Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2022-09-06 , DOI: 10.1016/j.jhazmat.2022.129919 Qiulan Li 1 , Hong Li 2 , Kexiang Li 1 , Yi Gu 1 , Yijie Wang 1 , Dezhi Yang 3 , Yaling Yang 1 , Lei Gao 4
Methylmercury (MeHg+) is one of the common organic species of mercury, and has much higher toxicity than inorganic mercury. Based on the selective enhancement of the activity of nanozyme (NA-CDs/AuNPs) by MeHg+, a novel colorimetric nanoprobe for MeHg+ assay is proposed. The noradrenaline-based carbon dots (NA-CDs) as the reducing agent was applied to prepare the NA-CDs/AuNPs. The formation of gold amalgamation (Au@HgNPs) between nanozyme and MeHg+ allows to simultaneously accelerate the electron transfer from Au and Hg to NA-CDs and the generation of radicals (i.e. ∙OH, ∙O2- and ∙CH3). The NA-CDs/AuNPs has an outstanding anti-interference performance even in the presence of different mercury. Further density functionality theory (DFT) calculations revealed that the formation of Au@HgNPs via MeHg+ contributes to the significantly lowered activation energy, resulting in the peroxidase-like activity generation and acceleration. This leads to rapid (10 min) and specific colorimetric detection of MeHg+ with the detection limit of 0.06 μg L−1. This introduces a novel method for simple and sensitive detection of MeHg+, giving a new horizon for the assay of organometallic compounds.
中文翻译:
基于碳点/Au NPs纳米酶类过氧化物酶活性调控的甲基汞特异性比色检测
甲基汞 (MeHg + ) 是常见的有机汞之一,其毒性远高于无机汞。基于MeHg + 对纳米酶(NA-CDs/AuNPs)活性的选择性增强,提出了一种用于MeHg +测定的新型比色纳米探针。应用去甲肾上腺素基碳点 (NA-CDs) 作为还原剂来制备 NA-CDs/AuNPs。纳米酶和 MeHg +之间的金融合 (Au@HgNPs) 的形成允许同时加速从 Au 和 Hg 到 NA-CDs 的电子转移和自由基(即 ∙OH、∙O 2 -和 ∙CH 3)。即使在不同的汞存在下,NA-CDs/AuNPs 也具有出色的抗干扰性能。进一步的密度泛函理论 (DFT) 计算表明,通过 MeHg +形成 Au@HgNPs有助于显着降低活化能,从而导致过氧化物酶样活性的产生和加速。这导致对 MeHg +的快速(10 分钟)和特异性比色检测,检测限为 0.06 μg L -1。这介绍了一种简单而灵敏地检测 MeHg +的新方法,为有机金属化合物的测定提供了新的视野。