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六氟合铁(III)三[六异硫氰酸根合铁(III)]三羟合铁配合物作为电化学 DNA 生物传感器的新型 DNA 嵌入剂。

Hexaferrocenium tri[hexa(isothiocyanato)iron(III)] trihydroxonium complex as a new DNA intercalator for electrochemical DNA biosensor.

机构信息

Department of Chemical Sciences, Faculty of Science and Technology, Universiti Kebangsaan Malaysia (UKM), 43600, Bangi, Selangor Darul Ehsan, Malaysia.

出版信息

Sci Rep. 2021 Apr 12;11(1):7883. doi: 10.1038/s41598-021-86939-z.

Abstract

Ferrocene or ferrocenium has been widely studied in the field of organometallic complexes because of its stable thermodynamic, kinetic and redox properties. Novel hexaferrocenium tri[hexa(isothiocyanato)iron(III)]trihydroxonium (HexaFc) complex was the product from the reaction of ferrocene, maleic acid and ammonium thiocyanate and was confirmed by elemental analysis CHNS, FTIR and single crystal X-ray crystallography. In this study, HexaFc was used for the first time as an electroactive indicator for porcine DNA biosensor. The UV-Vis DNA titrations with this compound showed hypochromism and redshift at 250 nm with increasing DNA concentrations. The binding constant (K) for HexaFc complex towards CT-DNA (calf-thymus DNA) was 3.1 × 10 M, indicated intercalator behaviour of the complex. To test the usefulness of this complex for DNA biosensor application, a porcine DNA biosensor was constructed. The recognition probes were covalently immobilised onto silica nanospheres (SiNSs) via glutaraldehyde linker on a screen-printed electrode (SPE). After intercalation with the HexaFc complex, the response of the biosensor to the complementary porcine DNA was measured using differential pulse voltammetry. The DNA biosensor demonstrated a linear response range to the complementary porcine DNA from 1 × 10 to 1 × 10 µM (R = 0.9642) with a limit detection of 4.83 × 10 µM and the response was stable up to 23 days of storage at 4 °C with 86% of its initial response. The results indicated that HexaFc complex is a feasible indicator for the DNA hybridisation without the use of a chemical label for the detection of porcine DNA.

摘要

二茂铁或二茂铁阳离子由于其稳定的热力学、动力学和氧化还原性质,在有机金属配合物领域得到了广泛的研究。新型六茂铁三[六(异硫氰酸根合铁(III))]三羟基合(六茂铁)配合物是由二茂铁、马来酸和硫氰酸铵反应得到的产物,通过元素分析 CHNS、傅里叶变换红外光谱(FTIR)和单晶 X 射线晶体学得到了证实。在这项研究中,六茂铁首次被用作猪 DNA 生物传感器的电活性指示剂。该化合物与 DNA 的紫外可见 DNA 滴定实验显示,随着 DNA 浓度的增加,在 250nm 处出现了减色和红移现象。六茂铁配合物与 CT-DNA(小牛胸腺 DNA)的结合常数(K)为 3.1×10M,表明该配合物具有嵌入剂的行为。为了测试该配合物用于 DNA 生物传感器应用的有用性,构建了猪 DNA 生物传感器。识别探针通过戊二醛连接子共价固定在硅纳米球(SiNSs)上,然后固定在丝网印刷电极(SPE)上。与六茂铁配合物嵌入后,使用差分脉冲伏安法测量生物传感器对互补猪 DNA 的响应。该 DNA 生物传感器对互补猪 DNA 的线性响应范围为 1×10至 1×10µM(R=0.9642),检测限为 4.83×10µM,在 4°C 下储存 23 天,其初始响应的 86%保持稳定。结果表明,六茂铁配合物是一种可行的指示剂,可用于杂交而无需使用化学标记物来检测猪 DNA。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c24/8041802/4276c7167c3a/41598_2021_86939_Fig1_HTML.jpg

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