A Metal–Organic Framework Based on a Nickel Bis(dithiolene) Connector: Synthesis, Crystal Structure, and Application as an Electrochemical Glucose Sensor,Journal of the American Chemical Society

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A Metal–Organic Framework Based on a Nickel Bis(dithiolene) Connector: Synthesis, Crystal Structure, and Application as an Electrochemical Glucose Sensor
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-11-13 , DOI: 10.1021/jacs.0c09009
Yan Zhou ₁ , Qin Hu ₂ , Fei Yu ₁ , Guang-Ying Ran ₂ , Hai-Ying Wang ₂ , Nicholas D Shepherd ₃ , Deanna M D'Alessandro ₃ , Mohamedally Kurmoo ₄ , Jing-Lin Zuo ₁

Affiliation

Functionalizing the redox-active tetrathiafulvalene (TTF) core with groups capable of coordination to metals provides new perspectives on the modulation of architectures and electronic properties of organic-inorganic hybrid materials. With a view to extending this concept, we have now synthesized nickel bis(dithiolene-dibenzoic acid), [Ni(C2S2(C6H4COOH)2)2], which can be considered as the inorganic analogue of the organic tetrathiafulvalene-tetrabenzoic acid (H4TTFTB). Likewise, [Ni(C2S2(C6H4COOH)2)2] is a redox-active linker for new functional metal-organic frameworks, as demonstrated here with the synthesis of [Mn2{Ni(C2S2(C6H4COO)2)2}(H2O)2]·2DMF, (1, DMF = N,N-dimethylformamide). 1 is isomorphic to the reported [Mn2(TTFTB)(H2O)2] (2) but is a better electrochemical glucose sensor due to the multiple oxidation-reduction states of the [NiS4] core, which allow glucose to be oxidized to glucolactone by the high oxidation state [NiS4] center. As a non-enzymatic glucose sensor, 1 on Cu foam (CF), 1-CF, was synthesized by a one-step hydrothermal method and exhibited an excellent electrochemical performance. The fabricated 1-CF electrode offers a high sensitivity of 27.9 A M-1 cm-2, with a wide linear detection range from 2.0 × 10-6 to 2.0 × 10-3 M, a low detection limit of 1.0 × 10-7 M (signal/noise = 3), and satisfactory stability and reproducibility.

中文翻译：

基于镍双（二硫醇）连接体的金属有机框架：合成、晶体结构及其作为电化学葡萄糖传感器的应用

用能够与金属配位的基团对氧化还原活性四硫富瓦烯（TTF）核进行功能化，为有机-无机杂化材料的结构和电子性能的调节提供了新的视角。为了扩展这个概念，我们现在合成了双(二硫杂环戊二烯-二苯甲酸)镍，[Ni(C2S2(C6H4COOH)2)2]，它可以被认为是有机四硫富瓦烯-四苯甲酸(H4TTFTB)的无机类似物）。同样，[Ni(C2S2(C6H4COOH)2)2] 是新型功能性金属有机框架的氧化还原活性连接体，如[Mn2{Ni(C2S2(C6H4COO)2)2}(H2O) 的合成所示2]·2DMF，（1，DMF=N,N-二甲基甲酰胺）。 1 与报道的 [Mn2(TTFTB)(H2O)2] (2) 同构，但由于 [NiS4] 核心的多种氧化还原态，它允许葡萄糖通过以下方式氧化为葡萄糖内酯，因此是一种更好的电化学葡萄糖传感器高氧化态[NiS4]中心。作为一种非酶葡萄糖传感器，1 on Cu foam (CF)，1-CF，是通过一步水热法合成的，并表现出优异的电化学性能。所制造的 1-CF 电极具有 27.9 A M-1 cm-2 的高灵敏度、2.0 × 10-6 至 2.0 × 10-3 M 的宽线性检测范围、1.0 × 10-7 的低检测限M（信号/噪声=3），以及令人满意的稳定性和再现性。

更新日期：2020-11-13

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