Collaborative Innovation Centre for Green Chemical Manufacturing and Accurate Detection, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, Shandong, China.
Collaborative Innovation Centre for Green Chemical Manufacturing and Accurate Detection, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, Shandong, China.
Biosens Bioelectron. 2023 Feb 1;221:114925. doi: 10.1016/j.bios.2022.114925. Epub 2022 Nov 24.
The wide and even whole pH range electrochemiluminescence (ECL) is attractive for steroid estrogens detection under harsh conditions (such as strong acid and alkali). Herein, we presented an efficient europium-based metal-organic framework (Eu-MOF) as ECL luminophore, which has been synthesized via the specific 2, 4-bis(3, 5-dicarboxyphenylamino)-6-oltriazine (HBDPO) ligand with acid-base buffering effect. The functional groups with weak acid and base endowed the HBDPO with eight ionogenic group states, thereout different total charges of HBDPO were derived, thus high and steady ECL signals of Eu-MOF were acquired under different environments with pH = 1.0-14.0. Most notably, combined with the means of UV-vis, fluorescence spectra, cyclic voltammetry (CV) and density functional theory (DFT) calculations, the Eu-MOF has been explored different luminescence mechanisms with variational total charges. The constructed ECL biosensor based on the Eu-MOF realized sensitive detection of trenbolone under wide pH range (In order to maintain the biological activity of antigen and antibody, the studied pH value is 5-8.5), in which the limits of detection were 3.95 fg/mL (pH = 5.0), 2.36 fg/mL (pH = 7.4) and 5.48 fg/mL (pH = 8.5) respectively. This work provides a considerable method to realize efficient trace detection of steroid estrogens under the wide or even whole pH conditions.
宽且均匀的整个 pH 范围电化学发光(ECL)在恶劣条件下(如强酸和强碱)对检测甾体雌激素具有吸引力。在此,我们提出了一种高效的基于铕的金属有机骨架(Eu-MOF)作为 ECL 发光体,它是通过具有酸碱缓冲作用的特定 2,4-双(3,5-二羧基苯氨基)-6-唑三嗪(HBDPO)配体合成的。具有弱酸和弱碱性的官能团赋予 HBDPO 具有八个离子基团状态,从而得出 HBDPO 的不同总电荷,从而在 pH = 1.0-14.0 的不同环境下获得了高且稳定的 Eu-MOF ECL 信号。值得注意的是,结合紫外-可见光谱、荧光光谱、循环伏安法(CV)和密度泛函理论(DFT)计算,Eu-MOF 已经探索了具有变化总电荷的不同发光机制。基于 Eu-MOF 的构建的 ECL 生物传感器实现了在宽 pH 范围内(为了保持抗原和抗体的生物活性,研究的 pH 值为 5-8.5)对 trenbolone 的灵敏检测,其中检测限分别为 3.95 fg/mL(pH = 5.0)、2.36 fg/mL(pH = 7.4)和 5.48 fg/mL(pH = 8.5)。这项工作提供了一种相当有意义的方法,可以在宽或甚至整个 pH 条件下实现对甾体雌激素的有效痕量检测。