First‐Principles Computational Screening of Dopants to Improve the Deacon Process over RuO₂

Abstract

Doping of metal oxides is a promising route to further optimize their catalytic performance. To guide corresponding experimental endeavors, we performed a DFT‐based computational screening study for a wide range of metal dopant atoms in rutile RuO2. With a focus on the Deacon process, that is, the catalytic oxidation of HCl to chlorine and water, we used the rate‐controlling Cl desorption energy as a reactivity descriptor. As stability descriptors, we employed the dopant surface segregation energy and as the dopant thermodynamic stability against precipitation into the metal oxide or bulk oxide grains. In the oxygen‐rich conditions of the Deacon process, particularly the instability against oxide precipitation, represents a strong limitation. In this respect, doping with Cu appears as an optimum compromise between stability and catalytic activity enhancement.

Selective Seawater Splitting Using Pyrochlore Electrocatalyst

“…The -OOH intermediates on the surface metal oxides (e.g., RuO 2 ) can be stabilized through metal doping having lower d-electrons than the host cation. 8 The formation of -OCl on the electrocatalyst can be destabilized through performing the reaction in higher pH medium (pH > 6.0). 9,10 Oxygen vacancy in the electrocatalyst lattice has also been found to promote OER.…”

Towardsoperandocomputational modeling in heterogeneous catalysis

“…The structures and stabilities of various nanoparticles used in catalysis were investigated as a function of synthesis conditions or “ operando ” environment, e.g. Mo 2 C, ZnO and Ni 2 P, 166 – 169 surface coverage as a function of T and p i , 161 , 170 – 172 doping effects, 173 metal alloying, 174 , 175 surfaces under electrochemical conditions, 176 , 177 water in the interlayer space, 178 or controlled growth conditions, 179 to name just some. Several recent reviews and perspectives are also available.…”

Peter J. Dunn Award: B. H. Lipshutz and S. Handa / International Solvay Chair in Chemistry: G. Frenking / Max Born Prize: A. Rubio / Terrae Rarae Prize: R. Kempe / Frontiers in Chemical Energy Science Award: K. Reuter / New Members of the Academia Europaea

“…Reuter's research interests center on the first‐principles‐based multiscale modeling of problems in materials, catalysis, and energy. He has reported in Angewandte Chemie on multiphoton absorption in metal–organic frameworks, and in ChemCatChem on the DFT‐based computational screening for dopants in RuO 2 …”