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具有可控电活性的 RuCu 笼/合金纳米粒子,用于特定的电化学生物传感应用。

RuCu Cage/Alloy Nanoparticles with Controllable Electroactivity for Specific Electroanalysis Applications.

机构信息

Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, International Joint Research Center for Photoresponsive Molecules and Materials, School of Chemical and Material Engineering, Jiangnan University, Wuxi, Jiangsu 214122, China.

出版信息

Anal Chem. 2021 Sep 28;93(38):13080-13088. doi: 10.1021/acs.analchem.1c03182. Epub 2021 Sep 15.

Abstract

Electrochemical nanotags with controllable and multiresponse electroactivity have a great capacity for overcoming the drawbacks of limited target monitoring and inaccurate detection results for electrochemical sensors. In this contribution, double electro-oxidative Ru and Cu metals were integrated into RuCu nanostructures for the generation of dual electro-oxidative signals. A facial approach was proposed for the controllable fabrication of RuCu cage nanoparticles (NPs) and RuCu alloy NPs by simply adjusting the pH value of the reaction system. RuCu cage NPs and RuCu alloy NPs demonstrated inherent different electro-oxidative responses owing to the remarkable distinction of structures with different metal valences. RuCu cage NPs showed a single electro-oxidization peak at 0.84 V, assigned to the exposure of more Ru electroactive sites on the hollow cage structures. RuCu alloy NPs illustrated dual electro-oxidization peak at 0.84 and -0.16 V, attributing to the presence of Ru and Cu electroactive sites on the alloy structures, respectively. RuCu cage NPs and RuCu alloy NPs served as specific electroactive tags, achieving the selective monitoring of NaS and ratiometric electrochemical detection of xanthine in monosodium glutamate, respectively. The limits of detection were as low as 27 pM for NaS and 70 nM for xanthine. The rational design of multimetal nanostructures holds enormous potential for the generation of multiresponse electroactivity with the impetus for exploring the capacity of specific electrochemical sensing.

摘要

具有可控多响应电活性的电化学纳米标签在克服电化学传感器对目标监测的局限性和检测结果的不准确性方面具有巨大的潜力。在本研究中,双电化学氧化的 Ru 和 Cu 金属被整合到 RuCu 纳米结构中,以产生双电化学氧化信号。提出了一种简便的方法,通过简单调节反应体系的 pH 值,可控地制备 RuCu 笼状纳米颗粒(NPs)和 RuCu 合金 NPs。由于不同金属价态的结构有显著的区别,RuCu 笼状 NPs 和 RuCu 合金 NPs 表现出固有的不同电氧化响应。RuCu 笼状 NPs 在 0.84 V 处显示出单个电氧化峰,归因于空心笼状结构上更多 Ru 电活性位点的暴露。RuCu 合金 NPs 在 0.84 V 和-0.16 V 处呈现出双电氧化峰,分别归因于合金结构上存在 Ru 和 Cu 电活性位点。RuCu 笼状 NPs 和 RuCu 合金 NPs 作为特定的电活性标签,分别实现了对 NaS 的选择性监测和对谷氨酸单钠中黄嘌呤的比率型电化学检测。对 NaS 的检测限低至 27 pM,对黄嘌呤的检测限低至 70 nM。多金属纳米结构的合理设计为产生多响应电活性提供了巨大的潜力,为探索特定电化学传感的能力提供了动力。

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