Effect of In-Situ Synthesis of Ni@B-HZSM-5 by Nitrilotriacetic Acid Coordination Assistance on Alkylation of Benzene With Methanol
In this work,nitrilotriacetic acid ion(NTA3-)was used to coordinate with Ni2+in strong alkaline solution for the in-situ synthesis of B-Ni-supported ZSM-5 zeolite(Ni@B-HZSM-5).The catalyst was characterized by means of X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray fluorescence spectroscopy(XRF),N2 adsorption-desorption,pyridine adsorption IR spectra(Py-IR),NH3 temperature programmed desorption(NH3-TPD)and H2 temperature programmed reduction(H2-TPR).Moreover,the alkylation of benzene with methanol was evaluated in a fixed-bed reactor,and was compared to that of Ni/HZSM-5 zeolite prepared using impregnation method.The results indicate that the Ni@B-HZSM-5 catalyst prepared by in-situ synthesis exhibits uniform distribution of B and Ni,abundant weak acid and suitable hydrogenation capability,and the side reaction of methanol hydrogenation to methane is inhibited to some extent.Under the temperature of 460 ℃,H2 pressure of 0.4 MPa,n(benzene)∶n(methanol)of 1.2∶1 and MHSV of 2 h 1,4%Ni@B2-HZSM-5 has good catalytic activity in alkylation of benzene with methanol,the benzene conversion can reach up to 46.4%,the total selectivity for toluene and xylene is 95.9%,the selectivity of C8 aromatics is 35.1%,and the molar fraction of ethylbenzene in C8 aromatics is 6.1%,exhibiting excellent stability,which has better catalytic performance than Ni/HZSM-5 zeolite prepared using impregnation method.