In situ monitoring multi-carbon alcohol oxidation by combined electrochemistry with spatially selective NMR spectroscopy

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2023-10-01 DOI:10.1016/S1872-2067(23)64526-7
Haolin Zhan , Lifei Ji , Shuohui Cao , Ye Feng , Yanxia Jiang , Yuqing Huang , Shigang Sun , Zhong Chen
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Abstract

In situ electrochemical nuclear magnetic resonance (EC-NMR) plays a pivotal role in electrochemical observation on liquid fuel cells, but its applications are generally trapped by insufficient spectral resolution caused by spatiotemporal variations of magnetic fields. Herein, we develop a general spectroelectrochemistry protocol to address this problem and facilitate real-time electrooxidation analyses. This protocol enables the direct extraction of well-resolved and undistorted NMR signals from standard NMR instruments, thus it is commonly applicable to in situ electrochemical studies. The effectiveness for electrooxidation mechanism investigations on multi-carbon alcohols is validated by 1-butanol electrooxidation. It is verified that the direct oxidation of 1-butanol to butyric acid becomes more significant along with higher potentials on Pt/C at 60 °C, while 1-butanol oxidation is more likely to yield gaseous products (mainly CO2) at lower potentials. Additionally, this protocol reveals that Pt/C rather than PtRu/C is inclined to accomplish the β -C–H bond breaking process for CO2 generation at a high potential of 1.2 V (vs. SCE) . Therefore, this study provides a promising paradigm for electrooxidation investigations on fuel cells, and it may take a meaningful step toward wider electrochemical studies and NMR applications.

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电化学与空间选择核磁共振相结合原位监测多碳醇氧化
原位电化学核磁共振(EC-NMR)在液体燃料电池的电化学观测中发挥着关键作用,但其应用通常因磁场的时空变化导致光谱分辨率不足而受阻。在此,我们开发了一个通用的光谱电化学协议来解决这个问题,并促进实时电氧化分析。该方案能够从标准NMR仪器中直接提取分辨率良好且未失真的NMR信号,因此通常适用于原位电化学研究。通过1-丁醇电氧化验证了多碳醇电氧化机理研究的有效性。经验证,在60°C下,随着Pt/C上电位的升高,1-丁醇直接氧化为丁酸变得更加显著,而在较低电位下,1-丁醇氧化更有可能产生气态产物(主要是CO2)。此外,该方案表明,Pt/C而不是PtRu/C倾向于在1.2 V(vs.SCE)的高电势下完成CO2生成的β-C–H键断裂过程。因此,这项研究为燃料电池的电氧化研究提供了一个有前景的范式,并可能朝着更广泛的电化学研究和NMR应用迈出有意义的一步。
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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