The mixed-ionic and electronic conductor Sr(Ti,Fe)O3-alpha, (STF) exhibits fast oxygen surface exchange kinetics, with electron concentration potentially playing a key role. The effect of La donor doping on electron concentration, Fermi level, and overall defect chemistry of STF is investigated on Sr1-yLayTi0.65Fe0.35O3-alpha (LSTF, 0 <= y <= 0.5) thin films. Defect chemical modeling, optical absorption, and electrical conductivity measurements in oxidizing conditions indicate compensation of donors by an increase in oxygen and electron concentrations, increase in Fermi level, decrease in oxygen vacancy and hole concentrations, and formation of cation vacancies (for [La] > [Fe]). The surface exchange coefficient, Measured by impedance spectroscopy, decreased with increasing donor concentration, suggesting that oxygen exchange kinetics in LSTF are limited by low oxygen vacancy and/or hole concentrations, rather than electron transfer. (C) 2014 Elsevier B.V. All rights reserved.