Influence of ZnO Facets on Pd/ZnO Catalysts for Methanol Steam Reforming

Influence of ZnO Facets on Pd/ZnO Catalysts for Methanol Steam Reforming
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DOI:
10.1021/cs500590t
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发表时间:
2014-06
期刊:
影响因子:
12.9
通讯作者:
He Zhang;Junming Sun;V. Dagle;B. Halevi;A. Datye;Yong Wang
He Zhang;Junming Sun;V. Dagle;B. Halevi;A. Datye;Yong Wang
中科院分区:
化学1区
文献类型:
--
作者:
He Zhang;Junming Sun;V. Dagle;B. Halevi;A. Datye;Yong Wang

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采用具有(10-10)个非极性晶面的针状ZnO微晶(ZnO-N)和没有任何主晶面的商品ZnO(ZnO-P)制备了一系列Pd/ZnO催化剂。Pd/ZnO催化剂的特征在于使用互补的技术,如氮气物理吸附,X射线衍射(XRD),高分辨率透射电子显微镜(HRTEM),和吸附CO的傅里叶变换红外光谱分析(CO-FTIR)。研究了ZnO微晶的小面化对Pd/ZnO催化剂甲醇水蒸气重整反应活性和选择性的影响。发现富Pd相(PdxZny,x > y)主要在两种ZnO载体(ZnO-N和ZnO-P)上在低Pd负载下形成,导致高CO选择性。随着Pd负载量的增加,PdxZny相中的x/y比降低,导致CO选择性降低。结果表明,Pd/ZnO-P催化剂具有更高的选择性,这是由于Pd/ZnO-N催化剂更容易形成活性中心,而Pd/ZnO-P催化剂具有更高的选择性。
A series of Pd/ZnO catalysts with different Pd loadings were prepared using needlelike ZnO crystallites (ZnO-N) with predominant (10–10) nonpolar facets exposed and commercial ZnO (ZnO-P) without any dominant facets. The Pd/ZnO catalysts were characterized using complementary techniques, such as nitrogen physisorption, X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), and Fourier transform infrared spectroscopy analysis of adsorbed CO (CO-FTIR). The effect of ZnO crystallite faceting on the activity and selectivity of the Pd/ZnO catalysts was studied in methanol steam reforming (MSR). It was found that the Pd-rich phases (PdxZny, x > y) are predominantly formed at low Pd loadings on both ZnO supports (ZnO-N and ZnO-P), resulting in high CO selectivity. As Pd loading increases, the x/y ratio in the PdxZny phases decreases, leading to decreased CO selectivity. At similar Pd loadings, Pd/ZnO-P catalysts are more selective in MSR than Pd/ZnO-N, which is due to more facile form...