Co/TUD-1催化1,2-二苯乙烯环氧化反应  

Epoxidation of trans-Stilbene over Highly Dispersed Co/TUD-1 Catalysts

作　　者：汤清虎[1] 石倩倩[1] 乔冉[1] 赵培正[1] 赵培真[1] 

机构地区：[1]河南师范大学化学与环境科学学院绿色化学介质与反应省部共建教育部重点实验室,河南新乡453007

出　　处：《石油化工》2012年第3期288-294,共7页Petrochemical Technology

基　　金：河南省高校科技创新人才支持计划(2010HASTIT028)

摘　　要：以乙酰丙酮钴(Ⅱ)为前体,采用原子层沉积法合成了Co/TUD-1催化剂,考察了该催化剂在以O2为氧化剂的1,2-二苯乙烯环氧化反应中的性能;并对催化剂进行了XRD、N2吸附-脱附、漫反射光谱和H2-TPR表征。表征结果显示,当Co负载量(w)小于等于4.0%时,TUD-1分子筛中Co主要以高度分散的CoOx形式存在;当Co负载量大于4.0%时,分子筛的孔道内外均有大量Co3O4形成。高度分散在分子筛中的CoOx是1,2-二苯乙烯环氧化的高活性组分。与采用浸渍法和水热法制备的催化剂相比,原子层沉积法制备的Co/TUD-1催化剂具有更高的活性。以负载量为4.0%的Co/TUD-1为催化剂,在100℃下反应6 h时,1,2-二苯乙烯转化率为49.3%,环氧化物选择性为96.8%。Co/TUD-1 catalysts with different Co loadings were synthesized by atomic layer deposition（ALD） method using cobalt acetylacetonate（ Ⅱ ） as the precursor and were characterized by means of XRD, N2 adsorption-desorption, DRS and HE-TPR. Activity of the prepared catalysts inepoxidation of trans-stilbene with oxygen was investigated. The results showed that the Co species on TUD-1 molecular sieves existed mainly in the form of highly dispersed CoOx when the Co content was not more than 4.0%（w）, whereas higher Co content would lead to formation of a large amount of Co304 clusters outside and inside the channels of the TUD-1 molecular sieves. Compared with the catalystsprepared by impregnation or hydrothermal method with the same Co content, Co/TUD-1 catalyst prepared by ALD method exhibited high activity in epoxidation of trans-stilbene. Under the conditions of reaction temperature 100 ℃, reaction time 6 h and Co/TUD-1 with Co loading 4.0% as the catalyst, the conversion of trans-stilbene and the selectivity to epoxide were 49.3% and 96.8%, respectively.

关 键 词：TUD-1分子筛 钴催化剂 1 2-二苯乙烯 氧气 乙酰丙酮钴 环氧化 

分 类 号：TQ426.8[化学工程]