Electro-carboxylation of butadiene and ethene over Pt and Ni catalysts
By Steinmann, Stephan N.; Michel, Carine; Schwiedernoch, Renate; Wu, Mengjia; Sautet, Philippe
Published in Journal of Catalysis
NULL
2016
Abstract
Abstract Electrochemical synthesis could provide an elegant and efficient means to exploit the largely available {C1} building block CO2. The electrocarboxylation of dienes is, in particular, an attractive goal. However, the presently known electrocatalysts are inefficient and not very selective since they work around ?2.3 V vs. SHE. In order to identify more active catalysts, we need to better understand the reaction mechanism. In this contribution, we present prototypical experimental results for the electrocarboxylation of 2,3-dimethyl-butadiene on a Ni catalyst and quantify the side-products, namely carbonates, oxalic and formic acid. Together with the extensive, state of the art, first principles investigation of the mechanism at the atomic scale, we reveal a highly activated process around the onset potential of ?1.3 V and a change in mechanism at the peak potential of ?2.3 V, suggesting that a more active catalyst could be engineered by modifying the morphology in order to facilitate the
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