Unique characteristics of MnOx-incorporated mesoporous silicate, Mn-FDU-5, prepared via evaporation induced self assembly
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- 作者：Gaffar Imran ; Vinju Vasudevan Srinivasan…
- 关键词：Manganese ; FDU ; 5 ; Epoxidation ; trans ; Stilbene
- 刊名：Journal of Porous Materials
- 出版年：2016
- 出版时间：February 2016
- 年：2016
- 卷：23
- 期：1
- 页码：57-65
- 全文大小：1,230 KB
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Vinju Vasudevan Srinivasan (1)
Rajamanickam Maheswari (1)
Anand Ramanathan (2)
Bala Subramaniam (2)
1. Department of Chemistry, Anna University, Chennai, 600025, India
2. Center for Environmentally Beneficial Catalysis, The University of Kansas, Lawrence, KS, 66047, USA - 刊物类别：Chemistry and Materials Science
- 刊物主题：Chemistry
Catalysis
Characterization and Evaluation Materials
Physical Chemistry - 出版者：Springer Netherlands
- ISSN：1573-4854
文摘
Mn containing 3D mesostructured FDU-5 (Ia3d) silicates with varying Si/Mn ratios were synthesized for the first time via evaporation induced self assembly (EISA) technique under acidic conditions at room temperature, employing Pl23 triblock copolymer as a structure directing agent. This method facilitates complete incorporation of higher amounts of Mn in the framework and extraframework locations of FDU-5 even under highly acidic synthesis conditions. The Mn-FDU-5 samples possessed surface areas of 300–500 m2/g, pore volumes of 0.42–0.55 cm3/g and narrow pore size distributions of 4.1–4.9 nm. Homogeneous dispersion of Mn species and aggregated Mn oxide clusters were evidenced from FIB-SEM micrographs. Complementary analytical techniques such as diffuse reflectance UV–Vis, FTIR, TPR and EPR analyses provide insights into the nature of the different types of Mn species (Mn2+, Mn3+ and Mn3O4 nanoparticles) that co-exist in FDU-5. The Mn-FDU-5 material is shown to be active for the epoxidation of trans-stilbene (TS, ~60 % conversion) to trans-stilbene epoxide (~64 % selectivity) with TBHP as oxidant. Although the activity of Mn-FDU-5 (~45 % TS conversion) is similar to those observed with MCM-41 and MCM-48 supports containing similar amounts of Mn (1 wt%), higher epoxide selectivity (~64 %) was observed with Mn-FDU-5. The mixed oxidation states of Mn (Mn2+, Mn3+) along with the extraframework Mn3O4 are found to be beneficial in catalyzing TS epoxidation. Keywords Manganese FDU-5 Epoxidation trans-Stilbene