N 掺杂碳纳米管负载 Fe-Mn 双单原子纳米酶，协同增强过氧化物酶活性，用于乙酰胆碱酯酶及其抑制剂的灵敏比色检测,Analytical Chemistry

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N 掺杂碳纳米管负载 Fe-Mn 双单原子纳米酶，协同增强过氧化物酶活性，用于乙酰胆碱酯酶及其抑制剂的灵敏比色检测
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-05-23 , DOI: 10.1021/acs.analchem.3c01070
Yan-Wen Mao ₁ , Juan Zhang ₂ , Rui Zhang ₁ , Jia-Qi Li ₁ , Ai-Jun Wang ₁ , Xiao-Cheng Zhou ₂ , Jiu-Ju Feng ₁

Affiliation

监测乙酰胆碱酯酶 (AChE) 及其抑制剂对于神经系统疾病的早期诊断和治疗具有重要意义。在此，N 掺杂的碳纳米管负载 Fe-Mn 双单原子 (FeMn DSAs/N-CNTs) 是通过简单的热解制备的，正如一系列表征技术所彻底弄清楚的那样。_{通过催化氧化 3,3',5,5'-四甲基联苯胺 (TMB) 在 H 2} O ₂中产生丰富的羟基自由基 (·OH)，研究了 FeMn DSAs/N-CNTs 的类过氧化物酶活性系统，有效催化无色TMB氧化成蓝色氧化TMB（ox-TMB）。此外，硫代胆碱（来源于 AChE）大大削弱了过氧化物酶样活性，同时使 blue ox-TMB 褪色。令人印象深刻的是，密度泛函理论 (DFT) 计算进一步证明了高度改善的类过氧化物酶特性，其中双单原子显示出较低的能垒 (0.079 eV)，并且它们与 N-CNT 的相互作用对于产生氧自由基。凭借纳米酶，构建了一种低成本、特异性和灵敏的比色传感器，用于检测 AChE，具有更宽的线性范围 0.1–30 UL ^–1和检测下限（LOD，0.066 UL ^–1), 结合其在人血清样本中的可行性分析。此外，该平台还用于测量线性范围为 5–500 nM 且 LOD 低至 4.17 nM 的石杉碱甲抑制剂。该策略为早期临床诊断和药物开发提供了一种低成本且方便的方法。

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N-Doped Carbon Nanotubes Supported Fe–Mn Dual-Single-Atoms Nanozyme with Synergistically Enhanced Peroxidase Activity for Sensitive Colorimetric Detection of Acetylcholinesterase and Its Inhibitor

Monitoring acetylcholinesterase (AChE) and its inhibitors is of importance for early diagnosis and therapy of neurological diseases. Herein, N-doped carbon nanotubes supported Fe–Mn dual-single-atoms (FeMn DSAs/N-CNTs) were fabricated by a simple pyrolysis, as thoroughly figured out by a series of the characterization techniques. The peroxidase-like activity of FeMn DSAs/N-CNTs was investigated by catalytic oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to generate rich hydroxyl radicals (·OH) in the H₂O₂ system, which effectively catalyzed colorless TMB oxidation to blue oxidized TMB (ox-TMB). Besides, the peroxidase-like activity was greatly weakened by thiocholine (derived from AChE), accompanied by making blue ox-TMB fade. Impressively, the highly improved peroxidase-like property is further evidenced by density functional theory (DFT) calculations, where the dual-single atoms show a lower energy barrier (0.079 eV) and their interactions with the N-CNTs played critical roles for producing the oxygen radicals. By virtue of the nanozyme, a low-cost, specific, and sensitive colorimetric sensor was built for detection of AChE with a broader linear range of 0.1–30 U L^–1 and a lower limit of detection (LOD, 0.066 U L^–1), combined with its feasible analysis in human serum samples. Also, this platform was applied for measuring huperzine A inhibitor with a wide linear scope of 5–500 nM and a LOD down to 4.17 nM. This strategy provides a low-cost and convenient approach for early clinical diagnosis and drug development.

更新日期：2023-05-23

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