Department of Applied Chemistry, College of Life Science , Fujian Agriculture and Forestry University , Fuzhou , Fujian 350002 , People's Republic of China.
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter , Chinese Academy of Sciences , Fuzhou 350002 , People's Republic of China.
Inorg Chem. 2018 Aug 6;57(15):9096-9104. doi: 10.1021/acs.inorgchem.8b01097. Epub 2018 Jul 11.
Natural enzyme mimetics with high catalytic activity at nearly neutral pH values are highly desired for their applications in biological systems. Herein for the first time a stable MOF, namely MOF-808, has been shown to possess high intrinsic peroxidase-like catalytic activity under acidic, neutral, and alkaline conditions. As a novel peroxidase mimetic, MOF-808 can effectively catalyze the oxidation of 3,3',5,5'-tetramethylbenzidine when HO serves as oxidant, accompanied by a significant color variation in the solution. The catalytic activity and the color variation were greatly dependent on HO concentration, and thus MOF-808 can be applied to the colorimetric sensing of HO. The HO detection limit is 4.5 μM, and the linear range is 10 μM to 15 mM. In view of the significant inhibition effect produced by ascorbic acid, a facile and sensitive approach for colorimetric sensing of ascorbic acid was successfully established. The AA detection limit is 15 μM, and the linear range is 30-1030 μM. Further investigation found that the catalytic activity of MOF-808 could be mainly ascribed to the Zr-OH(OH) groups. Such active Zr-OH(OH) groups can be effectively shielded by gluconic acid, and subsequently the catalytic activity of MOF-808 was significantly suppressed. With these findings, a facile and selective colorimetric assay for glucose sensing has been successfully explored via combination of the glucose oxidation with the TMB oxidation. The glucose detection limit is 5.7 μM, and the linear range is 5.7-1700 μM. MOF-808 is one of the best colorimetric biosensors among the peroxidase mimics reported for HO, AA, and glucose detection.
在生物系统中应用时,具有近中性 pH 值下高催化活性的天然酶模拟物是非常需要的。在此,首次表明稳定的 MOF(即 MOF-808)在酸性、中性和碱性条件下具有高固有过氧化物酶样催化活性。作为一种新型过氧化物酶模拟物,MOF-808 可以在 HO 作为氧化剂时有效催化 3,3',5,5'-四甲基联苯胺的氧化,同时溶液中的颜色发生明显变化。催化活性和颜色变化极大地依赖于 HO 的浓度,因此 MOF-808 可用于 HO 的比色检测。HO 的检测限为 4.5 μM,线性范围为 10 μM 至 15 mM。鉴于抗坏血酸产生的显著抑制作用,成功建立了一种用于比色检测抗坏血酸的简单灵敏方法。AA 的检测限为 15 μM,线性范围为 30-1030 μM。进一步的研究发现,MOF-808 的催化活性主要归因于 Zr-OH(OH)基团。这种活性 Zr-OH(OH)基团可以被葡萄糖酸有效地屏蔽,随后 MOF-808 的催化活性显著受到抑制。有了这些发现,通过将葡萄糖氧化与 TMB 氧化结合,成功探索了一种用于葡萄糖感测的简单选择性比色测定法。葡萄糖的检测限为 5.7 μM,线性范围为 5.7-1700 μM。MOF-808 是报道的用于 HO、AA 和葡萄糖检测的过氧化物酶模拟物中最好的比色生物传感器之一。