A zeolite designated as ZK-4 was synthesized hydrothermally in the system (TMA)2ONa2O-Al2O3- SiO2- H2O at 80 - 100℃ with tetramethylammonium hydroxide as an organic templating agent. The pure zeolite ZK-4 could be ...A zeolite designated as ZK-4 was synthesized hydrothermally in the system (TMA)2ONa2O-Al2O3- SiO2- H2O at 80 - 100℃ with tetramethylammonium hydroxide as an organic templating agent. The pure zeolite ZK-4 could be prepared by using the mother liquor obtained after filtration as the source of templating agent. The effect of some synthetic conditions such as the amount of tetramethylammonium hydroxide used, n [ (TMA)2O + Na2O] /n (Al2O3) ratio, n (SiO2)/n(Al2O3) ratio and crystallization time, etc. on the crystalline phase of the product was investigated. When the following molar ratios of the reaction mixture, n (SiO2)/n (Al2O3) 4-10, n[(TMA)2O+Na2O]/ n (Al2O3 ) > 7, n (Na2O)/n (Al2O3)=0. 5-2. 0, n (H2O)/ n(A12O3)=80-450, were used, pure zeolite ZK-4 could be obtained. The synthetic products were characterized by X-ray powder diffraction, atomic absorption spectrophotometry (AAS), adsorption measurement, thermogravimetric analysis(TGA), and 29Si magic angle spinning nuclear magnetic resonance technique. Zeolite ZK-4 has a higher thermal stability than sodium zeolite A due to higher n(Si)/n(Al) ratio of zeolite ZK-4.展开更多
It is essential to develop a cheap, recyclable, and efficient photocatalyst to help degrade pollutants contaminating the environment. Herein, mesoporous molecular sieve titanium phosphate （MMS-TiP） was used as an ef...It is essential to develop a cheap, recyclable, and efficient photocatalyst to help degrade pollutants contaminating the environment. Herein, mesoporous molecular sieve titanium phosphate （MMS-TiP） was used as an efficient nano-photocatalyst to degrade 2,4-dichlorophenol （2,4-DCP） and to oxidize CO. The catalyst was successfully synthesized by a simple and convenient hydrothermal method in the presence of a tri-block copolymer surfactant. Exceptional photoactivity of the optimized MMS-TiP mainly depends on its porous structure, with a large surface area by means of O2 temperature-programmed desorption curves and fluorescence spectra related to the amounts of produced hydroxyl radical. Interestingly, the photocatalytic activity of the prepared MMS-TiP could be greatly improved by coupling with nanocrystalline SnO2. This is likely due to the increase in the lifetime and separation of photogenerated charges by transferring electrons to SnO2 and was observed by steady-state surface photovoltage spectra and time-resolved surface photovoltage responses. The SnOa-coupled MMS-TiP exhibits better photocatalytic performance for 2,4-DCP degradation and better self-settlement than those of the commercial catalyst P25 TiO2. Moreover, it was confirmed by radical-trapping experiments that ·O2^- is the main activated species for the photocatalytic degradation of 2,4-DCP, and is photogenerated by electron transfer from MMS-TiP to SnO2. Furthermore, the main intermediates in the degradation of 2,4-DCP, like parachlorophenol superoxide and 1,2-benzenediol superoxide radicals, were detected, and a possible decomposition pathway related to ·O2^- attack is proposed. These experimental results provide new strategies for developing a recyclable molecular sieve- based nano-photocatalyst with high photocatalytic activity for environmental remediation.展开更多
In the study of heteroatom zeolite, Fe incorporated has displayed special properties,such as increasing selectivity of aromatics and alkenes, slow deactivation, and good antipoisoning ability. For the secondarily synt...In the study of heteroatom zeolite, Fe incorporated has displayed special properties,such as increasing selectivity of aromatics and alkenes, slow deactivation, and good antipoisoning ability. For the secondarily synthesized zeolite containing Fe, it has been an interesting subject to study the iron states and to distinguish the iron on the framework sites fom that on the nonframework sites. This note studies the secondarily展开更多
Large AlPO4-5 molecular sieve single crystals with high optical quality were synthesized hydrothermally by using TPA as template. As-synthesized crystals were calcined under O2 atmosphere to remove the organic templat...Large AlPO4-5 molecular sieve single crystals with high optical quality were synthesized hydrothermally by using TPA as template. As-synthesized crystals were calcined under O2 atmosphere to remove the organic templates in the channels. Disperse-Red-1 （DR1） and p-nitroaniline （pNA） molecules have been successfully incorporated into the one-dimensional channels of AlPO4-5 single crystals respectively by means of vapor phase diffusion. XRD patterns reveal that the loading of organic molecules has not destroyed the structures of AlPO4-5 crystals. Polarizing microscope and SHG results indicate that the DR1 and pNA molecules are well aligned in a preferred direction along the crystal channels. The different polarization-dependence SH intensity shows that different SHG processes occur in the DR1- and pNA-loaded AlPO4-5 crystals.展开更多
In this study, the improvement in the removal of chlorobenzene （C6H5Cl） in the air was investigated by combining dielectric barrier discharge （DBD） driven by bipolar pulse-power with catalysts. Molecular sieve 4A ...In this study, the improvement in the removal of chlorobenzene （C6H5Cl） in the air was investigated by combining dielectric barrier discharge （DBD） driven by bipolar pulse-power with catalysts. Molecular sieve 4A （MS-4A） and MnO2/γ-Al2O3 （MnO2/ALP） as two kinds of catalysts were tested at different positions in a DBD reactor. Catalysts were located either in the discharging area between two electrodes, or just behind the discharging area （in the afterglow area） closed to the outlet. The results indicated that DBD reactor with a bipolar pulse power-supply produced strong instant discharge and energetic particles, which can effectively activate catalysts of MS-4A and MnO2/ALP located in the afterglow area to achieve the synergistic effects on effective fission of chemical bonds of chlorobenzene. It was considered that the gas-chlorobenzene and the chlorobenzene adsorbed on the catalysts were decomposed simultaneously.展开更多
文摘A zeolite designated as ZK-4 was synthesized hydrothermally in the system (TMA)2ONa2O-Al2O3- SiO2- H2O at 80 - 100℃ with tetramethylammonium hydroxide as an organic templating agent. The pure zeolite ZK-4 could be prepared by using the mother liquor obtained after filtration as the source of templating agent. The effect of some synthetic conditions such as the amount of tetramethylammonium hydroxide used, n [ (TMA)2O + Na2O] /n (Al2O3) ratio, n (SiO2)/n(Al2O3) ratio and crystallization time, etc. on the crystalline phase of the product was investigated. When the following molar ratios of the reaction mixture, n (SiO2)/n (Al2O3) 4-10, n[(TMA)2O+Na2O]/ n (Al2O3 ) > 7, n (Na2O)/n (Al2O3)=0. 5-2. 0, n (H2O)/ n(A12O3)=80-450, were used, pure zeolite ZK-4 could be obtained. The synthetic products were characterized by X-ray powder diffraction, atomic absorption spectrophotometry (AAS), adsorption measurement, thermogravimetric analysis(TGA), and 29Si magic angle spinning nuclear magnetic resonance technique. Zeolite ZK-4 has a higher thermal stability than sodium zeolite A due to higher n(Si)/n(Al) ratio of zeolite ZK-4.
基金We are grateful to financial support from the National Natural Science of China （Nos. U1401245, 21501052, and 91622119）, the Program for Innovative Research Team in Chinese Universities （No. IRT1237）, the Research Project of Chinese Ministry of Education （No. 213011A）, Special Funding for Postdoctoral of Heilongjiang Province （No. LBH-TZ06019） and the Science Foundation for Excellent Youth of Harbin City of China （Nos. 2014RFYXJ002, 2016RQQXJ099 and UNPYSCT-2016173）.
文摘It is essential to develop a cheap, recyclable, and efficient photocatalyst to help degrade pollutants contaminating the environment. Herein, mesoporous molecular sieve titanium phosphate （MMS-TiP） was used as an efficient nano-photocatalyst to degrade 2,4-dichlorophenol （2,4-DCP） and to oxidize CO. The catalyst was successfully synthesized by a simple and convenient hydrothermal method in the presence of a tri-block copolymer surfactant. Exceptional photoactivity of the optimized MMS-TiP mainly depends on its porous structure, with a large surface area by means of O2 temperature-programmed desorption curves and fluorescence spectra related to the amounts of produced hydroxyl radical. Interestingly, the photocatalytic activity of the prepared MMS-TiP could be greatly improved by coupling with nanocrystalline SnO2. This is likely due to the increase in the lifetime and separation of photogenerated charges by transferring electrons to SnO2 and was observed by steady-state surface photovoltage spectra and time-resolved surface photovoltage responses. The SnOa-coupled MMS-TiP exhibits better photocatalytic performance for 2,4-DCP degradation and better self-settlement than those of the commercial catalyst P25 TiO2. Moreover, it was confirmed by radical-trapping experiments that ·O2^- is the main activated species for the photocatalytic degradation of 2,4-DCP, and is photogenerated by electron transfer from MMS-TiP to SnO2. Furthermore, the main intermediates in the degradation of 2,4-DCP, like parachlorophenol superoxide and 1,2-benzenediol superoxide radicals, were detected, and a possible decomposition pathway related to ·O2^- attack is proposed. These experimental results provide new strategies for developing a recyclable molecular sieve- based nano-photocatalyst with high photocatalytic activity for environmental remediation.
文摘In the study of heteroatom zeolite, Fe incorporated has displayed special properties,such as increasing selectivity of aromatics and alkenes, slow deactivation, and good antipoisoning ability. For the secondarily synthesized zeolite containing Fe, it has been an interesting subject to study the iron states and to distinguish the iron on the framework sites fom that on the nonframework sites. This note studies the secondarily
文摘Large AlPO4-5 molecular sieve single crystals with high optical quality were synthesized hydrothermally by using TPA as template. As-synthesized crystals were calcined under O2 atmosphere to remove the organic templates in the channels. Disperse-Red-1 （DR1） and p-nitroaniline （pNA） molecules have been successfully incorporated into the one-dimensional channels of AlPO4-5 single crystals respectively by means of vapor phase diffusion. XRD patterns reveal that the loading of organic molecules has not destroyed the structures of AlPO4-5 crystals. Polarizing microscope and SHG results indicate that the DR1 and pNA molecules are well aligned in a preferred direction along the crystal channels. The different polarization-dependence SH intensity shows that different SHG processes occur in the DR1- and pNA-loaded AlPO4-5 crystals.
基金National Natural Science Foundation of China(No.50678031)
文摘In this study, the improvement in the removal of chlorobenzene （C6H5Cl） in the air was investigated by combining dielectric barrier discharge （DBD） driven by bipolar pulse-power with catalysts. Molecular sieve 4A （MS-4A） and MnO2/γ-Al2O3 （MnO2/ALP） as two kinds of catalysts were tested at different positions in a DBD reactor. Catalysts were located either in the discharging area between two electrodes, or just behind the discharging area （in the afterglow area） closed to the outlet. The results indicated that DBD reactor with a bipolar pulse power-supply produced strong instant discharge and energetic particles, which can effectively activate catalysts of MS-4A and MnO2/ALP located in the afterglow area to achieve the synergistic effects on effective fission of chemical bonds of chlorobenzene. It was considered that the gas-chlorobenzene and the chlorobenzene adsorbed on the catalysts were decomposed simultaneously.
