Platinum(Pt)supported on Zinc(Zn)modified silicalite-1(S-1)zeolite(denoted as Pt-Zn/S-1)was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time.Both Le...Platinum(Pt)supported on Zinc(Zn)modified silicalite-1(S-1)zeolite(denoted as Pt-Zn/S-1)was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time.Both Lewis and Bronsted acid sites were detected in Pt-Zn/S-1 catalyst by means of FT-IR adsorption of NH3 experiment,which were identified as mostly weak and medium ones.Besides,Pt and Zn species showed strong interaction,as revealed by the TPR(Temperature-programmed reduction)and XPS(X-ray photoelectron spectroscopy)experiments.Pt-Zn/S-1 catalyst exhibited excellent aromatization function rather than isomerization and cracking side reactions in the conversion of n-hexane.Pulse experimental study showed that 75.6%of n-hexane conversion and 76.8%of benzene selectivity were obtained over Pt0.1-Zn60/S-l catalyst at 550℃ and under atmospheric pressure.By spectroscopy tests and pulse experimental results,it was concluded that the n-hexane aromatization over Pt-Zn/S-1 catalyst follows a metal-acid bifunctional mechanism.Furthermore,with the assistance of Zn,the electron-deficient Pt species in Pt-Zn/S-1 showed good sulfur tolerance performance.展开更多
Hierarchical silicalite-1 zeolites were obtained from the direct conversion of a mixture of ground solid raw materials via a steam-assisted crystallization(SAC) method without involvement of any mesoscale template. ...Hierarchical silicalite-1 zeolites were obtained from the direct conversion of a mixture of ground solid raw materials via a steam-assisted crystallization(SAC) method without involvement of any mesoscale template. Only a trace amount of water was necessary during the crystallization, implying that the amount of water can be dramatically reduced, which still offers easy separation and high yields. The simple procedure involved only grinding and heating, which not only saves resources and energy, but also significantly reduces the discharge of eco-friendly synthesis of zeolites for practical applications. Compared to conventional bulk silicalite-1, the nanosized hierarchical zeolites with MFI structure show enhanced removal capabilities for methylene blue owing to their hierarchical porosity.展开更多
Metal alloys have been widely applied for heterogeneous catalysis,especially alkane dehydrogenation.However,the catalysts always suffer from sintering and coke deposition due to the rigorous reaction conditions.Herein...Metal alloys have been widely applied for heterogeneous catalysis,especially alkane dehydrogenation.However,the catalysts always suffer from sintering and coke deposition due to the rigorous reaction conditions.Herein,we described an original approach to prepare a catalyst where highly dispersed Pt clusters alloying with copper were encapsulated in silicalite-1(S-1)zeolite for propane dehydrogenation(PDH).The introduction of Cu species significantly enhances the catalytic activity and prolongs the lifetime of the catalyst.0.1Pt0.4CuK@S-1 exhibits a propane conversion of 24.8%with 98.2%selectivity of propene,and the specific activity of propylene formation is up to 32 mol·gPt^(−1)·h^(−1)at 500℃.No obvious deactivation is observed even after 73 h on stream,affording an extremely low deactivation constant of 0.00032 h^(−1).The excellent activity and stability are ascribed to the confinement of zeolites and the stabilization of Cu species for Pt clusters.展开更多
ZEOLITES and molecular sieves are crystallite materials with well-defined and uniform micropore system that can recognize and discriminate molecules according to their sizes and shapes. Therefore, zeolite and molecula...ZEOLITES and molecular sieves are crystallite materials with well-defined and uniform micropore system that can recognize and discriminate molecules according to their sizes and shapes. Therefore, zeolite and molecular sieve crystals serve as host, organizing organic and inorganic guest atoms, molecules, and supramolecular compounds in their channels or cavities, which results in host-guest materials with novel properties in optical data storage, nonlinear optics, electrochemistry and optoelectronics. The general crystallite size of zeolites and展开更多
基金financially supported by the National Natural Science Foundation of China (21603023)
文摘Platinum(Pt)supported on Zinc(Zn)modified silicalite-1(S-1)zeolite(denoted as Pt-Zn/S-1)was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time.Both Lewis and Bronsted acid sites were detected in Pt-Zn/S-1 catalyst by means of FT-IR adsorption of NH3 experiment,which were identified as mostly weak and medium ones.Besides,Pt and Zn species showed strong interaction,as revealed by the TPR(Temperature-programmed reduction)and XPS(X-ray photoelectron spectroscopy)experiments.Pt-Zn/S-1 catalyst exhibited excellent aromatization function rather than isomerization and cracking side reactions in the conversion of n-hexane.Pulse experimental study showed that 75.6%of n-hexane conversion and 76.8%of benzene selectivity were obtained over Pt0.1-Zn60/S-l catalyst at 550℃ and under atmospheric pressure.By spectroscopy tests and pulse experimental results,it was concluded that the n-hexane aromatization over Pt-Zn/S-1 catalyst follows a metal-acid bifunctional mechanism.Furthermore,with the assistance of Zn,the electron-deficient Pt species in Pt-Zn/S-1 showed good sulfur tolerance performance.
基金Supported by the National Natural Science Foundation of China(Nos.21390394, 21261130584, 91022030, 21771082), the National Basic Research Program of China(Nos.2012CB821700, 2011CB808703), the "111" Project of China(No.B07016), the Award Project of King Abdullah University of Science & Technology(No.CRG-1-2012-LAI-009), the Science and Technology Development Center Project of the Ministry of Education of China(No.20120061130012) and the Science and Technology Research Program of the 13th Five Year Plan of China(No.20120061130012) and the Fund of Education Department of Jilin Province, China(No.2016405).
文摘Hierarchical silicalite-1 zeolites were obtained from the direct conversion of a mixture of ground solid raw materials via a steam-assisted crystallization(SAC) method without involvement of any mesoscale template. Only a trace amount of water was necessary during the crystallization, implying that the amount of water can be dramatically reduced, which still offers easy separation and high yields. The simple procedure involved only grinding and heating, which not only saves resources and energy, but also significantly reduces the discharge of eco-friendly synthesis of zeolites for practical applications. Compared to conventional bulk silicalite-1, the nanosized hierarchical zeolites with MFI structure show enhanced removal capabilities for methylene blue owing to their hierarchical porosity.
基金the National Key Research and Development Program of China(No.2020YFA0210900)the Science and Technology Key Project of Guangdong Province(No.2020B010188002)+1 种基金the National Natural Science Foundation of China(Nos.21905313 and 21938001)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01C102).
文摘Metal alloys have been widely applied for heterogeneous catalysis,especially alkane dehydrogenation.However,the catalysts always suffer from sintering and coke deposition due to the rigorous reaction conditions.Herein,we described an original approach to prepare a catalyst where highly dispersed Pt clusters alloying with copper were encapsulated in silicalite-1(S-1)zeolite for propane dehydrogenation(PDH).The introduction of Cu species significantly enhances the catalytic activity and prolongs the lifetime of the catalyst.0.1Pt0.4CuK@S-1 exhibits a propane conversion of 24.8%with 98.2%selectivity of propene,and the specific activity of propylene formation is up to 32 mol·gPt^(−1)·h^(−1)at 500℃.No obvious deactivation is observed even after 73 h on stream,affording an extremely low deactivation constant of 0.00032 h^(−1).The excellent activity and stability are ascribed to the confinement of zeolites and the stabilization of Cu species for Pt clusters.
文摘ZEOLITES and molecular sieves are crystallite materials with well-defined and uniform micropore system that can recognize and discriminate molecules according to their sizes and shapes. Therefore, zeolite and molecular sieve crystals serve as host, organizing organic and inorganic guest atoms, molecules, and supramolecular compounds in their channels or cavities, which results in host-guest materials with novel properties in optical data storage, nonlinear optics, electrochemistry and optoelectronics. The general crystallite size of zeolites and