4 years ago

Adsorption and Oxidation of Ethylene on the Stoichiometric and O-Rich RuO2(110) Surfaces

Adsorption and Oxidation of Ethylene on the Stoichiometric and O-Rich RuO2(110) Surfaces
Jason F. Weaver, Rahul Rai, Zhu Liang, Aravind Asthagiri, Minkyu Kim, Tao Li
We investigated the adsorption and oxidation of ethylene (C2H4) on stoichiometric and oxygen-rich RuO2(110) surfaces using temperature-programmed reaction spectroscopy (TPRS) and density functional theory (DFT) calculations. We find that C2H4 binds strongly on the coordinatively unsaturated (cus) Ru sites of RuO2(110), and desorbs in a peak at ∼315 K during TPRS. According to DFT, C2H4 initially adsorbs in a π-bonded configuration on atop Rucus sites but converts to a more stable di-σ species of the form C2H4O, prior to desorbing or reacting. Our TPRS results show that the stoichiometric RuO2(110) surface exhibits limited reactivity toward C2H4, whereas the O-rich surface is highly active toward promoting the extensive oxidation of C2H4. We find that the absolute yield of reacted C2H4 increases to a maximum with increasing initial coverage of on-top O atoms (Oot) on RuO2(110), and show that this behavior is accurately described by a model that assumes unit reaction probability of C2H4 molecules adsorbed at Rucus–Oot surface pairs. Our DFT calculations predict that the C–H bond cleavage of adsorbed C2H4 is energetically prohibitive on stoichiometric RuO2(110) relative to desorption, but that Obr–Rucus–Oot surface ensembles provide facile reaction pathways on O-rich RuO2(110), wherein C–H bond cleavage of adsorbed C2H4 is strongly preferred over desorption.

Publisher URL: http://dx.doi.org/10.1021/acs.jpcc.7b06865

DOI: 10.1021/acs.jpcc.7b06865

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