Mo Single-Atom Nanozyme Anchored to the 2D N-Doped Carbon Film: Catalytic Mechanism, Visual Monitoring of Choline, and Evaluation of Intracellular ROS Generation,ACS Applied Materials & Interfaces

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Mo Single-Atom Nanozyme Anchored to the 2D N-Doped Carbon Film: Catalytic Mechanism, Visual Monitoring of Choline, and Evaluation of Intracellular ROS Generation
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-07-19 , DOI: 10.1021/acsami.3c04761
Qijun Sun ₁ , Xiaoyu Xu ₁ , Song Liu ₁ , Xinzhao Wu ₂ , Chenhui Yin ₁ , Meng Wu ₁ , Yuxue Chen ₁ , Na Niu ₁ , Ligang Chen ₁ , Fuquan Bai ₂

Affiliation

Single-atom nanozymes (SANs) have attracted great attention in constructing devices for instant biosensing due to their excellent stability and atom utilization. Here, Mo atoms were immobilized in 2D nitrogen-doped carbon films by cascade-anchored one-pot pyrolysis to obtain Mo single-atom nanozyme (Mo-SAN) with high atomic loading (4.79 wt %) and peroxidase-like activity. The coordination environment and enzyme-like activity mechanism of Mo-SAN were studied by combining synchrotron radiation and density functional theory. The strong oxophilicity of single-atom Mo makes the catalytic center more capable of transferring electrons to free radicals to selectively generate ^•OH in the presence of H₂O₂. Choline oxidase and Mo-SAN were used as signal opening unit and signal amplification unit, respectively. Combining the portability and visualization functions of smartphone and test strips, a paper-based visual sensing platform was constructed, which can accurately identify choline at a concentration of 0.5–35 μM with a limit of detection as low as 0.12 μM. The recovery of human serum samples was 96.4–102.2%, with an error of less than 5%. Furthermore, the potential of Mo-SAN to efficiently generate toxic ^•OH in tumor cells was intuitively confirmed. This work provides a technical and theoretical basis for designing highly active SANs and detecting neurological markers.

中文翻译：

锚定在二维 N 掺杂碳膜上的 Mo 单原子纳米酶：催化机制、胆碱的可视化监测以及细胞内 ROS 生成的评估

单原子纳米酶（SAN）由于其优异的稳定性和原子利用率，在构建即时生物传感设备方面引起了极大的关注。在此，通过级联锚定一锅热解将Mo原子固定在二维氮掺杂碳膜中，获得具有高原子负载量（4.79 wt%）和类过氧化物酶活性的Mo单原子纳米酶（Mo-SAN）。结合同步辐射和密度泛函理论研究了Mo-SAN的配位环境和类酶活性机制。_{单原子Mo的强亲氧性使得催化中心在H 2} O ₂存在下更能够将电子转移给自由基选择性地生成^· OH 。胆碱氧化酶和Mo-SAN分别用作信号开放单元和信号放大单元。结合智能手机和试纸的便携性和可视化功能，构建了纸基视觉传感平台，可以准确识别浓度为0.5-35μM的胆碱，检测限低至0.12μM。人血清样品回收率为96.4%~102.2%，误差小于5%。此外，直观地证实了Mo-SAN 在肿瘤细胞中有效产生有毒^•· OH的潜力。该工作为设计高活性SANs和检测神经标志物提供了技术和理论基础。

更新日期：2023-07-19

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