铜掺杂氧化铈中铜物种对结构演变和CO催化氧化性能提高的影响
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摘要
在本文中,我们在碳纳米球作为模板的条件下,使用尿素作用下的均匀沉淀法~([1])制备了铜掺杂的氧化铈纳米球。结果显示,随着铜掺杂的投入量从0到7.5%mol的增加,纳米球的形貌从双壳空心球变成了单壳空心球。值得注意的是,最终产物中的Cu/Ce+Cu的摩尔比数值大约是投入值的五倍,这说明该制备方法能够实现被掺杂元素铜的高效利用。除此之外,铜掺杂的氧化铈催化剂与纯相氧化铈催化剂相比,较大程度上提高了CO催化氧化的性能~([2])(例如,纯相氧化铈催化剂在300℃催化完全,而铜铈催化剂的最佳样品在160℃就可以催化完全)。通过对催化剂结构的分析,我们证明了使催化性能提高的两个活性物种是CuO_x和Cu-[O_x]-Ce结构中的铜离子。
In this paper, copper doped ceria porous nanospheres were synthesized using carbon nanospheres as hard template via a homogenous precipitation method at low temperature. Results showed that the copper-doped ceria have undergone a morphology transformation from the initial double-shell spheres to hollow spheres as the copper doping concentration increased from 0 to 7.5% mol. Notably, the Cu/Ce+Cu atomic ratio in the final products were approximately five times of the initial design ratio, which confirmed an efficient utilization of copper in this system. Furthermore, the copper-ceria catalysts exhibited enhanced catalytic performance towards CO conversion when compared with pure ceria catalysts(e.g., for the optimal catalysts, the complete conversion temperature was 160 ℃, for the pure catalysts, complete conversion temperature was 300 ℃). Through the analysis of the catalysts structure, we proved that the superior catalytic performance was derived from a combination of CuO_x clusters and copper ions in the Cu-[O_x]-Ce bulk phase.
引文
[1]H.Qian,G.Lin,Y.Zhang,P.Gunawan and R.Xu,Nanotechnology 2007,18,355602.
    [2]W.Liu,X.Liu,L.Feng,J.Guo,A.Xie,S.Wang,J.Zhang and Y.Yang,Nanoscale 2014,6,10693-10700.

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