Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficien...Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.展开更多
A simple and convenient method, free of template, has been proposed to synthesize hollow carambolashaped Ag2 S microspheres with Ag NO3, thiourea（TU）, Na Cl and diethanolamine as reagents using a microwave-assisted ...A simple and convenient method, free of template, has been proposed to synthesize hollow carambolashaped Ag2 S microspheres with Ag NO3, thiourea（TU）, Na Cl and diethanolamine as reagents using a microwave-assisted method, at low temperatures of below 100 ℃. Powder X-ray diffraction（XRD）,scanning electron microscopy（FESEM） and high resolution transmission electron microscopy（HRTEM）were employed to characterize the morphology and composition of those microspheres. The results indicated that the hollow carambola-shaped silver sulfide microspheres（with high purity and homogeneous morphology） were prepared by an Ostwald ripening process. A possible formation mechanism of hollow carambola-shaped Ag2 S microspheres was proposed.展开更多
Hollow carbon-based nanostructures(HCNs)have found broad applications in various fields,particularly rechargeable batteries.However,the syntheses of HCNs usually rely on template methods,which are time-consuming,low-y...Hollow carbon-based nanostructures(HCNs)have found broad applications in various fields,particularly rechargeable batteries.However,the syntheses of HCNs usually rely on template methods,which are time-consuming,low-yield,and environmentally detrimental.Metal-organic frameworks(MOFs),constructed by organic ligands and inorganic metal nodes,have been identified as effective platforms for preparing HCNs without adding extra templates.This review summarized the recent progress in template-free synthesis of HCNs enabled by MOFs and their applications in rechargeable batteries.Different template-free strategies were introduced first with mechanistic insights into the hollowing mechanism.Then the electrochemical performances of the HCNs were discussed with highlight on the structure-function correlation.It is found that the built-in cavities and nonporous for HCNs is of critical importance to increase the storage sites for high capacity,to enhance charge and mass transport kinetics for high-rate capability,and to ensure the resilient electrode structure for stable cycling.Finally,the challenges and opportunities regarding MOFs-derived HCNs and their applications in rechargeable batteries were discussed.展开更多
Developing accurate and sensitive DNA methyltransferase(MTase) analysis methods is essential for early clinical diagnosis and development of antimicrobial drug targets. In this work, by coupling WO_(3-x) dotsencapsula...Developing accurate and sensitive DNA methyltransferase(MTase) analysis methods is essential for early clinical diagnosis and development of antimicrobial drug targets. In this work, by coupling WO_(3-x) dotsencapsulated metal-organic frameworks(MOFs) as co-reactants and terminal deoxynucleotidyl transferase(Td T)-mediated template-free branched polymerization, a dual signal-amplified electrochemiluminescent(ECL) biosensor was constructed to detect DNA adenine methylation(Dam) MTase. The employment of WO_(3-x) dots-encapsulated MOFs(i.e., NH_(2)-UIO66@WO_(3-x) ) was not only beneficial for biomolecule conjugation because of the abundant amino groups but also led to a 7-fold enhanced ECL response due to the increased loading of WO_(3-x). Moreover, Td T-mediated template-free branched polymerization promoted the capture of ECL emitters on the electrode surface, achieving 20-fold enhanced signal amplification. The presented ECL biosensor demonstrated a low detection limit of 2.4 × 10^(-4)U/m L, and displayed high reliability for the detection of Dam MTase in both spiked human serum and E. coli cell samples, and for the screening of potential inhibitors. This study opens a new avenue for designing a dual signal amplificationbased ECL bioassay for Dam MTase and screening inhibitors in the fields of clinical diagnosis and drug development.展开更多
Kbphillipsite was prepared using a hydrothermal method. Soluble glass and sodium aluminate were used as raw materials in the absence of an organic template. Investigations regarding the K＋ ions were con- ducted at ro...Kbphillipsite was prepared using a hydrothermal method. Soluble glass and sodium aluminate were used as raw materials in the absence of an organic template. Investigations regarding the K＋ ions were con- ducted at room temperature to determine the ion-exchange capacity in the seawater sample and the selectivity coefficient of the mixed K＋-Na~ solution. The sample was characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, and energy dispersion spectroscopy （EDS）. The K＋ ion- exchange capacity is 51 mg/g in seawater and the selectivity coefficient is 75.1 in the mixed K＋-Na＋ solution. The sample has a selectivity preference for K＋, and therefore can be used to selectively extract potassium from seawater. The sample composed of Si, Al, K, Na, and O exhibits a cross-like shape and is a typical K-phillipsite structure.展开更多
Mesoporous anatase TiO2 spheres with high surface area（119 m^2g^（-1）） were successfully synthesized via a facile and green template-free method. The prepared TiO2 was characterized by X-ray diffraction（XRD）,N2 a...Mesoporous anatase TiO2 spheres with high surface area（119 m^2g^（-1）） were successfully synthesized via a facile and green template-free method. The prepared TiO2 was characterized by X-ray diffraction（XRD）,N2 adsorption, scanning electron microscopy（SEM）, transmission electron microscopy（TEM） and UV–vis absorbance spectra. It was found that the prepared TiO2 is characterized by pure anatase phase, which shows uniform spheres and has a typical mesostructure with a high specific surface area and a large pore volume. The effects of complexant（acetylacetone） amount, crystallization temperature and calcination temperature were also investigated. Based on the results, a sketch for the preparation of mesoporous TiO2 was proposed. First, complex formed between tetrabutyl titanate and acetylacetone in ethanol. After introduction of aqueous of ammonia sulfate and urea, hydrolysis of tetrabutyl titanate would occur slowly,and sol of TiO2 was formed. Then, crystallization proceeded under hydrothermal conditions. Calcination process favored the formation of bigger TiO2 crystal through combining of the small crystals in TiO2.This led to the formation of bigger mesopores between TiO2 crystals. Photocatalytic activity of the prepared TiO2 was evaluated by decomposition of methyl orange.展开更多
基金The financial supports from the National Natural Science Foundation of China (22178059, 22208054 and 22072019)Natural Science Foundation of Fujian Province, China (2020J01513)+1 种基金Sinochem Quanzhou Energy Technology Co., Ltd. (ZHQZKJ-19-F-ZS0076)Qingyuan Innovation Laboratory (00121002)
文摘Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.
基金supported by the Fundamental Research Funds for the Central Universities(No.2232013A3-05)the National Science and Technology Ministry(No.ID 2012BAK30B03)
文摘A simple and convenient method, free of template, has been proposed to synthesize hollow carambolashaped Ag2 S microspheres with Ag NO3, thiourea（TU）, Na Cl and diethanolamine as reagents using a microwave-assisted method, at low temperatures of below 100 ℃. Powder X-ray diffraction（XRD）,scanning electron microscopy（FESEM） and high resolution transmission electron microscopy（HRTEM）were employed to characterize the morphology and composition of those microspheres. The results indicated that the hollow carambola-shaped silver sulfide microspheres（with high purity and homogeneous morphology） were prepared by an Ostwald ripening process. A possible formation mechanism of hollow carambola-shaped Ag2 S microspheres was proposed.
基金supported by the National Natural Science Foundation of China(21931012,22025507,22109052)Guangdong Basic and Applied Basic Research Foundation(2022B1515020001)+1 种基金Guangzhou Science and Technology Program(202201010703)the Fundamental Research Funds for the Central Universities(21621033)。
文摘Hollow carbon-based nanostructures(HCNs)have found broad applications in various fields,particularly rechargeable batteries.However,the syntheses of HCNs usually rely on template methods,which are time-consuming,low-yield,and environmentally detrimental.Metal-organic frameworks(MOFs),constructed by organic ligands and inorganic metal nodes,have been identified as effective platforms for preparing HCNs without adding extra templates.This review summarized the recent progress in template-free synthesis of HCNs enabled by MOFs and their applications in rechargeable batteries.Different template-free strategies were introduced first with mechanistic insights into the hollowing mechanism.Then the electrochemical performances of the HCNs were discussed with highlight on the structure-function correlation.It is found that the built-in cavities and nonporous for HCNs is of critical importance to increase the storage sites for high capacity,to enhance charge and mass transport kinetics for high-rate capability,and to ensure the resilient electrode structure for stable cycling.Finally,the challenges and opportunities regarding MOFs-derived HCNs and their applications in rechargeable batteries were discussed.
基金supported by the National Natural Science Foundation of China (Nos.22074015 and 22174014)。
文摘Developing accurate and sensitive DNA methyltransferase(MTase) analysis methods is essential for early clinical diagnosis and development of antimicrobial drug targets. In this work, by coupling WO_(3-x) dotsencapsulated metal-organic frameworks(MOFs) as co-reactants and terminal deoxynucleotidyl transferase(Td T)-mediated template-free branched polymerization, a dual signal-amplified electrochemiluminescent(ECL) biosensor was constructed to detect DNA adenine methylation(Dam) MTase. The employment of WO_(3-x) dots-encapsulated MOFs(i.e., NH_(2)-UIO66@WO_(3-x) ) was not only beneficial for biomolecule conjugation because of the abundant amino groups but also led to a 7-fold enhanced ECL response due to the increased loading of WO_(3-x). Moreover, Td T-mediated template-free branched polymerization promoted the capture of ECL emitters on the electrode surface, achieving 20-fold enhanced signal amplification. The presented ECL biosensor demonstrated a low detection limit of 2.4 × 10^(-4)U/m L, and displayed high reliability for the detection of Dam MTase in both spiked human serum and E. coli cell samples, and for the screening of potential inhibitors. This study opens a new avenue for designing a dual signal amplificationbased ECL bioassay for Dam MTase and screening inhibitors in the fields of clinical diagnosis and drug development.
基金the Natural Science Foundation of Shandong Province(ZR2010BQ024)the Specialized Research Fund for the Doctoral Program of Higher Education(20100132120004)the Fundamental Research Funds for the Central Universities (201013013)for financial support
文摘Kbphillipsite was prepared using a hydrothermal method. Soluble glass and sodium aluminate were used as raw materials in the absence of an organic template. Investigations regarding the K＋ ions were con- ducted at room temperature to determine the ion-exchange capacity in the seawater sample and the selectivity coefficient of the mixed K＋-Na~ solution. The sample was characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, and energy dispersion spectroscopy （EDS）. The K＋ ion- exchange capacity is 51 mg/g in seawater and the selectivity coefficient is 75.1 in the mixed K＋-Na＋ solution. The sample has a selectivity preference for K＋, and therefore can be used to selectively extract potassium from seawater. The sample composed of Si, Al, K, Na, and O exhibits a cross-like shape and is a typical K-phillipsite structure.
基金supported by the National Natural Science Foundation of China (Nos. 21206150, U1304209 and U1204215)the Foundation for University Young Key Teacher by Henan Province (No. 2014GGJS-005)
文摘Mesoporous anatase TiO2 spheres with high surface area（119 m^2g^（-1）） were successfully synthesized via a facile and green template-free method. The prepared TiO2 was characterized by X-ray diffraction（XRD）,N2 adsorption, scanning electron microscopy（SEM）, transmission electron microscopy（TEM） and UV–vis absorbance spectra. It was found that the prepared TiO2 is characterized by pure anatase phase, which shows uniform spheres and has a typical mesostructure with a high specific surface area and a large pore volume. The effects of complexant（acetylacetone） amount, crystallization temperature and calcination temperature were also investigated. Based on the results, a sketch for the preparation of mesoporous TiO2 was proposed. First, complex formed between tetrabutyl titanate and acetylacetone in ethanol. After introduction of aqueous of ammonia sulfate and urea, hydrolysis of tetrabutyl titanate would occur slowly,and sol of TiO2 was formed. Then, crystallization proceeded under hydrothermal conditions. Calcination process favored the formation of bigger TiO2 crystal through combining of the small crystals in TiO2.This led to the formation of bigger mesopores between TiO2 crystals. Photocatalytic activity of the prepared TiO2 was evaluated by decomposition of methyl orange.
