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Processes 2021, 9, 528 2 of 14 the fossil-fuel power station [17–19]. In this regard, among the mixed-conducting OTMs, recent attention to the development and application of dual-phase membranes has been growing exponentially due to their superior chemical and physical stability compared with the single-phase OTMs. The earliest discovery of dual-phase membranes was using noble metals as the electron-conducting (EC) phases and ceramic perovskite oxides as the pure oxygen ion-conducting (OIC) phases [20]. However, the high cost and mismatch between the conducting coefficients of two phases impeded their industrial application. In order to reduce costs and improve the oxygen permeability, researchers have proposed to use ceramic oxides instead of noble metals being as EC phases. Hence the noble-metal free dual-phase membranes usually consist of ceramic oxide electron conductor (EC) and oxygen ion conductor (OIC) [21–34]. During the exploration of a new dual-phase membrane, researchers have realized that doped CeO2 oxides are good candidates used as OIC phase in the dual-phase OTMs due to the following aspects: (i) Ce4+ in CeO2 fluorite phase is easy to be reduced to Ce3+ under low-oxygen partial pressure or reduction environment, resulting in a large number of oxygen vacancies in the material, showing n-type conductivity and good oxy- gen ion conductivity in high temperature environment [35]. (ii) CeO2 has strong tol- erance to the dissolution of other oxides, which will introduce more oxygen vacancies inside the material, resulting in a larger electrolysis zone [36]. (iii) CeO2 based oxides are insusceptible of corrosive gas (H2S, CO2, and SO2) atmospheres [37,38]. In view of these aforementioned characteristics, CeO2 has been widely adopted as OIC phase in the dual-phase OTMs. So far, abundant works on the CeO2-based dual-phase materials has been reported, such as Ce0.9Pr0.1O2-δ-NiFe2O4-δ (CP-NF), Ce0.8Tb0.2O2-δ-NiFe2O4-δ (CT- NF), Ce0.9Pr0.1O2-δ-Pr0.6Sr0.4FeO3-δ (CP-PSF), Ce0.85Sm0.15O1.925-Sm0.6Sr0.4Al0.3Fe0.7O3-δ (CS-NSAF), Ce0.8 Gd0.2 O2-δ -Ba0.95 La0.05 Fe1-x Nbx O3-δ (CG-BLFN), and Ce0.9 Nd0.1 O2-δ - Nd0.6Sr0.4Fe0.8Al0.2O3-δ (CN-NSFA), which show comparable oxygen permeability and CO2 resistance [29,39–42]. However, oxygen permeability is still not high enough to meet industrial requirements (≥1 mL cm−2 min−1). Therefore, development of new dual-phase membranes with both high oxygen permeability and stability is still highly demanded. Recently, Balagueret et al. has reported that transition metal cobalt doping into ceria- based oxides Ce1-xLnxO2-δ (Ln = Gd, La, Tb, Pr, Eu, Er, Yb, and Nd) can improve their total conductivity, and it is especially evident for Tb and Pr systems, which present remarkable improvements [43]. In addition, Fang et al. found that the electronic and ionic conductivity of Ce0.85Gd0.1Cu0.05O2-δ were improved by Cu doping and the obtained oxygen permeation membrane 75 wt.%Ce0.85Gd0.1Cu0.05O2-δ-25 wt.%La0.6Ca0.4FeO3-δ, which is composed of two mixed ionic electronic conductor phases and displays excellent oxygen permeability in the CO2 atmosphere [44]. The aforementioned findings imply that adding metal transition metals such as Co or Cu into Ce1-xLnxO2-δ oxides can enhance the electronic and ionic conductivity and further improve the oxygen permeability. In fact, many metal oxides such as MnO2, MnO3, GaO3, Co3O4, and Fe2O3 are considered to be able to improve the density because their melting point is much lower than those of lanthanide, meaning they also can act as sintering aids [45,46]. Currently, the 60 wt.%Ce0.9Pr0.1O2-δ-40 wt.%Pr0.6Sr0.4FeO3-δ (CP-PSF) membrane has been reported to yield 0.26 mL min−1 cm−2 oxygen permeation flux at 950 ◦C (with 0.5 mm thickness and He as sweeping gas) and has exhibited good stability in the par- tial oxidation of methane to syngas experiment [34]. More recently, we have designed Ce0.9Pr0.1O2-δ-Pr0.6Sr0.4Fe0.8Al0.2O3-δ (CP-PSFA) by doping Al in B-site of perovskite phase in CP-PSF and found higher oxygen permeability can be achieved [47]. Based on the above achievements, we further design a series of new dual-phase OTMs with the compositions of 60 wt.%Ce0.85Pr0.1M0.05O2-δ-40 wt.%Pr0.6Sr0.4Fe0.8Al0.2O3-δ (M = Fe, Co, Ni, and Cu) (CPM-PSFA) and the oxygen permeability. as well as systematically studying stability. The aim of the work will focus on the study of the effect of doping Fe, Co, Ni, and Cu transition metals into CP phase on the oxygen permeability and stability.PDF Image | CO2-Tolerant Oxygen Permeation Membranes
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