Dense and thin electrolyte films are desirable for solid oxide fuel cells (SOFCs) because of their low gas leakage and low ohmic resistances. This work aims at the preparation of thin dense Gd‐doped ceria (CGO) electrolyte films using a cost‐effective deposition method in ambient atmosphere–electrostatic spray deposition (ESD). The deposition parameters such as deposition temperature, concentration and flow rate of precursor solution were changed systematically to examine their effects on film morphology and hence electrochemical performance. While the film morphology was examined by a scanning electron microscope, the electrochemical performance was revealed by measuring open circuit voltages (OCVs) of NiO‐CGO/CGO/Ba0.5Sr0.5Co0.8Fe0.2O3‐δ (BSCF) cells in 500–700 °C with humidified hydrogen as fuel and air as oxidant. The results show that a CGO film of 25 μm thick obtained at a deposition temperature of 400 °C, a precursor solution flow rate of 6 ml h–1 and a precursor concentration of 0.3 M was dense with very few isolated pores and the OCV of the associated cell was 0.915 V at 500 °C. This implies that the CGO film has negligible gas leakage and ESD is a promising method for preparing thin dense electrolyte films for SOFCs.
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