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载体改性对Cu/B/Al2O3结构及其催化醋酸仲丁酯加氢性能的影响
引用本文:孙培永,贾长斌,罗学清,张胜红,姚志龙. 载体改性对Cu/B/Al2O3结构及其催化醋酸仲丁酯加氢性能的影响[J]. 化工学报, 2016, 67(4): 1313-1323. DOI: 10.11949/j.issn.0438-1157.20151221
作者姓名:孙培永  贾长斌  罗学清  张胜红  姚志龙
作者单位:1. 北京石油化工学院化学工程学院, 恩泽生物质精细化工北京市重点实验室, 北京 102617;2. 北京化工大学化学工程学院, 北京 100029
基金项目:北京市自然科学基金项目(2154048);北京市属高等学校高层次人才引进与培养计划项目(长城学者: CIT&TCD 20150316)。
摘    要:以γ-Al2O3为载体采用分步浸渍法制备了不同金属氧化物进行载体改性的Cu/B/M/Al2O3(M=Mg,Ca,Ni)催化剂,并测试了其催化醋酸仲丁酯加氢反应的性能。结果表明,以NiO进行载体改性的催化剂导致酯加氢反应中大量酸催化产物及烃类出现;以MgO进行载体改性不利于金属Cu的分散且催化剂的结构稳定性较差;以CaO对γ-Al2O3载体进行改性不仅能够促进金属Cu的分散,提高催化剂的酯加氢活性和产物选择性,而且可以有效减少反应中非活性碳物种在催化剂表面的沉积。

关 键 词:催化  加氢  载体改性    醋酸仲丁酯  仲丁醇  
收稿时间:2015-07-29
修稿时间:2015-11-17

Effects of support modifications on catalyst structure and catalytic performance for hydrogenation ofsec-butyl acetate over Cu/B/Al2O3 catalyst
SUN Peiyong,JIA Changbin,LUO Xueqing,ZHANG Shenghong,YAO Zhilong. Effects of support modifications on catalyst structure and catalytic performance for hydrogenation ofsec-butyl acetate over Cu/B/Al2O3 catalyst[J]. Journal of Chemical Industry and Engineering(China), 2016, 67(4): 1313-1323. DOI: 10.11949/j.issn.0438-1157.20151221
Authors:SUN Peiyong  JIA Changbin  LUO Xueqing  ZHANG Shenghong  YAO Zhilong
Affiliation:1. Beijing Key Laboratory of Enze Biomass Fine Chemicals, College of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing 102617, China;2. College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Abstract:Cu-based catalysts(Cu/B/M/Al2O3, M = Mg, Ca, Ni)supported on the modified γ-Al2O3 by incorporating MgO, CaO or NiO were prepared by an incipient wetness impregnation method, of which each active component was solely deposited on support. The catalysts were characterized by scanning electron microscopy(SEM), X-ray diffraction(XRD), NH3 temperature-programmed desorption(NH3-TPD), H2 temperature-programmed reduction(H2-TPR)and X-ray photoelectron spectroscopy(XPS)techniques. It showed that effects of the modifications of γ-Al2O3 support with varied metal oxides on the structure of Cu-based catalysts and the catalytic performances for the hydrogenation of sec-butyl acetate(SBA)were significant. NiO-modified catalysts exhibited dramatic increases in the yields of both ethyl acetate and butane, due to the intrinsic activity of Ni metal for alkene hydrogenation and the acidic support beneficial to transesterification and sec-butanol dehydration, while the modification with MgO resulted in a poor dispersion of Cu metal on support and an inferior catalyst stability for the SBA hydrogenation. For above two catalysts, the modification of NiO or MgO was conducted after loading B2O3 and Cu precursors on support. On the contrary, the modification with CaO was done before loading B2O3 and Cu precursors, which facilitated the Cu dispersion on support and improved both SBA conversions and the selectivity to sec-butanol. Moreover, formation and accumulation of non-reactive carbonaceous species on the surface of CaO-modified catalyst might be effectively minimized.
Keywords:catalysis  hydrogenation  support modification  copper  sec-butyl acetate  sec-butanol  
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