Enhanced performances in catalytic oxidation of <i>o</i>-xylene over hierarchical macro-/mesoporous silica-supported palladium catalysts

doi:10.1007/s11783-015-0802-1

Front. Environ. Sci. Eng.

2016, Vol. 10

Issue (3) : 458-466 https://doi.org/10.1007/s11783-015-0802-1

RESEARCH ARTICLE

Enhanced performances in catalytic oxidation of o-xylene over hierarchical macro-/mesoporous silica-supported palladium catalysts

Nanli QIAO¹,Xin ZHANG¹,Chi HE²,Yang LI¹,Zhongshen ZHANG¹,Jie CHENG¹,Zhengping HAO^1,^*(

)

1. Department of Environmental Nano-materials and Technologies, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
2. Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China

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Abstract

A series of hierarchical macro-/mesoporous silica supports (MMSs) were successfully synthesized using dual-templating technique employing polystyrene (PS) spheres and the Pluronic P123 surfactant. Pd was next loaded on the hierarchical silica supports via colloids precipitation method. Physicochemical properties of the synthesized samples were characterized by various techniques and all catalysts were tested for the total oxidation of o-xylene. Among them, the Pd/MMS-b catalyst with tetraethoxysilane/polystyrene weight ratio of 1.0 exhibited superior catalytic activity, and under a higher gas hourly space velocity (GHSV) of 70000 h^-1, the 90% conversion of o-xylene has been obtained at around 200°C. The BET and SEM results indicated that Pd/MMS-b catalyst possesses high surface area and large pore volume, and well-ordered, interconnected macropores and 2D hexagonally mesopores hybrid network. This novel ordered hierarchical porous structure was highly beneficial to the dispersion of active sites Pd nanoparticles with less aggregation, and facilitates diffusion of reactants and products. Furthermore, the Pd/MMS-b catalyst possessed good stability and durability.

Keywords hierarchical macro-/mesoporous silica palladium VOCs catalytic oxidation

Corresponding Author(s): Zhengping HAO

Online First Date: 17 July 2015 Issue Date: 05 April 2016

Cite this article:

Nanli QIAO,Xin ZHANG,Chi HE, et al. Enhanced performances in catalytic oxidation of o-xylene over hierarchical macro-/mesoporous silica-supported palladium catalysts[J]. Front. Environ. Sci. Eng., 2016, 10(3): 458-466.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-015-0802-1
https://academic.hep.com.cn/fese/EN/Y2016/V10/I3/458

Fig.1 Low angle powder XRD patterns of the support

Tab.1 The physical and textural properties of catalyst supports

Fig.2 N₂ adsorption/desorption isotherms (a) and pore size distribution calculated from the desorption branch (b) of the support

Fig.3 SEM images of the support: (a) SBA-15, (b) MMS-a (c) MMS-b and (d) MMS-c. The magnified SEM images of the MMS-d sample (e and f). TEM images of the MMS-b (g)

Tab.2 Characteristic data and catalytic activity of the synthesized catalysts

Fig.4 TEM images of Pd/MMS-b catalyst

Fig.5 H₂-TPR profiles of catalysts

Fig.6 Conversion profiles of o-xylene catalytic oxidation under different GHSV: (a) 42000h^-1; (b) 52500h^-1; (c) 70000h^-1

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