This article refers to the study on the performance of mesoporous silica used as the catalyst for oxidative desulfurization reactions. The test results revealed that under mild reaction conditions using tert-butyl hyd...This article refers to the study on the performance of mesoporous silica used as the catalyst for oxidative desulfurization reactions. The test results revealed that under mild reaction conditions using tert-butyl hydroperoxide as the oxidizing agent the content of dibenzothiophene(DBT) contained in oil samples could be reduced from 5000 ppm to less than 5 ppm. Furthermore,the mesoporous silica material can be easily regenerated and recycled.展开更多
Porous materials have regular three-dimensional pore structure, which has unique advantages in the field of modern pharmaceutical. At present, porous materials commonly used in the pharmaceutical field are mainly mole...Porous materials have regular three-dimensional pore structure, which has unique advantages in the field of modern pharmaceutical. At present, porous materials commonly used in the pharmaceutical field are mainly molecular sieves, macroporous adsorbent resins, activated carbon, etc. In this paper, the application status of these porous materials in the pharmaceutical field is reviewed, and the future development is prospected.展开更多
The mesoporous Al-SBA-15 zeolite was obtained via impregnation of pure silica-based SBA-15 zeolite with aluminum nitrate.The Al-SBA-15 sample was calcined in air at 800 ℃ for 6 h and hydrothermally treated at near 1...The mesoporous Al-SBA-15 zeolite was obtained via impregnation of pure silica-based SBA-15 zeolite with aluminum nitrate.The Al-SBA-15 sample was calcined in air at 800 ℃ for 6 h and hydrothermally treated at near 100 ℃ for 120 h,respectively,and then the thermal and hydrothermal stability of Al-SBA-15 sample was investigated by X-ray diffractometry (XRD),scanning electron microscopy (SEM),transmission electron microscopy (TEM) and nitrogen adsorption and desorption techniques.The Al-SBA-15 sample was also studied by 27 Al nuclear magnetic resonance (27 Al NMR) and ammonia temperature programmed desorption (NH 3-TPD) techniques.In addition,the catalytic activity of Al-SBA-15 zeolite was investigated by the Friedel-Crafts reactions of 2,4-di-tert-butylphenol with cinnamyl alcohol.The test results showed that the thermal and hydrothermal stability of Al-SBA-15 zeolite was better than that of SBA-15 zeo-lite.The Al-SBA-15 zeolite sample prepared by impregnation method exhibits more framework aluminum species and Al-O-Si units.Therefore,the number of the surface hydroxyl groups was reduced,resulting in the stabilization of framework structure ofAl-SBA-15 zeolite.The aluminum species can form weak and medium-strong acid sites with catalytic activity.展开更多
A Y-zeolite-containing composite material with micro/mesoporous structure had been synthesized from kaolin by means of the in-situ crystallization method. The obtained samples were investigated by XRD and BET methods....A Y-zeolite-containing composite material with micro/mesoporous structure had been synthesized from kaolin by means of the in-situ crystallization method. The obtained samples were investigated by XRD and BET methods. Evaluation of catalytic activity of both the commercial Y-zeolite and the novel Y-zeolite-containing composite material was carried out in the pulse micro-chromatography platform with two probe molecules of different molecular sizes: VGO feedstock and 1,3,5 tri-isopropyl benzene. It was found that the Y-zeolite-containing composite material was richer in external surface and meso-/macro-pores; the Y-zeolite-containing composite material demonstrated a smaller rate of deactivation compared to the commercial Y-zeolite.展开更多
This paper discusses an important issue related to filter divergence in the dimension-reduced projection,four-dimensional variational data assimilation(DRP-4-DVar) approach.Idealized experiments with the Lorenz-96 mod...This paper discusses an important issue related to filter divergence in the dimension-reduced projection,four-dimensional variational data assimilation(DRP-4-DVar) approach.Idealized experiments with the Lorenz-96 model over a period of 200 days showed that the amplitudes of the root mean square errors(RMSEs) reached the same levels as those of the state variables after approximately 100 days because of the accumulation of sampling errors following the cycle of assimilation.Strategies to reduce sampling errors are critical to ensure the quality of ensemble-based assimilation.Numerical experiments showed that localization and reducing observational errors can alleviate,but cannot completely overcome,the filter divergence in the DRP-4-DVar approach,while the method of perturbing observations and the inflation technique can efficiently eliminate the filter divergence problem.展开更多
Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their s...Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents.展开更多
Two-dimensional(2D)materials possess unique thickness-and lateral-size-dependent properties.Many efforts have been devoted to obtaining 2D materials with narrow structure heterogeneity while it is still challenging to...Two-dimensional(2D)materials possess unique thickness-and lateral-size-dependent properties.Many efforts have been devoted to obtaining 2D materials with narrow structure heterogeneity while it is still challenging to independently control their thickness and lateral size,limiting their widespread applications.Here,we develop a three-step method which achieves independent thickness and lateral size sorting of 2D materials.Taking 2D h-BN flakes as an example,their thickness and lateral size are independently sorted to different fractions with thicknesses smaller than 6 nm.In addition,the 2D h-BN flakes possess narrow distributions of both thickness and lateral size.We further develop a force field extraction method and achieve scalable size sorting of 2D h-BN,which is universal for sorting other 2D materials including MoS2 and graphene oxide.This work reports an effective method to produce structure homogenous 2D materials and will help fundamental studies and applications of 2D materials where thickness and lateral size are of concern.展开更多
High-throughput(HTP)experiments play key roles in accelerating the discovery of advanced materials,but the HTP preparation and characterization,especially for bulk samples,are extremely difficult.In this work,we devel...High-throughput(HTP)experiments play key roles in accelerating the discovery of advanced materials,but the HTP preparation and characterization,especially for bulk samples,are extremely difficult.In this work,we developed a novel and general strategy for HTP screening of high-performance bulk thermoelectric materials.The performed fullchain HTP experiments cover rapid synthesis of the bulk sample with quasi-continuous composition,microarea phase identification and structure analysis,and measurement of the spatial distribution of the sample composition,electrical and thermal transport properties.According to our experiments,bulk Bi_(2-x)Sb_(x)Te_(3)(x=1-2)and Bi_(2)Te_(3-x)Se_(x)(x=0-1.5)samples with quasi-continuous compositions have been rapidly fabricated by this HTP method.The target thermoelectric materials with the best Sb/Bi and Te/Se ratios are successfully screened out based on subsequent HTP characterization results,demonstrating that this HTP technique is effective in speeding up the exploration of novel high-performance thermoelectric materials.展开更多
文摘This article refers to the study on the performance of mesoporous silica used as the catalyst for oxidative desulfurization reactions. The test results revealed that under mild reaction conditions using tert-butyl hydroperoxide as the oxidizing agent the content of dibenzothiophene(DBT) contained in oil samples could be reduced from 5000 ppm to less than 5 ppm. Furthermore,the mesoporous silica material can be easily regenerated and recycled.
文摘Porous materials have regular three-dimensional pore structure, which has unique advantages in the field of modern pharmaceutical. At present, porous materials commonly used in the pharmaceutical field are mainly molecular sieves, macroporous adsorbent resins, activated carbon, etc. In this paper, the application status of these porous materials in the pharmaceutical field is reviewed, and the future development is prospected.
文摘The mesoporous Al-SBA-15 zeolite was obtained via impregnation of pure silica-based SBA-15 zeolite with aluminum nitrate.The Al-SBA-15 sample was calcined in air at 800 ℃ for 6 h and hydrothermally treated at near 100 ℃ for 120 h,respectively,and then the thermal and hydrothermal stability of Al-SBA-15 sample was investigated by X-ray diffractometry (XRD),scanning electron microscopy (SEM),transmission electron microscopy (TEM) and nitrogen adsorption and desorption techniques.The Al-SBA-15 sample was also studied by 27 Al nuclear magnetic resonance (27 Al NMR) and ammonia temperature programmed desorption (NH 3-TPD) techniques.In addition,the catalytic activity of Al-SBA-15 zeolite was investigated by the Friedel-Crafts reactions of 2,4-di-tert-butylphenol with cinnamyl alcohol.The test results showed that the thermal and hydrothermal stability of Al-SBA-15 zeolite was better than that of SBA-15 zeo-lite.The Al-SBA-15 zeolite sample prepared by impregnation method exhibits more framework aluminum species and Al-O-Si units.Therefore,the number of the surface hydroxyl groups was reduced,resulting in the stabilization of framework structure ofAl-SBA-15 zeolite.The aluminum species can form weak and medium-strong acid sites with catalytic activity.
文摘A Y-zeolite-containing composite material with micro/mesoporous structure had been synthesized from kaolin by means of the in-situ crystallization method. The obtained samples were investigated by XRD and BET methods. Evaluation of catalytic activity of both the commercial Y-zeolite and the novel Y-zeolite-containing composite material was carried out in the pulse micro-chromatography platform with two probe molecules of different molecular sizes: VGO feedstock and 1,3,5 tri-isopropyl benzene. It was found that the Y-zeolite-containing composite material was richer in external surface and meso-/macro-pores; the Y-zeolite-containing composite material demonstrated a smaller rate of deactivation compared to the commercial Y-zeolite.
基金the National Basic Research Program of China (973 Program) (Grant No. 2010CB951604)the National High Technology Research and Development Program of China (863 Program) (Grant No. 2010AA012304)+1 种基金the China Meteorological Administration for the R&D Special Fund for Public Welfare Industry (Meteorology) (Grant No. GYHY(QX)200906009)the LASG free exploration fund
文摘This paper discusses an important issue related to filter divergence in the dimension-reduced projection,four-dimensional variational data assimilation(DRP-4-DVar) approach.Idealized experiments with the Lorenz-96 model over a period of 200 days showed that the amplitudes of the root mean square errors(RMSEs) reached the same levels as those of the state variables after approximately 100 days because of the accumulation of sampling errors following the cycle of assimilation.Strategies to reduce sampling errors are critical to ensure the quality of ensemble-based assimilation.Numerical experiments showed that localization and reducing observational errors can alleviate,but cannot completely overcome,the filter divergence in the DRP-4-DVar approach,while the method of perturbing observations and the inflation technique can efficiently eliminate the filter divergence problem.
文摘Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents.
基金the National Natural Science Foundation of China(51920105002,51991340,and 51991343)Guangdong Innovative and Entrepreneurial Research Team Program(2017ZT07C341)+2 种基金the Bureau of Industry and Information Technology of Shenzhen for the“2017 Graphene Manufacturing Innovation Center Project”(201901171523)Shenzhen Basic Research Project(JCYJ20190809180605522,JCYJ20200109144620815 and JCYJ20200109144616617)China Postdoctoral Science Foundation(2020M680540)。
文摘Two-dimensional(2D)materials possess unique thickness-and lateral-size-dependent properties.Many efforts have been devoted to obtaining 2D materials with narrow structure heterogeneity while it is still challenging to independently control their thickness and lateral size,limiting their widespread applications.Here,we develop a three-step method which achieves independent thickness and lateral size sorting of 2D materials.Taking 2D h-BN flakes as an example,their thickness and lateral size are independently sorted to different fractions with thicknesses smaller than 6 nm.In addition,the 2D h-BN flakes possess narrow distributions of both thickness and lateral size.We further develop a force field extraction method and achieve scalable size sorting of 2D h-BN,which is universal for sorting other 2D materials including MoS2 and graphene oxide.This work reports an effective method to produce structure homogenous 2D materials and will help fundamental studies and applications of 2D materials where thickness and lateral size are of concern.
基金supported by the National Key Research and Development Program of China(2018YFB0703600 and 2018YFA0702100)the National Natural Science Foundation of China(51772186,51632005 and 51371194)。
文摘High-throughput(HTP)experiments play key roles in accelerating the discovery of advanced materials,but the HTP preparation and characterization,especially for bulk samples,are extremely difficult.In this work,we developed a novel and general strategy for HTP screening of high-performance bulk thermoelectric materials.The performed fullchain HTP experiments cover rapid synthesis of the bulk sample with quasi-continuous composition,microarea phase identification and structure analysis,and measurement of the spatial distribution of the sample composition,electrical and thermal transport properties.According to our experiments,bulk Bi_(2-x)Sb_(x)Te_(3)(x=1-2)and Bi_(2)Te_(3-x)Se_(x)(x=0-1.5)samples with quasi-continuous compositions have been rapidly fabricated by this HTP method.The target thermoelectric materials with the best Sb/Bi and Te/Se ratios are successfully screened out based on subsequent HTP characterization results,demonstrating that this HTP technique is effective in speeding up the exploration of novel high-performance thermoelectric materials.