化工学报2016,Vol.67Issue(4):1313-1323,11.DOI:10.11949/j.issn.0438-1157.20151221
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
Effects of support modifications on catalyst structure and catalytic performance for hydrogenation ofsec-butyl acetate over Cu/B/Al2O3 catalyst
摘要
Abstract
Cu-based catalysts(Cu/B/M/Al2O3, M = Mg, Ca, Ni)supported on the modifiedγ-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 ofγ-Al2O3 support with varied metal oxides on the structure of Cu-based catalysts and the catalytic performances for the hydrogenation ofsec-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 andsec-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 tosec-butanol. Moreover, formation and accumulation of non-reactive carbonaceous species on the surface of CaO-modified catalyst might be effectively minimized.关键词
催化/加氢/载体改性/铜/醋酸仲丁酯/仲丁醇Key words
catalysis/hydrogenation/support modification/copper/sec-butyl acetate/sec-butanol分类
化学化工引用本文复制引用
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):1313-1323,11.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)。@@@@supported by the Natural Science Foundation of Beijing (2154048) and the Changcheng Scholars Program of Beijing (CIT&TCD 20150316) (长城学者:CIT&TCD 20150316)