Yuehua Xiao, Yinjie Wang, Chengtao Wang*, Wei Fang, Pei Liu, Yu Hui, Hangjie Li, Hang Zhou and Feng-Shou Xiao*,
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引用次数: 0
Abstract
Tungstate-based catalysts for olefin metathesis generally suffer from insufficient reaction rates, which require relatively high temperatures for the satisfied activities. This issue is mainly due to the shortage of active WOx species related to intrinsic low adsorption and poor activation of olefin molecules. Herein, we found that the silanol nests in dealuminated Beta zeolite (DeAl-Beta) were favorable for high dispersion of tungsten species, forming active WOx species on the zeolite, which was helpful for the adsorption and activation of olefin molecules, thus facilitating the generation of metallocycle intermediates. As a result, the propene yield in the metathesis of ethene and 1-butene over WOx/DeAl-Beta was 2.3 times higher than that of the tungsten species supported on siliceous Beta zeolite with fewer silanol nests (WOx/Si-Beta) under the equivalent conditions. A propene yield as high as >50% was achieved by optimizing the silanol nests in the WOx/DeAl-Beta catalyst, outperforming those in the industrial silica supported tungsten species (W/SiO2) catalysts reported previously.
钨酸盐基烯烃复分解催化剂通常存在反应速率不足的问题,需要较高的温度才能达到满意的反应活性。这主要是由于烯烃分子固有的低吸附性和较差的活化性导致活性WOx种类的缺乏。我们发现脱铝β沸石(DeAl-Beta)中的硅醇巢有利于钨种的高度分散,在沸石上形成活性的WOx种,有利于烯烃分子的吸附和活化,从而促进金属环中间体的生成。结果表明,在同等条件下,在WOx/ del -Beta分子筛上进行乙烯- 1-丁烯复合反应时,丙烯的产率是在较少硅醇巢(WOx/Si-Beta)的硅质β分子筛上负载钨的2.3倍。通过优化WOx/DeAl-Beta催化剂中的硅醇巢,丙烯产率高达50%,优于之前报道的工业二氧化硅负载钨(W/SiO2)催化剂。