Natural Enzyme-Inspired Design of the Single-Atom Cu Nanozyme as Dual-Enzyme Mimics for Distinguishing Total Antioxidant Capacity and the Ascorbic Acid Level,Analytical Chemistry

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Natural Enzyme-Inspired Design of the Single-Atom Cu Nanozyme as Dual-Enzyme Mimics for Distinguishing Total Antioxidant Capacity and the Ascorbic Acid Level
Analytical Chemistry ( IF 6.7 ) Pub Date : 2024-01-14 , DOI: 10.1021/acs.analchem.3c05245
Chenyu Tao ₁ , Yuanyuan Jiang ₁ , Shushu Chu ₁ , Yanrong Miao ₁ , Jiqing Zhang ₁ , Yizhong Lu ₁ , Li Niu _{2,

3}

Affiliation

Although various oxidase mimetic or peroxidase (POD) mimetic nanozymes have been extensively studied, their poor substrate selectivity significantly inhibits their practical applications. Nanozymes with specific biomolecules as substrates, especially ascorbic acid oxidase (AAO) mimetic nanozymes with ascorbic acid (AA) as a substrate, have scarcely been studied. Herein, inspired by the multi-Cu atom sites and the redox electron transfer pathway of Cu²⁺/Cu⁺ in the natural AAO, atomically dispersed Cu sites immobilized on N-doped porous carbon (Cu-N/C) are artificially designed to simulate the function of natural AAO. Compared with their natural counterparts, the Cu-N/C catalysts exhibited higher catalytic efficiency and superior stability. Combined theoretical calculation and experimental characterizations reveal that the Cu-N/C nanozymes could catalyze the AA oxidation through a 2e^– oxygen reduction pathway with H₂O₂ as the product. Moreover, the Cu-N/C nanozymes also possess high POD activity. As a proof-of-concept application, Cu-N/C can simultaneously realize AA detection in fluorescent mode based on its AAO activity and total antioxidant capacity detection in colorimetric mode utilizing its POD activity.

中文翻译：

受天然酶启发的单原子铜纳米酶设计作为双酶模拟物，用于区分总抗氧化能力和抗坏血酸水平

尽管各种氧化酶模拟或过氧化物酶（POD）模拟纳米酶已被广泛研究，但它们较差的底物选择性显着抑制了它们的实际应用。以特定生物分子为底物的纳米酶，特别是以抗坏血酸（AA）为底物的抗坏血酸氧化酶（AAO）模拟纳米酶，几乎没有被研究过。在此，受天然AAO中多Cu原子位点和Cu ²⁺ /Cu ⁺氧化还原电子转移途径的启发，人工设计了固定在N掺杂多孔碳（Cu-N/C）上的原子分散的Cu位点，以实现模拟天然AAO的功能。与天然催化剂相比，Cu-N/C催化剂表现出更高的催化效率和优异的稳定性。结合理论计算和实验表征表明，Cu-N/C纳米酶可以通过^2e-氧还原途径催化AA氧化，产物为H ₂ O ₂ 。此外，Cu-N/C纳米酶还具有高POD活性。作为概念验证应用，Cu-N/C 可以同时实现基于其 AAO 活性的荧光模式下的 AA 检测和利用其 POD 活性的比色模式下的总抗氧化能力检测。

更新日期：2024-01-14

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