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Synthesis and characterization of Mn-Silicalite-1 by the hydrothermal conversion of Mn-magadiite under the neutral condition and its catalytic performance on selective oxidation of styrene
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2018-04-05
Jing Zhao, Yifu Zhang, Shaoqing Zhang, Qiushi Wang, Meng Chen, Tao Hu, Changgong Meng

The incorporation of manganese into the framework of Silicalite-1 (denoted as Mn-Silicalite-1) was achieved by the hydrothermal conversion manganese ion exchanged magadiite (Mn-magadiite) under the neutral condition. The influences of the synthetic conditions (the reaction time, the reaction temperatures and the precursors) on the synthesis of Mn-Silicalite-1 were studied in detail to reveal the successful synthesis of Mn-Silicalite-1. The introduction of the manganese into the framework of Silicalite-1 was demonstrated by the means of X-ray powder diffraction (XRD), energy-dispersive X-ray spectrometer (EDS), elemental mapping, X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR), Fourier transform infrared spectroscopy (FTIR), ultraviolet-visible spectroscopy (UV-Vis), field emission scanning electron microscopy (FE-SEM), N2 adsorption/desorption isotherms and temperature-programmed reduction (TPR). The BET surface area (SBET) and pore volume (Vp) of Mn-Silicalite-1 measured 323 m2/g and 0.052 cm3/g, respectively. All results confirmed that Mn atoms were successfully doped into the framework of Silicalite-1 and homogeneous solid-solutions of Mn-Silicalite-1 were synthesized. Furthermore, the catalytic properties of the as-synthesized Mn-Silicalite-1 were evaluated by the styrene oxidation reaction. Mn-Silicalite-1 significantly increased the active sites of the catalyst and improved the catalytic efficiency. Low temperature was beneficial to the formation of styrene oxide and high temperature was beneficial to the formation of benzaldehyde.



中文翻译:

锰铁辉石在中性条件下的水热转化合成Mn-Silicalite-1及其表征及其对苯乙烯选择性氧化的催化性能

通过在中性条件下水热转化锰离子交换的magadiite(Mn-magadiite)将锰掺入Silicalite-1(表示为Mn-Silicalite-1)的骨架中。详细研究了合成条件(反应时间,反应温度和前驱体)对Mn-Silicalite-1合成的影响,揭示了Mn-Silicalite-1的成功合成。通过X射线粉末衍射(XRD),能量色散X射线光谱仪(EDS),元素映射,X射线光电子能谱(XPS)证明了将锰引入Silicalite-1构架中,电子顺磁共振(EPR),傅立叶变换红外光谱(FTIR),紫外可见光谱(UV-Vis),场发射扫描电子显微镜(FE-SEM),2个吸附/解吸等温线和程序升温还原(TPR)。Mn-Silicalite-1的BET表面积(S BET)和孔体积(V p)分别为323 m 2 / g和0.052 cm 3/ g。所有结果证实,Mn原子被成功地掺杂到Silicalite-1的骨架中,并合成了Mn-Silicalite-1的均匀固溶体。此外,通过苯乙烯氧化反应评价了合成后的Mn-Silicalite-1的催化性能。Mn-Silicalite-1显着增加了催化剂的活性中心并提高了催化效率。低温有利于氧化苯乙烯的形成,而高温有利于苯甲醛的形成。

更新日期:2018-04-06
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