用于 ECL 光谱鉴别和发射器相互交互研究的敏感信号调制策略,Analytical Chemistry

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用于 ECL 光谱鉴别和发射器相互交互研究的敏感信号调制策略
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-02-19 , DOI: 10.1021/acs.analchem.1c05217
Xuemei Ma ₁ , Qi Kang ₁ , Mengmeng Li ₁ , Li Fu ₂ , Guizheng Zou ₂ , Dazhong Shen ₁

Affiliation

电化学发光 (ECL) 的强度通常会随着电化学过程的进行而迅速变化，这使得在波长扫描模型中使用常规光电倍增管很难确定 ECL 光谱。在此，提出了一种涉及带通滤波器（BPF）的调制策略，以在不改变其硬件的情况下将传统的 ECL 分析仪升级为高灵敏度的 ECL 光谱仪。ECL 光谱可以通过使用不同中心波长的 BPF 阵列快速和/或连续调制 ECL 强度-时间曲线的一部分以及通过单变量三次多项式模型在不同测量时间校正 ECL 强度来计算。该策略不仅可以通过在短时间内调制发射来高灵敏度地确定超弱发射光谱，₃²⁺或三丙胺（TPA），还可以证明共存发射体之间的相互作用。结果表明， Ru(bpy) ₃^{2+ /TPA体系的Ru(bpy)}₃²⁺和TPA的ECL可以在电化学电位和浓度依赖性方面相互促进。_{随着 Ru(bpy) 3}²⁺浓度从 0.01 增加到 0.8 μM ，TPA 在 1.24 V 电位下的自 ECL 可以从 4.9 倍提高到 51 倍。在 0.04 μM Ru(bpy) ₃^2+存在下，在 1.01 和 1.76 V 的电位下，TPA 的自身 ECL 分别增强了 94 倍和 10.2 倍。便携式廉价 BPF 转盘设备也可用于光谱分辨多分析物测定和比率 ECL 生物传感器。

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Sensitive, Signal-Modulation Strategy for Discrimination of ECL Spectra and Investigation of Mutual Interactions of Emitters

The intensity of electrochemiluminescence (ECL) usually changes rapidly with the progress of the electrochemical process, making it difficult to determine the ECL spectrum with a conventional photomultiplier in a wavelength scan model. Herein, a band-pass filter (BPF)-involved modulating strategy is proposed to upgrade a conventional ECL analyzer to a highly sensitive ECL spectrometer without changing its hardware. The ECL spectrum can be figured out by rapidly and/or continuously modulating a part of the ECL intensity–time curve with a BPF array of different central wavelengths as well as correcting the ECL intensity at different measurement times by a univariate cubic polynomial model. This strategy not only can determine the spectrum of ultra-weak emission with high sensitivity via merely modulating the emission within a short period, including the weak self-ECL from either Ru(bpy)₃²⁺ or tripropylamine (TPA), but also can demonstrate the interaction between the co-existing emitters. It is shown that the ECL from both Ru(bpy)₃²⁺ and TPA of the Ru(bpy)₃²⁺/TPA system can be mutually promoted in electrochemical potential and in a concentration-dependent way. The self-ECL of TPA at the potential of 1.24 V can be enhanced from 4.9- to 51-fold with the Ru(bpy)₃²⁺ concentration increasing from 0.01 to 0.8 μM. In the presence of 0.04 μM Ru(bpy)₃²⁺, the self-ECL of TPA is enhanced by 94- and 10.2-fold at the potential of 1.01 and 1.76 V, respectively. The portable inexpensive BPF turntable device is also useful in spectrum-resolved multi-analyte determination and ratiometric ECL biosensors.

更新日期：2022-02-19

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