Chemisorbed oxygen or surface oxides steer the selectivity in Pd electrocatalytic propene oxidation observed by operando Pd L-edge X-ray absorption spectroscopy
| العنوان: | Chemisorbed oxygen or surface oxides steer the selectivity in Pd electrocatalytic propene oxidation observed by operando Pd L-edge X-ray absorption spectroscopy |
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| المؤلفون: | Koroidov, Sergey, Winiwarter, Anna, Diaz-Morales, Oscar, Görlin, Mikaela, Stenlid, Joakim Halldin, Wang, Hsin-Yi, Börner, Mia, Goodwin, Christopher Matthew, Soldemo, Markus, Pettersson, Lars Gunnar Moody, Rossmeisl, Jan, Hansson, Tony, Chorkendorff, Ib, Nilsson, Anders |
| المصدر: | StandUp Catalysis Science & Technology. 11(10):3347-3352 |
| الوصف: | Controlled electrochemical oxidation of hydrocarbons to desired products is an attractive approach in catalysis. Here we study the electrochemical propene oxidation under operando conditions using Pd L-edge X-ray absorption spectroscopy (XAS) as a sensitive probe to elucidate surface processes occurring during catalysis. Together with ab initio multiple-scattering calculations, our XAS results enable assignment of characteristic changes of the Pd L-edge intensity and energy position in terms of a mechanistic understanding of the selective oxidation of propene. The results, supported by electrochemical density functional theory DFT simulations, show that in the potential range of 0.8-1.0 V vs. the reversible hydrogen electrode (RHE), selective oxidation of propene to acrolein and acrylic acid occurs on the metallic Pd surface. These reactions are proposed to proceed via the Langmuir-Hinshelwood mechanism. In contrast, for the potential range of 1.1-1.3 V vs. RHE, selective oxidation of propene to propylene glycol takes place on a Pd oxide surface. |
| وصف الملف: | electronic |
| URL الوصول: | https://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-444387 https://doi.org/10.1039/d0cy02134b https://uu.diva-portal.org/smash/get/diva2:1561542/FULLTEXT01.pdf |
| قاعدة البيانات: | SwePub |
| تدمد: | 20444753 |
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| DOI: | 10.1039/d0cy02134b |