化工学报2016,Vol.67Issue(10):4176-4186,11.DOI:10.11949/j.issn.0438-1157.20160187
工业氟硅酸合成钛硅介孔分子筛催化环己烯环氧化
Synthesis of mesoporous titanosilicates from industrial by-product hexafluosilicic acid and application for catalytic cyclohexene epoxidation
摘要
Abstract
The hexafluosilicic acid, a by-product in phosphate fertilizer industry, was used as the raw material for hydrothermal synthesis of mesoporous titanosilicates with cetyltrimethylammonium bromide (CTAB) as the cationic surfactant and ammonia as neutralization agent. The influence of synthesis conditions including hydrothermal time, the ratio of CTAB to silica, Si/Ti ratio, and surfactant removal methods on the structures and properties of mesoporous titanosilicates were investigated by characterization of the resulting product with techniques of X-ray diffraction (XRD), nitrogen adsorption/desorption, scanning electron microscopy (SEM), solid UV light scattering. At the optimized synthesis condition of the ratio of SiO2:CTAB:Ti(OC4H9)4:NH3:H2O = 1:1.50:0.03:10:150 and the hydrothermal time of 5 h, mesoporous titanosilicate had specific surface area of 1116 m2·g−1 and porosity of 0.79 cm3·g−1. When used as catalyst for cyclohexene epoxidation. this mesoporous titanosilicate showed good catalytic activities with cyclohexene conversion of 68.10%, cyclohexene epoxide selectivity of 96.60%, and turnover frequencies of Ti active sites of 99.5 h−1. This new synthesis technique will greatly improve profit of phosphate fertilizer industry by utilizing the by-product hexafluosilicic acid for the production of value-added mesoporous titanosilicate.关键词
氟硅酸/介孔/分子筛/水热/催化Key words
hexafluosilicic acid/mesoporous/molecular sieves/hydrothermal/catalysis分类
化学化工引用本文复制引用
金放,刘铁良,王先桥,吴元欣..工业氟硅酸合成钛硅介孔分子筛催化环己烯环氧化[J].化工学报,2016,67(10):4176-4186,11.基金项目
国家自然科学基金项目(21306143,E041102);湖北省中低品位磷矿资源开发利用协同创新中心开放基金项目;湖北省教育厅自然科学研究项目(D20161503)。@@@@Foundation item:supported by the National Natural Science Foundation of China(21306143, E041102) (21306143, E041102)