Barcellos Debora R, Coury Francisco G, Emery Antoine, Sanders Michael, Tong Jianhua, McDaniel Anthony, Wolverton Christopher, Kaufman Michael, O'Hayre Ryan
Metallurgical and Materials Engineering Department , Colorado School of Mines , Golden , Colorado , United States.
Department of Materials Science and Engineering , Northwestern University , Evanston , Illinois , United States.
Inorg Chem. 2019 Jun 17;58(12):7705-7714. doi: 10.1021/acs.inorgchem.8b03487. Epub 2019 May 30.
Ruddlesden-Popper (layered perovskite) phases are attracting significant interest because of their unique potential for many applications requiring mixed ionic and electronic conductivity. Here we report a new, previously undiscovered layered perovskite of composition, Ce SrMnO ( x = 0.1, 0.2, and 0.3). Furthermore, we demonstrate that this new system is suitable for solar thermochemical hydrogen production (STCH). Synchrotron radiation X-ray diffraction and transmission electron microscopy are performed to characterize this new system. Density functional theory calculations of phase stability and oxygen vacancy formation energy (1.76, 2.24, and 2.66 eV/O atom, respectively with increasing Ce content) reinforce the potential of this phase for STCH application. Experimental hydrogen production results show that this materials system produces 2-3 times more hydrogen than the benchmark STCH oxide ceria at a reduction temperature of 1400 °C and an oxidation temperature of 1000 °C.
鲁德尔斯登-波珀（层状钙钛矿）相因其在许多需要混合离子和电子传导性的应用中具有独特潜力而备受关注。在此，我们报告一种新的、此前未被发现的组成式为Ce SrMnO （x = 0.1、0.2和0.3）的层状钙钛矿。此外，我们证明这个新体系适用于太阳能热化学制氢（STCH）。通过同步辐射X射线衍射和透射电子显微镜对这个新体系进行了表征。相稳定性和氧空位形成能的密度泛函理论计算（随着Ce含量增加，分别为1.76、2.24和2.66 eV/氧原子）强化了该相在STCH应用方面的潜力。实验制氢结果表明，在1400°C的还原温度和1000°C的氧化温度下，该材料体系产生的氢气比基准STCH氧化物二氧化铈多2至3倍。
