The activation effect of boric acid as an activator is good,and we investigate the best activation conditions for the boric acid impregnation method.To represent the structural characteristics and adsorption performan...The activation effect of boric acid as an activator is good,and we investigate the best activation conditions for the boric acid impregnation method.To represent the structural characteristics and adsorption performance of the Stellera Chamaejasme based carbon molecular sieves,we use Brunner-Emmet-Teller(BET)measurements,scan-ning electron microscope(SEM),Raman spectra(Raman),X-ray diffraction(XRD),and adsorption property measurement.When the loading ratio was 0.68:1,the specific surface area was 532.21 m^(2)/g,the total pore volume was 0.24 cm 3/g,the average pore size was 1.81 nm,the adsorption value of methylene blue was 145.28 mg/g,and the adsorption value of iodine was 713.33 mg/g,the results showed that boric acid had better activation effect.The carbon molecular sieves made from Stellera Chamaejasme and activated with boric acid produce two peaks on the aperture distribution graph that are densely distributed in the micropore range.This indicates that boric acid’s pore-forming tendency is primarily micropore.展开更多
To improve oil quality,ZSM-22/SAPO-11 composite molecular sieves were synthesized by adding ZSM-22 into a synthetic gel of SAPO-11 for n-decane hydroisomerization.The mass ratios of ZSM-22/(ZSM-22+SAPO-11)in the compo...To improve oil quality,ZSM-22/SAPO-11 composite molecular sieves were synthesized by adding ZSM-22 into a synthetic gel of SAPO-11 for n-decane hydroisomerization.The mass ratios of ZSM-22/(ZSM-22+SAPO-11)in the composite molecular sieves were optimized and the optimal ZSM-22/SAPO-11 composite(ZS-9)was obtained.The electrostatic repulsions between the ZSM-22 precursors and the SAPO-11 crystalline nuclei produced small ZSM-22 and SAPO-11 crystallites in ZS-9,which increased the specific surface area and mesopore volume and thereby exposed more acid sites.In comparison with conventional SAPO-11,ZSM-22 and their mechanical mixture,ZS-9 with smaller crystallites and the optimal medium and strong Brønsted acid centers(MSBAC)content displayed a higher yield of branched C_(10) isomers(81.6%),lower cracking selectivity(11.9%)and excellent stability.The correlation between the i-C_(10) selectivity and the MSBAC density of molecular sieves indicated that the selectivity for branched C_(10) isomers first increased and then decreased with increasing MSBAC density on the molecular sieves,and the maximum selectivity(87.7%)occurred with a density of 9.6×10^(−2)μmol m^(−2).展开更多
Hydrogen is a green clean fuel and chemical feedstock. Its separation and purification from hydrogencontaining mixtures is the key step in the production of hydrogen with high purity(>99.99%). In this work, carbon ...Hydrogen is a green clean fuel and chemical feedstock. Its separation and purification from hydrogencontaining mixtures is the key step in the production of hydrogen with high purity(>99.99%). In this work, carbon molecular sieve(CMS) membranes with ultrahigh permselectivity for hydrogen purification were fabricated by high-temperature(700–900 ℃) pyrolysis of polymeric precursor of phenolphthaleinbased cardo poly(arylene ether ketone)(PEK-C). The evolution of the microstructural texture and ultramicroporous structure and gas separation performance of the CMS membrane were characterized via TG-MS, FT-IR, XRD, TEM, CO2 sorption analysis and gas permeation measurements. CMS membranes prepared at 700 ℃ exhibited amorphous turbostratic carbon structures and high H2 permeability of 5260 Barrer with H2/CH4, H2/N2 and H2/CO selectivities of 311, 142, 75, respectively. When carbonized at900 ℃, the CMS membrane with ultrahigh H2/CH4 selectivity of 1859 was derived owing to the formation of the dense and ordered carbon structure. CMS membranes with ultrahigh permselectivity exhibit an attractive application prospect in hydrogen purification.展开更多
Thermally stable mesoporous silica and Ti-containing molecular sieves have been synthesized at mild temperature using low-cost and biodegradable---amphoteric tetradecyl betaine as template. The physicochemical charact...Thermally stable mesoporous silica and Ti-containing molecular sieves have been synthesized at mild temperature using low-cost and biodegradable---amphoteric tetradecyl betaine as template. The physicochemical characterizations proved that Ti(Ⅳ) could be incorporated in the mesoporous struture.展开更多
Research and development of efficient, economical and resource-based flue gas desulfurization technology has always been a hot spot in the field of air pollution control. Molecular sieve materials have been paid atten...Research and development of efficient, economical and resource-based flue gas desulfurization technology has always been a hot spot in the field of air pollution control. Molecular sieve materials have been paid attention to by SO<sub>2</sub> adsorbent researchers due to their huge specific surface area. In this paper, 13X zeolite was modified with Cu(NO<sub>3</sub>) <sub>2</sub>·3H<sub>2</sub>O to obtain 13x-Xwt %CuO (calculated by the amount of CuO loaded). The adsorption time and capacity of SO<sub>2</sub> penetration sorbent and the isothermal curve of N<sub>2</sub> adsorption-desorption were studied. The results are as follows: 13X-3wt%CuO has the best adsorption effect, the penetration adsorption time is 110 min, the penetration adsorption capacity is 43.41 mg·g<sup>-1</sup>, the saturation adsorption capacity is 49.27 mg·g<sup>-1</sup>;The amount of CuO loading has a great influence on the adsorption effect of modified 13X molecular sieve on SO<sub>2</sub>. SEM and BET characterization showed that CuO modification did not change the external morphology of 13X molecular sieve, changed the pore size, but did not block the original channel of the molecular sieve, before and after modification belong to the type I adsorption isothermal curve. The pore size distribution and type of molecular sieve, as well as the content and type of alkali metal cations jointly control the adsorption process of SO<sub>2</sub> by 13X-xwt %CuO. XPS characterization showed that Cu(NO<sub>3</sub>) <sub>2</sub> decomposed into CuO and Cu<sub>2</sub>O during roasting at 450°C, CuO/Cu<sub>2</sub>O ≈ 1.5. The R<sup>2</sup> values of the quasi-second-order kinetic models obtained from the 13X-Xwt %CuO particle diffusion kinetic models were all above 0.99, indicating that the quasi-second-order kinetic equations were more relevant. Particle diffusion dynamics model in fitting results show that the adsorption process can be divided into two stages, the first phase of surface adsorption and diffusion rate in the granules common control process, more accurate dynamics model of the secondary in the second phase particle diffusion rate control stage, mainly for the micropore adsorption or chemical adsorption, quasi level 2 dynamic model conformity of variation;C is a constant not equal to 0, indicating that the adsorption of SO<sub>2</sub> is not completely through the form of intra-particle diffusion, and a small amount of chemisorption exists. And it is the compound effect of multiple adsorption mechanisms.展开更多
Mesoporous molecularsieve MCM-41 has been synthesized in the extremely dense system (with H2O/Si<10) and characterized by XRD, N2 adsorption isotherm as well as probe reactions of cracking of cumene and isomerizati...Mesoporous molecularsieve MCM-41 has been synthesized in the extremely dense system (with H2O/Si<10) and characterized by XRD, N2 adsorption isotherm as well as probe reactions of cracking of cumene and isomerization of o-xylene.展开更多
In the experiment,PDMS membrane with NaY molecular sieve filling were chosen as the experimental objects and the flux of phenol and removal efficiency of phenol as evaluation index,the effect of the system operating t...In the experiment,PDMS membrane with NaY molecular sieve filling were chosen as the experimental objects and the flux of phenol and removal efficiency of phenol as evaluation index,the effect of the system operating temperature,the flow rate,liquid membrane downstream pressure,operation time,and filling proportion of NaY molecular sieve on pervaporation treatment efficiency for wastewater from coal gasification were investigated. With the increase of temperature and feed flow rate,pervaporation flux and phenol removal efficiency increases. The decrease of the membrane downstream pressure and elevating NaY molecular sieve filling proportion may result in the increase of flux and then phenol removal efficiency improves. When NaY molecular sieve filling proportion is 45% ,treatment efficiency is the best for coal gasification wastewater containing 1850 mg/L phenol as the flux of phenol was 12948. 23 mg/(h·m2) .展开更多
Mesoporous molecular sieves, NbFAPO-5 and NbFAPSO-5 were hydrothermally synthesized with AlPO-5 type structure. Characterization of these molecular sieves was performed by X-ray diffraction to determine their structur...Mesoporous molecular sieves, NbFAPO-5 and NbFAPSO-5 were hydrothermally synthesized with AlPO-5 type structure. Characterization of these molecular sieves was performed by X-ray diffraction to determine their structure, ICP-EAS for their elemental composition and infrared spectrometry to access their acidic properties. X-ray diffraction patterns confirmed well AlPO-5 type structure. ICP-EAS analysis confirmed the incorporation of silicon (12.9%), aluminium (15.4%), phosphorous (21.9%), iron (5.62%) and niobium (0.39%) into AlPO-5 framework. Infrared spectrometry analysis showed that both Bronsted and Lewis sites were found in the synthesized samples. The presence of both Bronsted and Lewis acid site led to bifunctional function of NbFAPO-5 and NbFAPSO-5 molecular sieve in promoting both oxidation and esterification reactions. NbFAPSO-5 Bronsted acidity was higher than that of NbFAPO-5 and for Lewis acidity, NbFAPO-5 was higher than that of NbFAPO-5.展开更多
After my graduation as a chemistry major from Shanghai Jiaotong University in 1952. I was assigned to work at the People’s University of Northeast China (the predecessor of today’s Jilin University) in Changchun Cit...After my graduation as a chemistry major from Shanghai Jiaotong University in 1952. I was assigned to work at the People’s University of Northeast China (the predecessor of today’s Jilin University) in Changchun City, serving as a teaching assistant.I)uring my career on campus.I have lectured on a dozen courses on inorganic chemistry,general chemistry,analytic chemistry. rare-element chemistry, complex chemistry. inorganic synthesis,solid-state chemistry展开更多
Samples of methane molecules grade diameter channel CHA-type molecular sieves(Chabazite-K, SAPO-34 and SSZ-13) were investigated using the adsorption separation of CH4/N2 mixtures. The isotherms recorded for CH4 and N...Samples of methane molecules grade diameter channel CHA-type molecular sieves(Chabazite-K, SAPO-34 and SSZ-13) were investigated using the adsorption separation of CH4/N2 mixtures. The isotherms recorded for CH4 and N2 follow a typical type-Ι behavior, which were fitted well with the Sips model(R2>0.999) and the selectivity was calculated using IAST theory. The results reveal that Chabazite-K has the highest selectivity(SCH4/N= 5.5).2 SSZ-13 has the largest capacity, which can adsorb up to a maximum of 30.957 cm3·g-1(STP) of CH4, due to it having the largest pore volume and surface area, but the lowest selectivity(SCH4/N2= 2.5). From the breakthrough test, we can conclude that SSZ-13 may be a suitable candidate for the recovery of CH4 from low concentration methane(CH4<20%) based on its larger pore volume and higher CH4 capacity. Chabazite-K is more suited to the separation of high concentration methane(CH4>50%) due to its higher selectivity.展开更多
HZSM-5/MCM-41 molecular sieve (H-ZM) catalysts with well-defined micro/mesoporous structures were synthesized and showed high performance for selective synthesis of triacetin via the esterification reaction of glycero...HZSM-5/MCM-41 molecular sieve (H-ZM) catalysts with well-defined micro/mesoporous structures were synthesized and showed high performance for selective synthesis of triacetin via the esterification reaction of glycerol with acetic acid. The conversion of glycerol was demonstrated to be 100% and the triacetin selectivity was over 91%, which can be attributed to the synergistic effect regarding suitable acidic property, excellent diffusion efficiency and good stability derived from the combined advantages of microporous molecular sieve HZSM-5 and mesoporous molecular sieve MCM-41.展开更多
Recent decades witnessed the significant progress made in the research field of 2D molecular sieve membranes.In comparison with their 3D counterparts, 2D molecular sieve membranes possessed several unique advantages l...Recent decades witnessed the significant progress made in the research field of 2D molecular sieve membranes.In comparison with their 3D counterparts, 2D molecular sieve membranes possessed several unique advantages like significantly reduced membrane thickness(one atom thick in theory) and diversified molecular sieving mechanisms(in-plane pores within nanosheets & interlayer galleries between nanosheets). M. Tsapatsis first carried out pioneering work on fabrication of lamellar ZSM-5 membrane. Since then, diverse 2D materials typically including graphene oxides(GOs) have been fabricated into membranes showing promising prospects in energy-efficient gas separation, pervaporation, desalination and nanofiltration. In addition to GOs, other emerging 2D materials, including 2D zeolites, 2D metal–organic frameworks(MOFs), 2 D covalent-organic frameworks(COFs), layered double hydroxides(LDHs), transition metal dichalcogenides(TMDCs), MXenes(typically Ti3C2TX), graphitic carbon nitrides(typically g-C3N4), hexagonal boron nitride(h-BN) and montmorillonites(MT) are showing intriguing performance in membrane-based separation process. This article summarized the most recent developments in the field of 2D molecular sieve membranes aside from GOs with particular emphasis on their structure–performance relationship and application prospects in industrial separation.展开更多
ZSM-5/MCM-41 composite molecular sieve was prepared by the nano-assembling method.The ZSM-5 molecular sieve,the MCM-41 molecular sieve,the ZSM-5/MCM-41 mechanical mixture and the ZSM-5/MCM-41 composite molecular sieve...ZSM-5/MCM-41 composite molecular sieve was prepared by the nano-assembling method.The ZSM-5 molecular sieve,the MCM-41 molecular sieve,the ZSM-5/MCM-41 mechanical mixture and the ZSM-5/MCM-41 composite molecular sieve were characterized by X-ray powder diffractometry,N<sub>2</sub> adsorption isotherms,temperature programmed desorption of ammonia and scanning electron microscopy and their properties were analyzed.Using FCC gasoline as the feed,activities of different molecular sieves for reducing olefin content were investigated in a continuous high-pressure micro-reactor unit under the following conditions:a reaction temperature of 400℃,a reaction time of 2 h,a weight hourly space velocity of 3h<sup>-1</sup>,and a reaction pressure of 2.0 MPa.The results showed that the HMCM-41 molecular sieve had low reaction performance,and the HZSM-5 molecular sieve demonstrated high aromatization activity,while the ZSM-5/MCM- 41 composite molecular sieve exhibited a best olefin-reducing performance because of its high isomerization activity and moderate aromatization activity.With a largest olefin-reducmg capability and a reasonable distribution of products,the composite molecular sieve was more suitable for FCC gasoline upgrading compared to other three catalysts.展开更多
To deeply clean oily wastewater,molecular sieve residues(MSRs)were sufficiently recycled and utilized due to their high specific surface area,porous structure,and outstanding adsorption property.Molding MSRs(MMSRs)wer...To deeply clean oily wastewater,molecular sieve residues(MSRs)were sufficiently recycled and utilized due to their high specific surface area,porous structure,and outstanding adsorption property.Molding MSRs(MMSRs)were prepared by adding additives(starch,citric acid,and soluble glass)to MSRs and were then filled into a fixed bed for adsorbing and separating the oil in wastewater.Sodium dodecylbenzenesulfonate was used to modify the MMSRs,and their adsorption property was also investigated.In addition,the MSRs were characterized by scanning electron microscopy,energy-dispersive X-ray spectroscopy,Brunauer–Emmett–Teller analysis,and Fourier transform infrared spectroscopy.The results indicated that MMSRs satisfied the filling requirement of fixed bed,and their dynamic adsorption capacity could reach 0.1854 mg g^?1.Furthermore,the static adsorption capacity of MMSRs achieved 1.7346 mg g^?1 in the optimum conditions,and the oil adsorption performance of modified MMSRs was further enhanced.Therefore,this work suggests that MSRs are promising alternatives in cleaning oily wastewater.展开更多
Lead, a heavy metal, is a well known contaminant in water and has been reported to cause serious health implications to humans, animals, and plants. One of the processes for heavy metal remediation of contaminated wat...Lead, a heavy metal, is a well known contaminant in water and has been reported to cause serious health implications to humans, animals, and plants. One of the processes for heavy metal remediation of contaminated water is chemical precipitation. In this present work, chemical precipitation of lead from a contaminated aqueous matrix by chlorides, carbonates, and sulfates of sodium and calcium was compared to lead removal by molecular sieves and biomaterials (fishbone, grape and spinach). The order of lead removal from 1400 ppm of lead solution is sodium chloride (31%) < calcium chloride (62%) burnt grape (83%) < charred spinach (92.3%) < sodium phosphate (95.8%) < sodium carbonate (97%) < molecular sieve sphere (98.7%) < sodium sulfate (99.3%) s ground (99.71%) < fishbone (99.87%)展开更多
A simulated gasoline consisting of model sulfur compounds of thiophene(C4H4S)and 3-methythiophene (3-MC4H4S)dissolved in n-heptane was tested for the oxidative desulfurization in the hydrogen peroxide(H2O2) and formic...A simulated gasoline consisting of model sulfur compounds of thiophene(C4H4S)and 3-methythiophene (3-MC4H4S)dissolved in n-heptane was tested for the oxidative desulfurization in the hydrogen peroxide(H2O2) and formic acid oxidative system over metal oxide-loaded molecular sieve.The effects of the oxidative system, loaded metal oxides,phase transfer catalyst,the addition of olefin and aromatics on sulfur removal were investi- gated in details.The results showed that the sulfur removal rate of simulated gasoline in the H2O2/formic acid sys- tem was higher than in other oxidative systems.The cerium oxide-loaded molecular sieve was found very active catalyst for oxidation of simulated gasoline in this system.The sulfur removal rates of C4H4S and 3-MC4H4S were enhanced when phase transfer catalyst(PTC)was added.However,the sulfur removal rate of simulated gasoline was reduced with the addition of olefin and aromatics.展开更多
Photochemical oxidation of thiophene in n-octane/water extraction system using O2 as oxidant was studied. The reaction mechanism of thiophene oxidation was proposed. Results obtained here can be used as the reference ...Photochemical oxidation of thiophene in n-octane/water extraction system using O2 as oxidant was studied. The reaction mechanism of thiophene oxidation was proposed. Results obtained here can be used as the reference for the oxidative desulfurization of gasoline because thiophene is one of the main components containing sulfur in fluid catalytic cracking gasoline. Thiophene dissolved in n-octane was photodecomposed and removed into the water phase at ambient temperature and atmospheric pressure. A 500 W high-pressure mercury lamp (main wave length 365 nm, 0.22 kW/m) was used as light source for irradiation, and air was introduced by a gas pump to supply O2. Thiophene can be photo-oxidized to sulfone, oxalic acid, SO42?, and CO2. The desulfurization yield of thiophene in n-octane is 58.9% under photo-irradiation for 5 h under the conditions of air flow at 150 mL/min and V(water):V(n-octane)=1:1. It can be improved to 92.3% by adding 0.15 g zeoliteartificial into 100 mL reaction system, which is the adsorbent for O2 and thiophene. And under such conditions, the photo-oxidation kinetics of thiophene with O2/zeoliteartificial is first-order with an apparent rate constant of 0.5047 h-1 and a half-time of 1.37 h. The sulfur content can be depressed from 800 μL/L to less than 62 μL/L.展开更多
KL molecular sieves with different framework compositions were secondarily synthesized by substituting Si for AI with a solution of (NH4)2SiF6. The internal tetrahedron symmetric stretch frequency, at ～770 cm^-1, i...KL molecular sieves with different framework compositions were secondarily synthesized by substituting Si for AI with a solution of (NH4)2SiF6. The internal tetrahedron symmetric stretch frequency, at ～770 cm^-1, is linear with the molar fraction of Al (XAl= Al/(Si+Al)) in the framework of KL samples: XAl = -7.309×10.3 (v770-760) + 0.3242.展开更多
基金Graduate Innovation Project of Qinghai University for Nationalities(2021XJXS12)Graduate Innovation Project of Qinghai University for Nationalities(12M2021018).
文摘The activation effect of boric acid as an activator is good,and we investigate the best activation conditions for the boric acid impregnation method.To represent the structural characteristics and adsorption performance of the Stellera Chamaejasme based carbon molecular sieves,we use Brunner-Emmet-Teller(BET)measurements,scan-ning electron microscope(SEM),Raman spectra(Raman),X-ray diffraction(XRD),and adsorption property measurement.When the loading ratio was 0.68:1,the specific surface area was 532.21 m^(2)/g,the total pore volume was 0.24 cm 3/g,the average pore size was 1.81 nm,the adsorption value of methylene blue was 145.28 mg/g,and the adsorption value of iodine was 713.33 mg/g,the results showed that boric acid had better activation effect.The carbon molecular sieves made from Stellera Chamaejasme and activated with boric acid produce two peaks on the aperture distribution graph that are densely distributed in the micropore range.This indicates that boric acid’s pore-forming tendency is primarily micropore.
基金The authors gratefully acknowledge the financial support of Science Foundation of China University of Petroleum,Beijing(Grant No.KYJJ2012-03-03).
文摘To improve oil quality,ZSM-22/SAPO-11 composite molecular sieves were synthesized by adding ZSM-22 into a synthetic gel of SAPO-11 for n-decane hydroisomerization.The mass ratios of ZSM-22/(ZSM-22+SAPO-11)in the composite molecular sieves were optimized and the optimal ZSM-22/SAPO-11 composite(ZS-9)was obtained.The electrostatic repulsions between the ZSM-22 precursors and the SAPO-11 crystalline nuclei produced small ZSM-22 and SAPO-11 crystallites in ZS-9,which increased the specific surface area and mesopore volume and thereby exposed more acid sites.In comparison with conventional SAPO-11,ZSM-22 and their mechanical mixture,ZS-9 with smaller crystallites and the optimal medium and strong Brønsted acid centers(MSBAC)content displayed a higher yield of branched C_(10) isomers(81.6%),lower cracking selectivity(11.9%)and excellent stability.The correlation between the i-C_(10) selectivity and the MSBAC density of molecular sieves indicated that the selectivity for branched C_(10) isomers first increased and then decreased with increasing MSBAC density on the molecular sieves,and the maximum selectivity(87.7%)occurred with a density of 9.6×10^(−2)μmol m^(−2).
基金the National Key R&D Program of China(2017YFB0603403)National Natural Science Foundation of China(21676044,21878033,21978034)+1 种基金High Level Innovation Team of Liaoning Province(XLYC1908033)Fundamental Research Funds for the Central Universities(DUT19ZD211,DUT 2018TB02)for the financial support。
文摘Hydrogen is a green clean fuel and chemical feedstock. Its separation and purification from hydrogencontaining mixtures is the key step in the production of hydrogen with high purity(>99.99%). In this work, carbon molecular sieve(CMS) membranes with ultrahigh permselectivity for hydrogen purification were fabricated by high-temperature(700–900 ℃) pyrolysis of polymeric precursor of phenolphthaleinbased cardo poly(arylene ether ketone)(PEK-C). The evolution of the microstructural texture and ultramicroporous structure and gas separation performance of the CMS membrane were characterized via TG-MS, FT-IR, XRD, TEM, CO2 sorption analysis and gas permeation measurements. CMS membranes prepared at 700 ℃ exhibited amorphous turbostratic carbon structures and high H2 permeability of 5260 Barrer with H2/CH4, H2/N2 and H2/CO selectivities of 311, 142, 75, respectively. When carbonized at900 ℃, the CMS membrane with ultrahigh H2/CH4 selectivity of 1859 was derived owing to the formation of the dense and ordered carbon structure. CMS membranes with ultrahigh permselectivity exhibit an attractive application prospect in hydrogen purification.
文摘Thermally stable mesoporous silica and Ti-containing molecular sieves have been synthesized at mild temperature using low-cost and biodegradable---amphoteric tetradecyl betaine as template. The physicochemical characterizations proved that Ti(Ⅳ) could be incorporated in the mesoporous struture.
文摘Research and development of efficient, economical and resource-based flue gas desulfurization technology has always been a hot spot in the field of air pollution control. Molecular sieve materials have been paid attention to by SO<sub>2</sub> adsorbent researchers due to their huge specific surface area. In this paper, 13X zeolite was modified with Cu(NO<sub>3</sub>) <sub>2</sub>·3H<sub>2</sub>O to obtain 13x-Xwt %CuO (calculated by the amount of CuO loaded). The adsorption time and capacity of SO<sub>2</sub> penetration sorbent and the isothermal curve of N<sub>2</sub> adsorption-desorption were studied. The results are as follows: 13X-3wt%CuO has the best adsorption effect, the penetration adsorption time is 110 min, the penetration adsorption capacity is 43.41 mg·g<sup>-1</sup>, the saturation adsorption capacity is 49.27 mg·g<sup>-1</sup>;The amount of CuO loading has a great influence on the adsorption effect of modified 13X molecular sieve on SO<sub>2</sub>. SEM and BET characterization showed that CuO modification did not change the external morphology of 13X molecular sieve, changed the pore size, but did not block the original channel of the molecular sieve, before and after modification belong to the type I adsorption isothermal curve. The pore size distribution and type of molecular sieve, as well as the content and type of alkali metal cations jointly control the adsorption process of SO<sub>2</sub> by 13X-xwt %CuO. XPS characterization showed that Cu(NO<sub>3</sub>) <sub>2</sub> decomposed into CuO and Cu<sub>2</sub>O during roasting at 450°C, CuO/Cu<sub>2</sub>O ≈ 1.5. The R<sup>2</sup> values of the quasi-second-order kinetic models obtained from the 13X-Xwt %CuO particle diffusion kinetic models were all above 0.99, indicating that the quasi-second-order kinetic equations were more relevant. Particle diffusion dynamics model in fitting results show that the adsorption process can be divided into two stages, the first phase of surface adsorption and diffusion rate in the granules common control process, more accurate dynamics model of the secondary in the second phase particle diffusion rate control stage, mainly for the micropore adsorption or chemical adsorption, quasi level 2 dynamic model conformity of variation;C is a constant not equal to 0, indicating that the adsorption of SO<sub>2</sub> is not completely through the form of intra-particle diffusion, and a small amount of chemisorption exists. And it is the compound effect of multiple adsorption mechanisms.
文摘Mesoporous molecularsieve MCM-41 has been synthesized in the extremely dense system (with H2O/Si<10) and characterized by XRD, N2 adsorption isotherm as well as probe reactions of cracking of cumene and isomerization of o-xylene.
文摘In the experiment,PDMS membrane with NaY molecular sieve filling were chosen as the experimental objects and the flux of phenol and removal efficiency of phenol as evaluation index,the effect of the system operating temperature,the flow rate,liquid membrane downstream pressure,operation time,and filling proportion of NaY molecular sieve on pervaporation treatment efficiency for wastewater from coal gasification were investigated. With the increase of temperature and feed flow rate,pervaporation flux and phenol removal efficiency increases. The decrease of the membrane downstream pressure and elevating NaY molecular sieve filling proportion may result in the increase of flux and then phenol removal efficiency improves. When NaY molecular sieve filling proportion is 45% ,treatment efficiency is the best for coal gasification wastewater containing 1850 mg/L phenol as the flux of phenol was 12948. 23 mg/(h·m2) .
文摘Mesoporous molecular sieves, NbFAPO-5 and NbFAPSO-5 were hydrothermally synthesized with AlPO-5 type structure. Characterization of these molecular sieves was performed by X-ray diffraction to determine their structure, ICP-EAS for their elemental composition and infrared spectrometry to access their acidic properties. X-ray diffraction patterns confirmed well AlPO-5 type structure. ICP-EAS analysis confirmed the incorporation of silicon (12.9%), aluminium (15.4%), phosphorous (21.9%), iron (5.62%) and niobium (0.39%) into AlPO-5 framework. Infrared spectrometry analysis showed that both Bronsted and Lewis sites were found in the synthesized samples. The presence of both Bronsted and Lewis acid site led to bifunctional function of NbFAPO-5 and NbFAPSO-5 molecular sieve in promoting both oxidation and esterification reactions. NbFAPSO-5 Bronsted acidity was higher than that of NbFAPO-5 and for Lewis acidity, NbFAPO-5 was higher than that of NbFAPO-5.
文摘After my graduation as a chemistry major from Shanghai Jiaotong University in 1952. I was assigned to work at the People’s University of Northeast China (the predecessor of today’s Jilin University) in Changchun City, serving as a teaching assistant.I)uring my career on campus.I have lectured on a dozen courses on inorganic chemistry,general chemistry,analytic chemistry. rare-element chemistry, complex chemistry. inorganic synthesis,solid-state chemistry
基金financial support from the National Natural Science Foundation of China (Nos. 51672186, 21676175)
文摘Samples of methane molecules grade diameter channel CHA-type molecular sieves(Chabazite-K, SAPO-34 and SSZ-13) were investigated using the adsorption separation of CH4/N2 mixtures. The isotherms recorded for CH4 and N2 follow a typical type-Ι behavior, which were fitted well with the Sips model(R2>0.999) and the selectivity was calculated using IAST theory. The results reveal that Chabazite-K has the highest selectivity(SCH4/N= 5.5).2 SSZ-13 has the largest capacity, which can adsorb up to a maximum of 30.957 cm3·g-1(STP) of CH4, due to it having the largest pore volume and surface area, but the lowest selectivity(SCH4/N2= 2.5). From the breakthrough test, we can conclude that SSZ-13 may be a suitable candidate for the recovery of CH4 from low concentration methane(CH4<20%) based on its larger pore volume and higher CH4 capacity. Chabazite-K is more suited to the separation of high concentration methane(CH4>50%) due to its higher selectivity.
基金Supported by the National Natural Science Foundation of China(21620102007)the Natural Science Foundation for High Education of Jiangsu Province(17KJB530011)+1 种基金the Science and Technology Innovation Foundation of Yangzhou University(2017CXJ015)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘HZSM-5/MCM-41 molecular sieve (H-ZM) catalysts with well-defined micro/mesoporous structures were synthesized and showed high performance for selective synthesis of triacetin via the esterification reaction of glycerol with acetic acid. The conversion of glycerol was demonstrated to be 100% and the triacetin selectivity was over 91%, which can be attributed to the synergistic effect regarding suitable acidic property, excellent diffusion efficiency and good stability derived from the combined advantages of microporous molecular sieve HZSM-5 and mesoporous molecular sieve MCM-41.
基金Supported by the National Natural Science Foundation of China(21176231)the Fundamental Research Funds for the Central Universities(DUT16RC(3)103)Thousand Youth Talents Program
文摘Recent decades witnessed the significant progress made in the research field of 2D molecular sieve membranes.In comparison with their 3D counterparts, 2D molecular sieve membranes possessed several unique advantages like significantly reduced membrane thickness(one atom thick in theory) and diversified molecular sieving mechanisms(in-plane pores within nanosheets & interlayer galleries between nanosheets). M. Tsapatsis first carried out pioneering work on fabrication of lamellar ZSM-5 membrane. Since then, diverse 2D materials typically including graphene oxides(GOs) have been fabricated into membranes showing promising prospects in energy-efficient gas separation, pervaporation, desalination and nanofiltration. In addition to GOs, other emerging 2D materials, including 2D zeolites, 2D metal–organic frameworks(MOFs), 2 D covalent-organic frameworks(COFs), layered double hydroxides(LDHs), transition metal dichalcogenides(TMDCs), MXenes(typically Ti3C2TX), graphitic carbon nitrides(typically g-C3N4), hexagonal boron nitride(h-BN) and montmorillonites(MT) are showing intriguing performance in membrane-based separation process. This article summarized the most recent developments in the field of 2D molecular sieve membranes aside from GOs with particular emphasis on their structure–performance relationship and application prospects in industrial separation.
文摘ZSM-5/MCM-41 composite molecular sieve was prepared by the nano-assembling method.The ZSM-5 molecular sieve,the MCM-41 molecular sieve,the ZSM-5/MCM-41 mechanical mixture and the ZSM-5/MCM-41 composite molecular sieve were characterized by X-ray powder diffractometry,N<sub>2</sub> adsorption isotherms,temperature programmed desorption of ammonia and scanning electron microscopy and their properties were analyzed.Using FCC gasoline as the feed,activities of different molecular sieves for reducing olefin content were investigated in a continuous high-pressure micro-reactor unit under the following conditions:a reaction temperature of 400℃,a reaction time of 2 h,a weight hourly space velocity of 3h<sup>-1</sup>,and a reaction pressure of 2.0 MPa.The results showed that the HMCM-41 molecular sieve had low reaction performance,and the HZSM-5 molecular sieve demonstrated high aromatization activity,while the ZSM-5/MCM- 41 composite molecular sieve exhibited a best olefin-reducing performance because of its high isomerization activity and moderate aromatization activity.With a largest olefin-reducmg capability and a reasonable distribution of products,the composite molecular sieve was more suitable for FCC gasoline upgrading compared to other three catalysts.
基金supported by the National Natural Science Foundation of China (No. 21676180 and No. 21076143)the Key Technologies R&D Program of Tianjin (No. 15ZCZDSF00160)Tianjin Municipal Science and Technology Xinghai Program (No. KJXH2014-05)
文摘To deeply clean oily wastewater,molecular sieve residues(MSRs)were sufficiently recycled and utilized due to their high specific surface area,porous structure,and outstanding adsorption property.Molding MSRs(MMSRs)were prepared by adding additives(starch,citric acid,and soluble glass)to MSRs and were then filled into a fixed bed for adsorbing and separating the oil in wastewater.Sodium dodecylbenzenesulfonate was used to modify the MMSRs,and their adsorption property was also investigated.In addition,the MSRs were characterized by scanning electron microscopy,energy-dispersive X-ray spectroscopy,Brunauer–Emmett–Teller analysis,and Fourier transform infrared spectroscopy.The results indicated that MMSRs satisfied the filling requirement of fixed bed,and their dynamic adsorption capacity could reach 0.1854 mg g^?1.Furthermore,the static adsorption capacity of MMSRs achieved 1.7346 mg g^?1 in the optimum conditions,and the oil adsorption performance of modified MMSRs was further enhanced.Therefore,this work suggests that MSRs are promising alternatives in cleaning oily wastewater.
文摘Lead, a heavy metal, is a well known contaminant in water and has been reported to cause serious health implications to humans, animals, and plants. One of the processes for heavy metal remediation of contaminated water is chemical precipitation. In this present work, chemical precipitation of lead from a contaminated aqueous matrix by chlorides, carbonates, and sulfates of sodium and calcium was compared to lead removal by molecular sieves and biomaterials (fishbone, grape and spinach). The order of lead removal from 1400 ppm of lead solution is sodium chloride (31%) < calcium chloride (62%) burnt grape (83%) < charred spinach (92.3%) < sodium phosphate (95.8%) < sodium carbonate (97%) < molecular sieve sphere (98.7%) < sodium sulfate (99.3%) s ground (99.71%) < fishbone (99.87%)
基金Supported by the National Natural Science Foundation of China （No.20276015） and the Natural Science Foundation of Hebei Province （No.203364）.
文摘A simulated gasoline consisting of model sulfur compounds of thiophene(C4H4S)and 3-methythiophene (3-MC4H4S)dissolved in n-heptane was tested for the oxidative desulfurization in the hydrogen peroxide(H2O2) and formic acid oxidative system over metal oxide-loaded molecular sieve.The effects of the oxidative system, loaded metal oxides,phase transfer catalyst,the addition of olefin and aromatics on sulfur removal were investi- gated in details.The results showed that the sulfur removal rate of simulated gasoline in the H2O2/formic acid sys- tem was higher than in other oxidative systems.The cerium oxide-loaded molecular sieve was found very active catalyst for oxidation of simulated gasoline in this system.The sulfur removal rates of C4H4S and 3-MC4H4S were enhanced when phase transfer catalyst(PTC)was added.However,the sulfur removal rate of simulated gasoline was reduced with the addition of olefin and aromatics.
基金Science and Technology Development Planning Foundation of Jilin Province, China(No.20030405)
文摘Photochemical oxidation of thiophene in n-octane/water extraction system using O2 as oxidant was studied. The reaction mechanism of thiophene oxidation was proposed. Results obtained here can be used as the reference for the oxidative desulfurization of gasoline because thiophene is one of the main components containing sulfur in fluid catalytic cracking gasoline. Thiophene dissolved in n-octane was photodecomposed and removed into the water phase at ambient temperature and atmospheric pressure. A 500 W high-pressure mercury lamp (main wave length 365 nm, 0.22 kW/m) was used as light source for irradiation, and air was introduced by a gas pump to supply O2. Thiophene can be photo-oxidized to sulfone, oxalic acid, SO42?, and CO2. The desulfurization yield of thiophene in n-octane is 58.9% under photo-irradiation for 5 h under the conditions of air flow at 150 mL/min and V(water):V(n-octane)=1:1. It can be improved to 92.3% by adding 0.15 g zeoliteartificial into 100 mL reaction system, which is the adsorbent for O2 and thiophene. And under such conditions, the photo-oxidation kinetics of thiophene with O2/zeoliteartificial is first-order with an apparent rate constant of 0.5047 h-1 and a half-time of 1.37 h. The sulfur content can be depressed from 800 μL/L to less than 62 μL/L.
文摘KL molecular sieves with different framework compositions were secondarily synthesized by substituting Si for AI with a solution of (NH4)2SiF6. The internal tetrahedron symmetric stretch frequency, at ～770 cm^-1, is linear with the molar fraction of Al (XAl= Al/(Si+Al)) in the framework of KL samples: XAl = -7.309×10.3 (v770-760) + 0.3242.
