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Adsorption and Electrochemistry of Carbon Monoxide at the Ionic Liquid-Pt Interface.
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2019-05-22 , DOI: 10.1021/acs.jpcb.8b11602 Yongan Tang 1 , Xiaojun Liu 1 , Jordan McMahan 1 , Anil Kumar 1 , Asim Khan 1 , Michael Sevilla 1 , Xiangqun Zeng 1
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2019-05-22 , DOI: 10.1021/acs.jpcb.8b11602 Yongan Tang 1 , Xiaojun Liu 1 , Jordan McMahan 1 , Anil Kumar 1 , Asim Khan 1 , Michael Sevilla 1 , Xiangqun Zeng 1
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In this work, CO adsorption and oxidation processes were studied with cyclic voltammetry and anodic adsorptive stripping chronoamperometry in two structural different ionic liquids (ILs) (i.e., 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide [Bmpy][NTf2] and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide [Bmim][NTf2]). Multiple redox processes were observed in the ILs. During the anodic oxidation processes, the NTf2- anion is oxidized to form NTf2• radical and CO is oxidized to CO2 and produces a proton in these ILs when a trace amount of water is present. The products of oxidation processes (NTf2• radical and proton) can be reduced at cathodic processes. Results show that the cation in these ILs can facilitate the formation of an electrolyte-electrode interface structure that influences the amount of CO adsorbed as well as the subsequent CO oxidation current and charge. By selecting the anodic and cathodic potentials, we developed an innovative electroanalytical method for CO sensing based on a simple double-potential adsorptive stripping chronoamperometry. The method allows calibration of the concurrent NTf2- anion and CO redox processes as well as the double-layer charging and discharging processes in the IL with the presence of a trace amount of water providing quantitative analysis of CO concentration with high accuracy and sensitivity. The reported method is the first work to show that quantitative CO detection can be achieved in the presence of complex dynamic interfacial processes in the ILs. The trace water present in the ILs is beneficial for CO oxidation, but a large amount of water is detrimental for the CO oxidation in ambient condition.
中文翻译：
一氧化碳在离子液体-Pt界面的吸附和电化学。
在这项工作中，使用循环伏安法和阳极吸附溶出计时电流法研究了两种结构不同的离子液体（即1-丁基-1-甲基吡咯烷鎓双（三氟甲基磺酰基）酰亚胺[Bmpy] [NTf2]和1-丁基-3-甲基咪唑鎓双（三氟甲基磺酰基）酰亚胺[Bmim] [NTf2]）。在IL中观察到多个氧化还原过程。在阳极氧化过程中，当存在痕量水时，NTf2-阴离子被氧化形成NTf2•自由基，CO被氧化成CO2并在这些IL中产生质子。氧化过程的产物（NTf2•自由基和质子）可在阴极过程中还原。结果表明，这些IL中的阳离子可以促进电解质-电极界面结构的形成，从而影响吸附的CO量以及随后的CO氧化电流和电荷。通过选择阳极和阴极电位，我们基于简单的双电位吸附剥离计时电流法开发了一种用于CO感测的创新电分析方法。该方法允许校准同时存在的NTf2-阴离子和CO氧化还原过程以及IL中的双层充放电过程，其中存在痕量水，从而以高精度和高灵敏度对CO浓度进行定量分析。报道的方法是证明在IL中存在复杂动态界面过程时可以实现定量CO检测的第一项工作。IL中存在的微量水有利于CO氧化，但大量水对环境条件下的CO氧化有害。
更新日期：2019-05-24
中文翻译：
一氧化碳在离子液体-Pt界面的吸附和电化学。
在这项工作中，使用循环伏安法和阳极吸附溶出计时电流法研究了两种结构不同的离子液体（即1-丁基-1-甲基吡咯烷鎓双（三氟甲基磺酰基）酰亚胺[Bmpy] [NTf2]和1-丁基-3-甲基咪唑鎓双（三氟甲基磺酰基）酰亚胺[Bmim] [NTf2]）。在IL中观察到多个氧化还原过程。在阳极氧化过程中，当存在痕量水时，NTf2-阴离子被氧化形成NTf2•自由基，CO被氧化成CO2并在这些IL中产生质子。氧化过程的产物（NTf2•自由基和质子）可在阴极过程中还原。结果表明，这些IL中的阳离子可以促进电解质-电极界面结构的形成，从而影响吸附的CO量以及随后的CO氧化电流和电荷。通过选择阳极和阴极电位，我们基于简单的双电位吸附剥离计时电流法开发了一种用于CO感测的创新电分析方法。该方法允许校准同时存在的NTf2-阴离子和CO氧化还原过程以及IL中的双层充放电过程，其中存在痕量水，从而以高精度和高灵敏度对CO浓度进行定量分析。报道的方法是证明在IL中存在复杂动态界面过程时可以实现定量CO检测的第一项工作。IL中存在的微量水有利于CO氧化，但大量水对环境条件下的CO氧化有害。
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