The conversion of CO_(2) into specific aromatics by modulating the morphology of zeolites is a promising strategy.HZSM-5 zeolite with hollow tubular morphology is reported.The morphology of zeolite was precisely contr...The conversion of CO_(2) into specific aromatics by modulating the morphology of zeolites is a promising strategy.HZSM-5 zeolite with hollow tubular morphology is reported.The morphology of zeolite was precisely controlled,and the acid sites on its outer surface were passivated by steam-assisted crystallization method,so that the zeolite exhibits higher aromatic selectivity than sheet HZSM-5 zeolite and greater p-xylene selectivity than chain HZSM-5 zeolite.The tandem catalyst was formed by combining hollow tubular HZSM-5 zeolites with ZnZrO_(x)metal oxides.The para-selectivity of p-xylene reached 76.2%at reaction temperature of 320℃,pressure of 3.0 MPa,and a flow rate of 2400 mL g^(-1)h^(-1)with an H_(2)/CO_(2) molar ratio of 3/1.Further research indicates that the high selectivity of p-xylene is due to the pore structure of hollow tubular HZSM-5 zeolite,which is conducive to the formation of p-xylene.Moreover,the passivation of the acid site located on the outer surface of zeolite effectively prevents the isomerization of p-xylene.The reaction mechanism of CO_(2) hydrogenation over the tandem catalyst was investigated using in-situ diffuse reflectance Fourier transform infrared spectroscopy and density functional theory.The results showed that the CO_(2) to p-xylene followed a methanol-mediated route over ZnZrO_(x)/hollow tubular HZSM-5 tandem catalysts.In addition,the catalyst showed no significant deactivation in the 100 h stability test.This present study provides an effective strategy for the design of catalysts aimed at selectively preparing aromatics through CO_(2)hydrogenation.展开更多
The alkylation of toluene with methanol for the selective formation of p-xylene was systematically studied. Very few studies have been reported on the use of superacids such as heteropolyacids on cheap supports, such ...The alkylation of toluene with methanol for the selective formation of p-xylene was systematically studied. Very few studies have been reported on the use of superacids such as heteropolyacids on cheap supports, such as clay. This article deals with the use of different heteropoly acids （HPAs）, viz, Dodeca-Tungstophosphoric acid [H3PO4.12WO3.xH2O] （TPA）, Dodeca-Molyhdo phosphoric acid ammonium salt hydrate [H12Mo12N3O40P＋aq] （DMAA）, Dodeca-Molyhdo Phosphoric acid （PMA） on clay （MontmoriUonite, K-10） and as such plain clay. This comparative study reveals that 20%PMA/Clay shows 62% toluene conversion and 100% selectivity toward p-xylene.展开更多
The alkylation of toluene with methanol to selective formation of p-xylene has been systematically studied. ZSM-12 （MTW）/ZSM-5 co-crystalline zeolite in 40：60 proportions have been synthesized by the same molar gel...The alkylation of toluene with methanol to selective formation of p-xylene has been systematically studied. ZSM-12 （MTW）/ZSM-5 co-crystalline zeolite in 40：60 proportions have been synthesized by the same molar gel composition, but at different temperatures and periods than that of ZSM-12 and ZSM-5, separately. All the prepared samples are characterized by XRD, SEM, BET, and XRF. The activity of toluene alkylation was investigated with a mixture of toluene and methanol as a feed over the ZSM-12, ZSM-12/ZSM-5 co-crystalline, ZSM-5, and physical mixture of ZSM-12/ZSM-5. From characterization, it is observed that the ZSM-12/ZSM-5 co-crystalline material is different from that of ZSM-12, ZSM-5, and their physical mixture. Further, the ZSM-12/ZSM-5 co-crystalline zeolite produces the highest content of xylene and has better selectivity for p-xylene than ZSM-12, ZSM-5, and their physical mixture.展开更多
基金financially supported by the National Natural Science Foundation of China(22268039)the Natural Science Foundation for Distinguished Young Scholars of Gansu Province(23JRRA682)。
文摘The conversion of CO_(2) into specific aromatics by modulating the morphology of zeolites is a promising strategy.HZSM-5 zeolite with hollow tubular morphology is reported.The morphology of zeolite was precisely controlled,and the acid sites on its outer surface were passivated by steam-assisted crystallization method,so that the zeolite exhibits higher aromatic selectivity than sheet HZSM-5 zeolite and greater p-xylene selectivity than chain HZSM-5 zeolite.The tandem catalyst was formed by combining hollow tubular HZSM-5 zeolites with ZnZrO_(x)metal oxides.The para-selectivity of p-xylene reached 76.2%at reaction temperature of 320℃,pressure of 3.0 MPa,and a flow rate of 2400 mL g^(-1)h^(-1)with an H_(2)/CO_(2) molar ratio of 3/1.Further research indicates that the high selectivity of p-xylene is due to the pore structure of hollow tubular HZSM-5 zeolite,which is conducive to the formation of p-xylene.Moreover,the passivation of the acid site located on the outer surface of zeolite effectively prevents the isomerization of p-xylene.The reaction mechanism of CO_(2) hydrogenation over the tandem catalyst was investigated using in-situ diffuse reflectance Fourier transform infrared spectroscopy and density functional theory.The results showed that the CO_(2) to p-xylene followed a methanol-mediated route over ZnZrO_(x)/hollow tubular HZSM-5 tandem catalysts.In addition,the catalyst showed no significant deactivation in the 100 h stability test.This present study provides an effective strategy for the design of catalysts aimed at selectively preparing aromatics through CO_(2)hydrogenation.
文摘The alkylation of toluene with methanol for the selective formation of p-xylene was systematically studied. Very few studies have been reported on the use of superacids such as heteropolyacids on cheap supports, such as clay. This article deals with the use of different heteropoly acids （HPAs）, viz, Dodeca-Tungstophosphoric acid [H3PO4.12WO3.xH2O] （TPA）, Dodeca-Molyhdo phosphoric acid ammonium salt hydrate [H12Mo12N3O40P＋aq] （DMAA）, Dodeca-Molyhdo Phosphoric acid （PMA） on clay （MontmoriUonite, K-10） and as such plain clay. This comparative study reveals that 20%PMA/Clay shows 62% toluene conversion and 100% selectivity toward p-xylene.
文摘The alkylation of toluene with methanol to selective formation of p-xylene has been systematically studied. ZSM-12 （MTW）/ZSM-5 co-crystalline zeolite in 40：60 proportions have been synthesized by the same molar gel composition, but at different temperatures and periods than that of ZSM-12 and ZSM-5, separately. All the prepared samples are characterized by XRD, SEM, BET, and XRF. The activity of toluene alkylation was investigated with a mixture of toluene and methanol as a feed over the ZSM-12, ZSM-12/ZSM-5 co-crystalline, ZSM-5, and physical mixture of ZSM-12/ZSM-5. From characterization, it is observed that the ZSM-12/ZSM-5 co-crystalline material is different from that of ZSM-12, ZSM-5, and their physical mixture. Further, the ZSM-12/ZSM-5 co-crystalline zeolite produces the highest content of xylene and has better selectivity for p-xylene than ZSM-12, ZSM-5, and their physical mixture.
