Citation: YU Shan-Qing, TIAN Hui-Ping, ZHU Yu-Xia, DAI Zhen-Yu, LONG Jun. Mechanism of Rare Earth Cations on the Stability and Acidity of Y Zeolites[J]. Acta Physico-Chimica Sinica, ;2011, 27(11): 2528-2534. doi: 10.3866/PKU.WHXB20111101 shu

Mechanism of Rare Earth Cations on the Stability and Acidity of Y Zeolites

1.
Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, P. R. China

Received Date: 17 May 2011
Available Online: 26 August 2011
Fund Project: 国家重点基础研究发展规划项目(973) (2010CB732301)资助 (973) (2010CB732301)

The influences of rare earth (RE) cations on the stability and acidity of Y zeolites were studied by X-ray powder diffraction (XRD), solid-state magic-angle spinning nuclear magnetic resonance spectroscopy (MAS NMR), temperature-programmed desorption (TPD) of ammonia, and Fourier transform infrared of pyridine (Py-FTIR). The results showed that the stability of Y zeolites was enhanced markedly and the medium acid amount increased, but the strong acid amount of Y zeolites decreased with the introduction of RE cations. Combined with the density functional theory (DFT) calculations, a comprehensive model was proposed to describe the mechanism of RE cations on the stability and acidity of Y zeolites. RE cations located at the sodalite β cage I' sites of Y zeolites bonded strongly with O atoms, which strengthened the interaction between framework Al and its neighbouring O atoms and then enhanced evidently the stability of Y zeolites. It was the enhanced stability of REHY zeolites that restrained the release of framework Al and the formation of extra-framework Al, hence led to weaker Brönsted acid strength of REHY than that of USY. Meanwhile, RE cations located at the sodalite β cage I' sites of Y zeolites made the negative charge of O1 reduce and the bond length of Al―O1 shorten, which resulted in stronger Brönsted acid strength of REHY than that of HY. Moreover, the Bro? nsted acid amount of REHY was more than that of USY, but less than that of HY.
- Density functional theory,
- Y zeolite,
- Rare earth,
- Acidity,
- Stability
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沈阳化工大学材料科学与工程学院沈阳 110142