| Autor: |
Yue Lu, Feng Lu, Zhi Yang, Jie Wu, Hongyun Yu, Xinjian Xie, Jianping Xu, Fangyi Cheng, Jun Chen, Ka Xiong, Hui Liu, Wei-Hua Wang, Jianzhou Zhao, Weichao Wang |
| Jazyk: |
angličtina |
| Rok vydání: |
2016 |
| Předmět: |
|
| Zdroj: |
AIP Advances, Vol 6, Iss 9, Pp 095210-095210-7 (2016) |
| Druh dokumentu: |
article |
| ISSN: |
2158-3226 |
| DOI: |
10.1063/1.4963079 |
| Popis: |
3d-orbital filling in transition metal oxide is crucial to govern the catalytic activity in oxygen evolution reduction, nevertheless, it is not fundamentally accessible why specific orbital occupation produces a highest catalytic performance. Here, we utilize brownmillerite Ca2Mn2O5 to clarify the orbital selective catalytic behavior due to the crystal field splitting and on-site coulomb interactions. Within density functional theory plus dynamical mean field theory, Ca2Mn2O5 shows a paramagnetic Mott insulating behavior at room temperature, consistent with optical adsorption spectra and magnetic susceptibility. As the center of the dz2 orbital locates in the lower Hubbard sub-band, the unit occupation on dz2 orbital provides a moderate bonding with external O* species to cause a high catalytic activity of Ca2Mn2O5 with a square pyramid crystal field. Such concept of unit occupation of dz2 near Fermi level could be extended to other crystal fields for future design of oxide catalysts. |
| Databáze: |
Directory of Open Access Journals |
| Externí odkaz: |
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