钨含量对W/SiO2/Al2O3催化剂上1-丁烯自歧化反应的影响

引用本文: 柳娜, 张辉, 薛念华, 丁维平. 钨含量对W/SiO₂/Al₂O₃催化剂上1-丁烯自歧化反应的影响[J]. 物理化学学报, 2015, 31(5): 933-940. doi: 10.3866/PKU.WHXB201503032 shu

Citation: LIU Na, ZHANG Hui, XUE Nian-Hua, DING Wei-Ping. Influence of Tungsten Loadings on the 1-Butene Metathesis Reaction over W/SiO₂/Al₂O₃ Catalysts[J]. Acta Physico-Chimica Sinica, 2015, 31(5): 933-940. doi: 10.3866/PKU.WHXB201503032 shu

钨含量对W/SiO₂/Al₂O₃催化剂上1-丁烯自歧化反应的影响

柳娜 ^1, ,
张辉 ^1, ,
薛念华 ^2, ,
丁维平 ^2,

基金项目:
国家自然科学基金(21403164) (21403164)

国家大学生创新创业训练项目(S14024)资助 (S14024)

摘要:

采用浸渍法制备了一系列钨负载量不同的W/SiO₂/Al₂O₃ 催化剂. 采用X 射线衍射(XRD)、激光拉曼(Raman)光谱、紫外-可见(UV-Vis)光谱、氢气程序升温还原(H₂-TPR)和氨程序升温脱附(NH₃-TPD)等技术对催化剂进行了表征. 实验结果表明: 钨的负载量对催化剂上氧化钨物种的分散程度、还原性以及催化剂的酸性有非常重要的影响. 对该类催化剂上1-丁烯自歧化反应进行了详细考察, 结果表明: 当钨的质量分数为6.0%时,W/SiO₂/Al₂O₃催化剂表现出最佳的歧化活性和稳定性. 原因在于6.0%的钨负载量可以使催化剂上氧化钨物种具有中等程度的分散性、合适的还原性, 并且使催化剂具有一定程度的酸性, 这些因素有利于在催化剂上形成烯烃歧化活性位.

关键词:

1-丁烯
/ 丙烯
/ 歧化
/ 钨负载量
/ 催化活性

English

Influence of Tungsten Loadings on the 1-Butene Metathesis Reaction over W/SiO₂/Al₂O₃ Catalysts

1.
1 College of Chemistry and Chemical Engineering, Xi'an University of Science and Technology, Xi'an 710054, P. R. China;
2 Key Laboratory of Mesoscopic Chemistry of MOE, College of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, P. R. China
Received Date: 30 December 2014
Available Online: 08 May 2015
Fund Project:
国家自然科学基金(21403164)

国家大学生创新创业训练项目(S14024)资助

Abstract:

A series of W/SiO₂/Al₂O₃ catalysts with various tungsten loadings were synthesized via the impregnation method. The as-synthesized catalysts were characterized by X-ray diffraction (XRD), Raman spectroscopy, ultraviolet-visible (UV-Vis) spectroscopy, H2 temperature-programmed reduction (H₂-TPR), and NH₃ temperature-programmed desorption (NH₃-TPD). The results reveal that the tungsten loadings were crucial to the dispersion and reducibility of the tungsten oxide species and the acidity of catalysts. The catalytic performances were also investigated during the metathesis of 1-butene to propene. Amongst these catalysts, W/SiO₂/Al₂O₃ with a tungsten mass fraction of 6.0% gave the highest activity and stability during the 1-butene metathesis reaction. The excellent catalytic performance of the catalyst containing a tungsten mass fraction of 6.0% is attributed to its moderate dispersion, suitable reducibility of the WO_x species and suitable acidity. We speculate that these factors are favorable for the formation of active centers for olefin metathesis.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

钨含量对W/SiO₂/Al₂O₃催化剂上1-丁烯自歧化反应的影响

English

Influence of Tungsten Loadings on the 1-Butene Metathesis Reaction over W/SiO₂/Al₂O₃ Catalysts

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