The alkylation of methylnaphthalene(MN) with methanol in the presence of HZSM-5 is a promising route for producing 2,6-dimetylnaphthalene(2,6-DMN) with a high selectivity. However, the conversion of MN is very low...The alkylation of methylnaphthalene(MN) with methanol in the presence of HZSM-5 is a promising route for producing 2,6-dimetylnaphthalene(2,6-DMN) with a high selectivity. However, the conversion of MN is very low and the catalyst will be deactivated rapidly with increasing time on stream. In this study, the effects of the reaction pressure on the reactivity, selectivity and life of the catalyst of alkylation of MN over HZSM-5 modified by BaO were investigated. It was observed that with the enhancement of pressure, the conversion of MN increased, but the selectivity of 2,6-DMN kept unchanged, which was about 40% -42%. When the alkylation was carried out under a supercritical condition, the conversion of MN was 3-6 times higher and the life of catalyst was 25-30 times longer than those at an ambient pressure. The thermogravimetric analyses of the deactivated catalysts at different reaction pressures indicate that the amount of coke deposited on the catalysts was about 10% to 12 %, and the coke-burning reactions mainly took place in a temperature range from 720 to 860 K, and the apparent activation energies of the coke-burning catalysts at 0. 1 MPa( 10 h) and 7. 6 MPa( 108 h) were, respectively, 65.90 and 84. 72 kJ/mol. It is concluded from tile results that the supercritical condition is advantageous to enhancing the conversion of alkylation and extraction in situ, and to transporting those high molecular-weight poly-aromatic compounds so as to extend the catalyst life successively.展开更多
Alkylation of methylnaphthalene with methanol is one promising technology for producing 2,6-dimethylnaphthalene. When the alkylation is carried out under ambient pressure by using HZMS-5 catalysis, the reaction activi...Alkylation of methylnaphthalene with methanol is one promising technology for producing 2,6-dimethylnaphthalene. When the alkylation is carried out under ambient pressure by using HZMS-5 catalysis, the reaction activity is very low and obvious deactivation of catalyst is observed in a short run.This paper aims at slowing down catalyst deactivation and improving reaction activity of alkylation of methylnaphthalene with methanol by taking advantage of some special properties of supercritical fluids, such as higher solubility than gases and higher diffusivity than liquids. The results indicate that the reaction under supercritical condition will achieve high reaction activity and long catalyst life. When the reaction was carried out at 460 ℃ and 7.0 MPa which is above the critical temperature and pressure of the inert reaction solvent,1,3,5-trimethylbenzene, the reaction activity increased by 3 times and catalyst life was extended by 25 to 30 times than those under ambient pressure and at the same temperature.展开更多
文摘The alkylation of methylnaphthalene(MN) with methanol in the presence of HZSM-5 is a promising route for producing 2,6-dimetylnaphthalene(2,6-DMN) with a high selectivity. However, the conversion of MN is very low and the catalyst will be deactivated rapidly with increasing time on stream. In this study, the effects of the reaction pressure on the reactivity, selectivity and life of the catalyst of alkylation of MN over HZSM-5 modified by BaO were investigated. It was observed that with the enhancement of pressure, the conversion of MN increased, but the selectivity of 2,6-DMN kept unchanged, which was about 40% -42%. When the alkylation was carried out under a supercritical condition, the conversion of MN was 3-6 times higher and the life of catalyst was 25-30 times longer than those at an ambient pressure. The thermogravimetric analyses of the deactivated catalysts at different reaction pressures indicate that the amount of coke deposited on the catalysts was about 10% to 12 %, and the coke-burning reactions mainly took place in a temperature range from 720 to 860 K, and the apparent activation energies of the coke-burning catalysts at 0. 1 MPa( 10 h) and 7. 6 MPa( 108 h) were, respectively, 65.90 and 84. 72 kJ/mol. It is concluded from tile results that the supercritical condition is advantageous to enhancing the conversion of alkylation and extraction in situ, and to transporting those high molecular-weight poly-aromatic compounds so as to extend the catalyst life successively.
基金国家自然科学基金 (No 2 0 2 760 112 0 3 760 12 )黑龙江省科学院重点基金 (No 2 0 0 0 0 1 12)资助项目~~
文摘Alkylation of methylnaphthalene with methanol is one promising technology for producing 2,6-dimethylnaphthalene. When the alkylation is carried out under ambient pressure by using HZMS-5 catalysis, the reaction activity is very low and obvious deactivation of catalyst is observed in a short run.This paper aims at slowing down catalyst deactivation and improving reaction activity of alkylation of methylnaphthalene with methanol by taking advantage of some special properties of supercritical fluids, such as higher solubility than gases and higher diffusivity than liquids. The results indicate that the reaction under supercritical condition will achieve high reaction activity and long catalyst life. When the reaction was carried out at 460 ℃ and 7.0 MPa which is above the critical temperature and pressure of the inert reaction solvent,1,3,5-trimethylbenzene, the reaction activity increased by 3 times and catalyst life was extended by 25 to 30 times than those under ambient pressure and at the same temperature.