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Highlights: [•] WGS reaction mechanism on Pt/Ce1−x Ti x O2−δ was studied by SSITKA-operando methodology. [•] WGS on Pt/Ce0.8Ti0.2O2−δ at 300°C largely follows both the “redox” and “associative formate” mechanisms. [•] CeO2-doped (Zr4+, La3+ and Ti4+) largely affects the concentration of active C-pool and H-pool on Pt/CeO2-doped catalyst. [•] The extent (Δx, nm) of a reactive zone around Pt nanoparticles strongly depends on the dopant. [•] A very good correlation between the active C-pool and the specific WGS reaction rate as a function of dopant exists. [ABSTRACT FROM AUTHOR]