Cobalt oxide encapsulated hydrophilic hierarchical Silicalite-1 for highly efficient conversion of cyclohexyl hydroperoxide

催化作用 氧化钴 环己烷 硅烷化 氧化物 吸附 化学工程 多相催化 化学 材料科学 无机化学 有机化学 工程类
作者
Baorong Wang,Tao Guo,Yao Zhang,Feibiao Chen,Peixin Rui,Xianqing Xie,Weilin Liao,Yibin Luo,Xingtian Shu
出处
期刊:Microporous and Mesoporous Materials [Elsevier BV]
卷期号:302: 110186-110186 被引量:13
标识
DOI:10.1016/j.micromeso.2020.110186
摘要

CHHP is the main product of the cyclohexane oxidation process, the rational design and preparation of solid catalysts are vital important for the development of an environmental benign CHHP conversion process. Herein, cobalt oxide encapsulated hydrophilic hierarchical Silicalite-1 was developed for CHHP conversion. In the presence of an organosilane, the encapsulation of cobalt oxide, creation of intracrystalline secondary porosity, and introduction of surface silanols were simultaneously achieved via hydrothermal synthesis. The particle size of the encapsulated cobalt oxide was about 4.7–6.3 nm, while the SBET, VT and VME are 527 m2/g, 0.417 cm3/g and 0.3 cm3/g, respectively. Moreover, the SBET further increases to 692 m2/g when the silanization process was intensified by surfactants, and the hydrophilic substrates could more easily be adsorbed by the catalyst for the abundant terminal silanols. Then, the dilute CHHP could selectively be adsorbed and activated by the catalyst, and a CHHP conversion of more than 99% could be achieved in 20min. More importantly, the catalyst exhibits outstanding activity in both the CHHP decomposition reactions and cyclohexane oxidation reaction with CHHP as the oxidant, the oxygen utilization efficiency (60%) and KA oil selectivity (120%) were notably improved. The stability of the catalyst is excellent, the activity retained after recycling for 20 times. This strategy is general, which could further be applied for the development of heterogeneous catalysts for more environmental benign chemical processes.
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