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Processes 2021, 9, 528 h RT lnP σ σ J = ion e d(lnP) (2) o Considering that in dual-phase mixed-conducting OTM, electronic conductivit8yofis14 often much larger than ionic conductivity (σe ˃˃ σi) making the equation approximately to be as follows: O2 16F2L σ +σ lnP ion e l ln p'' mixed-conducting phases, i.e., both fluorRitTe phase Oand perovskite phase can conduct both oxygen ions and electrons, thus2 making the membrane exhibit2 better oxygen permeability. O 16F2lnp' i O J ⋅L=− 2σdlnp (3) O2 At the same time, we compare the average grain sizes of the CPM-PSFA (M = Fe, Co, Ni, The calculated ionic conductivity of CPM-PSFA (M = Fe, Co, Ni, Cu) are 0.0182, and Cu) composite membranes after sintering at 1275 C in Table S2. We find that the 0.0194, 0.0181, and 0.0243 S∙cm−1, respectively, which are higher than that of CP-PSFA average grain size for CPCu-PSFA is the largest, followed by the system doped with Co (0.0179 S∙cm−1). This indicates that the oxygen vacancies in CPM phase are enhanced due element among these four dual-phase membranes. It seems like that the large grain size tohathsealpoows-ivtiavlenefcfecotfotrnatnhseitoioxnygmeentapleormxyegaetinonioflnus,xthinusouexrhstibuidtinedg dbeutatle-rpihoansiecmcoenmdburcatnive-s, itwy.hich is similar to the findings in some single-type oxygen permeable membranes [50,51]. Figure 4. (a) Oxygen permeation rates through the CPMPSFA (M = Fe, Co, Ni, Cu) composite Figure 4. (a) Oxygen permeation rates through the CPMPSFA (M = Fe, Co, Ni, Cu) composite membranes. (b) Arrhenius plot of oxygen permeation rates for CPM-PSFA (M = Fe, Co, Ni, and Cu) membranes. (b) Arrhenius plot of oxygen permeation rates for CPM-PSFA (M = Fe, Co, Ni, and ◦ Processes 2021, 9, x FOR PEER REVIEW −1 −1 −1−1 9 of 14 Ccuo)mcopmospitoesmitembemrabnreasn.eCso.nCdointidointi:o1n5:01m50LmLinminairaiarsatshethfeefedegdags,a4s,94m9LmmLimninHHeeasasththeesweep −1 −1 swgaese,p1gmasL, m1 minL mNine asNaenaisnatenrninatlesrtnaanldsatardndgarsd. Mgaesm. Mbreamnebrtahnicektnheiscsk:n0e.s6sm: 0m.6.mm. Figure 5. Comparison of oxygen permeation rates through the CPM-PSFA (M = Fe, Co, Ni, and Figure 5. Comparison of oxygen permeation rates through the CPM-PSFA (M = Fe, Co, Ni, and Cu) C u ) c o m p o s i t e m e m b r a n e s a t 1 0◦ 0 0 ° C . C o n d i t i o n : 1 5 0 m L m− 1i n − 1 a i r a s t h e f e e d g a s , 4 9 m L m−i n1 − 1 H e composite membranes at 1000 C. Condition: 150 mL min air as the feed gas, 49 mL min He as −1 asthesweepgas,and1mLm−in1 Neasaninternalstandardgas.Membranethickness:0.6mm. the sweep gas, and 1 mL min Ne as an internal standard gas. Membrane thickness: 0.6 mm. Table 2 shows the comparison of oxygen permeation fluxes of different oxygen per- In addition, to study the activation energy of oxygen in the process of permeation, meable membranes. As shown in Table 2, we can see that our dual-phase membranes have we draw Arrhenius plots based on the relationship between temperature and oxygen lower oxygen permeability than that of co-based SrSc0.05Co0.95O3-δ single perovskite mem- permeation rates (Figure 4b). The apparent activation energy of CPM-PSFA (M = Fe, Co, −1 brane [53] but have near double higher [33,54] or comparable oxygen permeability com- Ni, and Cu) were 88.71, 61.43, 88.05, and 70.80 kJ mol , respectively. The CPCu-PSFA poaxryegdewniptheromtheearbdleumal-epmhbarsaenmeemxhbirbaintsesth[e55s,m56a]l.lTesotfaucrttihveartiboennecnhemrgayrk, atnhde pthoetecnatlicaullpartaiocn- tsichaolwapspthliactaitiohnasotfhOeTlaMrgseisntporxey--efxupeolnceonmtibaulsfaticotonr,,ownheiochftmheaimnsptohrattatnhtefamcetomrsbrisanwehdeothperd twheithOTcoMppcearnhoapsethraetemsotsatbrleyaicntiorinchsitceasrbfornindtieorxfaidceeaxtmchoasnpgheepreroscaetsshiagmhotnegmtphersaetustrued.iSeod fmare,mborsatnoesf.tIhneoprdrervitoufsurftihnedrinegxpslornetheesfifnegclteo-pfhFae,seCop,eNroi,vasnkidteC(uAdBoOp3i)ngmoenmflburaonreitse adopted alkali-earth elements in A or B site. This leads to the formation of carbonates in CO2 rich atmosphere at high temperature and the stop of oxygen permeation [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 and CPCo- PSFA materials from 30 to 1000 °C. In situ XRD patterns show that there is no carbonates or other impurity phase that can be observed in the CPCu-PSFA and CPCo-PSFA compo-PDF Image | CO2-Tolerant Oxygen Permeation Membranes
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