Zeolite synthesis in contemporary chemical industries is predominantly conducted using organic structure‐directing agents(OSDAs),which are chronically hazardous to humans and the environment.It is a growing trend to ...Zeolite synthesis in contemporary chemical industries is predominantly conducted using organic structure‐directing agents(OSDAs),which are chronically hazardous to humans and the environment.It is a growing trend to develop an eco‐friendly and nuisanceless OSDA for zeolite synthesis.Herein,choline is employed as a non‐toxic and green OSDA to synthesize high silica Y zeolite with SiO2/Al2O3 ratios of 6.5–6.8.The prepared Y zeolite samples exhibited outstanding(hydro)thermal stability at ultrahigh temperature owing to the higher SiO2/Al2O3 ratio.The XRF,SEM,29Si‐NMR and 13Na+results suggested that choline plays a structure‐directing role in the synthesis of Y zeolite,while the feed molar fraction of Na+is a crucial determinant for the framework SiO2/Al2O3 ratio and the crystal morphology.展开更多
K-Chabazite(K-CHA)zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective“one-pot”method.By solely employing colloidal silica and aluminum hydroxide in the K^(+)/Sr^(2+)syste...K-Chabazite(K-CHA)zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective“one-pot”method.By solely employing colloidal silica and aluminum hydroxide in the K^(+)/Sr^(2+)system without the assistance of seeds,fluorides or organic structure as directing agents,the K-CHA nano-aggregates were successfully synthesized in a few hours.The crystallization behavior of the gels with different SiO_(2)/Al_(2)O_(3) molar ratios(SARs)was investigated using X-ray diffraction(XRD);scanning electron microscope(SEM);X-ray fluorescence(XRF);27Al and 29Si magic angle spinning nuclear magnetic resonance(MAS NMR);Fourier-transform infrared spectra(FTIR);UV-Raman characterizations.As the nucleation rates were changed with the SARs,three kinds of K-CHA nano-aggregates,namely,hamburger-,disk-and walnut-shaped,were obtained.A possible formation mechanism of the K-CHA nano-aggregates was proposed.Additionally,the walnut-shaped sample with an SAR of 7 possessed the largest pore volume and specific surface area,resulting in the highest methane adsorption capacity.Furthermore,it exhibited a CH_(4)/N_(2) selectivity of more than 3 under relative pressures ranging from 0 to 0.6.This work offers guidance for modifying the stacking modes of other nano-sized zeolites.展开更多
Curcurbit[n]uril(Q[n])-based supramolecular frameworks(QSFs) constructed from the outer surface interaction of Q[n]s(OSIQ) have the characteristic of simplicity,diversity and modulability.Their simplicity is reflected...Curcurbit[n]uril(Q[n])-based supramolecular frameworks(QSFs) constructed from the outer surface interaction of Q[n]s(OSIQ) have the characteristic of simplicity,diversity and modulability.Their simplicity is reflected in their simple composition and preparation methods used for QSFs.The diversity of supramolecular organic frameworks(SOFs) is reflected in the synthesis methods and structural characteristics of the as-obtained QSFs,as well as the variety of structural directing agents and basic building blocks used to prepare QSFs.The modulability is reflected by the controllable channel size in the QSFs,which can be adjusted using different sizes of Q[n]s.In this work,the first re ported cucurbituril Q[6]was selected as the basic building block and three Q[6]-based su p ramolecular frameworks were obtained from aqueous HCl solutions in the presence of [CdCl_(4)]^(2-)respectively.The OSIQs are the main driving forces for the formation of these frameworks.This study shows the diversity of the QSFs.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.21802136)~~
文摘Zeolite synthesis in contemporary chemical industries is predominantly conducted using organic structure‐directing agents(OSDAs),which are chronically hazardous to humans and the environment.It is a growing trend to develop an eco‐friendly and nuisanceless OSDA for zeolite synthesis.Herein,choline is employed as a non‐toxic and green OSDA to synthesize high silica Y zeolite with SiO2/Al2O3 ratios of 6.5–6.8.The prepared Y zeolite samples exhibited outstanding(hydro)thermal stability at ultrahigh temperature owing to the higher SiO2/Al2O3 ratio.The XRF,SEM,29Si‐NMR and 13Na+results suggested that choline plays a structure‐directing role in the synthesis of Y zeolite,while the feed molar fraction of Na+is a crucial determinant for the framework SiO2/Al2O3 ratio and the crystal morphology.
基金supported by the National Natural Science Foundation of China(No.21276183).
文摘K-Chabazite(K-CHA)zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective“one-pot”method.By solely employing colloidal silica and aluminum hydroxide in the K^(+)/Sr^(2+)system without the assistance of seeds,fluorides or organic structure as directing agents,the K-CHA nano-aggregates were successfully synthesized in a few hours.The crystallization behavior of the gels with different SiO_(2)/Al_(2)O_(3) molar ratios(SARs)was investigated using X-ray diffraction(XRD);scanning electron microscope(SEM);X-ray fluorescence(XRF);27Al and 29Si magic angle spinning nuclear magnetic resonance(MAS NMR);Fourier-transform infrared spectra(FTIR);UV-Raman characterizations.As the nucleation rates were changed with the SARs,three kinds of K-CHA nano-aggregates,namely,hamburger-,disk-and walnut-shaped,were obtained.A possible formation mechanism of the K-CHA nano-aggregates was proposed.Additionally,the walnut-shaped sample with an SAR of 7 possessed the largest pore volume and specific surface area,resulting in the highest methane adsorption capacity.Furthermore,it exhibited a CH_(4)/N_(2) selectivity of more than 3 under relative pressures ranging from 0 to 0.6.This work offers guidance for modifying the stacking modes of other nano-sized zeolites.
基金the financial support of the National Natural Science Foundation of China(Nos.21761007,51663005 and 21871064)Science and Technology Plan Project of Guizhou Province(Nos.20175788 and 20185781)。
文摘Curcurbit[n]uril(Q[n])-based supramolecular frameworks(QSFs) constructed from the outer surface interaction of Q[n]s(OSIQ) have the characteristic of simplicity,diversity and modulability.Their simplicity is reflected in their simple composition and preparation methods used for QSFs.The diversity of supramolecular organic frameworks(SOFs) is reflected in the synthesis methods and structural characteristics of the as-obtained QSFs,as well as the variety of structural directing agents and basic building blocks used to prepare QSFs.The modulability is reflected by the controllable channel size in the QSFs,which can be adjusted using different sizes of Q[n]s.In this work,the first re ported cucurbituril Q[6]was selected as the basic building block and three Q[6]-based su p ramolecular frameworks were obtained from aqueous HCl solutions in the presence of [CdCl_(4)]^(2-)respectively.The OSIQs are the main driving forces for the formation of these frameworks.This study shows the diversity of the QSFs.