Probing the Local Reaction Environment During High Turnover Carbon Dioxide Reduction with Ag-Based Gas Diffusion Electrodes.
Probing the Local Reaction Environment During High Turnover Carbon Dioxide Reduction with Ag-Based Gas Diffusion Electrodes.
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DOI：
10.1002/chem.202100387
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发表时间：
2021-04-01
期刊：
影响因子：
--
通讯作者：
Schuhmann W
中科院分区：
文献类型：
--
作者：
Dieckhöfer S;Öhl D;Junqueira JRC;Quast T;Turek T;Schuhmann W
了解电化学反应对电极微环境的影响是涉及OH−产生和水消耗的电化学反应不可避免的话题。这对于二氧化碳还原反应（CO2 RR）来说尤其如此，它与竞争性析氢反应（HER）一起在局部OH-和H2O活性中产生变化，这反过来可能影响CO2 RR的活性，稳定性和选择性。我们使用气相色谱法通过产物分析确定了靠近CO2转换Ag基气体扩散电极（GDE）的局部OH−和H2O活性。使用基于剪切力的扫描电化学显微镜（SECM）接近曲线将Pt纳米传感器定位在工作GDE附近，这允许通过Pt尖端纳米传感器处的动电位测量来监测在否则不可接近的多孔GDE内进行的反应引起的变化。我们表明，高营业额HER/CO2 RR在GDE导致调制的局部电解质的碱度，这类似于一个16 m的KOH溶液，变化，这反过来又与反应的选择性。 地方情：现代电化学中气体扩散电极（GDE）的数量急剧增加，特别是随着人们对CO2电化学还原的兴趣日益增加。由于这些电极和反应的几个方面尚未澄清，我们在本文中将局部反应环境的评估与基于Ag的GDE的析氢/CO2还原反应系统的实际产物分布相结合。
Discerning the influence of electrochemical reactions on the electrode microenvironment is an unavoidable topic for electrochemical reactions that involve the production of OH− and the consumption of water. That is particularly true for the carbon dioxide reduction reaction (CO2RR), which together with the competing hydrogen evolution reaction (HER) exert changes in the local OH− and H2O activity that in turn can possibly affect activity, stability, and selectivity of the CO2RR. We determine the local OH− and H2O activity in close proximity to a CO2‐converting Ag‐based gas diffusion electrode (GDE) with product analysis using gas chromatography. A Pt nanosensor is positioned in the vicinity of the working GDE using shear‐force‐based scanning electrochemical microscopy (SECM) approach curves, which allows monitoring changes invoked by reactions proceeding within an otherwise inaccessible porous GDE by potentiodynamic measurements at the Pt‐tip nanosensor. We show that high turnover HER/CO2RR at a GDE lead to modulations of the alkalinity of the local electrolyte, that resemble a 16 m KOH solution, variations that are in turn linked to the reaction selectivity. Local affection: The abundance of gas diffusion electrodes (GDE) in modern electrochemistry has grown drastically, especially with the increasing interest in electrochemical reduction of CO2. Since several aspects of those electrodes and that reaction are not clarified yet, we herein couple assessment of the local reaction environment to the actual product distribution of the hydrogen evolution/CO2 reduction reaction system at Ag‐based GDEs.
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影响因子：
12.9
作者：
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10.1016/j.cep.2011.11.003
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