第一种超薄纯多金属氧酸盐二维材料作为过氧化物酶模拟催化剂用于检测氧化应激生物标志物,ACS Applied Materials & Interfaces

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第一种超薄纯多金属氧酸盐二维材料作为过氧化物酶模拟催化剂用于检测氧化应激生物标志物
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-12-28 , DOI: 10.1021/acsami.2c15579
Jun Jiang ₁ , Yanzhou Li ₁ , Lulu Liu ₁ , Lijuan Chen ₁ , Junwei Zhao ₁ , Carsten Streb ₂ , Yu-Fei Song ₃

Affiliation

尽管具有超薄几何形状和非凡电学特性的二维 (2D) 材料引起了广泛关注，但开发新型二维材料仍然是一个巨大的挑战。在这项工作中，通过超声剥离一维 (1D) 链异金属结晶锗钨酸盐 Na ₄ [Ho(H ₂ O) ₆ ] ₂制备了前所未有的单层纯多金属氧酸盐 (POM) 二维材料 (2D- 1 ) [Fe ₄ (H ₂ O) ₂ (pic) ₆ Ge ₂ W ₂₀ O ₇₂ ]·16H ₂ O ( 1) (Hpic = 吡啶甲酸)。1的一维聚合链由特定的 {Ge ₂ W ₂₀ } 基 [Fe ₄ (H ₂ O) ₂ (pic) ₆ Ge ₂ W ₂₀ O ₇₂ ] ^10–链段通过桥接 [Ho(H ₂ O) ₆ ] ³⁺阳离子。2D- 1是由 1 的相邻一维聚合链之间的 π-π 相互作用驱动力形成的。此外，2D- 1的过氧化物酶模拟特性可用于检测 H ₂ O ₂进行了评估，并观察到良好的检测结果，检测限 (LOD) 为 58 nM。密度泛函理论 (DFT) 计算进一步证实 2D- 1具有出色的催化活性，活性位点位于 Fe 中心和 Hpic 配体上。在尿酸酶的催化下，尿酸可转化为尿囊素和H ₂ O ₂，然后H ₂ O _2在2D-1作为催化剂存在下将TMB氧化成蓝色ox-TMB 。然后，我们利用这种级联反应检测尿酸，结果也很突出。该研究为制备超薄纯 POM 二维材料打开了一扇大门，并拓宽了 POM 在生物学和医学领域的潜在应用范围。

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First Ultrathin Pure Polyoxometalate 2D Material as a Peroxidase-Mimicking Catalyst for Detecting Oxidative Stress Biomarkers

Although two-dimensional (2D) materials with ultrathin geometry and extraordinary electrical attributes have attracted substantial concern, exploiting new-type 2D materials is still a great challenge. In this work, an unprecedented single-layer pure polyoxometalate (POM) 2D material (2D-1) was prepared by ultrasonically exfoliating a one-dimensional (1D)-chain heterometallic crystalline germanotungstate Na₄[Ho(H₂O)₆]₂[Fe₄(H₂O)₂(pic)₆Ge₂W₂₀O₇₂]·16H₂O (1) (Hpic = picolinic acid). The 1D polymeric chain of 1 is assembled from particular {Ge₂W₂₀}-based [Fe₄(H₂O)₂(pic)₆Ge₂W₂₀O₇₂]^10– segments through bridging [Ho(H₂O)₆]³⁺ cations. 2D-1 is formed by π–π interaction driving force among adjacent 1D polymeric chains of 1. Also, the peroxidase-mimicking properties of 2D-1 toward detecting H₂O₂ were evaluated and good detection result was observed with a limit of detection (LOD) of 58 nM. Density functional theory (DFT) calculation further confirms that 2D-1 displays outstanding catalytic activity and active sites are located on Fe centers and Hpic ligands. Under the catalysis of uricase, uric acid can be transformed to allantoin and H₂O₂, and then, H₂O₂ oxidizes TMB to its blue ox-TMB in the presence of 2D-1 as a catalyst. Then, we utilized this cascade reaction to detect uric acid, which also exhibits prominent results. This research opens a door to prepare ultrathin pure POM 2D materials and broadens the scope of potential applications of POMs in biology and iatrology.

更新日期：2022-12-28

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