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Zinc-Based Metal–Organic Framework with MLCT Properties as an Efficient Electrochemiluminescence Probe for Trace Detection of Trenbolone
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-09-29 , DOI: 10.1021/acs.analchem.2c03615 Xianzhen Song 1 , Lu Zhao 1 , Nuo Zhang 1 , Lei Liu 1 , Xiang Ren 1 , Hongmin Ma 1 , Chuannan Luo 1 , Yuyang Li 1 , Qin Wei 1
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-09-29 , DOI: 10.1021/acs.analchem.2c03615 Xianzhen Song 1 , Lu Zhao 1 , Nuo Zhang 1 , Lei Liu 1 , Xiang Ren 1 , Hongmin Ma 1 , Chuannan Luo 1 , Yuyang Li 1 , Qin Wei 1
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In this work, we utilized polycyclic aromatic hydrocarbon (PAH) derivatives as ligands to develop a zinc-based metal–organic framework (Zn-MOF) as an effective detection probe to construct an electrochemiluminescence (ECL) sensor for trenbolone detection. As traditional ECL emitters, PAHs and their derivatives have limited luminescence efficiency because of the aggregation-induced quenching (ACQ) effect. Therefore, Zn-PTC was designed by the coordination of 3,4,9,10-perylenetetracarboxylic (PTC) in the MOF to eliminate the ACQ effect. Meanwhile, Zn-PTC formed based on an aromatic ligand possessed the metal-to-ligand charge-transfer (MLCT) effect, which could transfer the energy of Zn2+ to the aromatic ligand for strong luminescence. The ECL efficiency of Zn-PTC was calculated to be approximately 2.2 times that of the ligand (K4PTC). Second, the Ag@Fe core–shell bimetallic nanocrystal was prepared for efficient activation of persulfate (S2O82–), thereby generating more sulfate radicals (SO4•–) to further promote ECL emission. According to ECL characterizations, UV–vis and fluorescence spectra, and density functional theory calculations, the luminescence and signal amplification mechanisms were investigated. In addition, NKFRGKYKC (NKF) was introduced as an affinity ligand to directionally immobilize the target antibodies, thus releasing specific sites in their Fab fragment to enhance binding activity. Based on the above strategies, the constructed biosensor exhibited high sensitivity, realizing trace detection of TBE with a wide detection range (10 fg/mL–100 ng/mL) and a low detection limit (3.28 fg/mL). This study provided an important reference for sensitive monitoring of steroid pollutants in the environment.
中文翻译：
具有 MLCT 特性的锌基金属有机骨架作为高效电化学发光探针用于痕量群勃龙检测
在这项工作中，我们利用多环芳烃 (PAH) 衍生物作为配体，开发了一种锌基金属有机骨架 (Zn-MOF) 作为有效的检测探针，构建了用于群勃龙检测的电化学发光 (ECL) 传感器。作为传统的 ECL 发光体，多环芳烃及其衍生物由于聚集诱导猝灭 (ACQ) 效应而限制了发光效率。因此，Zn-PTC 是通过 MOF 中的 3,4,9,10-苝四羧酸 (PTC) 的配位设计的，以消除 ACQ 效应。同时，基于芳香族配体形成的Zn-PTC具有金属-配体电荷转移（MLCT）效应，可以转移Zn 2+的能量用于强发光的芳香配体。经计算，Zn-PTC 的 ECL 效率约为配体 (K 4 PTC) 的 2.2 倍。其次，制备了 Ag@Fe 核壳双金属纳米晶，用于高效活化过硫酸盐 (S 2 O 8 2– )，从而产生更多的硫酸根 (SO 4 •–)进一步促进ECL排放。根据ECL表征、紫外可见光谱和荧光光谱以及密度泛函理论计算，研究了发光和信号放大机制。此外，引入NKFRGKYKC（NKF）作为亲和配体，定向固定目标抗体，从而释放其Fab片段中的特定位点，增强结合活性。基于上述策略，构建的生物传感器表现出高灵敏度，实现了TBE的痕量检测，检测范围广（10 fg/mL–100 ng/mL），检测限低（3.28 fg/mL）。该研究为环境中类固醇污染物的灵敏监测提供了重要参考。
更新日期：2022-09-29
中文翻译：
具有 MLCT 特性的锌基金属有机骨架作为高效电化学发光探针用于痕量群勃龙检测
在这项工作中，我们利用多环芳烃 (PAH) 衍生物作为配体，开发了一种锌基金属有机骨架 (Zn-MOF) 作为有效的检测探针，构建了用于群勃龙检测的电化学发光 (ECL) 传感器。作为传统的 ECL 发光体，多环芳烃及其衍生物由于聚集诱导猝灭 (ACQ) 效应而限制了发光效率。因此，Zn-PTC 是通过 MOF 中的 3,4,9,10-苝四羧酸 (PTC) 的配位设计的，以消除 ACQ 效应。同时，基于芳香族配体形成的Zn-PTC具有金属-配体电荷转移（MLCT）效应，可以转移Zn 2+的能量用于强发光的芳香配体。经计算，Zn-PTC 的 ECL 效率约为配体 (K 4 PTC) 的 2.2 倍。其次，制备了 Ag@Fe 核壳双金属纳米晶，用于高效活化过硫酸盐 (S 2 O 8 2– )，从而产生更多的硫酸根 (SO 4 •–)进一步促进ECL排放。根据ECL表征、紫外可见光谱和荧光光谱以及密度泛函理论计算，研究了发光和信号放大机制。此外，引入NKFRGKYKC（NKF）作为亲和配体，定向固定目标抗体，从而释放其Fab片段中的特定位点，增强结合活性。基于上述策略，构建的生物传感器表现出高灵敏度，实现了TBE的痕量检测，检测范围广（10 fg/mL–100 ng/mL），检测限低（3.28 fg/mL）。该研究为环境中类固醇污染物的灵敏监测提供了重要参考。
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