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基于单原子钴的纳米酶比色传感器阵列用于区分含硫金属盐。

Nanozyme colorimetric sensor array based on monatomic cobalt for the discrimination of sulfur-containing metal salts.

机构信息

College of Food Science and Engineering, Jilin University, Changchun 130062, PR China.

Institute of Physical Chemistry, College of Chemistry, Jilin University, 2519 Jiefang Road, Changchun 130021, PR China.

出版信息

J Hazard Mater. 2023 Aug 15;456:131643. doi: 10.1016/j.jhazmat.2023.131643. Epub 2023 May 14.

Abstract

The identification of sulfur-containing metal salts (SCMs) is of great interest because they play an important role in many biological processes and diseases. Here, we constructed a ternary channel colorimetric sensor array to detect multiple SCMs simultaneously, relying on monatomic Co embedded in nitrogen-doped graphene nanozyme (CoN-G). Due to the unique structure, CoN-G exhibits activity similar to native oxidases, capable of catalysing directly the oxidization of 3,3',5,5'-tetramethylbenzidine (TMB) by O molecules independent of HO. Density functional theory (DFT) calculations suggest that CoN-G has no potential barrier in the whole reaction route, thus presenting higher oxidase-like catalytic activity. Based on different degrees of TMB oxidation, different colorimetric response changes are obtained as "fingerprints" on the sensor array. The sensor array can discriminate different concentrations of unitary, binary, ternary, and quaternary SCMs and has been successfully applied to detect six real samples (soil, milk, red wine and egg white). To advance the field detection of the above four types of SCMs, we creatively propose a smartphone-based autonomous detection platform with a linear range of 1.6-320 μM and a limit of detection of 0.0778-0.218 μM, which demonstrates the potential use of sensor arrays in the application of disease diagnosis and food and environment monitoring.

摘要

含硫金属盐(SCMs)的鉴定具有重要意义,因为它们在许多生物过程和疾病中发挥着重要作用。在这里,我们构建了一个三元通道比色传感器阵列,以依赖于嵌入氮掺杂石墨烯纳米酶(CoN-G)中的单原子 Co 来同时检测多种 SCMs。由于独特的结构,CoN-G 表现出类似于天然氧化酶的活性,能够独立于 HO 直接催化 O 分子对 3,3',5,5'-四甲基联苯胺(TMB)的氧化。密度泛函理论(DFT)计算表明,CoN-G 在整个反应途径中没有势垒,因此表现出更高的氧化酶样催化活性。基于 TMB 氧化程度的不同,传感器阵列获得了不同的比色响应变化,作为“指纹”。传感器阵列可以区分不同浓度的单一、二元、三元和四元 SCMs,并已成功应用于检测六种实际样品(土壤、牛奶、红酒和蛋清)。为了推进上述四种 SCMs 的现场检测,我们创造性地提出了一种基于智能手机的自主检测平台,具有 1.6-320 μM 的线性范围和 0.0778-0.218 μM 的检测限,这表明传感器阵列在疾病诊断和食品及环境监测中的应用具有潜力。

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