Abstract
Operando Pd X-ray absorption spectroscopy elucidates how the surface oxygen species steer the selectivity in the electrochemical oxidation of propene.
Highlights
Controlled electrochemical oxidation of hydrocarbons to desired products is an attractive approach in catalysis
We focus on the anodic propene oxidation on Pd using Pd L3-edge X-ray absorption spectroscopy (XAS, for experimental details see Electronic supplementary information (ESI)†) under operando conditions
XAS has been used before to examine the electronic structure of catalytic intermediates,[13] as well as to probe catalysts in situ in electrochemistry with similar spectral resolution.[14]
Summary
Controlled electrochemical oxidation of hydrocarbons to desired products is an attractive approach in catalysis. 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. Propene (C3H6) is a simple HC molecule and an essential feedstock chemical for the synthesis of a large number of important chemicals and polymers.[4,5] Electrochemical oxidation of propene using noble-metal electrodes facilitates generation of a wide variety of products,[6,7,8,9,10] where one of the most promising electrocatalysts reported so far is Pd.[7,11] Electrochemical propene oxidation on Pd leads to the formation of several highly valuable and industrially relevant products such as acrolein, acrylic acid, and propylene glycol. This will in turn provide important information to guide the design for more efficient catalysts
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