An integrated approach to Deacon chemistry on RuO2-based catalysts

• DOI: 10.1016/j.jcat.2011.09.039
• Publication Date: 2011-11-09T07:31:15Z
• Authors: Detre Teschner; Ramzi Farra; Lide Yao; Robert Schlögl; Hary Soerijanto; Reinhard Schomäcker; Timm Schmidt; László Szentmiklósi; Amol P. Amrute; Cecilia Mondelli; Javier Pérez-Ramírez; Gerard Novell-Leruth; Núria López
• Keywords: Reactivity

Rationally designed RuO2-based Deacon catalysts can contribute to massive energy saving compared the current electrolysis process in chemically recycling HCl produce molecular chlorine. Here, we report on our integrated approach between state-of-the-art experiments and calculations. The aim is understand industrial catalyst its realistic surface state derive mechanistic insights into this sustainable reaction. We show that practically relevant RuO2/SnO2 consists of two major RuO2 morphologies, namely 2–4 nm-sized particles 1–3-ML-thick epitaxial films attached SnO2 support particles. A large fraction small nanoparticles expose {1 1 0} 0 1} facets, whereas film grows with same orientations, due preferential orientation rutile-type support. Steady-state kinetics indicate a medium-to-strong positive effect partial pressures reactants deep inhibition by both water chlorine products. Temporal Analysis Products situ Prompt Gamma Activation strongly suggest Langmuir–Hinshelwood mechanism adsorbed Cl poisons surface. Under operation conditions, reactivity proportional coverage specific atomic oxygen species. On extensively chlorinated be described as oxy-chloride, activation rate-determining step. DFT-based micro-kinetic modeling reproduced all experimental observations additionally suggested reaction structure sensitive. Out investigated models, 2 ML film-covered gives rise significantly higher than (1 1) surface, seems inactive.