Porous Oxyhydroxide Derived from Metal–Organic Frameworks as Efficient Triphosphatase-like Nanozyme for Chromium(III) Ion Colorimetric Sensing,ACS Applied Bio Materials

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Porous Oxyhydroxide Derived from Metal–Organic Frameworks as Efficient Triphosphatase-like Nanozyme for Chromium(III) Ion Colorimetric Sensing
ACS Applied Bio Materials ( IF 4.6 ) Pub Date : 2021-08-18 , DOI: 10.1021/acsabm.1c00628
Yuhao Xiong _{1,

2} , Linjing Su ₂ , Fanggui Ye ₁ , Shulin Zhao ₁

Affiliation

The dephosphorylation that involves the removal of a phosphate group from a substrate molecule plays a significant role in living organisms. An enzyme mimic (nanozyme) with phosphatase-like catalytic activity has recently received attention in terms of its capacity for dephosphorylation. In this study, three types of highly porous oxyhydroxide with remarkable triphosphatase-like catalytic activities, ZrOOH, GdOOH, and HfOOH, have been prepared through the transformation of metal–organic frameworks (MOFs) using a simple alkaline hydrolysis method. The triphosphatase mimetic activities of ZrOOH, GdOOH, and HfOOH were then thoroughly investigated and verified. In particular, an isotopic tracing experiment revealed that abundant surface hydroxyls could serve as nucleophilic agents to directly attack the electropositive phosphorus atom, causing the cleavage of the terminal phosphoester bonds of phosphoester substrate molecules. The kinetic analysis provided calculated values of K_m of 105.7, 90.5, and 46.1 μM, while the V_max values were 3.57, 4.76, and 2.74 × 10^–8 M s^–1 and E_a values were estimated to be 47.52, 41.15, and 52.79 kJ/mol for ZrOOH, GdOOH, and HfOOH, respectively. The chromium(III) ions acting as “poisoning” inhibitors efficiently downregulated the triphosphatase mimetic activity of GdOOH. On the basis of this effect, a colorimetric chromium(III) ion-sensing system was explored, which provided a relevant linear response range for the detection of chromium(III) ions of 5.0–200 μM and a low detection limit of 0.84 μM. This work not only shows the great potential of ZrOOH, GdOOH, and HfOOH as triphosphatase nanozymes but also deepens our understanding of the role of surface hydroxyls on phosphatase-mimicking nanozyme catalytic dephosphorization, which could be used in the rational design of phosphatase-mimicking nanozymes. Furthermore, the developed colorimetric sensing system could be applied to chromium(III) ion detection in biological systems.

中文翻译：

金属-有机骨架衍生的多孔羟基氧化物作为高效的三磷酸酶类纳米酶用于铬 (III) 离子比色传感

涉及从底物分子中去除磷酸基团的去磷酸化在活生物体中起着重要作用。具有磷酸酶样催化活性的酶模拟物（纳米酶）最近因其去磷酸化能力而受到关注。在本研究中，通过使用简单的碱性水解方法转化金属有机骨架（MOF），制备了三种具有显着类三磷酸酶催化活性的高孔羟基氧化物 ZrOOH、GdOOH 和 HfOOH。然后彻底研究和验证 ZrOOH、GdOOH 和 HfOOH 的三磷酸酶模拟活性。特别是，同位素示踪实验表明，丰富的表面羟基可以作为亲核试剂直接攻击带正电的磷原子，导致磷酸酯底物分子的末端磷酸酯键断裂。动力学分析提供了计算值K _m为 105.7、90.5 和 46.1 μM，而V_最大值为 3.57、4.76 和 2.74 × 10 ^–8 M s ^–1和E _aZrOOH、GdOOH 和 HfOOH 的值估计分别为 47.52、41.15 和 52.79 kJ/mol。作为“中毒”抑制剂的铬 (III) 离子有效地下调了 GdOOH 的三磷酸酶模拟活性。基于这种效应，探索了一种比色铬（III）离子传感系统，该系统为检测铬（III）离子提供了5.0-200 μM的相关线性响应范围和0.84 μM的低检测限。该工作不仅展示了 ZrOOH、GdOOH 和 HfOOH 作为三磷酸酶纳米酶的巨大潜力，而且加深了我们对表面羟基在模拟磷酸酶纳米酶催化脱磷中的作用的理解，可用于磷酸酶模拟纳米酶的合理设计. 此外，

更新日期：2021-09-20

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