金属取代型 AlPO-5 分子筛催化剂上环己烷亚硝化一步法合 ...？ http://www.chxb.cn/CN/Y2012/V33/I4/670 金属取代型 AlPO-5 分子筛催化剂 上环己烷亚硝化一步法合成 己内酰胺 郝芳1, 钟俊1, 刘平乐1,*, 游奎一1, 魏超2, 罗和安1 1 湘潭大学化工学院, 湖南湘潭 411105; 2 长沙理工大学化学与生物工程学院, 湖南长沙 410004 HAO Fang1, ZHONG Jun1, LIU Pingle1,*, YOU Kuiyi1, WEI Chao2, LUO He’an1 1College of Chemical Engineering, Xiangtan University, Xiangtan 411105, Hunan, China; 2College of Chemical and Biological Engineering, Changsha University of Science & Technology, Changsha 410004, Hunan, China Download: PDF (590KB) HTML (1KB) Export: BibTeX or EndNote (RIS) Supporting Info 摘要 采用水热法制备了一系列结晶态的 AlPO-5 (磷酸铝分子筛), SAPO-5 (硅磷酸铝分子筛) 和 MeAlPOs (金属取代型磷酸铝分子筛) 催化剂, 利用 X 射线衍射、N2 吸附脱附法、扫描电镜、粒度分布、电感耦合等离子光谱、 红外光谱 、NH3 程序升温脱附、H2 程序升温还原和热重-微分热重分析对催化剂进行了表征, 并考察了其催化环己烷亚硝化一步法制备己内酰胺的反应活性. 结果表明, 随着 Si 或金属原子引入 AlPO-5 结构中, 催化剂的 Lewis 弱酸中心增加, 同时出现了 Brønsted 强酸中心. 相对于 AlPO-5, 具有较大比表面积和较多酸中心的 SAPO-5 和 CrAPO-5 表现出较好的环己烷亚硝化反应活性, 后者环己烷转化率为 8.16%, 己内酰胺选择性达 68.17%. Service 把本文推荐给朋友 加入我的书架 加入引用管理器 Email Alert RSS 作者相关文章 郝芳 钟俊 刘平乐 游奎一 魏超 罗和安 关键词 ： 金属取代型磷酸铝分子筛 己内酰胺 环己烷 一步法 亚硝化 Abstract ： Crystalline AlPO-5, SAPO-5, and metal substituted AlPO-5 (MeAlPOs) were prepared by the hydrothermal method and characterized by X-ray diffraction, N2 adsorption-desorption, scanning electron microscopy, particle size distribution, inductively coupled plasma (ICP) spectroscopy, Fourier transform infrared (FT-IR) spectroscopy, NH3 temperature-programmed desorption (TPD), H2 temperature-programmed reduction, and thermogravimetric-differential thermogravimetric (TG-DTG) analysis. All the samples crystallized with the AFI structure. TPD profiles showed that stronger Brønsted acid sites appeared and the number of Lewis acid sites increased when Si or a metal was introduced into the framework of AlPO-5. ICP, FT-IR spectra, and TG-DTG curves confirmed that Si or the metals were incorporated into the framework of the AlPO-5. The catalytic properties of the samples in cyclohexane nitrosation to ε-caprolactam were studied. SAPO-5 with a larger BETsurface area, more Lewis acid sites, and stronger Brønsted acid sites gave better activity and selectivity thanAlPO-5. Among the MeAlPOs, CrAPO-5 with the larger BET surface area, more Lewis acid sites, and stronger Brønsted acid sites gave the better result with a conversion of 8.16% and ε-caprolactam selectivity of 68.17%. Keywords ： metal substituted aluminophosphate molecular sieve , ε-caprolactam , cyclohexane , one-step method , nitrosation 收稿日期: 2011-10-25; 出版日期: 2012-02-29 引用本文: 郝芳, 钟俊, 刘平乐等 .金属取代型 AlPO-5 分子筛催化剂上环己烷亚硝化一步法合成己内酰胺[J] 催化学报, 2012,V33(4): 670-676 HAO Fang, ZHONG Jun, LIU Ping-Le etc .One-Step Cyclohexane Nitrosation to ε-Caprolactam over Metal Substituted AlPO-5[J] Chinese Journal of Catalysis, 2012,V33(4): 670-676 链接本文: http://www.chxb.cn/CN/10.1016/S1872-2067(11)60354-9 或 http://www.chxb.cn/CN/Y2012/V33/I4/670 查看更多1个回答 . 4人已关注
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