The ionic liquid 1‐ethyl‐3‐methylimidazolium ethylsulfate [EMIM][EtOSO3] was supported on Pd‐Al2O3 to yield a solid catalyst with ionic liquid layer (SCILL) material. During the hydrogenation of ethene, it was found that ethene was incorporated into the imidazolium moiety in a reaction catalyzed by the palladium surface. The formation of 1,2‐diethyl‐3‐methylimidazolium ethylsulfate was confirmed ex situ by means of NMR spectroscopy. Moreover, the reaction itself could be monitored in situ by diffuse reflection infrared Fourier transformation (DRIFT) spectroscopy. A reaction mechanism involving surface carbene species was proposed on the basis of the analytical data.
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