苯乙烯
催化作用
选择性
煅烧
硅醇
苯乙烯氧化物
沸石
分子
介孔材料
化学
过氧化氢
化学工程
纳米孔
堆积
氧化物
材料科学
有机化学
共聚物
聚合物
工程类
作者
Xue Liu,Zhongrui Wang,Tingyu Yan,Yulin Ma,Zhiguo Zhu,Xinqing Lu,Han Peng,Huiliang Li,Yuting Wang,Zejiang Liu,Sen Liu
标识
DOI:10.1016/j.cej.2023.147455
摘要
Co-zeolites with hierarchical porous are significantly desirable for the liquid-phase selective epoxidation of styrene that required relatively open reaction spaces. A typical UTL germanosilicate with the absence of organic structure-directing agent molecules inside pore channels suffered from severe structural collapse after ultrasonic treatment under pure water medium, originating from the unstable germanium-rich double four ring subunits. The simple strategy cleaved the weak linkage Ge-O bands and caused the irregular location of silicon-rich cfi layers. Subsequently, Co activity centers was incorporated into the framework through reacting with the abundant silanol groups located in the hydroxyl nests at room temperature. The random arrangement of mono- or multi- cfi layers induced the stacking faults and generated a large amount of intracrystal mesopores after calcination. The resultant Co-Meso-UTL catalysts favored the molecules diffusion of large-sized styrene and target products, improving the accessibility of Co active sites and exhibiting excellent catalytic performance in the styrene epoxidation reaction with single hydrogen peroxide (H2O2) oxidant. Especially, high styrene oxide product selectivity was also obtained through controlling appropriate H2O2-added content as well as reaction time, which possessed a highest turnover frequency value of 403 h−1 among the reported catalysts.
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