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钛硅分子筛催化1-丁烯环氧化反应溶剂效应和酸碱效应研究
引用本文:马书启,李钢,王祥生.钛硅分子筛催化1-丁烯环氧化反应溶剂效应和酸碱效应研究[J].分子催化,2005,19(1):7-11.
作者姓名:马书启  李钢  王祥生
作者单位:1. 大连理工大学,催化化学与工程系,辽宁,大连,116012
2. 大连理工大学,催化化学与工程系,辽宁,大连,116012;大连理工大学,精细化工国家重点实验室,辽宁,大连,116012
基金项目:全国高等学校优秀博士学位论文作者专项基金
摘    要:研究了用双氧水为氧化剂,钛硅分子筛TS-1催化1-丁烯环氧化反应的溶剂效应.研究发现,在质子性溶剂中1-丁烯环氧化反应活性高于非质子性溶剂,而以甲醇为溶剂H2O2转化率最高.分别利用碱性添加物稀氨水溶液和酸性添加物稀盐酸溶液调变反应介质的pH值,考察了介质的pH值对1-丁烯环氧化反应的影响,结果表明,随pH值提高,1,2-环氧丁烷(B0)的选择性略提高,但是过量稀氨水的加入会导致催化剂失活,双氧水的转化率及利用率明显下降.与钛硅分子筛催化丙烯环氧化相比,酸性添加物的加入对反应结果的影响不大,随反应介质的pH值降低1,2-环氧丁烷的选择性没有明显下降.

关 键 词:钛硅分子筛  1-丁烯  环氧化  溶剂效应  酸碱效应
文章编号:1001-3555(2005)01-0007-05

The Effect of Solvent and Acid-base on 1-Butylene Epoxidation Catalyzed by Titanium Silicalite
MA Shuqi,LI Gang,WANG Xiang-sheng.The Effect of Solvent and Acid-base on 1-Butylene Epoxidation Catalyzed by Titanium Silicalite[J].Journal of Molecular Catalysis (China),2005,19(1):7-11.
Authors:MA Shuqi  LI Gang  WANG Xiang-sheng
Abstract:The solvent effect of 1-butylene epoxidation was investigated over titanium silicate TS-1 using hydrogen peroxide as oxidant. Epoxidation activity is better in protic solvents than that in nonprotic solvents, and the conversion of H_2O_2 is the highest using methanol as solvent. Basic additive ammonia and acid additive hydrochloric acid were added respectively to change the pH value of the reaction medium. It has been shown that the selectivity of 1,2-epoxybutane(BO) was improved as the pH value increased, but excessive ammonia additive inhibited the activity of TS-1 catalyst, the conversion and the utilization of H_2O_2 decreased sharply. Compared with propylene epoxidation catalyzed by titanium silicate TS-1, the effect of acid addition on 1-butylene epoxidation is neglectable, the selectivity of BO has not obviously decreased as the pH value fell.
Keywords:TS-1
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