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Perovskite-type oxides BaCe0.90Sm0.10O3−δ (BCS) and BaCe0.80Gd0.10Sm0.10O3−δ (BCGS) were synthesized by the sol–gel method and characterized by thermal analysis (TG-DTA), X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). Using the sintered samples as solid electrolytes and silver–palladium alloy as electrodes, ammonia was synthesized from nitrogen and hydrogen at atmospheric pressure in a solid-state proton-conducting cell reactor. The maximum rate of production of ammonia was 5.82×10−9 mol s−1 cm−2.