Citation: YAN Jing-Sen, WANG Hai-Yan, ZHANG Jing-Ru, XU Hui-Juan. Effect of TiO₂-Al₂O₃ Support Preparation Technique on Hydrodenitrogenation of Ni₂P/TiO₂-Al₂O₃ Catalysts[J]. Acta Physico-Chimica Sinica, ;2014, 30(7): 1309-1317. doi: 10.3866/PKU.WHXB201405043 shu

Effect of TiO₂-Al₂O₃ Support Preparation Technique on Hydrodenitrogenation of Ni₂P/TiO₂-Al₂O₃ Catalysts

1.
1. Department of Chemical Engineering, China University of Petroleum East China, Qingdao 266555, Shandong Province, P. R. China;
2. Institute of Petrochemical Technology, Liaoning Shihua University, Fushun 113001, Liaoning Province, P. R. China;
3. Institute of Biomedical and Chemical Engineering, Liaoning Institute of Science and Technology, Benxi 117004, Liaoning Province, P. R. China

Received Date: 11 February 2014
Available Online: 4 May 2014

TiO₂-Al₂O₃ composite supports were prepared by in situ sol-gel and co-precipitation methods, and the supported nickel phosphide catalysts were prepared by incipient wetness impregnation and the in situ H₂ reduction method. The catalysts were characterized by X-ray diffraction (XRD), N₂ adsorption (BET), transmission electron microscopy (TEM), temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), and inductive couple plasma atomic emission spectrometry techniques (ICP-AES). The hydrodenitrogenation (HDN) activity of the supported nickel phosphide catalysts were evaluated on a continuousflow fixed-bed reactor using quinoline as the model molecule. The results showed that the composite support prepared by the in situ sol-gel method basically retained the original pore properties of γ-Al₂O₃ but with a larger surface area and decentralized pore size distribution, and TiO₂ was enriched on the tubular γ-Al₂O₃ surface. The composite support prepared by the co-precipitation method had a smaller surface area and a centralized pore size distribution, and TiO₂ was evenly dispersed on the massive γ-Al₂O₃ surface. The main active phases after reduction were Ni₂P and Ni₁₂P₅ for the catalyst supported on sol-gel prepared TiO₂-Al₂O₃, but only Ni₂P for the catalyst supported on co-precipitated TiO₂-Al₂O₃. Different TiO₂-Al₂O₃ preparation techniques and different Ti/Al atomic ratios had a great effect on the HDN activity of the catalysts. The catalyst supported on co-precipitated TiO₂-Al₂O₃ exhibited better reducibility and HDN activity than the catalyst supported on in situ sol-gel prepared TiO₂-Al₂O₃. The optimal HDN activity occurred for the catalyst supported on co-precipitated TiO₂-Al₂O₃ with an initial Ti/Al atomic ratio of 1:8. At a reaction temperature of 340 ℃, pressure of 3 MPa, hydrogen/oil volume ratio of 500, and liquid hourly space velocity of 3 h^-1, the HDN conversion of quinoline was 91.3%.
- Nickel phosphide,
- Titania,
- Alumina,
- Composite support,
- Co-precipitation method,
- Sol-gel method,
- Hydrodenitrogenation
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Effect of TiO2-Al2O3 Support Preparation Technique on Hydrodenitrogenation of Ni2P/TiO2-Al2O3 Catalysts

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通讯作者: 陈斌, bchen63@163.com

Effect of TiO₂-Al₂O₃ Support Preparation Technique on Hydrodenitrogenation of Ni₂P/TiO₂-Al₂O₃ Catalysts