Rapid Gas-Phase Synthesis of the Perovskite-Type BaCe_0.7Zr_0.1Y_0.1Yb_0.1O_3−δ Proton-Conducting Nanocrystalline Electrolyte for Intermediate-Temperature Solid Oxide Fuel Cells

Abstract

Perovskite-type proton-conducting materials, such as BaCe 0.7 Zr 0.1 Y 0.1 Yb 0.1 O 3−δ (BCZYYb), are very attractive for the nextgeneration equipment of electrochemical energy conversion and storage owing to their excellent conductivity in the intermediate-temperature range (300−750 °C), as well as good thermo-chemical stability, coking resistance, and sulfur tolerance. However, the lack of a reliable and costeffective synthesis method for such multi-component co-doping oxides limits their large-scale application. In this study, for the first time, we successfully synthesize BCZYYb electrolyte nanopowders by using a rapid, scalable flame-based gas-phase synthesis method with two different barium precursors Ba(NO 3 ) 2 and Ba(CH 3 COO) 2 , named as BCZYYb (N) and BCZYYb (CA). The as-synthesized nanoparticles exhibit good crystallinity of the pure orthorhombic perovskite BCZYYb phase. BCZYYb (CA) shows more uniform doping with the element ratio of 1:0.74:0.12:0.08:0.1, which is very close to the theoretical value. The shrinkage and surface SEM (scanning electron microscope) results indicate that the flame-made powders have superior sinterability compared to the sol−gel-made powders because of the smaller primary particle size (∼20 nm). Electrochemical impedance spectroscopy tests show that BCZYYb (CA) sintered at 1450 °C has the highest protonic conductivity of 1.31 × 10 −2 S cm −1 in wet H 2 when operating at 600 °C and still maintains a high-level conductivity of 1.19 × 10 −2 S cm −1 even when the sintering temperature is reduced to 1350 °C, which is mainly attributed to uniform doping and good sinterability. The activation energy for the conductivity of BCZYYb (CA) is also significantly lower than that of conventional electrolytes, which suggests much better conductivity in the intermediate (∼600 °C) and even lower operating temperature. The excellent conductivity performance combined with the high-throughput production capability makes the swirling spray flame a promising synthesis method for promoting the BCZYYb electrolytes from lab to industrial-scale solid oxide fuel cells.

Nanotechnologies in ceramic electrochemical cells

“…Wu et al developed a flame-based gas-phase fabrication method. 263 The combustion process was modified, by using a swirling spray flame burner. The primary particle size was about 20 nm, which was considered to be helpful for achieving an advanced electrolyte.…”

Fundamental Understanding and Applications of Protonic Y‐ and Yb‐Coped Ba(Ce,Zr)O3 Perovskites: State‐of‐the‐Art and Perspectives

“…The same positive effects of NiO addition on the BCZYYb densification have been additionally obtained using other synthesis methods: co-precipitation, [123] and sol-gel. [124,125] A combination of wet chemical approaches and sintering additive allows the preparation of dense ceramics at 1250-1350 °C.…”