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微等离子体诱导的原位快速合成 CoSe 纳米球@ZIF-67 衍生的 N 掺杂聚合物碳点用于高灵敏多巴胺检测。

Microplasma-induced in situ rapid synthesis of CoSe nanosphere@N-doped polymeric carbon dots derived from ZIF-67 for highly sensitive dopamine detection.

机构信息

Key Laboratory of Land Resources Evaluation and Monitoring in Southwest, Ministry of Education, College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610068, China.

Key Lab of Process Analysis and Control of Sichuan Universities, Yibin University, Yibin, 644000, China.

出版信息

Anal Chim Acta. 2024 Nov 15;1329:343236. doi: 10.1016/j.aca.2024.343236. Epub 2024 Sep 11.

Abstract

BACKGROUND

Designing a fast and sensitive electrochemical sensing platform to achieve selective quantitative detection of dopamine (DA) is a great challenge. Combining transition metal selenides (TMSs) with a variety of conductive carbonaceous materials is one of the effective strategies to improve the electrocatalytic activity of TMSs. However, most of the reported preparation methods of TMSs/carbon-based composite nanomaterials need to be annealed at a high temperature for a long time, which does not meet the requirements of sustainable development. Therefore, it is of great significance to explore an energy-efficient and fast method to prepare these compounds.

RESULTS

In this work, CoSe nanosphere@nitrogen-doped polymeric carbon dots are rapid prepared using ZIF precursor by simple dielectric barrier discharge (DBD) microplasma-induced on carbon cloth (CoSe NSs@N-PCDs/CC) for the first time. Owing to the fact that CoSe can promote rapid proton transfer, N-CDs has a high specific surface area, rich functional groups and electrical conductivity, this electrode exhibits highly sensitive non-enzymatic electrochemical sensing performance for DA detection. The linear range and detection limit are 0.1 μM-50 μM and 40.2 nM, respectively, and it have been successfully applied to the determination of DA levels in real human serum samples. Theoretical DFT calculations show that the most efficient interaction with DA on the surface of CoSe (101) can promote electrochemical reactions and catalyze DA oxidation.

SIGNIFICANCE

Using ZIF as precursor, CoSe NSs@N-PCDs/CC electrochemical electrode was synthesized in situ by simple and energy-saving DBD microplasma. CoSe NSs can effectively prevent the aggregation of function-rich N-PCDs and significantly improve the electrocatalytic activity of the composite. The mechanism of high selectivity of CoSe NSs@N-PCDs/CC electrode to DA was studied by DFT calculation. This work provides a new idea for the fast and green synthesis of transition metal and carbon-based nanomaterials by microplasma.

摘要

背景

设计快速灵敏的电化学传感平台以实现对多巴胺(DA)的选择性定量检测是一项巨大的挑战。将过渡金属硒化物(TMSs)与各种导电碳质材料结合是提高 TMSs 电催化活性的有效策略之一。然而,大多数报道的 TMSs/基于碳的复合纳米材料的制备方法需要在高温下长时间退火,这不符合可持续发展的要求。因此,探索一种节能且快速的方法来制备这些化合物具有重要意义。

结果

在这项工作中,首次使用 ZIF 前体制备了 CoSe 纳米球@氮掺杂聚合物碳点(CoSe NSs@N-PCDs/CC),通过简单的介电阻挡放电(DBD)微等离子体在碳布上快速制备。由于 CoSe 可以促进快速质子转移,N-CDs 具有高比表面积、丰富的官能团和导电性,因此该电极对 DA 检测表现出高度灵敏的非酶电化学传感性能。线性范围和检测限分别为 0.1 μM-50 μM 和 40.2 nM,已成功应用于真实人血清样品中 DA 水平的测定。理论 DFT 计算表明,在 CoSe(101)表面与 DA 最有效的相互作用可以促进电化学反应并催化 DA 氧化。

意义

使用 ZIF 作为前体,通过简单且节能的 DBD 微等离子体原位合成 CoSe NSs@N-PCDs/CC 电化学电极。CoSe NSs 可以有效防止富含功能的 N-PCDs 的聚集,并显著提高复合材料的电催化活性。通过 DFT 计算研究了 CoSe NSs@N-PCDs/CC 电极对 DA 具有高选择性的机制。这项工作为通过微等离子体快速绿色合成过渡金属和基于碳的纳米材料提供了新的思路。

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