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Molecularly Imprinted Polymers Electrochemical Sensing: The Effect of Inhomogeneous Binding Sites on the Measurements. A Comparison between Imprinted Polyaniline versus nanoMIP-Doped Polyaniline Electrodes for the EIS Detection of 17β-Estradiol
ACS Sensors ( IF 8.2 ) Pub Date : 2024-08-29 , DOI: 10.1021/acssensors.4c01787 Alice Marinangeli 1 , Iva Chianella 2 , Eros Radicchi 1 , Devid Maniglio 3 , Alessandra Maria Bossi 1
ACS Sensors ( IF 8.2 ) Pub Date : 2024-08-29 , DOI: 10.1021/acssensors.4c01787 Alice Marinangeli 1 , Iva Chianella 2 , Eros Radicchi 1 , Devid Maniglio 3 , Alessandra Maria Bossi 1
Affiliation
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Molecularly imprinted polymers (MIPs) are synthetic receptors made by template-assisted synthesis. MIPs might be ideal receptors for sensing devices, given the possibility to custom-design selectivity and affinity toward a targeted analyte and their robustness and ability to withstand harsh conditions. However, the synthesis of MIP is an inherently random process that produces a statistical distribution of binding sites, characterized by a variety of affinities. This is verified both for bulk MIP materials and for MIP’s thin layers. In the present work, we aimed at assessing the effects of inhomogeneous versus homogeneous imprinted binding sites on electrochemical sensing measurements, and the possible implications on the sensor’s performance. In the example of an Electrochemical Impedance Spectroscopy (EIS) sensor for the 17β-estradiol (E2) hormone, the scenario of inhomogeneous binding sites was studied by modifying electrodes with an E2-MIP polyaniline (PANI) thin layer, called the “Imprinted PANI layer”. In contrast, the condition of discrete and uniform binding sites was epitomized by electrodes modified with a thin PANI layer purposedly doped with E2-MIP nanoparticles (nanoMIPs), which were referred to as “nanoMIP-doped PANI”. The behaviors of the two EIS sensors were compared. Interestingly, the sensitivity of the nanoMIP-doped PANI was almost twice with respect to that of the imprinted PANI layer, strongly suggesting that the homogeneity of the binding sites has a fundamental role in the sensor’s development. The nanoMIP-doped PANI sensor, which showed a response for E2 in the range 36.7 pM–36.7 nM and had a limit of detection of 2.86 pg/mL, was used to determine E2 in wastewater.
中文翻译：
分子印迹聚合物电化学传感：不均匀结合位点对测量的影响。印迹聚苯胺电极与 nanoMIP 掺杂聚苯胺电极用于 17β-雌二醇 EIS 检测的比较
分子印迹聚合物（MIP）是通过模板辅助合成制成的合成受体。 MIP 可能是传感设备的理想受体，因为它可以定制设计对目标分析物的选择性和亲和力，并且具有鲁棒性和承受恶劣条件的能力。然而，MIP 的合成本质上是一个随机过程，会产生结合位点的统计分布，其特征在于各种亲和力。这对于块状 MIP 材料和 MIP 薄层都得到了验证。在目前的工作中，我们的目的是评估不均匀与均匀印记结合位点对电化学传感测量的影响，以及对传感器性能的可能影响。在 17β-雌二醇 (E2) 激素的电化学阻抗谱 (EIS) 传感器示例中，通过使用 E2-MIP 聚苯胺 (PANI) 薄层（称为“印迹 PANI”）修改电极来研究不均匀结合位点的情况。层”。相比之下，离散且均匀的结合位点的情况是通过特意掺杂 E2-MIP 纳米粒子 (nanoMIP) 的薄 PANI 层修饰的电极来体现的，这被称为“nanoMIP 掺杂的 PANI”。比较了两个 EIS 传感器的行为。有趣的是，nanoMIP 掺杂的 PANI 的灵敏度几乎是印迹 PANI 层的两倍，强烈表明结合位点的均匀性在传感器的开发中具有重要作用。掺杂 nanoMIP 的 PANI 传感器对 E2 的响应范围为 36.7 pM–36.7 nM，检测限为 2.86 pg/mL，用于测定废水中的 E2。
更新日期：2024-08-29
中文翻译：
分子印迹聚合物电化学传感：不均匀结合位点对测量的影响。印迹聚苯胺电极与 nanoMIP 掺杂聚苯胺电极用于 17β-雌二醇 EIS 检测的比较
分子印迹聚合物（MIP）是通过模板辅助合成制成的合成受体。 MIP 可能是传感设备的理想受体，因为它可以定制设计对目标分析物的选择性和亲和力，并且具有鲁棒性和承受恶劣条件的能力。然而，MIP 的合成本质上是一个随机过程，会产生结合位点的统计分布，其特征在于各种亲和力。这对于块状 MIP 材料和 MIP 薄层都得到了验证。在目前的工作中，我们的目的是评估不均匀与均匀印记结合位点对电化学传感测量的影响，以及对传感器性能的可能影响。在 17β-雌二醇 (E2) 激素的电化学阻抗谱 (EIS) 传感器示例中，通过使用 E2-MIP 聚苯胺 (PANI) 薄层（称为“印迹 PANI”）修改电极来研究不均匀结合位点的情况。层”。相比之下，离散且均匀的结合位点的情况是通过特意掺杂 E2-MIP 纳米粒子 (nanoMIP) 的薄 PANI 层修饰的电极来体现的，这被称为“nanoMIP 掺杂的 PANI”。比较了两个 EIS 传感器的行为。有趣的是，nanoMIP 掺杂的 PANI 的灵敏度几乎是印迹 PANI 层的两倍，强烈表明结合位点的均匀性在传感器的开发中具有重要作用。掺杂 nanoMIP 的 PANI 传感器对 E2 的响应范围为 36.7 pM–36.7 nM，检测限为 2.86 pg/mL，用于测定废水中的 E2。
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