Cobalt(II) acetylacetonate complex immobilized on aminosilane-modified SBA-15 as an efficient catalyst for epoxidation of trans-stilbene with molecular oxygen
Tang, Qinghu1,2; Wang, Yanyan2; Zhang, Jian2; Qiao, Ran2; Xie, Xiaopei2; Wang, Yi3; Yang, Yanhui1
2016-06-01
发表期刊APPLIED ORGANOMETALLIC CHEMISTRY
ISSN0268-2605
卷号30期号:6页码:435-440
摘要From environmental and economic points of view, it is highly desirable to develop a clean and efficient catalytic process to produce epoxides. An attractive approach is to use a solid, recyclable catalyst and molecular oxygen as the oxidant without any sacrificial reductant or other additives. Nonetheless, the catalysts reported up to now still cannot balance catalytic activity with epoxide selectivity. It is of great importance to explore novel catalysts with both high activity and selectivity for the epoxidation of olefins. In this work, cobalt(II) acetylacetonate (Co(acac)(2)) was covalently bonded to the silica surface of SBA-15 molecular sieve by multi-step grafting using 3-aminopropytrimethoxysilane (APTS) as coupling agent. Characterizations with nitrogen physisorption, X-ray diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy and thermogravimetric analysis suggested that the metal complex was successfully immobilized on the aminosilane-modified SBA-15 surface and the channel structure remained intact. The synthesized Co(acac)(2)APTS@SBA-15 catalyst was used in the epoxidation of trans-stilbene (TS) with molecular oxygen. Compared to the sample prepared by the impregnation method as well as Co(acac)(2) solutions under the same reaction conditions, the Co(acac)(2) immobilized catalyst exhibited remarkably higher TS conversion and trans-stilbene oxide (TSO) selectivity. An increase in TS conversion with Co content was observed when the Co loading was lower than 0.70% and the 0.70Co(acac)(2)APTS@SBA-15 sample exhibited the best catalytic performance. Up to 50.1% of TS conversion could be achieved within 6 h, affording TSO selectivity as high as 96.7%. The superior catalytic performance of this particular catalyst is attributed to the high activity of the immobilized Co(acac)(2) species on SBA-15. Copyright (C) 2016 John Wiley & Sons, Ltd.
关键词Sba-15 Cobalt Acetylacetonate Trans-stilbene Epoxidation Molecular Oxygen
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1002/aoc.3451
收录类别SCI
语种英语
关键词[WOS]SELECTIVE EPOXIDATION ; MESOPOROUS SILICA ; STYRENE ; ALKENES ; MCM-41 ; AIR
WOS研究方向Chemistry
WOS类目Chemistry, Applied ; Chemistry, Inorganic & Nuclear
项目资助者scientific research key project fund of Department of Education of Henan Province(14A150043) ; Program for Innovative Research Team in Science and Technology in University of Henan Province(15IRTSTHN003) ; National Research Foundation (NRF) ; AcRF Tier 1 grant, Ministry of Education, Singapore(RG129/14) ; Prime Minister's Office, Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) program
WOS记录号WOS:000375998000009
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被引频次:5[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/21087
专题湿法冶金清洁生产技术国家工程实验室
作者单位1.Nanyang Technol Univ, Sch Chem & Biomed Engn, N1-2-B1-18,62 Nanyang Dr, Singapore 637459, Singapore
2.Henan Normal Univ, Minist Educ, Key Lab Green Chem Media & React, Collaborat Innovat Ctr Henan Prov Green Mfg Fine, Xinxiang 453007, Henan, Peoples R China
3.Chinese Acad Sci, Inst Proc Engn, Natl Engn Lab Hydromet Cleaner Prod Technol Techn, Beijing 100190, Peoples R China
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Tang, Qinghu,Wang, Yanyan,Zhang, Jian,et al. Cobalt(II) acetylacetonate complex immobilized on aminosilane-modified SBA-15 as an efficient catalyst for epoxidation of trans-stilbene with molecular oxygen[J]. APPLIED ORGANOMETALLIC CHEMISTRY,2016,30(6):435-440.
APA Tang, Qinghu.,Wang, Yanyan.,Zhang, Jian.,Qiao, Ran.,Xie, Xiaopei.,...&Yang, Yanhui.(2016).Cobalt(II) acetylacetonate complex immobilized on aminosilane-modified SBA-15 as an efficient catalyst for epoxidation of trans-stilbene with molecular oxygen.APPLIED ORGANOMETALLIC CHEMISTRY,30(6),435-440.
MLA Tang, Qinghu,et al."Cobalt(II) acetylacetonate complex immobilized on aminosilane-modified SBA-15 as an efficient catalyst for epoxidation of trans-stilbene with molecular oxygen".APPLIED ORGANOMETALLIC CHEMISTRY 30.6(2016):435-440.
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