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CO as a Probe Molecule to Study Surface Adsorbates during Electrochemical Oxidation of Propene
ChemElectroChem ( IF 4 ) Pub Date : 2020-12-10 , DOI: 10.1002/celc.202001162
Anna Winiwarter 1, 2 , Michael J. Boyd 3, 4 , Soren B. Scott 1, 5 , Drew C. Higgins 3, 4, 6 , Brian Seger 1 , Ib Chorkendorff 1 , Thomas F. Jaramillo 3, 4
Affiliation  

A major challenge in the electrochemical oxidation of hydrocarbons is understanding the formation of intermediate species, some of which continue to react, while others are non‐reactive or poisonous species that block adsorption of further reactants. Herein we investigate the identity and behavior of adsorbates formed during partial oxidation of propene. We employ two techniques: Electrochemistry‐Mass Spectrometry (EC‐MS) and Attenuated Total Reflection Infrared Spectroscopy (ATR‐FTIR). In both cases, we use CO as a probe molecule, to perturb the ad‐layer of propene intermediates. In the EC‐MS experiments, propene and its intermediates were quantified by triggering their desorption via displacement with CO. We show evidence for at least two distinct classes of propene adsorbates, via CO displacement and electrochemical stripping. A redshift in the ν(C−O) mode was observed, during IR spectroscopy, reflecting the chemical environment arising from strongly bound propene intermediates.

中文翻译:

CO作为探针分子,用于研究丙烯电化学氧化过程中的表面吸附物

碳氢化合物电化学氧化的一个主要挑战是了解中间物质的形成,其中一些继续反应,而另一些则是非反应性或有毒物质,阻碍了其他反应物的吸附。本文中,我们研究了丙烯部分氧化过程中形成的吸附物的特性和行为。我们采用两种技术:电化学质谱法(EC-MS)和衰减全反射红外光谱法(ATR-FTIR)。在这两种情况下,我们都使用CO作为探针分子,以扰动丙烯中间体的吸附层。在EC-MS实验中,通过用CO置换触发脱附来量化丙烯及其中间体。我们通过CO置换和电化学汽提显示了至少两类不同类型的丙烯吸附物的证据。
更新日期:2021-01-16
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