Electrolytic manganese residue(EMR)can cause serious environmental and biological hazards.In order to solve the problem,zeolite A(EMRZA)and zeolite X(EMRZX)were synthesized by EMR.The pure phase zeolites were synthesi...Electrolytic manganese residue(EMR)can cause serious environmental and biological hazards.In order to solve the problem,zeolite A(EMRZA)and zeolite X(EMRZX)were synthesized by EMR.The pure phase zeolites were synthesized by alkaline melting and hydrothermal two-step process,which had high crystallinity and excellent crystal control.And the optimum conditions for synthesis of zeolite were investigated:NaOH-EMR mass ratio=1.2,L/S=10,hydrothermal temperature=90℃,and hydrothermal time=6 h.Then,EMRZA and EMRZX showed excellent adsorption of Cd^(2+).When T=25℃,time=120min,pH=6,C0=518 mg·L^(-1),and quantity of absorbent=1.5 g·L^(-1),the adsorption capacities of EMRZA and EMRZX reached 314.2 and 289,5 mg·g^(-1),respectively,In addition,after three repeated adsorption-desorption cycles,EMRZA and EMRZX retained 80%and 74%of the initial zeolites removal rates,respectively.Moreover,adsorption results followed quasi-second-order kinetics and monolayer adsorption,which was regulated by a combination of chemisorption and intra-particle diffusion mechanisms.The adsorption mechanism was ions exchange between Cd^(2+)and Na+.In summary,it has been confirmed that EMRZA and EMRZX can be reused as highly efficient adsorbents to treat Cd^(2+)-contaminated wastewater.展开更多
Zeolite X was synthesized by a two-step hydrothermal method using natural stellerite zeolite as the silicon seed,and its adsorption performance for Cd^(2+)and Ni^(2+)ions was experimentally and comprehensively investi...Zeolite X was synthesized by a two-step hydrothermal method using natural stellerite zeolite as the silicon seed,and its adsorption performance for Cd^(2+)and Ni^(2+)ions was experimentally and comprehensively investigated.The effects of p H,zeolite X dosage,contact time,and temperature on adsorption performance for Cd^(2+)and Ni^(2+)ions over were studied.The adsorption process was endothermic and spontaneous,and followed the pseudo-second-order kinetic and the Langmuir isotherm models.The maximum adsorption capacitiesfor Cd^(2+)and Ni^(2+)ions at 298 K were 173.553 and 75.897 mg.g-1,respectively.Ion exchange and precipitation were the principal mechanisms for the removal of Cd^(2+)ions from aqueous solutions by zeolite X,followed by electrostatic adsorption.Ion exchange was the principal mechanisms for the removal of Ni^(2+)ions from aqueous solutions by zeolite X,followed by electrostatic adsorption and precipitation.The zeolite X converted from stellerite zeolite has a low n(Si/Al),abundant hydroxyl groups,and high crystallinity and purity,imparting a good adsorption performance for Cd^(2+)and Ni^(2+)ions.This study suggests that zeolite X converted from stellerite zeolite could be a useful environmentally-friendly and effective tool for the removal of Cd^(2+)and Ni^(2+)ions from aqueous solutions.展开更多
This work describes the development of a process to produce zeolite X from mined kaolin clay from Kono-Boue and Chokocho, Rivers State, Nigeria. The procedures involved the beneficiation of the raw kaolin and calcinat...This work describes the development of a process to produce zeolite X from mined kaolin clay from Kono-Boue and Chokocho, Rivers State, Nigeria. The procedures involved the beneficiation of the raw kaolin and calcinations at 850<span style="font-family:Verdana, Helvetica, Arial;white-space:normal;background-color:#FFFFFF;">°</span>C, to transform the kaolin to a more reactive metakaolin. Afterwards, the extremely reactive metakaolin was purge with sulphuric acid to obtain the much needed silica-alumina ratio for zeolite X synthesis. An alkaline fusion stage was then carried out to transform the metakaolin into zeolite by mixing with aqueous NaOH to form gel then allowed to stay for a duration of seven days at room temperature. The samples were then charged into a propylene container and placed in an oven at a temperature of 100<span style="font-family:Verdana, Helvetica, Arial;white-space:normal;background-color:#FFFFFF;">°</span>C for the reaction to take place for 6 h. Identification of the crystalline phases by X-ray Diffraction (XRD), chemical/elemental compositions by X-ray Fluorescence (XRF)/Energy Dispersive Spectroscopic analyses (EDS), surface morphology by Scanning Electron Microscopy (SEM) and molecular vibration of units by Fourier Transform Infrared Spectrophotometry (FT-IR) were done. The results showed that the zeolite synthesized from Chokocho kaolin (CK) was more crystalline/larger with sharper peaks on both XRD and FTIR than that from Kono-Boue. This was also supported by slightly rougher surface morphology of CK over KK on SEM. XRF Si:Al ratios of 10.73 and 14.36 were obtained for KK and CK respectively. EDS results supported the XRF ratios. Sharper zeolitic characteristic O-H stretching bands at 3488 and 3755 cm<sup>-1</sup> were recorded for CK than KK. However, both results showed that zeolite X have been produced from both Kono-Boue and Chokocho kaolin clays respectively.展开更多
A single phrase Na - X zeolite was synthesized from pretreated oil shale ash by alkaline fusion and hydrotherreal treatment. Eff3cts of the NaOH concentration, crystallization time ant temperature on the formation of ...A single phrase Na - X zeolite was synthesized from pretreated oil shale ash by alkaline fusion and hydrotherreal treatment. Eff3cts of the NaOH concentration, crystallization time ant temperature on the formation of Na-X zeolite were studied in detail. The single phase Na- X zeolite powders can. be prepared by alkaline fusion o.f pretreated oil shale ash at 600 ℃ .for 1 h, and crystalli-zation at 80 - 100 ℃ .for 8 - 10 h with NaOH concentration of 3 -3. 5 tool · L-1. Na - A zeolite appears when decreasing NaOH concentration, crystallization time or temperature, ant an unnamed zeolite emerges when prolonging crystallization time or raising crystalli-zation, temperature. SEM micrographs suggest that the aggregates of Na-X zeolite particles have perfect dispersity and uniform granular with about 1.5 μm in size, and most of the Na-X zeolite crystals display a regular octahedral structure with the size of about 500 nm. The specific surface area of the powders with single Na-X zeolite phase reaches the maximum value of 488. 163 2 m2· g -1, larger than that of multiple zeolite powders.展开更多
Rational design is important to achieve high-performance sorbents used to remove the contaminants of emerging concern(CECs) from water.However, it is hard to propose effective design guidelines due to the lack of a cl...Rational design is important to achieve high-performance sorbents used to remove the contaminants of emerging concern(CECs) from water.However, it is hard to propose effective design guidelines due to the lack of a clear understanding of the interaction mechanisms. By means of systematic quantum chemical computations, as a case study, we investigated the interactions between zeolite X/M^(n+)-zeolite X(Si/Al=1,M^(n+)=Cu^(2+) and Ni^(2+)) and three commonly used CECs(namely salicylic acid, carbamazepine and ciprofloxacin) in water to clarify the adsorption mechanisms. Our computations found that anionic salicylic acid cannot be adsorbed by neither zeolite X nor M^(n+)-zeolite X in neutral water due to the high electrostatic repulsion. In comparison, carbamazepine and ciprofloxacin have favorable binding energies with both zeolite X and M^(n+)-zeolite X, and their interactions with M^(n+)-zeolite X are stronger due to the joint effects of H-bond, metal complexation and electrostatic interaction. The adsorption loading of ciprofloxacin, which has a large molecular size, on M^(n+)-zeolite X is limited due to the steric hindrance. In general, steric hindrance, electrostatic interaction, H-bond and metal complexation are dominant factors for the examined systems in this study. Thus, for the design of high-performance absorbing materials, we should fully consider the molecular properties of pollutants(molecular size, surface electrostatic potential and atomic type, etc.), and properly enhance the favorable effects and avoid the unfavorable factors as much as possible under the guidance of the interaction mechanisms.展开更多
A two-stage vacuum pressure swing adsorption(VPSA)process that coupled kinetically controlled and equilibrium controlled separation process with reflux has been investigated for capturing carbon dioxide from dry flue ...A two-stage vacuum pressure swing adsorption(VPSA)process that coupled kinetically controlled and equilibrium controlled separation process with reflux has been investigated for capturing carbon dioxide from dry flue gas(85%N_(2)/15%CO_(2)).In the first enriching stage,carbon molecular sieve(CMS),which shows kinetic selectivity for CO_(2)/N_(2),is adopted as the adsorbent to remove most N_(2)in feed gas,thereby upgrading CO_(2)and significantly reducing the amount for further refinement.The second stage loads zeolite 13X as adsorbent to purify the CO_(2)-rich flow from the first stage for meeting the requirements of National Energy Technology Laboratory.Series of experiments have been conducted for adsorption isotherms measuring and lab-scale experimental validation as well as analysis.The effect of feed composition on the separation performance of the PSA system was studied experimentally and theoretically here.The optimal results achieved 95.1%purity and 92.9%recovery with a high CO_(2)productivity(1.89 mol CO_(2)·h^(-1)·kg^(-1))and an appropriate energy consumption of 1.07 MJ·(kg CO_(2))^(-1).Further analysis has been carried out by simulation for explicating the temperature,pressure,and concentration distribution at cyclic steady state.展开更多
A method is presented for the synthesis of zeolite ZSM-2 by adding zeolite X as seeds in the synthetic mixture containing both lithium and sodium. At the presence of zeolite X seeds, highly crystalline zeolite ZSM-2 w...A method is presented for the synthesis of zeolite ZSM-2 by adding zeolite X as seeds in the synthetic mixture containing both lithium and sodium. At the presence of zeolite X seeds, highly crystalline zeolite ZSM-2 with com-position of (0.3—0.7)Li2O·(0.7—0.3)Na2O·Al2O3·(2.5—4.0)SiO2·nH2O can be obtained in a wide range of SiO2/Al2O3 ratios from 2.5 to 16, and the optimum Li2O/(Li2O+Na2O) fraction is between 0.3 and 0.7. The ZSM-2 products were characterized by XRD, SEM, IR, 29Si MAS NMR and DTA/TG analysis etc. By 29Si MAS NMR spectroscopy, it was found that ZSM-2 contained nearly equal FAU and EMT phase, and the Si/Al ratios in FAU were slightly lower than those in EMT domains in most cases. The lithium form zeolite ZSM-2 has comparable N2 adsorption capacity with LiX.展开更多
The strength of basic sites has been measured by pyrrole-IR on alkali metal cation exchanged β and X zeolites, as well as NaOH loaded Naβ. The influence of cation type and the structure of zeolites on their basicity...The strength of basic sites has been measured by pyrrole-IR on alkali metal cation exchanged β and X zeolites, as well as NaOH loaded Naβ. The influence of cation type and the structure of zeolites on their basicity has been studied. The acidic and basic properties of the samples were investigated by NH3-TPD and isopropanol reaction. It was shown that the strength of basic sites on samples could be characterized by the shift of vNH band in the pyrrole-IR spectra. The framework oxygen charges were calculated from the Sanderson electronegativity. The changes in basic properties with various alkali metal cation are consistent with the changes of local oxygen charges of the zeolite framework.展开更多
基金supported by the National Natural Science Foundation of China(52164036,U1960201,51764007)the Guizhou Province Graduate Research Fund(YJSKYJJ(2021)003).
文摘Electrolytic manganese residue(EMR)can cause serious environmental and biological hazards.In order to solve the problem,zeolite A(EMRZA)and zeolite X(EMRZX)were synthesized by EMR.The pure phase zeolites were synthesized by alkaline melting and hydrothermal two-step process,which had high crystallinity and excellent crystal control.And the optimum conditions for synthesis of zeolite were investigated:NaOH-EMR mass ratio=1.2,L/S=10,hydrothermal temperature=90℃,and hydrothermal time=6 h.Then,EMRZA and EMRZX showed excellent adsorption of Cd^(2+).When T=25℃,time=120min,pH=6,C0=518 mg·L^(-1),and quantity of absorbent=1.5 g·L^(-1),the adsorption capacities of EMRZA and EMRZX reached 314.2 and 289,5 mg·g^(-1),respectively,In addition,after three repeated adsorption-desorption cycles,EMRZA and EMRZX retained 80%and 74%of the initial zeolites removal rates,respectively.Moreover,adsorption results followed quasi-second-order kinetics and monolayer adsorption,which was regulated by a combination of chemisorption and intra-particle diffusion mechanisms.The adsorption mechanism was ions exchange between Cd^(2+)and Na+.In summary,it has been confirmed that EMRZA and EMRZX can be reused as highly efficient adsorbents to treat Cd^(2+)-contaminated wastewater.
基金supported by the National Natural Science Foundation of China(51564008,41662005)Natural Science Foundation of Guangxi Province(2019GXNSFBA245083)。
文摘Zeolite X was synthesized by a two-step hydrothermal method using natural stellerite zeolite as the silicon seed,and its adsorption performance for Cd^(2+)and Ni^(2+)ions was experimentally and comprehensively investigated.The effects of p H,zeolite X dosage,contact time,and temperature on adsorption performance for Cd^(2+)and Ni^(2+)ions over were studied.The adsorption process was endothermic and spontaneous,and followed the pseudo-second-order kinetic and the Langmuir isotherm models.The maximum adsorption capacitiesfor Cd^(2+)and Ni^(2+)ions at 298 K were 173.553 and 75.897 mg.g-1,respectively.Ion exchange and precipitation were the principal mechanisms for the removal of Cd^(2+)ions from aqueous solutions by zeolite X,followed by electrostatic adsorption.Ion exchange was the principal mechanisms for the removal of Ni^(2+)ions from aqueous solutions by zeolite X,followed by electrostatic adsorption and precipitation.The zeolite X converted from stellerite zeolite has a low n(Si/Al),abundant hydroxyl groups,and high crystallinity and purity,imparting a good adsorption performance for Cd^(2+)and Ni^(2+)ions.This study suggests that zeolite X converted from stellerite zeolite could be a useful environmentally-friendly and effective tool for the removal of Cd^(2+)and Ni^(2+)ions from aqueous solutions.
文摘This work describes the development of a process to produce zeolite X from mined kaolin clay from Kono-Boue and Chokocho, Rivers State, Nigeria. The procedures involved the beneficiation of the raw kaolin and calcinations at 850<span style="font-family:Verdana, Helvetica, Arial;white-space:normal;background-color:#FFFFFF;">°</span>C, to transform the kaolin to a more reactive metakaolin. Afterwards, the extremely reactive metakaolin was purge with sulphuric acid to obtain the much needed silica-alumina ratio for zeolite X synthesis. An alkaline fusion stage was then carried out to transform the metakaolin into zeolite by mixing with aqueous NaOH to form gel then allowed to stay for a duration of seven days at room temperature. The samples were then charged into a propylene container and placed in an oven at a temperature of 100<span style="font-family:Verdana, Helvetica, Arial;white-space:normal;background-color:#FFFFFF;">°</span>C for the reaction to take place for 6 h. Identification of the crystalline phases by X-ray Diffraction (XRD), chemical/elemental compositions by X-ray Fluorescence (XRF)/Energy Dispersive Spectroscopic analyses (EDS), surface morphology by Scanning Electron Microscopy (SEM) and molecular vibration of units by Fourier Transform Infrared Spectrophotometry (FT-IR) were done. The results showed that the zeolite synthesized from Chokocho kaolin (CK) was more crystalline/larger with sharper peaks on both XRD and FTIR than that from Kono-Boue. This was also supported by slightly rougher surface morphology of CK over KK on SEM. XRF Si:Al ratios of 10.73 and 14.36 were obtained for KK and CK respectively. EDS results supported the XRF ratios. Sharper zeolitic characteristic O-H stretching bands at 3488 and 3755 cm<sup>-1</sup> were recorded for CK than KK. However, both results showed that zeolite X have been produced from both Kono-Boue and Chokocho kaolin clays respectively.
文摘A single phrase Na - X zeolite was synthesized from pretreated oil shale ash by alkaline fusion and hydrotherreal treatment. Eff3cts of the NaOH concentration, crystallization time ant temperature on the formation of Na-X zeolite were studied in detail. The single phase Na- X zeolite powders can. be prepared by alkaline fusion o.f pretreated oil shale ash at 600 ℃ .for 1 h, and crystalli-zation at 80 - 100 ℃ .for 8 - 10 h with NaOH concentration of 3 -3. 5 tool · L-1. Na - A zeolite appears when decreasing NaOH concentration, crystallization time or temperature, ant an unnamed zeolite emerges when prolonging crystallization time or raising crystalli-zation, temperature. SEM micrographs suggest that the aggregates of Na-X zeolite particles have perfect dispersity and uniform granular with about 1.5 μm in size, and most of the Na-X zeolite crystals display a regular octahedral structure with the size of about 500 nm. The specific surface area of the powders with single Na-X zeolite phase reaches the maximum value of 488. 163 2 m2· g -1, larger than that of multiple zeolite powders.
基金the Postdoctoral Fellowships Program from the NSF-sponsored Puerto Rico Institute for Functional Nanomaterials under Grant EPS-1002410support from NSF CREST Phase 2 Grant HRD-1345156
文摘Rational design is important to achieve high-performance sorbents used to remove the contaminants of emerging concern(CECs) from water.However, it is hard to propose effective design guidelines due to the lack of a clear understanding of the interaction mechanisms. By means of systematic quantum chemical computations, as a case study, we investigated the interactions between zeolite X/M^(n+)-zeolite X(Si/Al=1,M^(n+)=Cu^(2+) and Ni^(2+)) and three commonly used CECs(namely salicylic acid, carbamazepine and ciprofloxacin) in water to clarify the adsorption mechanisms. Our computations found that anionic salicylic acid cannot be adsorbed by neither zeolite X nor M^(n+)-zeolite X in neutral water due to the high electrostatic repulsion. In comparison, carbamazepine and ciprofloxacin have favorable binding energies with both zeolite X and M^(n+)-zeolite X, and their interactions with M^(n+)-zeolite X are stronger due to the joint effects of H-bond, metal complexation and electrostatic interaction. The adsorption loading of ciprofloxacin, which has a large molecular size, on M^(n+)-zeolite X is limited due to the steric hindrance. In general, steric hindrance, electrostatic interaction, H-bond and metal complexation are dominant factors for the examined systems in this study. Thus, for the design of high-performance absorbing materials, we should fully consider the molecular properties of pollutants(molecular size, surface electrostatic potential and atomic type, etc.), and properly enhance the favorable effects and avoid the unfavorable factors as much as possible under the guidance of the interaction mechanisms.
基金financially supported by the Renewable Energy and Hydrogen Projects National Key Research&Development Program of China(2019YFB1505000)。
文摘A two-stage vacuum pressure swing adsorption(VPSA)process that coupled kinetically controlled and equilibrium controlled separation process with reflux has been investigated for capturing carbon dioxide from dry flue gas(85%N_(2)/15%CO_(2)).In the first enriching stage,carbon molecular sieve(CMS),which shows kinetic selectivity for CO_(2)/N_(2),is adopted as the adsorbent to remove most N_(2)in feed gas,thereby upgrading CO_(2)and significantly reducing the amount for further refinement.The second stage loads zeolite 13X as adsorbent to purify the CO_(2)-rich flow from the first stage for meeting the requirements of National Energy Technology Laboratory.Series of experiments have been conducted for adsorption isotherms measuring and lab-scale experimental validation as well as analysis.The effect of feed composition on the separation performance of the PSA system was studied experimentally and theoretically here.The optimal results achieved 95.1%purity and 92.9%recovery with a high CO_(2)productivity(1.89 mol CO_(2)·h^(-1)·kg^(-1))and an appropriate energy consumption of 1.07 MJ·(kg CO_(2))^(-1).Further analysis has been carried out by simulation for explicating the temperature,pressure,and concentration distribution at cyclic steady state.
文摘A method is presented for the synthesis of zeolite ZSM-2 by adding zeolite X as seeds in the synthetic mixture containing both lithium and sodium. At the presence of zeolite X seeds, highly crystalline zeolite ZSM-2 with com-position of (0.3—0.7)Li2O·(0.7—0.3)Na2O·Al2O3·(2.5—4.0)SiO2·nH2O can be obtained in a wide range of SiO2/Al2O3 ratios from 2.5 to 16, and the optimum Li2O/(Li2O+Na2O) fraction is between 0.3 and 0.7. The ZSM-2 products were characterized by XRD, SEM, IR, 29Si MAS NMR and DTA/TG analysis etc. By 29Si MAS NMR spectroscopy, it was found that ZSM-2 contained nearly equal FAU and EMT phase, and the Si/Al ratios in FAU were slightly lower than those in EMT domains in most cases. The lithium form zeolite ZSM-2 has comparable N2 adsorption capacity with LiX.
基金supported by the National Natural Science Foundation of China.
文摘The strength of basic sites has been measured by pyrrole-IR on alkali metal cation exchanged β and X zeolites, as well as NaOH loaded Naβ. The influence of cation type and the structure of zeolites on their basicity has been studied. The acidic and basic properties of the samples were investigated by NH3-TPD and isopropanol reaction. It was shown that the strength of basic sites on samples could be characterized by the shift of vNH band in the pyrrole-IR spectra. The framework oxygen charges were calculated from the Sanderson electronegativity. The changes in basic properties with various alkali metal cation are consistent with the changes of local oxygen charges of the zeolite framework.