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Highly selective epoxidation of styrene at ambient temperature under photo-assisted condition over bimetallic Eu and Ti-doped amino-functionalized mesoporous molecular sieve

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Abstract

Mesoporous molecular sieves silica materials had been functionalized employing 3-aminopropyltriethoxysilane as the surface decoration agent by a post-synthesis method and Eu and Ti with different loading ratio were synchronously anchored on amino-functionalized silica framework by incipient wetness impregnation method, respectively. The structures of the synthesized samples were evaluated by means of X-ray diffraction, Fourier transform infrared spectroscopy, ultraviolet-visible spectra, scanning electron microscope, transmission electron microscope, X-ray photoelectron spectroscopy and solid-state 29Si magic angle spinning nuclear magnetic resonance spectra. The results revealed that the highly ordered mesoporous two dimensional hexagonal structure and the mesoporous channel structure were well preserved and isolated tetrahedral surface Eu3+ and isolated [TiO4] or [HOTiO3] species were found to be grafted and highly dispersed in the amino-functionalized mesoporous framework. A significant enhancement in selectivity and conversion for the photocatalytic epoxidation of styrene has been achieved by synergistic effect based on surface ligand effect and electron density effect between Eu3+ and Ti4+ species on amino-functionalized mesoporous silica framework. The factors associated with the conversion of styrene and selectivity to styrene oxide such as the solvent, metal loading, the amount of NaOH, H2O2/Styrene, the amount of catalyst and reaction time were also investigated in details. The desired selectivity (84%) to styrene oxide and excellent conversion (32%) of styrene for the photocatalytic epoxidation of styrene with turnover frequency of 3.1 ×  10−4s−1 were obtained using aqueous H2O2 as an oxidant in the presence of acetonitrile solvent under ambient temperature.

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Funding

This work was financially supported by the National Natural Science Foundation of Anhui Province (No: 1208085MB32).

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  1. School of Chemistry and materials Science, Huaibei Normal University, No. 100 Dongshan Road, Anhui Province, 235000, Huaibei, P.R. China

    Wang Guangjian, Gao Hongyu & Cao Qingxi

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  1. Wang Guangjian
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  2. Gao Hongyu
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  3. Cao Qingxi
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Contributions

GW: contributed to the conception of the study, data analyses with constructive discussions, manuscript preparation and modification. HG: performed the experiments and contributed to data analyses and wrote manuscript. QC: contributed to experiment, data analyses and plotting in the manuscript.

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Correspondence to Wang Guangjian.

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I would like to declare on behalf of my co-authors that the work described was original research that has not been published previously, and not under consideration for publication elsewhere, in whole or in part. All the authors listed have approved the manuscript that is enclosed. All authors declared that: (i) no support, financial or otherwise, has been received from any organization that may have an interest in the submitted work; and (ii) there are no other relationships or activities that could appear to have influenced the submitted work. To the best of our knowledge, the named authors have no conflict of interest, financial or otherwise. No conflict of interest exits in the submission of this manuscript, and manuscript is approved by all authors for publication. The original manuscript and figures will be transferred, following the instruction by the Editorial Committee when the paper is accepted. I hope your favorable consideration for publication to your journal.

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Guangjian, W., Hongyu, G. & Qingxi, C. Highly selective epoxidation of styrene at ambient temperature under photo-assisted condition over bimetallic Eu and Ti-doped amino-functionalized mesoporous molecular sieve. J Porous Mater 30, 921–936 (2023). https://doi.org/10.1007/s10934-022-01396-x

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