Template-free nanosized ZSM-5 seeds with an average size of 15 nm were prepared from a synthesis solution with the composition 12Na2O∶100SiO2∶2Al2O3∶2500H2O. By the use of these seeds, thin ZSM-5 zeolite membranes ...Template-free nanosized ZSM-5 seeds with an average size of 15 nm were prepared from a synthesis solution with the composition 12Na2O∶100SiO2∶2Al2O3∶2500H2O. By the use of these seeds, thin ZSM-5 zeolite membranes were prepared on the outer surface of a porous α-alumina tube with a pore size of 2 μm in a gel system by varying-concentration synthesis with organic-free template. The first composition synthesis sol-gel was the same as seeds of molar composition and the second one was 12Na2O∶100SiO2∶2Al2O3∶5000H2O at 180 ℃ for 10 h, respectively. XRD shows that the film consists of well-crystallized ZSM-5 zeolite. SEM investigation indicats that the zeolite films on the supports are defect free and the film thickness is approximately 8 μm. The permeances for H2, N2, CH4 and CO2 are 8.94×10-7, 3.27×10-7, 3.9×10-7, 3.14×10-7 and 0.874×10-7 mol·m2·s-1·Pa-1, respectively. The ideal selectivity of membrane at room temperature for H2/CO2, H2/N2, H2/CH4 are 2.84, 2.73 and 2.29, respectively.展开更多
Synthesis of zeolite LTN (“Linde Type N”) was investigated under insertion of a SiO2-rich filtration residue (FR) from waste water cleaning of the silane production. A new synthesis procedure was therefore developed...Synthesis of zeolite LTN (“Linde Type N”) was investigated under insertion of a SiO2-rich filtration residue (FR) from waste water cleaning of the silane production. A new synthesis procedure was therefore developed applying a flotation mechanism with the aim to grow LTN in form of thin membrane like sheets. Preparation starts with preactivation of FR by slurrying first in alkaline solution, followed by an addition of aluminate solution and citric acid. The latter was added as suitable chelating agent for the initiation of the flotation process. In the course of these experiments, we succeeded in synthesizing zeo-lite LTN with more or less zeolite SOD as byproduct in the form of a stable compact membrane-like layer at low temperature of 60℃. The crystallization was performed under isotherm static conditions in an open reaction system without addition of organic templates as structure directing agents (OSDA’s). FR was utilized as a total substitute of sodium silicate in all experiments and an expansive pre-treatment procedure like calcinations was not needed. Furthermore, membrane formation with LTN of usual synthesis needs chemically functionalized supports. In contrast self-supporting membranous LTN layers were grown for the first time in the present study.展开更多
Ultrathin zeolite membranes are of paramount importance in accelerating gas transport during membrane separation,and lowering down their membrane thicknesses to submicron scale is deemed to be very challenging.Herein,...Ultrathin zeolite membranes are of paramount importance in accelerating gas transport during membrane separation,and lowering down their membrane thicknesses to submicron scale is deemed to be very challenging.Herein,we develop an advanced approach of surface gel conversion for synthesis of submicron-thick pure silica MFI(silicalite-1)zeolite membranes.Viscous gel is prepared by finely adjusting the precursor composition,enabling its reduced wettability.The unfavorable wetting of the support surface can effectively prevent gel penetration into alumina support voids.Aided by the seeds,the surface gel is directly and fully crystallized into an MFI zeolite membrane with minimal water steam.A membrane with a thickness of 500 nm is successfully acquired and it is free of visible cracks.Additionally,the as-synthesized membranes exhibit rapid and selective separation of hexane isomers by virtue of unprecedentedly high n-hexane permeance of 24.5×10^−7 mol m^−2 s^−1 Pa^−1 and impressive separation factors of 13.3-22.6 for n-hexane over its isomers.This developed approach is of practical interest for sustainable synthesis of high-quality zeolite membranes.展开更多
Silicalite-1/ceramic composite membrane was prepared on the outer surface of the α-Al2O3 tubular support byin-situ hydrothermal synthesis. The membrane was characterized by X-ray diffraction (XRD) and scanning electr...Silicalite-1/ceramic composite membrane was prepared on the outer surface of the α-Al2O3 tubular support byin-situ hydrothermal synthesis. The membrane was characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM). The pure gas permeances of H2, N2, Ar, CH4, C2H4, C2H6, C3H8, n-C4H10 and i-C4H10 were measured as a function of the pressure difference at 298 and 473 K. The permeances of H2, N2 and Ar showed little dependence on the pressure differences; the permselectivities of H2/i-C4H10 were 249 and 36.2 at 298 and 473 K respectively, which is a characteristic of molecular transport in silicalite-1 channels. The permeances of light alkanes decreased in the following order: CH4】C2H6】C3H8】n-C4H10】i-C4H10. The permselectivity of n-C4H10/i-C4H10 was above 15 at 298 K. As the temperature increased, the permeances of all gases increased except those of N2 and Ar, and a significant increment was found for alkanes. The permselectivity ofn-C4H10/i-C4H10 decreased to about 9 at 473 K. The gas permeation results showed that the silicalite-1/ceramic composite membrane was defect-free.展开更多
A-type zeolite membranes were prepared on the nonporous metal supports by using electrophoretic tech- nique. The as-synthesized membranes were characterized by XRD and SEM. The effect of the applied potential on the f...A-type zeolite membranes were prepared on the nonporous metal supports by using electrophoretic tech- nique. The as-synthesized membranes were characterized by XRD and SEM. The effect of the applied potential on the formation of the A-type zeolite membrane was investigated, and the formation mechanism of zeolite membrane in the electric field was discussed. The results showed that the negative charged zeolite particles could migrate to the anode metal surface homogenously and rapidly under the action of the applied electric field, consequently formed uniform and dense membranes in short time. The applied potential had great effect on the membrane formation, and more uniform and denser zeolite membranes were prepared on the non- porous metal supports with 1 V potential.展开更多
基金This work was financially supported by the Specialized Research Fund for the Doctoral Program of High Education (SRFDP)(No.B20020288015).
文摘Template-free nanosized ZSM-5 seeds with an average size of 15 nm were prepared from a synthesis solution with the composition 12Na2O∶100SiO2∶2Al2O3∶2500H2O. By the use of these seeds, thin ZSM-5 zeolite membranes were prepared on the outer surface of a porous α-alumina tube with a pore size of 2 μm in a gel system by varying-concentration synthesis with organic-free template. The first composition synthesis sol-gel was the same as seeds of molar composition and the second one was 12Na2O∶100SiO2∶2Al2O3∶5000H2O at 180 ℃ for 10 h, respectively. XRD shows that the film consists of well-crystallized ZSM-5 zeolite. SEM investigation indicats that the zeolite films on the supports are defect free and the film thickness is approximately 8 μm. The permeances for H2, N2, CH4 and CO2 are 8.94×10-7, 3.27×10-7, 3.9×10-7, 3.14×10-7 and 0.874×10-7 mol·m2·s-1·Pa-1, respectively. The ideal selectivity of membrane at room temperature for H2/CO2, H2/N2, H2/CH4 are 2.84, 2.73 and 2.29, respectively.
文摘Synthesis of zeolite LTN (“Linde Type N”) was investigated under insertion of a SiO2-rich filtration residue (FR) from waste water cleaning of the silane production. A new synthesis procedure was therefore developed applying a flotation mechanism with the aim to grow LTN in form of thin membrane like sheets. Preparation starts with preactivation of FR by slurrying first in alkaline solution, followed by an addition of aluminate solution and citric acid. The latter was added as suitable chelating agent for the initiation of the flotation process. In the course of these experiments, we succeeded in synthesizing zeo-lite LTN with more or less zeolite SOD as byproduct in the form of a stable compact membrane-like layer at low temperature of 60℃. The crystallization was performed under isotherm static conditions in an open reaction system without addition of organic templates as structure directing agents (OSDA’s). FR was utilized as a total substitute of sodium silicate in all experiments and an expansive pre-treatment procedure like calcinations was not needed. Furthermore, membrane formation with LTN of usual synthesis needs chemically functionalized supports. In contrast self-supporting membranous LTN layers were grown for the first time in the present study.
基金the National Natural Science Foundation of China(21531003,21501024 and 21971035)Jilin Scientific and Technological Development Program(20170101198JC and 20190103017JH)+2 种基金Jilin Education Office(JJKH20180015KJ)“111”Program(B18012)open projects from the State Key Laboratory of Inorganic Synthesis&Preparative Chemistry and State Key Laboratory of Heavy Oil Processing(2018-8,SKLOP201902003)。
文摘Ultrathin zeolite membranes are of paramount importance in accelerating gas transport during membrane separation,and lowering down their membrane thicknesses to submicron scale is deemed to be very challenging.Herein,we develop an advanced approach of surface gel conversion for synthesis of submicron-thick pure silica MFI(silicalite-1)zeolite membranes.Viscous gel is prepared by finely adjusting the precursor composition,enabling its reduced wettability.The unfavorable wetting of the support surface can effectively prevent gel penetration into alumina support voids.Aided by the seeds,the surface gel is directly and fully crystallized into an MFI zeolite membrane with minimal water steam.A membrane with a thickness of 500 nm is successfully acquired and it is free of visible cracks.Additionally,the as-synthesized membranes exhibit rapid and selective separation of hexane isomers by virtue of unprecedentedly high n-hexane permeance of 24.5×10^−7 mol m^−2 s^−1 Pa^−1 and impressive separation factors of 13.3-22.6 for n-hexane over its isomers.This developed approach is of practical interest for sustainable synthesis of high-quality zeolite membranes.
文摘Silicalite-1/ceramic composite membrane was prepared on the outer surface of the α-Al2O3 tubular support byin-situ hydrothermal synthesis. The membrane was characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM). The pure gas permeances of H2, N2, Ar, CH4, C2H4, C2H6, C3H8, n-C4H10 and i-C4H10 were measured as a function of the pressure difference at 298 and 473 K. The permeances of H2, N2 and Ar showed little dependence on the pressure differences; the permselectivities of H2/i-C4H10 were 249 and 36.2 at 298 and 473 K respectively, which is a characteristic of molecular transport in silicalite-1 channels. The permeances of light alkanes decreased in the following order: CH4】C2H6】C3H8】n-C4H10】i-C4H10. The permselectivity of n-C4H10/i-C4H10 was above 15 at 298 K. As the temperature increased, the permeances of all gases increased except those of N2 and Ar, and a significant increment was found for alkanes. The permselectivity ofn-C4H10/i-C4H10 decreased to about 9 at 473 K. The gas permeation results showed that the silicalite-1/ceramic composite membrane was defect-free.
文摘A-type zeolite membranes were prepared on the nonporous metal supports by using electrophoretic tech- nique. The as-synthesized membranes were characterized by XRD and SEM. The effect of the applied potential on the formation of the A-type zeolite membrane was investigated, and the formation mechanism of zeolite membrane in the electric field was discussed. The results showed that the negative charged zeolite particles could migrate to the anode metal surface homogenously and rapidly under the action of the applied electric field, consequently formed uniform and dense membranes in short time. The applied potential had great effect on the membrane formation, and more uniform and denser zeolite membranes were prepared on the non- porous metal supports with 1 V potential.
