摘要
构建了以H2O2为氧化剂催化环己烯合成环氧环己烷的高效、绿色催化反应体系.在不加入铝源的情况下,以四乙基氢氧化铵(TEAOH)为模板剂,通过改进的干胶转化法控制H2O/SiO2摩尔比为1.5合成出Ti-Beta分子筛.实验结果表明,适宜的酸碱性、含水量以及模板剂用量显著影响分子筛的结晶度,同时影响晶粒尺寸和晶粒尺寸的均一性.通过对Ti-Beta分子筛原粉进行焙烧处理制得Ti-Beta分子筛催化剂,再通过对反应溶剂、反应温度和反应时间的筛选和优化,获得最优催化反应条件,在该条件下,环己烯转化率可达33.5%,环氧环己烷选择性可达99.6%.实验结果表明该催化剂是一种高效的多相催化剂.
The construction of a green catalytic reaction system with characteristic of high efficiency for the synthesis of epoxycyclohexane by catalytic epoxidation of cyclohexene with H2O2 was focused. We succeeded in synthesizing Ti-Beta zeolites in the absence of Al by the dry-gel conversion method using tetraethylammonium hydroxide(TEAOH) as the structure directing agent with n(H2O)/ n(Si) of about 1.5. We found that the crystallization, the uniformity of crystal and size of Ti-Beta were significantly affected by proper acidity and basicity , the amount of water and template dosage. Then, highly efficient Ti-Beta catalyst was prepared by calcination treatment of the raw powder. Under the optimal catalytic reaction conditions, the cyclohexene conversion of 33.5% and the epoxidation selectivity of 99.6% were achieved. The results indicate that Ti-Beta is an excellent heterogeneous catalyst.
作者
刘新超
赵亚榕
袁珍闫
周丹
鲁新环
夏清华
LIU Xinchao;ZHAO Yarong;YUAN Zhenyan;ZHOU Dan;LU Xinhuan;XIA Qinghua(Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials,Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules,Hubei University,Wuhan 430062,China)
出处
《高等学校化学学报》
SCIE
EI
CAS
CSCD
北大核心
2019年第6期1222-1228,共7页
Chemical Journal of Chinese Universities
基金
国家自然科学基金(批准号:21571055,21673069,21503074)
湖北省自然科学基金杰青项目(批准号:2016CFA040)资助~~
作者简介
联系人:周丹,女,博士,教授,博士生导师,主要从事分子筛类孔材料的合成、表征及应用研究.E-mail:d.zhou@hubu.edu.cn;联系人:夏清华,男,博士,教授,博士生导师,主要从事多孔催化材料的开发及催化性能研究. E-mail: xiaqh518@aliyun.com.
