Leverhulme Research Centre for Forensic Science, University of Dundee, Dundee, DD1 4HN, UK.
Materials Science & Engineering Research Cluster, School of Science & Engineering, University of Dundee, Dundee, DD1 4HN, UK.
Chemosphere. 2022 Nov;307(Pt 4):136108. doi: 10.1016/j.chemosphere.2022.136108. Epub 2022 Aug 19.
Explosives are powerful destructive weapons used by criminals and terrorists across the globe and their use within military installation sites poses serious environmental health problems. Existing colorimetric sensors for triacetone triperoxide (TATP) relies on detecting its hydrolysed HO form. However, such detection strategy limits the practicability for on-site TATP sensing. In this work, we have developed a novel peroxidase mimic catalytic colorimetric sensor for direct recognition of TATP. Ceria (Ce)-doped FeO nanoparticles (CeFeO) were synthesized via the hot-injection organic synthetic route in the presence of metal precursors and organic ligands. Thereafter, the organic-capped CeFeO nanoparticles were surface-functionalized with amphiphilic polymers (Amp-poly) to render the nanoparticle stable, compact and biocompatible. Thiolated γ-cyclodextrin (γ-CD) was adsorbed on the Amp-poly-CeFeO nanocomposite (NC) surface to form a γ-CD-Amp-poly-CeFeO NC. γ-CD served both as a receptor and as a catalytic enhancer for TATP. Hemin (H), used as a catalytic signal amplifier was adsorbed on the γ-CD-Amp-poly-CeFeO NC surface to form a γ-CD-Amp-poly-CeFeO-H NC that served as a functional nanozyme for the enhanced catalytic colorimetric detection of TATP. Under optimum experimental reaction conditions, TATP prepared in BIS-TRIS-Trisma Ac-KAc-NAc buffer, pH 3, was selectively and ultrasensitively detected without the need for acid hydrolysis based on the catalytic oxidation of 3,3',5,5'-tetramethylbenzidine by HO in the presence of the γ-CD-Amp-poly-CeFeO-H hybrid nanozyme. The obtained limit of detection of ∼0.05 μg/mL when compared with other published probes demonstrated superior sensitivity. The developed peroxidase mimic γ-CD-Amp-poly-CeFeO-H catalytic colorimetric sensor was successfully applied to detect TATP in soil, river water and tap water samples.
爆炸物是全球犯罪分子和恐怖分子使用的强大破坏性武器，其在军事设施场所的使用给环境健康带来了严重问题。目前用于三乙酰基过氧化物（TATP）的比色传感器依赖于检测其水解的 HO 形式。然而，这种检测策略限制了现场 TATP 传感的实用性。在这项工作中，我们开发了一种新颖的过氧化物酶模拟催化比色传感器，用于直接识别 TATP。通过在金属前体和有机配体存在下通过热注入有机合成途径合成了掺铈的 FeO 纳米粒子（CeFeO）。此后，用两亲聚合物（Amp-poly）对有机封端的 CeFeO 纳米粒子进行表面功能化，使纳米粒子稳定、紧凑且具有生物相容性。巯基化的γ-环糊精（γ-CD）吸附在 Amp-poly-CeFeO 纳米复合材料（NC）表面上形成γ-CD-Amp-poly-CeFeO NC。γ-CD 既是 TATP 的受体又是其催化增强剂。用作催化信号放大器的血红素（H）被吸附在γ-CD-Amp-poly-CeFeO NC 表面上，形成γ-CD-Amp-poly-CeFeO-H NC，用作增强 TATP 催化比色检测的功能纳米酶。在最佳实验反应条件下，在存在γ-CD-Amp-poly-CeFeO-H 杂化纳米酶的情况下，无需基于 HO 的酸水解，在 BIS-TRIS-Trisma Ac-KAc-NAc 缓冲液，pH3 中制备的 TATP 被选择性和超灵敏地检测到，用于 TATP 的比色检测。与其他已发表的探针相比，获得的检出限约为 0.05μg/mL，表现出更高的灵敏度。开发的过氧化物酶模拟γ-CD-Amp-poly-CeFeO-H 催化比色传感器成功应用于检测土壤、河水和自来水中的 TATP。
