With the development of hydrogen energy,palladium-based membranes have been widely used in hydrogen separation and purification.However,the poor chemical stability of palladium composite membranes limits their commerc...With the development of hydrogen energy,palladium-based membranes have been widely used in hydrogen separation and purification.However,the poor chemical stability of palladium composite membranes limits their commercial applications.In this study,a zeolite-palladium composite membrane with a sandwich-like structure was obtained by using a TS-1 zeolite film grown on the surface of palladium membrane.The membrane microstructure was characterized by SEM and EDX.The effects of the TS-1 film on the hydrogen permeability and stability of palladium composite membrane were investigated in details.Benefited from the protection of the TS-1 zeolite film,the stability of palladium composite membrane was enhanced.The results indicate that the TS-1-Pd composite membrane was stable after eight cycles of the temperature exchange cycles between 773 K and 623 K.Especially,the loss of hydrogen permeance for TS-1-Pd composite membrane was much smaller than that of the pure palladium membrane when the membrane was tested in the presence of C3H6atmosphere.It indicated that the TS-1-Pd composite membrane had better chemical stability in comparison with pure palladium membrane,owing to its sandwich-like structure.This work provides an efficient way for the deposition of zeolite film on palladium membrane to enhance the membrane stability.展开更多
Zeolite A/CS xerogel hybrid films were prepared by in-situ crystallization method with uniform structure and good strength.The hybrid films prepared from the precursor films dried at 50℃showed zeolite A was well crys...Zeolite A/CS xerogel hybrid films were prepared by in-situ crystallization method with uniform structure and good strength.The hybrid films prepared from the precursor films dried at 50℃showed zeolite A was well crystallized.The hybrid films show high water absorption,good elastic strength and Young modulus.The antimicrobial ability of the hybrid films was investigated after Ag^(+)-ion exchanged.The Ag^(+)-exchanged hybrid films with 35%(mass)content of zeolite A showed the highest antimicrobial activity,which could reduce the concentration of the microbial to zero after 7 h.展开更多
Ti02 coatings on natural feather zeolite are respectively prepared by a collosol （Sol-gel） method and two powder coating methods with deionizod water or dehydrated ethanol as a dispersant. During degradation of orth...Ti02 coatings on natural feather zeolite are respectively prepared by a collosol （Sol-gel） method and two powder coating methods with deionizod water or dehydrated ethanol as a dispersant. During degradation of orthomono- chlorphenol solutions by ultraviolet, the strong adsorption capability of the zeolite results in increased concentration of substrate on its surface. The Ti（h film coated on feather zeolite further enhances the photocatalytic activity. The TiO~ film on the zeolite prepared by the Sol-gel method is found more effective as a catalyst than that by two powder coating methods.展开更多
Recently, the development of high-performance bifunctional oxygen catalysts integrated with flexible conductive scaffolds f or rechargeable metal-air batteries has attracted considerable interest, driving by fastgrowi...Recently, the development of high-performance bifunctional oxygen catalysts integrated with flexible conductive scaffolds f or rechargeable metal-air batteries has attracted considerable interest, driving by fastgrowing wearable electronics. Herein, we report a flexible bifunctional oxygen catalyst thin film consisting of Co–N–C bifunctional catalysts embedding in carbon nanotube(CNT) networks. The catalyst is readily prepared by pyrolysis of cobalt-based zeolitic imidazolate frameworks(ZIF-67) that are in-situ synthesized in CNT networks. Such catalyst film demonstrates very high catalytic activities for oxygen reduction(onset potential: 0.91 V, and half-wave potential: 0.87 V vs. RHE) and oxygen evolution(10 m Acm^-2 at 1.58 V) reactions, high methanol tolerance property, and long-term stability(97% current retention). Moreover, our integrated catalyst film shows very good structure flexibility and robustness. Based on the obtained film air electrodes, flexible Zn–air batteries demonstrate low charging and discharging overpotentials(0.82 V at 1 m A cm^-1) and excellent structure stability in the bending tests. These results indicate that presently reported catalyst films are potential air electrodes for flexible metal–air batteries.展开更多
In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics(MTA)technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthesized via hydrot...In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics(MTA)technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthesized via hydrothermal crystallization. The Si/Al ratio of SAPO-34 film was used as the only variable to study this material. The composite zeolite material with 0.6Si/Al ratio of SAPO-34 has the largest mesoporous specific surface area and the most suitable acid distribution. The catalytic performance for the MTA process showed that 0.6-SAPO-34/ZSM-5/quartz film has as high as 50.3% benzene-toluenexylene selectivity and 670 min lifetime. The MTA reaction is carried out through the path we designed to effectively avoid the hydrocarbon pool circulation of ZSM-5 zeolite, so as to improve the aromatics selectivity and inhibit the occurrence of deep side reactions to a great extent. The coke deposition behavior was monitored by thermogravimetric analysis and gas chromatograph/mass spectrometer, it is found that with the increase of Si/Al ratio, the active intermediates changed from low-substituted methylbenzene to high-substituted methylbenzene, which led to the rapid deactivation of the catalyst. This work provides a possibility to employ the synergy effect of composite zeolite film synthesizing anti-carbon deposition catalyst in MTA reaction.展开更多
A novel zeolite-coated fiber sensors for detection of volatile organic compounds （VOCs） based on the Fabry-Perot interferometer was proposed and demonstrated. The sensor comprised a polycrystalline silicalite thin f...A novel zeolite-coated fiber sensors for detection of volatile organic compounds （VOCs） based on the Fabry-Perot interferometer was proposed and demonstrated. The sensor comprised a polycrystalline silicalite thin film grown up on the cleaved end face of a standard single-mode fiber. The inline Fabry-Perot cavity was composed by the end face of the single-mode fiber and the thin film. The sensor device operated by measuring the interference signal, which was a function of the amount of chemical vapor adsorption in its crystalline micro porous structure. Experimental results showed that the proposed VOC sensor worked well and the sensitivities were 2.78×10^-3dB/ppm when the concentration ranged from 350ppm to 2100ppm and 1.23×10^-3 dB/ppm when the concentration ranged from 2100ppm to 5250 ppm.展开更多
Exploring the native defects of zeolites is highly important for understanding the properties of zeolites, such as catalysis and optics. Here, ITQ-16 films were prepared via the secondary growth method in the presence...Exploring the native defects of zeolites is highly important for understanding the properties of zeolites, such as catalysis and optics. Here, ITQ-16 films were prepared via the secondary growth method in the presence of Ge atoms. Various intrinsic defects of ITQ-16 films were fully studied through photoluminescence and FTIR characterizations. It was found that both the as-synthesized and calcined ITQ-16 films displayed multicolor photolumines- cence including ultraviolet, blue, green and red emissions by exciting upon appropriate wavelengths. The results in- dicate that Si--OH and non-bridging oxygen hole centers（NBOHCs） are responsible for the origin of green and red emissions at 540--800 nm, while according to a variety of emission bands of calcined ITQ-16 film, blue emission bands at around 446 and 462 nm are attributed to peroxy free radicals（≡SiO2＊）, ultraviolet emissions ranging from 250 nm to 450 nm are suggested originating from a singlet-to-triplet transition of two-fold-coordinated Si and Ge, respectively.展开更多
Detection of oxygen and carbon dioxide is important in the field of chemical and biosensors for atmosphere and biosystem monitoring and fermentation processes. The present study reports on the preparation of zeolite f...Detection of oxygen and carbon dioxide is important in the field of chemical and biosensors for atmosphere and biosystem monitoring and fermentation processes. The present study reports on the preparation of zeolite films doped with iron nanoparticles for detection of CO2 and O2 in gas phase. Pure nanosized LTL type zeolite with monomodal particle size distribution loaded with iron （Fe-LTL） was prepared under hydrothermal condition from colloidal precursor suspensions. The zeolite was loaded with iron to different levels by ion exchange. The Fe-LTL suspensions were used for preparation of thin films on silicon wafers via spin coating method. The reduction of the iron in the zeolite films was carried out under H2 flow （50% H2 in Ar） at 300 ℃. The presence of iron nanoparticles is proved by in situ ultra-violet-visible spectroscopy. The properties of the films including surface roughness, thickness, porosity, and mechanical stability were studied. In addition, the loading and distribution of iron in the zeolite films were investigated. The Fe-LTL zeolite films were used to detect O2 and CO2 in a concentration dependent mode, followed by IR spectroscopy. The changes in the IR bands at 855 and 642 cm^-1 （Fe O-H and Fe-O bending vibrations） and at 2363 and 2333 cm^-1 （CO2 asymmetric stretching） corresponding to the presence of O2 and CO2, respectively, were evaluated. The response to O2 and CO2 was instant, which was attributed to great accessibility of the iron in the nanosized zeolite crystals. The saturation of the Fe-LTL films with CO2 and O2 at each concentration was reached within less than a minute. The Fe-LTL films detected both oxygen and carbon dioxide in contrast, to the pure LTL zeolite film.展开更多
基金financial support provided by Liaoning Revitalization Talents Program(XLYC2007171)the Natural Science Foundation of Liaoning Province(2021-MS-321)Research funding project of Liaoning Provincial Education Department(LJKZZ20220086)。
文摘With the development of hydrogen energy,palladium-based membranes have been widely used in hydrogen separation and purification.However,the poor chemical stability of palladium composite membranes limits their commercial applications.In this study,a zeolite-palladium composite membrane with a sandwich-like structure was obtained by using a TS-1 zeolite film grown on the surface of palladium membrane.The membrane microstructure was characterized by SEM and EDX.The effects of the TS-1 film on the hydrogen permeability and stability of palladium composite membrane were investigated in details.Benefited from the protection of the TS-1 zeolite film,the stability of palladium composite membrane was enhanced.The results indicate that the TS-1-Pd composite membrane was stable after eight cycles of the temperature exchange cycles between 773 K and 623 K.Especially,the loss of hydrogen permeance for TS-1-Pd composite membrane was much smaller than that of the pure palladium membrane when the membrane was tested in the presence of C3H6atmosphere.It indicated that the TS-1-Pd composite membrane had better chemical stability in comparison with pure palladium membrane,owing to its sandwich-like structure.This work provides an efficient way for the deposition of zeolite film on palladium membrane to enhance the membrane stability.
基金We are grateful for financial support from the National&Local Joint Engineering Research Center for Deep Utilization Technology of Rock-salt Resource(SF201804)Opening Topic of Key Laboratory of Attapulgite Resources Utilization in Jiangsu Province(HPK201804)Jiangsu Province Industry University Research Project(BY2019133).
文摘Zeolite A/CS xerogel hybrid films were prepared by in-situ crystallization method with uniform structure and good strength.The hybrid films prepared from the precursor films dried at 50℃showed zeolite A was well crystallized.The hybrid films show high water absorption,good elastic strength and Young modulus.The antimicrobial ability of the hybrid films was investigated after Ag^(+)-ion exchanged.The Ag^(+)-exchanged hybrid films with 35%(mass)content of zeolite A showed the highest antimicrobial activity,which could reduce the concentration of the microbial to zero after 7 h.
文摘Ti02 coatings on natural feather zeolite are respectively prepared by a collosol （Sol-gel） method and two powder coating methods with deionizod water or dehydrated ethanol as a dispersant. During degradation of orthomono- chlorphenol solutions by ultraviolet, the strong adsorption capability of the zeolite results in increased concentration of substrate on its surface. The Ti（h film coated on feather zeolite further enhances the photocatalytic activity. The TiO~ film on the zeolite prepared by the Sol-gel method is found more effective as a catalyst than that by two powder coating methods.
基金financial supports from the National Natural Science Foundation of China(21773293 , 21603264)CAS Pioneer Hundred Talents Program (J. Di)+1 种基金The National Key Research and Development Program of China(2016YFA0203301)Key Research Program of Frontier Science of Chinese Academy of Sciences(QYZDB-SSW-SLH031)
文摘Recently, the development of high-performance bifunctional oxygen catalysts integrated with flexible conductive scaffolds f or rechargeable metal-air batteries has attracted considerable interest, driving by fastgrowing wearable electronics. Herein, we report a flexible bifunctional oxygen catalyst thin film consisting of Co–N–C bifunctional catalysts embedding in carbon nanotube(CNT) networks. The catalyst is readily prepared by pyrolysis of cobalt-based zeolitic imidazolate frameworks(ZIF-67) that are in-situ synthesized in CNT networks. Such catalyst film demonstrates very high catalytic activities for oxygen reduction(onset potential: 0.91 V, and half-wave potential: 0.87 V vs. RHE) and oxygen evolution(10 m Acm^-2 at 1.58 V) reactions, high methanol tolerance property, and long-term stability(97% current retention). Moreover, our integrated catalyst film shows very good structure flexibility and robustness. Based on the obtained film air electrodes, flexible Zn–air batteries demonstrate low charging and discharging overpotentials(0.82 V at 1 m A cm^-1) and excellent structure stability in the bending tests. These results indicate that presently reported catalyst films are potential air electrodes for flexible metal–air batteries.
基金supported by the National Natural Science Foundation of China (51974312, 51974308)the National Key Research & Development Program of China (2019YFE0100100)。
文摘In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics(MTA)technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthesized via hydrothermal crystallization. The Si/Al ratio of SAPO-34 film was used as the only variable to study this material. The composite zeolite material with 0.6Si/Al ratio of SAPO-34 has the largest mesoporous specific surface area and the most suitable acid distribution. The catalytic performance for the MTA process showed that 0.6-SAPO-34/ZSM-5/quartz film has as high as 50.3% benzene-toluenexylene selectivity and 670 min lifetime. The MTA reaction is carried out through the path we designed to effectively avoid the hydrocarbon pool circulation of ZSM-5 zeolite, so as to improve the aromatics selectivity and inhibit the occurrence of deep side reactions to a great extent. The coke deposition behavior was monitored by thermogravimetric analysis and gas chromatograph/mass spectrometer, it is found that with the increase of Si/Al ratio, the active intermediates changed from low-substituted methylbenzene to high-substituted methylbenzene, which led to the rapid deactivation of the catalyst. This work provides a possibility to employ the synergy effect of composite zeolite film synthesizing anti-carbon deposition catalyst in MTA reaction.
文摘A novel zeolite-coated fiber sensors for detection of volatile organic compounds （VOCs） based on the Fabry-Perot interferometer was proposed and demonstrated. The sensor comprised a polycrystalline silicalite thin film grown up on the cleaved end face of a standard single-mode fiber. The inline Fabry-Perot cavity was composed by the end face of the single-mode fiber and the thin film. The sensor device operated by measuring the interference signal, which was a function of the amount of chemical vapor adsorption in its crystalline micro porous structure. Experimental results showed that the proposed VOC sensor worked well and the sensitivities were 2.78×10^-3dB/ppm when the concentration ranged from 350ppm to 2100ppm and 1.23×10^-3 dB/ppm when the concentration ranged from 2100ppm to 5250 ppm.
基金Supported by the Postdoctoral Science Foundation of China（No.2013M541716）, the Postdoctoral Science Foundation of Jiangsu Province, China（No.1301055C） and the Scientific Research Foundation for the Returned Overseas Chinese Scholars Sponsored by the Ministry of Education of China（No.K510900314）.
文摘Exploring the native defects of zeolites is highly important for understanding the properties of zeolites, such as catalysis and optics. Here, ITQ-16 films were prepared via the secondary growth method in the presence of Ge atoms. Various intrinsic defects of ITQ-16 films were fully studied through photoluminescence and FTIR characterizations. It was found that both the as-synthesized and calcined ITQ-16 films displayed multicolor photolumines- cence including ultraviolet, blue, green and red emissions by exciting upon appropriate wavelengths. The results in- dicate that Si--OH and non-bridging oxygen hole centers（NBOHCs） are responsible for the origin of green and red emissions at 540--800 nm, while according to a variety of emission bands of calcined ITQ-16 film, blue emission bands at around 446 and 462 nm are attributed to peroxy free radicals（≡SiO2＊）, ultraviolet emissions ranging from 250 nm to 450 nm are suggested originating from a singlet-to-triplet transition of two-fold-coordinated Si and Ge, respectively.
文摘Detection of oxygen and carbon dioxide is important in the field of chemical and biosensors for atmosphere and biosystem monitoring and fermentation processes. The present study reports on the preparation of zeolite films doped with iron nanoparticles for detection of CO2 and O2 in gas phase. Pure nanosized LTL type zeolite with monomodal particle size distribution loaded with iron （Fe-LTL） was prepared under hydrothermal condition from colloidal precursor suspensions. The zeolite was loaded with iron to different levels by ion exchange. The Fe-LTL suspensions were used for preparation of thin films on silicon wafers via spin coating method. The reduction of the iron in the zeolite films was carried out under H2 flow （50% H2 in Ar） at 300 ℃. The presence of iron nanoparticles is proved by in situ ultra-violet-visible spectroscopy. The properties of the films including surface roughness, thickness, porosity, and mechanical stability were studied. In addition, the loading and distribution of iron in the zeolite films were investigated. The Fe-LTL zeolite films were used to detect O2 and CO2 in a concentration dependent mode, followed by IR spectroscopy. The changes in the IR bands at 855 and 642 cm^-1 （Fe O-H and Fe-O bending vibrations） and at 2363 and 2333 cm^-1 （CO2 asymmetric stretching） corresponding to the presence of O2 and CO2, respectively, were evaluated. The response to O2 and CO2 was instant, which was attributed to great accessibility of the iron in the nanosized zeolite crystals. The saturation of the Fe-LTL films with CO2 and O2 at each concentration was reached within less than a minute. The Fe-LTL films detected both oxygen and carbon dioxide in contrast, to the pure LTL zeolite film.
