Molecular Catalysis ( IF 3.9 ) Pub Date : 2021-01-04 , DOI: 10.1016/j.mcat.2020.111370 Yongzhao Wang , Xiang Zhou , Xuhui Wei , Xiao Li , Ruifang Wu , Xiaobo Hu , Yongxiang Zhao
Different methods including ion exchange, impregnation and hydrothermal method were used to prepare Co/hydroxyapatite catalysts with various Co species. The catalytic activities for N2O decomposition were studied. It was concluded that Co2+ⅡOh existed in Co(1.2)-IE prepared by ion exchange is more active than Co2+Td, Co3+Oh and Co2+Ⅰ obtained by impregnation and hydrothermal methods, respectively. Meanwhile, Co(1.2)-IE shows better stability and stronger resistance against 2.0 vol.% O2 or 2.3 vol.% H2O in the feed gas. The higher catalytic activity of Co2+ⅡOh is attributed to its octahedral coordination geometrical structure, which make Co2+ⅡOh tend to donate electrons to activate N2O. Furthermore, the closer spacing distance between two Co2+ⅡOh sites can facilitate the combination and desorption of oxygen species. The above mentioned reasons ultimately lead to the increased catalytic activity. Finally, the results of density functional theory calculations indicate that the Co2+ⅡOh possesses the highest d-band center, which means the excellent catalytic activity.
中文翻译:
用于N 2 O催化分解的Co /羟基磷灰石催化剂:具有几何和间距效应的明确活性位点的设计
使用包括离子交换,浸渍和水热法在内的各种方法来制备具有各种Co物种的Co /羟基磷灰石催化剂。研究了N 2 O分解的催化活性。得出的结论是联合2+ Ⅱ噢在存在钴(1.2)-IE制备通过离子交换是比Co更活跃2+ TD,钴3+噢和Co 2+ Ⅰ通过浸渍和水热法,分别获得。同时,Co(1.2)-IE显示出更好的稳定性和对进料气体中的2.0体积%的O 2或2.3体积%的H 2 O的更强的耐受性。Co 2 + Ⅱ的较高催化活性哦归因于其八面体配位的几何结构,这使钴2+ Ⅱ喔倾向于将电子给予激励N- 2 O.而且,两个联合之间的间隔更近的距离2+ Ⅱ噢位点可以促进氧的组合和解吸。上述原因最终导致增加的催化活性。最后,密度泛函理论计算结果表明,Co 2 + ⅡOh具有最高的d带中心,这意味着优异的催化活性。