Structure and Electronic Properties of [Ca24Al28O64]4+・4e? Surfaces: Opportunities for Termination-Controlled Electron Transfer
Structure and Electronic Properties of [Ca24Al28O64]4+・4e? Surfaces: Opportunities for Termination-Controlled Electron Transfer
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[Ca24Al28O64]4+·4e 表面的结构和电子性质：终止控制电子转移的机会
DOI：
10.1021/acs.jpcc.8b11866
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Sushko Peter V.
中科院分区：
文献类型：
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作者：
Ong Phuong-Vu;Hosono Hideo;Sushko Peter V.
利用密度泛函理论模拟研究了钙铝石（12CaO·7Al2O3或C12A7）在其缺氧相中的结构、热力学稳定性和（001）、（110）和（111）表面的电子性质.七种类型的表面终端进行了鉴定，这取决于相对于表面平面的晶格纳米尺寸笼的取向。我们发现，表面终止的电子阴离子的分布在近表面区域有很强的影响，表现出的离子电荷和吸附的Au原子和二聚体的结合能的范围。值得注意的是，在所有情况下，Au物质获得负电荷，并优先吸附为孤立的离子，而不是聚集成簇。这些结果表明，C12A7双金属氧化物可以提供一种简单而通用的底物，以实现单原子催化剂的高吸附容量和空间选择性。
We investigate the structure, thermodynamic stability, and electronic properties of (001), (110), and (111) surfaces of mayenite (12CaO·7Al2O3or C12A7) in its oxygen-deficient phase known as mayenite-derived electride Ca12Al14O32using simulations based on the density functional theory. Seven types of surface terminations were identified, depending on the orientation of the lattice nanosize cages with respect to the surface plane. We find that the surface termination has a strong effect on the distribution of electron anions in the near-surface region, as demonstrated by the range of the ionic charges and binding energies of adsorbed Au atoms and dimers. Notably, in all cases, Au species acquire a negative charge and preferentially adsorb as isolated ions rather than aggregate into clusters. These results show that C12A7 electride can provide a simple, yet versatile substrate to achieve high adsorption capacity and steric selectivity for single atom catalysts.