TS-1 supported highly dispersed sub-5 nm gold nanoparticles toward direct propylene epoxidation using H-2 and O-2
作者:Li, NX (Li, Naixu)[ 1 ] ; Chen, Y (Chen, Yong)[ 1 ] ; Shen, QH (Shen, Quanhao)[ 1 ] ; Yang, B (Yang,
关键字:Gold nanoparticle; Titanium silicalite-1; Homogeneous deposition; Propylene epoxidation; Structure-reactivity relationship
论文来源:期刊
具体来源:JOURNAL OF SOLID STATE CHEMISTRY
发表时间:2018年
We report a simple and efficient method for the preparation of highly dispersed Au nanoparticles (< 5 nm) on TS-1 substrate. The synthesis relies on the use of NaBH4 as a reductant for rapid Au atom generation, as well as PVA as a capping agent confining the particle size and dispersion. The samples were characterized by N-2 physisorption, inductively coupled plasma mass spectrometry, power X-ray diffraction, scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, CO pulse chemisorption and thermogravimetric analysis. The size of Au particles can be controlled in the range of 3-5 nm. The supported catalyst shows both good activity and selectivity for propylene oxide (PO) generation from direct propylene epoxidation. An optimal performance with PO formation rate of 102.94 gpo h(-1) kg(-1) eat and selectivity of 84.83% is achieved over 2.0 wt% Au/TS-1 catalyst, which is prepared by controlling PVA/Au3+'''' mass ratio of 1.5/1 and NaBH4/Au3+ mole ratio of 5/1. After 50 h test at 200 degrees C, no significant decrement of both catalytic activity and PO selectivity can be observed,indicating the excellent thermally stability of the catalyst. Furthermore, a possible reaction mechanism is described on basis of the previous researches and our experimental results.