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One-pot synthesis of ethylene glycol by oxidative hydration of ethylene with hydrogen peroxide over titanosilicate catalysts
Journal of Catalysis ( IF 6.5 ) Pub Date : 2017-12-18 , DOI: 10.1016/j.jcat.2017.12.002
Xinqing Lu , Hao Xu , Jiaying Yan , Wen-Juan Zhou , Armin Liebens , Peng Wu

The oxidative hydration of ethylene with aqueous hydrogen peroxide was investigated over various titanosilicate catalysts for the purpose of one-pot synthesis of ethylene glycol (EG). The effect of titanosilicate topology (Ti-MWW, TS-1, Ti-MCM-68 and Ti-MOR), solvent, Ti content, catalyst amount, H2O/H2O2 ratio, reaction temperature and time on the EG production have been studied in detail. The Ti-MWW/H2O2/H2O catalytic system showed the highest EG yield together with high H2O2 conversion and utilization efficiency for the oxidative hydration of ethylene. The mechanism for the titanosilicate-catalyzed hydration of ethylene oxide (EO) has also been considered, which then shed light on the active sites for the second step in the oxidative hydration of ethylene. The catalyst deactivation could be ascribed to that the target product of EG and other heavy by-products with high boiling points were deposited inside the channels. The used Ti-MWW can be reusable when subjected to the regeneration by high-temperature calcination. Amine-assisted structural rearrangement of Ti-MWW not only enhanced the catalytic activity but also improved its stability in the oxidative hydration of ethylene.



中文翻译:

钛硅酸盐催化剂上乙烯与过氧化氢的氧化水合反应一锅法合成乙二醇

为了一锅法合成乙二醇(EG),在各种钛硅酸盐催化剂上研究了乙烯与过氧化氢水溶液的氧化水合反应。钛硅酸盐拓扑结构(Ti-MWW,TS-1,Ti-MCM-68和Ti-MOR),溶剂,Ti含量,催化剂量,H 2 O / H 2 O 2比率,反应温度和时间对EG的影响对生产进行了详细的研究。Ti-MWW / H 2 O 2 / H 2 O催化体系显示出最高的EG收率和较高的H 2 O 2乙烯氧化水化反应的转化率和利用效率。还考虑了钛硅酸盐催化环氧乙烷(EO)水合的机理,然后揭示了乙烯氧化水合第二步的活性部位。催化剂失活可以归因于EG的目标产物和其他具有高沸点的重质副产物沉积在通道内。当通过高温煅烧进行再生时,所使用的Ti-MWW可以是可重复使用的。Ti-MWW的胺辅助结构重排不仅增强了催化活性,而且还提高了其在乙烯氧化水合中的稳定性。

更新日期:2017-12-18
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