Hydrodealkylation of Trimethylbenzene over Silicon-based Catalyst†

doi:10.7503/cjcu20160461

Abstract

Abstract:

A series of Ni/SiO₂ catalysts, prepared via sol-gel and impregnation methods, respectively, was tested in the reaction of hydrodealkylation of 1,2,4-trimethylbenzene(1,2,4-TMB). The results showed that the volume of citric acid anhydrous(CA) have great influence on the structure, surface properties, particle size and catalytic properties. 1,2,4-TMB hardly reacted disproportionation and isomerization reaction on Lewis acid sites. The hydrogenation of benzene ring was main adverse reaction on Ni/SiO₂ catalysts. The particle size of Ni on the catalyst could be adjusted in a certain range by changing the amount of CA, and the resultant catalysts exhibited high selectivity for Benzene-Toluene-Xylene(BTX). With the optimum reaction conditions, the highest conversion of 1,2,4-Trimethylbenzene was 29.4% and the selectivity of BTX was 99.9% on the 10Ni/Si-2.0 catalyst.

Key words: Nickel catalyst, Sol-gel method, 1, 2, 4-Ttrimethylbenzene, Hydrodealkylation

CLC Number:

O643.3

TrendMD:

XIA Yanyang, BU Tiantong, WANG Licheng, ZHU Wanchun, YANG Xuwei, BAO Qiang, HAO Mengmeng, CHENG Dongdong, WANG Zhenlü. Hydrodealkylation of Trimethylbenzene over Silicon-based Catalyst^†[J]. Chem. J. Chinese Universities, 2016, 37(12): 2215.

Figures/Tables 8

Fig.1 XRD patterns of catalysts 10Ni/Si-0(a), 10Ni/Si-1.5(b), 10Ni/Si-2.0(c), 10Ni/Si-2.5(d) and 10Ni@Si(e)

Fig.2 N2 absorption-desorption isotherms(A) and pore size distribution(B) of catalysts 10Ni/Si-0(a),10Ni/Si-1.5(b), 10Ni/Si-2.0(c), 10Ni/Si-2.5(d) and 10Ni@Si(e)

Table 1 Structural properties of catalysts 10Ni/Si-X and 10Ni@Si

Catalyst	S_BET/ (m²·g^-1)	Pore volume/ (cm³·g^-1)	Average pore diameter/nm	Catalyst	S_BET/ (m²·g^-1)	Pore volume/ (cm³·g^-1)	Average pore diameter/nm
10Ni/Si-0	465.7	0.2	1.9	10Ni/Si-2.5	666.1	0.4	2.6
10Ni/Si-1.5	578.7	0.2	2.0	10Ni@Si	342.3	0.6	7.4
10Ni/Si-2.0	599.1	0.3	2.3

Fig.3 TPR spectra of fresh catalysts 10Ni/Si-1.5(a), 10Ni/Si-2.0(b), 10Ni/Si-2.5(c), 10Ni@Si(d) and aged catalyst 10Ni/Si-2.0(e)

Fig.4 Py-IR spectra of catalysts 10Ni/Si-1.5(a), 10Ni/Si-2.0(b), 10Ni/Si-2.5(c) and 10Ni@Si(d)

Fig.5 NH3-TPD spectra of catalysts 10Ni/Si-1.5(a), 10Ni/Si-2.0(b), 10Ni/Si-2.5(c) and 10Ni@Si(d)

Table 2 Catalytic results of 1,2,4-TMB hydrodealkylation over 10Ni/Si-X and 10Ni@Si catalysts*

Catalyst	Time/h	Conversion(%)	Selectivity(%)
Catalyst	Time/h	Conversion(%)	Ben.	Tol.	Xyl.
10Ni/Si-0	2	9.6	5.7	3.3	81.5
10Ni/Si-1.5	2	9.8	18.6	0.6	55.6
10Ni/Si-2.0	2	29.4	97.1	0	2.8
10Ni/Si-2.5	2	5.1	73.3	0.9	18.3
10Ni@Si	2	21.3	21.9	1.0	23.6

Fig.6 1,2,4-TMB selectivity vs. time on catalysts 10Ni/Si-1.5(a), 10Ni/Si-2.0(b), 10Ni/ Si-2.5(c) and 10Ni@Si(d)

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