Abstract
Ru/TiO2 catalysts are highly active and selective in the selective methanation of CO in the presence of large amounts of CO2 but suffer from a considerable deactivation and loss of selectivity during time on stream. Aiming at a fundamental understanding of these processes, we have systematically investigated the physical reasons responsible for these effects, using catalysts with different surface areas and combining time-resolved kinetic and in situ/operando spectroscopy measurements as well as ex situ catalyst characterization. This allowed us to identify and disentangle contributions from different effects such as structural effects, adlayer effects, such as site blocking effects, and changes in the chemical (surface) composition of the catalysts. Operando X-ray absorption near edge spectroscopy (XANES)/extended X-ray absorption fine structure analysis (EXAFS) measurements revealed that an initial activation phase is largely due to the reduction of oxidized Ru species, together with a distinct change i...
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