Adsorption of Nin (n = 1-4) clusters on perfect and O-defective CuAl_2O_4 surfaces: A DFT study
Adsorption of Nin (n = 1-4) clusters on perfect and O-defective CuAl_2O_4 surfaces: A DFT study
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Nin (n = 1-4) 团簇在完美和 O 缺陷 CuAl_2O_4 表面上的吸附：DFT 研究
DOI：
10.1016/j.cclet.2019.03.047
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发表时间：
2019
影响因子：
9.1
通讯作者：
Zhang Rongbin
中科院分区：
文献类型：
--
作者：
Li Li;Shi Liu;Yu Xiaohu;Qing Shaojun;Gao Zhixian;Luo Qiquan;Feng Gang;Zhang Rongbin
用密度泛函理论研究了NiN(n=1-4)在CuAl_2O_4完美表面和O-缺陷表面的吸附。计算结果表明，单个Ni原子在完美的尖晶石(100)表面上的吸附能为-5.30 eV，远大于Ni在CuAl2O4表面的吸附能。Ni_n(n=1-4)在氧缺陷CuAl_2O_4(100)表面上的吸附不如在完美CuAl_2O_4(100)表面上吸附稳定。而NiN(n=1-4)在氧缺陷CuAl_2O_4(110)表面上的吸附能接近于在完美CuAl_2O_4(110)表面上。Bader电荷和偏态密度(PDOS)分析表明，Ni在CuAl_2O_4表面的吸附伴随着从金属到载体的电荷转移。生长和聚集分析表明，NiN团簇的总体生长和聚集能力顺序为：气相>；γ-Al_2O_3(110)>；CuAl_2O_4(110)>；CuAl_2O_4(100)。这一结果可以合理地解释以CuAl_2O_4为载体的Ni的稳定性远好于以γ-Al_2O_3为载体的实验现象。
The density functional theory was employed to investigate the adsorption of Nin (n = 1-4) on the perfect and O-defect CuAl_2O_4 surfaces. The computational results show that for single Ni atom on the perfect spinel (100) surface, the adsorption energy is-5.30 eV, much larger than Ni on other CuAl_2O_4 surfaces. The adsorption of Ni_n (n = 1-4) absorbed on the O-defect CuAl_2O_4 (100) surface is less stable than on the perfect CuAl_2O_4 (100) surface. However, the adsorption energy for Nin (n = 1-4) on the O-defect CuAl_2O_4 (110) surface is close to on the perfect CuAl_2O_4 (110) surface. Bader charge and partial density of states (PDOS) analysis revel that the adsorption of Ni on the CuAl_2O_4 spinel surface is accompanied by charge transfer from the metal to the support. The growth and aggregations analysis show that the general growth and aggregation ability for Nin clusters follow the order: gas phase > γ-Al_2O_3 (110) > CuAl_2O_4 (110) > CuAl_2O_4 (100). This result can give reasonable explanations for the experimental phenomenon that Ni supported on the CuAl_2O_4 spinel performs much better stability than on the γ-Al_2O_3.