This dataset includes all data presented in the figures of the main manuscript: XPS work function changes, ab-initio calculated work functions, O2p band center shifts, Densities of state for LSC and PCO, i-PLD results for LSC, LSF, STF and PCO, Densities of state for adsorbed O2 on differently decorated PCO surfaces. In this work, we investigated surface dipole changes which were induced by modification of mixed conducting surfaces with binary oxides via pulsed laser deposition.