Ionic Liquid Sheath Stabilizes Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Complexes during Ethylene Hydrogenation Catalysis

An atomically dispersed reduced graphene aerogel (rGA)-supported iridium catalyst having reactive ethylene ligands was synthesized at an iridium loading of 9.9 wt % and coated with an ionic liquid, 1-ethyl-3-methylimidazolium acetate ([EMIM][OAc]). Continuous-scan X-ray absorption spectra demonstrated that the iridium remained site-isolated in flowing equimolar C2H4 and H-2 during a temperature ramp to 100 degrees C. The data further showed the lack of detectable iridium aggregation when the feed was H-2-rich or even pure H-2 at 100 degrees C. An Arrhenius plot determined for ethylene hydrogenation catalysis with the sample in flowing equimolar ethylene and hydrogen showed no variation in the apparent activation energy at temperatures up to 100 degrees C, confirming that the active sites remained intact at the higher temperatures. The results point to opportunities for overcoming the stability limitations of atomically dispersed supported noble metal catalysts by choice of electron-donor supports and ionic liquid sheaths.