Hg(II) [66] luminol/MnO 4 À > 7 Ag(I) [67] DNA-linked-Luminol-AuNps/ O 2 , APS as enhancer 8 Hg(II) [57] Luminol/H 2 O 2 7.4 Hg(II) [68] successfully applied as an emitter to measure Cu(II) in glycine buffer solution pH 10.15 [54] and Co(II) in H 3 BO 3 -NaOH solution pH 10. [55] The ECL intensity of luminol decreases in the presence of metals in alkaline solutions.…”

“…Meanwhile, Liu et al. applied luminol@Au‐cysteamine‐thymine (luminol@Au‐Cys‐T) composites as luminophores gravitationally assembled on the electrode surface [58] . This method can significantly improve the sensitivity of the ECL system to detect Hg(II) with a detection limit of 0.002 nM.…”

Highly Sensitive and Selective Detection of Pb(II) by NH2−SiO2/Ru(bpy)32+−UiO66 based Solid‐state ECL Sensor

“…These properties limit their wide applications. Electrochemiluminescence (ECL) is considered as a promising and powerful analytical technique because of its unique advantages [16,17]: ECL integrates the advantages of high sensitivity of luminescence analysis and controllable potential of electrochemical analysis, which shows the characteristics of good reproducibility, high sensitivity and good selectivity [18,19]. Zhu et al firstly applied Ru(bpy) 3 2 + derivative as ECL signal molecule and labeled it on DNA by coupling agent to obtain a DNA off-based signal off type lead ion sensor, this sensor could detect lead ions up to 1.1 × 10 À 5 μM [20]; Hai et al modified an aptamer probe with a hairpin structure to the surface of Fe 3 O 4 À Au magnetic nanoparticles, and formed a G-quadruplex with lead ions to construct a signal on-type Pb(II) biosensor and showed high selectivity for Pb(II) with a detection limit of 1.1 × 10 À 5 μM [21].…”

“…These properties limit their wide applications. Electrochemiluminescence (ECL) is considered as a promising and powerful analytical technique because of its unique advantages : ECL integrates the advantages of high sensitivity of luminescence analysis and controllable potential of electrochemical analysis, which shows the characteristics of good reproducibility, high sensitivity and good selectivity . Zhu et al.…”