College of Chemistry, Chemical Engineering and Resource Utilization, Key Laboratory of Forest Plant Ecology, Northeast Forestry University, Harbin 150040, People's Republic of China.
Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun 130023, People's Republic of China.
Nano Lett. 2024 Jul 3;24(26):8071-8079. doi: 10.1021/acs.nanolett.4c01846. Epub 2024 Jun 20.
Single-atom nanozymes (SANs) are considered to be ideal substitutes for natural enzymes due to their high atom utilization. This work reported a strategy to manipulate the second coordination shell of the Ce atom and reshape the carbon carrier to improve the oxidase-like activity of SANs. Internally, S atoms were symmetrically embedded into the second coordination layer to form a Ce-NS-C structure, which reduced the energy barrier for O reduction, promoted the electron transfer from the Ce atom to O atoms, and enhanced the interaction between the d orbital of the Ce atom and p orbital of O atoms. Externally, polymerization of mussel-inspired polydopamine on the precursor helps capture metal sources and protects the 3D structure of the carrier during pyrolysis. On the other hand, polyethylene glycol (PEG) modulated the interface of the material to enhance water dispersion and mass transfer efficiency. As a proof of concept, the constructed PEG@P@Ce-N/S-C was applied to the multimodal assay of butyrylcholinesterase activity.
单原子纳米酶 (SANs) 由于其高原子利用率，被认为是天然酶的理想替代品。本工作报道了一种操纵 Ce 原子第二配位壳并重塑碳载体以提高 SANs 氧化酶样活性的策略。在内部，S 原子对称地嵌入到第二配位层中，形成 Ce-NS-C 结构，降低了 O 还原的能量势垒，促进了 Ce 原子向 O 原子的电子转移，并增强了 Ce 原子的 d 轨道和 O 原子的 p 轨道之间的相互作用。在外部，贻贝启发的聚多巴胺在前驱体上聚合有助于在热解过程中捕获金属源并保护载体的 3D 结构。另一方面，聚乙二醇 (PEG) 调节材料的界面以增强水的分散性和质量转移效率。作为概念验证，构建的 PEG@P@Ce-N/S-C 被应用于丁酰胆碱酯酶活性的多模态测定。
