摘要
Zn/ZSM-5（NZ2） and Zn/Ni/ZSM-5（NZ3） as the catalysts for methanol to aromatics（MTA） were synthesized by a simple ultrasonic impregnation. The textural and acid properties of all catalysts were characterized using XRD, HRTEM, NH;-TPD, Py-IR, XPS, XRF and TG techniques. The XRD and HRTEM results showed that the basic zeolite structures were not affected much with the incorporation of Zn and Ni species. However, great changes have taken place in acid properties. The Py-IR and XPS results indicated that the Zn-Lewis acid sites（ZnOH;species）, which have stronger interaction with the zeolite framework compared with ZnO species, were generated at the expense of B acid sites with the incorporation of zinc species. Moreover, the product analysis results showed that the incorporation of zinc species promoted the primary aromatization by enhancing the dehydroaromatization and suppressing the cracking and subsequent H-transfer reaction. Furthermore, the addition of Ni species well inhibited the loss of zinc species by converting partial ZnO species to ZnOH;species, and thus improved the aromatization activity and catalyst stability. The catalytic performance results showed that the NZ3 possess higher conversion of methanol in a longer time and lower average rate of coke formation compared with NZ2. In addition,the NZ3 also exhibited the highest yield of BTX as the reaction proceeds.
Zn/ZSM-5(NZ2) and Zn/Ni/ZSM-5(NZ3) as the catalysts for methanol to aromatics(MTA) were synthesized by a simple ultrasonic impregnation. The textural and acid properties of all catalysts were characterized using XRD, HRTEM, NH_3-TPD, Py-IR, XPS, XRF and TG techniques. The XRD and HRTEM results showed that the basic zeolite structures were not affected much with the incorporation of Zn and Ni species. However, great changes have taken place in acid properties. The Py-IR and XPS results indicated that the Zn-Lewis acid sites(ZnOH^+ species), which have stronger interaction with the zeolite framework compared with ZnO species, were generated at the expense of B acid sites with the incorporation of zinc species. Moreover, the product analysis results showed that the incorporation of zinc species promoted the primary aromatization by enhancing the dehydroaromatization and suppressing the cracking and subsequent H-transfer reaction. Furthermore, the addition of Ni species well inhibited the loss of zinc species by converting partial ZnO species to ZnOH^+ species, and thus improved the aromatization activity and catalyst stability. The catalytic performance results showed that the NZ3 possess higher conversion of methanol in a longer time and lower average rate of coke formation compared with NZ2. In addition,the NZ3 also exhibited the highest yield of BTX as the reaction proceeds.
基金
entrusted by the Project of "utilization of low rank coal" strategic leading special fund
strategic leading special fund of CAS (XDA-07070800 and XDA-07070400)
the Opening Foundation of State Key Laboratory of Coal Conversion (J16-17-602)
