4.7 Article

Confinement of Mn3+ redox sites in Mn-KIT-6 and its catalytic activity for styrene epoxidation

期刊

MICROPOROUS AND MESOPOROUS MATERIALS
卷 247, 期 -, 页码 190-197

出版社

ELSEVIER SCIENCE BV
DOI: 10.1016/j.micromeso.2017.03.049

关键词

Mn3+; Isomorphous substitution; KIT-6; Epoxidation

资金

  1. UGC MANF [F.40-8(C/M)/2009(SA-III/MANF)]
  2. DST (FIST) [SR/FST/CS II-028/2014(C)]
  3. UGC (SAP) [F.540/3/DRS-III/2016 (SAP-I)]

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In the present study, a series of manganese (Mn) containing 3D cubic mesoporous KIT-6 materials with different Si/Mn ratio (100, 50 25 & 10) having laid space group were synthesized for the first time by a facile one-pot hydrothermal process. The synthesized materials were methodically characterized by various analytical techniques including XRD, N-2 sorption, HR-TEM, diffuse reflectance UV vis (DRS-UVvis), EPR and FT-IR. The well ordered mesoporous nature of Mn incorporated KIT-6 materials are realized by XRD, N-2 adsorption-desorption isotherm and HR-TEM analysis. Surface area, pore volume and pore size of Mn-KIT-6 with different Si/Mn ratio are in the range of 451-786 m(2)/g, 0.57-0.9 cm(3)/g and 4.5-4.9 nm respectively. The incorporation of Mn3+ in the framework and fine dispersion of Mn2+ species over silica matrix of Mn-KIT-6 are confirmed by the results of UV-DRS, Fr-IR and EPR. Further, the presence of higher amount of Mn2+ extra-framework species in Mn-KIT-6(10) is realized by the presence of high amplitude signal and the contraction in H1 hysteresis loop as shown in EPR and BET isotherm respectively. Catalytic behavior of Mn-KIT-6 material was evaluated for the epoxidation of styrene with various oxidants in which t-butyl hydro peroxide (TBHP) promotes the desired formation of styrene oxide under mild liquid phase conditions. Mn-KIT-6 shown to be highly stable and active which mainly depends on the framework substituted Mn3+ sites. (C) 2017 Elsevier Inc. All rights reserved.

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