Nb-modified Pd/Al2O3 Catalysts for Benzene Catalytic Combustion†

doi:10.7503/cjcu20130808

Abstract

Abstract:

Pd/Al₂O₃ catalyst modified by Nb promoter was prepared and tested for benzene catalytic combustion. The catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, temperature-programmed desorption of NH₃, H₂ temperature-programmed reduction, and N₂ adsorption. The results showed that the addition of Nb effectively improved the activity and stability of Pd/Al₂O₃ catalyst by increasing the dispersion of Pd active components, changing the oxidation state of partial palladium and increasing oxygen species concentration on the surface of catalyst. In case of Pd-Nb/Al₂O₃ catalyst, the benzene conversion of 90%was obtained at temperature as low as 195 ℃. Moreover, the 1%Pd-5%Nb/Al₂O₃ catalyst was more active than the 2%Pd/Al₂O₃ catalyst. It is concluded that Pd and Nb have a synergistic effect in benzene catalytic combustion.

Key words: Palladium niobium catalyst, Niobium oxide, Benzene, Catalytic combustion

CLC Number:

O643

TrendMD:

HE Zhanfeng, WANG Dan, LIU Tao, WANG Huanyi, JIANG Yi. Nb-modified Pd/Al₂O₃ Catalysts for Benzene Catalytic Combustion^†[J]. Chem. J. Chinese Universities, 2014, 35(1): 92.

Figures/Tables 11

Fig.1 Benzene conversion vs. reaction temperature over different catalystsa. 5%Nb/Al2O3; b. 1%Pd/Al2O3; c. 2%Pd/Al2O3;d. 1%Pd-5%Nb/Al2O3.

Table 1 Textural properties of different catalysts and supports

Sample	Surface area/(m²·g^-1)	Pore volume/(cm³·g^-1)	Sample	Surface area/(m²·g^-1)	Pore volume/(cm³·g^-1)
Al₂O₃	184	0.34	5%Nb/Al₂O₃	176	0.32
1%Pd/Al₂O₃	179	0.33	1%Pd-5%Nb/Al₂O₃	172	0.31
2%Pd/Al₂O₃	174	0.32

Fig.2 XRD patterns of different catalystsa. 5%Nb/Al2O3; b. 1%Pd/Al2O3;c. 1%Pd-5%Nb/Al2O3.

Fig.3 H2-TPR profiles of different catalystsa. 5%Nb/Al2O3; b. 1%Pd/Al2O3; c. 1%Pd-5%Nb/Al2O3.

Fig.4 NH3-TPD profiles of different catalystsa. 1%Pd/Al2O3; b. 1%Pd-5%Nb/Al2O3.

Fig.5 XPS Pd3d spectra of 1%Pd/Al2O3(A) and 1%Pd-5%Nb/Al2O3 catalysts(B)

Fig.6 XPS Nb3d spectra of 5%Nb/Al2O3 (A) and 1%Pd-5%Nb/Al2O3 catalysts(B)

Table 2 Elemental content and binding energy on the catalyst surface

Catalyst	Elemental content(%)				E_b/eV
Catalyst	Pd	Nb	Al	O	P $d 3 d 52$ (Pd⁰)	P $d 3 d 52$ (PdO)	N $b 3 d 52$	Al₂_p	O₁_s
5%Nb/Al₂O₃		1.3	36.0	63.0			207.2	74.4	531.4
1%Pd/Al₂O₃	0.30		36.3	63.4		336.5		74.4	531.5
1%Pd-5%Nb/Al₂O₃	0.40	1.4	32.2	66.0	335.7	337.1	207.5	74.4	531.8

Table 2 Elemental content and binding energy on the catalyst surface

Catalyst	Elemental content(%)				E_b/eV
Catalyst	Pd	Nb	Al	O	P $d 3 d 52$ (Pd⁰)	P $d 3 d 52$ (PdO)	N $b 3 d 52$	Al₂_p	O₁_s
5%Nb/Al₂O₃		1.3	36.0	63.0			207.2	74.4	531.4
1%Pd/Al₂O₃	0.30		36.3	63.4		336.5		74.4	531.5
1%Pd-5%Nb/Al₂O₃	0.40	1.4	32.2	66.0	335.7	337.1	207.5	74.4	531.8

Fig.7 HAADF-STEM images(A1,B1) and EDS(A2,A3,B2,B3) of 1%Pd/Al2O3(A1—A3) and 1%Pd-5%Nb/Al2O3(B1—B3) catalysts

Fig.8 Catalytic cycle of benzene combustion

Fig.9 Stabilities of the 1%Pd/Al2O3(a) and 1%Pd-5%Nb/Al2O3(b) catalystsBenzene concentration: 1%; space velocity: 8000 h-1; temperature: 260 ℃.

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Nb-modified Pd/Al₂O₃ Catalysts for Benzene Catalytic Combustion^†

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