Effect of thermal pretreatment on the surface structure of PtSn/SiO<sub>2</sub> catalyst and its performance in acetic acid hydrogenation

doi:10.1007/s11705-016-1583-1

Front. Chem. Sci. Eng.

2016, Vol. 10

Issue (3) : 417-424 https://doi.org/10.1007/s11705-016-1583-1

RESEARCH ARTICLE

Effect of thermal pretreatment on the surface structure of PtSn/SiO₂ catalyst and its performance in acetic acid hydrogenation

Guozhen Xu,Jian Zhang(

),Shengping Wang,Yujun Zhao(

),Xinbin Ma

Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Centre of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

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Abstract

The effect of thermal pretreatment on the active sites and catalytic performances of PtSn/SiO₂ catalyst in acetic acid (AcOH) hydrogenation was investigated in this article. The catalysts were characterized by N₂ physical adsorption, X-ray diffraction, transmission electron microscopy, pyridine Fourier-transform infrared spectra, and H₂-O₂ titration on its physicochemical properties. The results showed that Pt species were formed primarily in crystalline structure and no PtSn_x alloy was observed. Meanwhile, with the increment of thermal pretreatment temperature, Pt dispersion showed a decreasing trend due to the aggregation of Pt particles. Simultaneously, the amount of Lewis acid sites was remarkably influenced by such thermal pretreatment owning to the consequent physicochemical property variation of Sn species. Interestingly, the catalytic activity showed the similar variation trend with that of Lewis acid sites, confirming the important roles of Lewis acid sites in AcOH hydrogenation. Moreover, a balancing effect between exposed Pt and Lewis acid sites was obtained, resulting in the superior catalytic performance in AcOH hydrogenation.

Keywords thermal pretreatment acetic acid hydrogenation ethanol PtSn/SiO₂

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Corresponding Author(s): Jian Zhang,Yujun Zhao

Just Accepted Date: 08 July 2016 Online First Date: 10 August 2016 Issue Date: 23 August 2016

Cite this article:

Guozhen Xu,Jian Zhang,Shengping Wang, et al. Effect of thermal pretreatment on the surface structure of PtSn/SiO₂ catalyst and its performance in acetic acid hydrogenation[J]. Front. Chem. Sci. Eng., 2016, 10(3): 417-424.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-016-1583-1
https://academic.hep.com.cn/fcse/EN/Y2016/V10/I3/417

Tab.1 Physical properties of supported PtSn/SiO₂ catalysts

Fig.1 (A) N₂adsorption-desorption isotherms; (B) pore size distribution of catalysts

Fig.2 XRD patterns of the reduced catalysts

Fig.3 TEM images of the reduced catalysts. (A) PtSn/SiO₂-100, (B) PtSn/SiO₂-200, (C) PtSn/SiO₂-300, (D) PtSn/SiO₂-400, (E) PtSn/SiO₂-500, and (F) the lattice fringe image of the selected particle in (E)

Fig.4 (A,C) HAADF-STEM images, (B) EDX analysis of point 4 in A, (D) EDX line scans across individual particle (the red line 1) in C of reduced PtSn/SiO₂-500

Fig.5 FTIR spectra of chemisorbed pyridine on reduced catalysts

Fig.6 Thermogravimetric analysis (TGA) and the differential results (DTG) of fresh catalyst

Tab.2 Hydrogenation of AcOH over supported PtSn/SiO₂ catalysts^a)_.

Fig.7 Effect of L/Pt molar ratio on the catalytic performance. Reaction conditions: 270 °C, 2.6 MPa, H₂/AcOH (mol/mol) = 20

Fig.8 A hypothesized mechanism of AcOH hydrogenation over PtSn/SiO₂ catalysts

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