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在单个纳米颗粒电极上监测二硫化钼量子点催化的析氢反应。

Monitoring Hydrogen Evolution Reaction Catalyzed by MoS Quantum Dots on a Single Nanoparticle Electrode.

作者信息

Lu Si-Min, Li Yuan-Jie, Zhang Jian-Fang, Wang Yan, Ying Yi-Lun, Long Yi-Tao

机构信息

School of Chemistry and Molecular Engineering , East China University of Science and Technology , Shanghai 200237 , P. R. China.

School of Materials Science and Engineering, Key Laboratory of Advanced Functional Materials and Devices of Anhui Province , Hefei University of Technology , Hefei 230009 , P. R. China.

出版信息

Anal Chem. 2019 Aug 20;91(16):10361-10365. doi: 10.1021/acs.analchem.9b02364. Epub 2019 Aug 5.

Abstract

Hydrogen evolution reaction (HER) catalyzed by molybdenum sulfide quantum dots (MoS QDs) has attracted extensive attention in the energy field. Monitoring HER catalyzed by MoS QDs based on a glass nanopore with an electrochemically confined effect was proposed for the first time. MoS QDs inside the glass nanopore is driven toward the orifice of the nanopore and bonded with the Ag nanoparticles (Ag NPs) to form a single nanocomposite. When enough voltage is applied across the orifice, the single Ag NP acts as a single nanoparticle electrode to conduct the electrochemically bipolar reaction on its two extremities. In the process, HER is catalyzed by MoS QDs, and Ag NPs are oxidized at the same time. The appearance of blockages on the elevated ionic current is attributed to the generation of a H bubble. Furthermore, by analyzing the modulations in the ionic current oscillation, the frequency of hydrogen bubble generation that is related to the catalytic efficiency of MoS QDs could be estimated. The results reveal the capability of the glass nanopore for the real-time monitoring electrocatalytic behavior, which makes the glass nanopore an ideal candidate to further reveal the heterogeneity of catalytic capability at the single particle level.

摘要

硫化钼量子点(MoS QDs)催化的析氢反应(HER)在能源领域引起了广泛关注。首次提出基于具有电化学限制效应的玻璃纳米孔监测MoS QDs催化的HER。玻璃纳米孔内的MoS QDs被驱动至纳米孔口并与银纳米颗粒(Ag NPs)结合形成单一纳米复合材料。当在孔口施加足够电压时,单个Ag NP充当单个纳米颗粒电极在其两端进行电化学双极反应。在此过程中,HER由MoS QDs催化,同时Ag NPs被氧化。离子电流升高时出现的堵塞现象归因于H气泡的产生。此外,通过分析离子电流振荡中的调制情况,可以估算与MoS QDs催化效率相关的氢气泡产生频率。结果揭示了玻璃纳米孔实时监测电催化行为的能力,这使得玻璃纳米孔成为进一步揭示单颗粒水平催化能力异质性的理想候选者。

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