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Processes 2021, 9, 528 9 of 14 phase, we calculated the ionic conductivity of 0.6 mm-thickness CPM-PSFA membrane at 1273.15 K according to the Wagner equation: [52] lnP h lnPl Considering that in dual-phase mixed-conducting OTM, electronic conductivity is often much larger than ionic conductivity (σe ≫ σi) making the equation approximately to be JO = RT 2 16F2L σionσe d(lnPo) (2) σion +σe as follows: JO ·L=− RT lnp′′O2 σidlnpO (3) 2 2 16F2 lnp′ O2 The calculated ionic conductivity of CPM-PSFA (M = Fe, Co, Ni, Cu) are 0.0182, 0.0194, 0.0181, and 0.0243 S·cm−1, respectively, which are higher than that of CP-PSFA (0.0179 S·cm−1). This indicates that the oxygen vacancies in CPM phase are enhanced due to the low-valence of transition metal oxygen ions, thus exhibiting better ionic conductivity. Table 2 shows the comparison of oxygen permeation fluxes of different oxygen per- meable membranes. As shown in Table 2, we can see that our dual-phase membranes have lower oxygen permeability than that of co-based SrSc0.05Co0.95O3-δ single perovskite membrane [53] but have near double higher [33,54] or comparable oxygen permeability compared with other dual-phase membranes [55,56]. To further benchmark the poten- tial practical application of OTMs in oxy-fuel combustion, one of the important factors is whether the OTM can operate stably in rich carbon dioxide atmospheres at high tem- perature. So far, most of the previous findings on the single-phase perovskite (ABO3) ation [57]. Thus, it is necessary to check the stability for our CPM-PSFA membranes under low oxygen atmosphere. Figure 6a,b shows the in situ XRD patterns for the CPCu-PSFA ◦ membranes adopted alkali-earth elements in A or B site. This leads to the formation of Processes 2021, 9, x FOR PEER REVIEW 10 of 14 carbonates in CO2 rich atmosphere at high temperature and the stop of oxygen perme- 60 wt.%Ce0.9Pr0.1O2-δ- 0.6 1000 0.77 [33] and CPCo-PSFA materials from 30 to 1000 C. In situ XRD patterns show that there is no 40 wt.%Pr0.6Sr0.4Fe1-xAlxO3-δ carbonates or other impurity phase that can be observed in the CPCu-PSFA and CPCo-PSFA 60 wt.%Ce0.85Pr0.1Fe0.05O2-δ- 0.6 ◦ 1000 0.82 This com4p0owsti.%tePsr0 n h eO3 Moreover, Figure 6c,d shows the XRD patterns for the CPNi-PSFA and CPFe-PSFA com- i r g o . 0 .8 .2 -δ 6Srt .4Fee0 f 30 to 1000 C, indicating they are stablewionrkpure CO condition. 2 aAnl0 60 wt.%Ce0.85Pr0.1Co0.05O2-δ- This 40 wt.%Pr0.6Sr0.4Fe0.8Al0.2O3-δ 0.6 1000 0.87 work ◦ ◦ C, 600 ◦ C, posites after treating in pure CO2 condition at several temperatures (200 C, 400 60 wt.%Ce0.85Pr0.1Ni0.05O2-δ- This 800◦C,and1000◦C)for24h.Ass0h.6owninF1i0g0u0re6c,d,a0ll.8t2hesecompositesalsomaintain 40 wt.%Pr0.6Sr0.4Fe0.8Al0.2O3-δ work fluorite and perovskite two phases, and neither carbonates nor other impurity can be found. 60 wt.%Ce0.85Pr0.1Cu0.05O2-δ-40 0.6 1000 1.05 This Collectively,allthesefourstudiedcompoundsarephasestableinpureCO atmosphere. wt.%Pr0.6Sr0.4Fe0.8Al0.2O3-δ work 2 Figure 6. In-situ XRD patterns for (a) CPCu-PSFA and (b) CPCo-PSFA powders under CO2 atmos- Figure 6. In-situ XRD patterns for (a) CPCu-PSFA and (b) CPCo-PSFA powders under CO2 atmo- phere in the temperature range of 25-1000 oC; XRD patterns of (c) CPNi-PSFA and (d) CPFe-PSFA sphere in the temperature range of 25–1000 ◦C; XRD patterns of (c) CPNi-PSFA and (d) CPFe-PSFA powders calcined at 25–1000 °C for 24 h under CO2 atmosphere. powders calcined at 25–1000 ◦C for 24 h under CO2 atmosphere. Subsequently, we carried out the long-time oxygen permeability test for the optimal CPCu-PSFA membrane in the range of 900–1000 °C. Encouragingly, CPCu-PSFA compo- site membrane still maintains both high oxygen flux and acceptable stability in CO2 envi- ronment. As illustrated in Figure 7, during the first 40 h of the test, the oxygen permeabil- ity increases with the increase of temperature. When the temperature is stable at 1000 °C, the J also stabilizes at the level of about 1.05 mL min−1 cm−2. When the sweep gas isPDF Image | CO2-Tolerant Oxygen Permeation Membranes
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