Catalytic performance and characterization of Ni-doped HZSM-5 catalysts for selective trimerization of n-butene
Catalytic performance and characterization of Ni-doped HZSM-5 catalysts for selective trimerization of n-butene
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DOI：
10.1016/j.fuproc.2009.04.011
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发表时间：
2009-07
影响因子：
7.5
通讯作者：
Xin Zhang;Jin Zhong;Jianwei Wang;Linhui Zhang;Junkui Gao;Aisong Liu
中科院分区：
文献类型：
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作者：
Xin Zhang;Jin Zhong;Jianwei Wang;Linhui Zhang;Junkui Gao;Aisong Liu
制备了一系列Ni掺杂的HZSM-5催化剂，并考察了其在正丁烯三聚反应中的催化性能。Ni负载量、HZSM-5的Si/Al比以及反应条件（温度、压力和空速）对催化剂的催化性能有很大影响。77.5重量百分比正丁烯的转化率和50.5重量%在1 NiHZSM-5（320）催化剂上，在420 °C，空速为2 h-1，压力为1.0MPa的条件下，反应148 h，三聚体的选择性和产率为19.6×10 - 2g/（gcath）。采用粉末X射线衍射（XRD）、N2等温吸附-脱附、红外光谱（IR）和吡啶吸附红外光谱（Py-IR）等技术对催化剂的物化性能进行了比较表征。Ni的掺杂改变了HZSM-5（320）的比表面积和酸性，进而影响了催化剂在正丁烯三聚反应中的催化性能。催化剂外表面的酸量和刘易斯酸/布朗斯特酸（L/B）比值与催化剂的催化性能密切相关。1 NiHZSM-5（320）催化剂由于其外表面具有合适的酸量和L/B比，在正丁烯三聚反应中表现出最佳的催化性能。
A series of Ni-doped HZSM-5 catalysts were prepared and the catalytic performance of these catalysts in n-butene trimerization was investigated. The Ni-loading, the Si/Al ratio of HZSM-5 and the reaction conditions (temperature, pressure and WHSV) played great influences on the catalytic performance of these catalysts in the reaction. 77.5 wt.% conversion of n-butene and 50.5 wt.% selectivity of trimers as well as 19.6×10−2gtrimers/(gcath) yield of trimers were obtained on 1NiHZSM-5(320) catalyst up to 148 h at 420 °C, WHSV=2 h−1and 1.0 MPa. In addition, the physicochemical properties of these catalysts were comparatively characterized by powder X-ray diffraction (XRD), N2isothermal adsorption–desorption, infrared red spectroscopy (IR) and pyridine adsorbed infrared red spectroscopy (Py-IR) techniques. The doping of Ni into HZSM-5(320) modified the specific surface area and the acidity of these catalysts, which in turn affected the catalytic performance of these catalysts in n-butene trimerization. The acidic amount and the ratio of Lewis/Brönsted acid sites (L/B) on the external surface of these catalysts were close relative to the catalytic performance of these catalysts. 1NiHZSM-5(320) catalyst showed the highest catalytic performance in n-butene trimersization among the investigated catalysts because it had the proper acidic amount and the proper L/B ratio on its external surface.