High-Performance and Long-Lived Pd Nanocatalyst Directed by Shape Effect for CO Oxidative Coupling to Dimethyl Oxalate
High-Performance and Long-Lived Pd Nanocatalyst Directed by Shape Effect for CO Oxidative Coupling to Dimethyl Oxalate
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DOI：
10.1021/cs300759h
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发表时间：
2013-02
期刊：
影响因子：
12.9
通讯作者：
Zhong-Ning Xu;Jing Sun;Chensheng Lin;Xiaoming Jiang;Qing‐Song Chen;Si-Yan Peng;Ming‐Sheng Wang;G. Guo
中科院分区：
文献类型：
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作者：
Zhong-Ning Xu;Jing Sun;Chensheng Lin;Xiaoming Jiang;Qing‐Song Chen;Si-Yan Peng;Ming‐Sheng Wang;G. Guo
我们采用择优取向晶面生长技术合成了具有（111）和（100）晶面的单分散Pd纳米晶。首次发现Pd纳米晶的（111）晶面是CO氧化偶联合成草酸二甲酯（DMO）的活性晶面。这一结论是基于实验结果、反应机理和密度泛函理论计算得出的。在此形状效应的指导下，采用湿沉淀-溶液化学还原法成功制备了一种高性能、长寿命、Pd负载量低的CO氧化偶联制DMO纳米催化剂，该方法能够很好地控制Pd纳米晶的（111）晶面暴露和尺寸。
We synthesized monodisperse Pd nanocrystals with exposed (111) and (100) facets through preferentially oriented facet growth technology. We then supported them on α-Al2O3as catalysts for application in CO oxidative coupling to dimethyl oxalate (DMO) and find, for the first time, that the (111) facets of Pd nanocrystals are active planes for CO oxidative coupling to DMO. This conclusion is based on experiment results, reaction mechanism, and density functional theory calculation. Directed by this shape effect, a high-performance and long-lived nanocatalyst with much lower Pd load for CO oxidative coupling to DMO was successfully prepared by a new wet impregnation–solution chemical reduction method, which can well control the exposure of (111) facets and sizes of Pd nanocrystals.