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Polydopamine-based molecularly imprinted thin films for electro-chemical sensing of nitro-explosives in aqueous solutions.
Bioelectrochemistry ( IF 4.8 ) Pub Date : 2020-05-01 , DOI: 10.1016/j.bioelechem.2020.107541 Nadja Leibl 1 , Luminita Duma 1 , Carlo Gonzato 1 , Karsten Haupt 1
Bioelectrochemistry ( IF 4.8 ) Pub Date : 2020-05-01 , DOI: 10.1016/j.bioelechem.2020.107541 Nadja Leibl 1 , Luminita Duma 1 , Carlo Gonzato 1 , Karsten Haupt 1
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A sensitive electrochemical sensor was developed for the detection of nitro-explosives in aqueous solutions based on thin molecularly imprinted polydopamine films. Dopamine was identified in silico, based on DFT (density functional theory) calculations with the ωB97X-D/6-31G* basis set, as the best functional monomer and electropolymerized via cyclic voltammetry (CV) in the presence of carboxylic acid-based structural analogues ('dummy' templates) for two model nitro-explosives: TNT (2,4,6-trinitrotoluene) and RDX (Research Department eXplosive, 1,3,5-trinitroperhydro-1,3,5-triazine). This approach afforded a homogenous coverage of gold electrodes with imprinted films of tunable thickness. The electropolymerized molecularly imprinted polydopamine films allowed for a 105-fold sensitivity improvement over a bare gold electrode based on tracking the redox peaks of the targets by CV. This improved sensitivity is ascribed to the ability of the MIP to concentrate its target in proximity to the transduction element. The MIP films showed reproducible binding in phosphate buffer (10 mM, pH 7.4), with a dynamic range from 0.1 nM to 10 nM for both TNT and RDX and an increased selectivity over closely related structural analogues.
中文翻译：
基于聚多巴胺的分子印迹薄膜，用于水溶液中硝基炸药的电化学感应。
基于分子印迹的聚多巴胺薄膜，开发了一种灵敏的电化学传感器，用于检测水溶液中的硝基爆炸物。根据DFT（密度泛函理论）计算，使用ωB97X-D/ 6-31G *基组在计算机上将多巴胺确定为最佳功能单体，并在基于羧酸的结构存在下通过循环伏安法（CV）进行电聚合两种模型硝基炸药的类似物（“虚拟”模板）：TNT（2,4,6-三硝基甲苯）和RDX（研究部门eXplosive，1,3,5-三硝基过氢-1,3,5-三嗪）。这种方法可以用可调厚度的压印膜均匀覆盖金电极。基于CV追踪靶的氧化还原峰，电聚合的分子印迹聚多巴胺薄膜比裸金电极提高了105倍的灵敏度。这种提高的敏感性归因于MIP将其靶标集中在转导元件附近的能力。MIP膜在磷酸盐缓冲液（10 mM，pH 7.4）中显示可重现的结合，对TNT和RDX的动态范围为0.1 nM至10 nM，并且与紧密相关的结构类似物相比具有更高的选择性。
更新日期：2020-05-01
中文翻译：
基于聚多巴胺的分子印迹薄膜，用于水溶液中硝基炸药的电化学感应。
基于分子印迹的聚多巴胺薄膜，开发了一种灵敏的电化学传感器，用于检测水溶液中的硝基爆炸物。根据DFT（密度泛函理论）计算，使用ωB97X-D/ 6-31G *基组在计算机上将多巴胺确定为最佳功能单体，并在基于羧酸的结构存在下通过循环伏安法（CV）进行电聚合两种模型硝基炸药的类似物（“虚拟”模板）：TNT（2,4,6-三硝基甲苯）和RDX（研究部门eXplosive，1,3,5-三硝基过氢-1,3,5-三嗪）。这种方法可以用可调厚度的压印膜均匀覆盖金电极。基于CV追踪靶的氧化还原峰，电聚合的分子印迹聚多巴胺薄膜比裸金电极提高了105倍的灵敏度。这种提高的敏感性归因于MIP将其靶标集中在转导元件附近的能力。MIP膜在磷酸盐缓冲液（10 mM，pH 7.4）中显示可重现的结合，对TNT和RDX的动态范围为0.1 nM至10 nM，并且与紧密相关的结构类似物相比具有更高的选择性。
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