In this study,seven coal-based activated carbons(ACs)were adopted to remove trimethylamine(TMA)in an aqueous solution as environmentally friendly and harmless adsorbents.The results showed that columnar AC(CAC)had a c...In this study,seven coal-based activated carbons(ACs)were adopted to remove trimethylamine(TMA)in an aqueous solution as environmentally friendly and harmless adsorbents.The results showed that columnar AC(CAC)had a clear scale and honeycomb structures with few fragments and micropores,contributing to superior TMA removal capacity compared to granular AC(GAC)(71.67%for 6.0 mm CAC and 69.92%for 40–60 mesh GAC).In addition,the process of adsorption was accompanied by desorption,and the recommended absorbed time was 120–180 min.The short time to achieve equilibrium indicated that adsorption was kinetically controlled,and pseudo-second-order kinetics was more appropriate than pseudo-first-order kinetics in explaining the adsorption mechanism in both water and oyster enzymatic hydrolysate.The intraparticle diffusion model presented that the adsorption processes could be divided into three steps for GAC and two steps for CAC.The adsorption processes were consistent with the Freundlich model,indicating the existence of physisorption and chemisorption as multilayer adsorption.The results indicated that AC,especially CAC,has great potential for TMA elimination in aquatic product processing.展开更多
Support vector regression (SVR) combined with particle swarm optimization for its parameter optimization is employed to establish a model for predicting the Henry constants of multi-walled carbon nanotubes (MWNTs)...Support vector regression (SVR) combined with particle swarm optimization for its parameter optimization is employed to establish a model for predicting the Henry constants of multi-walled carbon nanotubes (MWNTs) for adsorption of volatile organic compounds (VOCs). The prediction performance of SVR is compared with those of the model of theoretical linear salvation energy relationship (TLSER). By using leave-one-out cross validation of SVR test Henry constants for adsorption of 35 VOCs on MWNTs, the root mean square error is 0.080, the mean absolute percentage error is only 1.19~, and the correlation coefficient (R2) is as high as 0.997. Compared with the results of the TLSER model, it is shown that the estimated errors by SVR are ali smaller than those achieved by TLSER. It reveals that the generalization ability of SVR is superior to that of the TLSER model Meanwhile, multifactor analysis is adopted for investigation of the influences of each molecular structure descriptor on the Henry constants. According to the TLSER model, the adsorption mechanism of adsorption of carbon nanotubes of VOCs is mainly a result of van der Waals and interactions of hydrogen bonds. These can provide the theoretical support for the application of carbon nanotube adsorption of VOCs and can make up for the lack of experimental data.展开更多
The large accumulation of coal gangue,a common industrial solid waste,causes severe environmental problems,and green development strategies are required to transform this waste into high-value-added products.In this s...The large accumulation of coal gangue,a common industrial solid waste,causes severe environmental problems,and green development strategies are required to transform this waste into high-value-added products.In this study,low-cost ceramsites adsorbents were prepared from waste gangue,silt coal,and peanut shells and applied to remove the organic dye methylene blue from wastewater.We investigated the microstructure of ceramsites and the effects of the sintering atmosphere,sintering temperature,and solution pH on their adsorption performance.The ceramsites sintered at 800℃under a nitrogen atmosphere exhibited the largest three-dimensional-interconnected hierarchical porous structure among the prepared ceramsites;further,it exhibited the highest methylene blue adsorption performance,with an adsorption capacity of 0.954 mg·g^(−1),adsorption efficiency of over 95%,and adsorption equilibrium time of 1 h at a solution pH of 9.The removal efficiency remained greater than 75%after five adsorption cycles.The adsorption kinetics data were analyzed using various models,including the pseudosecond-order kinetic model and Langmuir equation,and the adsorption was attributed to electrostatic interactions between the dyes and ceramsites,n-interactions,and hydrogen bonds.The prepared coal gangue ceramsites exhibited excellent adsorption capacities,removal rates,and cyclic stabilities,demonstrating their promising application prospects for the comprehensive utilization of solid waste and for wastewater treatment.展开更多
To explore the kinetic adsorption under continuous and nonequilibrium states, an integration of continuous measurement and adsorption platform kinetics method was proposed, which was initially called the ICM-AP kineti...To explore the kinetic adsorption under continuous and nonequilibrium states, an integration of continuous measurement and adsorption platform kinetics method was proposed, which was initially called the ICM-AP kinetics method, and a corresponding kinetic adsorption experimental method was developed. Adsorption experiments of europium(Eu) on Ca-bentonite,Na-bentonite, and the D231 cation exchange resin were performed using the ICM-AP kinetics method and continuous measurements. Because the kinetic experimental results observed in this study were different from those of traditional batch adsorption data, pseudo-first-order or pseudo-second-order kinetic models were unsuitable for fitting the experimental data.Hence, a liquid membrane diffusion(LMD) model was developed based on the assumption of simultaneous adsorption/desorption to discuss the mechanism of kinetic adsorption. The kinetic adsorption mechanism was also studied by using XPS.The results indicated that the proposed adsorption model can fit the experimental data more suitably, and the adsorption/desorption behaviors of Eu on bentonite and the D231 resin were simultaneously observed, suggesting that the adsorption kinetics of Eu(Ⅲ) was mainly dominated by hydrated Eu(Ⅲ) ions on the liquid membrane.展开更多
Polyvinylpyrrolidone-reduced graphene oxide was prepared by modified hummers method and was used as adsorbent for removing Cu ions from wastewater. The effects of contact time and ions concentration on adsorption capa...Polyvinylpyrrolidone-reduced graphene oxide was prepared by modified hummers method and was used as adsorbent for removing Cu ions from wastewater. The effects of contact time and ions concentration on adsorption capacity were examined. The maximum adsorption capacity of 1689 mg/g was observed at an initial p H value of 3.5 after agitating for 10 min. It was demonstrated that polyvinylpyrrolidone-reduced graphene oxide had a huge adsorption capacity for Cu ions, which was 10 times higher than maximal value reported in previous works. The adsorption mechanism was also discussed by density functional theory. It demonstrates that Cu ions are attracted to surface of reduced graphene oxide by C atoms in reduced graphene oxide modified by polyvinylpyrrolidone through physisorption processes, which may be responsible for the higher adsorption capacity. Our results suggest that polyvinylpyrrolidone-reduced graphene oxide is an effective adsorbent for removing Cu ions in wastewater. It also provides a new way to improve the adsorption capacity of reduced graphene oxide for dealing with the heavy metal ion in wastewater.展开更多
Carbonate shells have an astonishing ability in the removal of Cd^2+ in a short time period with emphasis on being a low cost adsorbent. In the present study, the sorption capacity of carbonate shells was studied for...Carbonate shells have an astonishing ability in the removal of Cd^2+ in a short time period with emphasis on being a low cost adsorbent. In the present study, the sorption capacity of carbonate shells was studied for Cd^2+ in batch experiments. The influence of different carbonate shell sizes and physico-chemical factors were evaluated and the results were analyzed for its correlation matrices by using Predictive Analytics Software (PASW). The miner- alogy state of aqueous solution regarding the saturation index was simulated using PHREEQC to identify the Cd^2+ uptake mechanism. The Cd uptake rates were calculated as well as Ca^2+, HCO3- concentration, pH, ambient humidity and temperature were measured. Cd2+ removal of 91.52% was achieved after 5 h adsorption. The adsorption efficiencies were significantly influenced by pH as they increased with the increase of pH from acidic solution (5.50±0.02) to slightly alkaline (7.60±0.05). In addition, the mineralogy state of aqueous solution calculated from PHREEQC confirmed that the increment of Ca^2+ and HCO3- concentrations in solution was attributed to the dissolution of carbonate shells. Moreover, the ion exchange adsorption mechanism of Cd^2+ toward Ca^2+ was identified as the process involved in Cd^2+ uptake.展开更多
Mercury(Hg)ions can lead to a serious impact on the environment;therefore,it was necessary to find an effective method for absorbing these toxic Hg ions.Here,the adsorbent(Zn-AHMT)was synthesized from zinc nitrate and...Mercury(Hg)ions can lead to a serious impact on the environment;therefore,it was necessary to find an effective method for absorbing these toxic Hg ions.Here,the adsorbent(Zn-AHMT)was synthesized from zinc nitrate and 4-amino 3-hydrazine-5 mercapto-1,2,4-triazole(AHMT)by one-step method and,characterized the microstruc-ture and absorption performance by fourier transform infrared spectroscopy(FTIR),field emission scanning electron microscopy(FESEM),X-ray diffraction(XRD),Brunauer-Emmett Teller(BET),Thermal Gravimetric Analyzer(TGA)and X-ray photoelectron spectroscopy(XPS).Through a plethora of measurements,we found that the maximum adsorption capacity was 802.8 mg/g when the optimal pH of Zn-AHMT was 3.0.The isothermal and kinetic experiments confirm that the reaction process of Zn-AHMT was chemisorption,while the adsorption process conforms to the Hill model and pseudo second order kinetic model.Thermodynamic experiments showed that the adsorption process was spontaneous and exothermic.Selective experiments were performed in the simulated wastewater containing Mn,Mg,Cr,Al,Co,Ni,Hg ions.Our results showed that the Zn-AHMT has a stronger affinity for Hg ions.The removal rate of Zn-AHMT remained above 98%,indicating that the Zn-AHMT had a good stability validated by three adsorption-desorption repeatable tests.According to the XPS results,the adsorption reaction of Zn-AHMT was mainly attributed to the chelation and ion exchange.This was further explained by both density functional theory(DFT)calculation and frontier molecular orbital theory.We therefore propose the adsorption mechanism of Zn-AHMT.The adsorption reaction facilitates via the synergistic action of S and N atoms.Moreover,the bonding between the adsorbent and the N atom has been proved to be more stable.Our study demonstrated that Zn-AHMT had a promising application prospect in mercury removal.展开更多
When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PF...When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PFOA) from groundwater. With favorable tailoring, QAE-AC removed PFOA from groundwater for 118,000 bed volumes before halfbreakthrough in rapid small scale column tests, while the influent PFOA concentration was 200 ng/L. The tailoring involved pre-dosing QAE at an array of proportions onto this carbon, and then monitoring bed life for PFOA removal. When pre-dosing with 1 mL QAE, this PFOA bed life reached an interim peak, whereas bed life was less following 3 mL QAE pre-dosing, then PFOA bed life exhibited a steady rise for yet subsequently higher QAE pre-dosing levels. Large-scale atomistic modelling was used herein to provide new insight into the mechanism of PFOA removal by QAE-AC. Based on experimental results and modelling, the authors perceived that the QAE's epoxide functionalities cross-linked with phenolics that were present along the activated carbon's graphene edge sites, in a manner that created mesopores within macroporous regions or created micropores within mesopores regions. Also, the QAE could react with hydroxyls outside of these pore, including the hydroxyls of both graphene edge sites and other QAE molecules. This latter reaction formed new pore-like structures that were external to the activated carbon grains. Adsorption of PFOA could occur via either charge balance between negatively charged PFOA with positively charged QAE, or by van der Waals forces between PFOA's fluoro-carbon tail and the graphene or QAE carbon surfaces.展开更多
The nanowires-reticulated calcium silicate with a specific surface area more than 100 m^2/g was prepared by a hydrothermalprocess using hydrated lime(Ca(OH)_2,HL)and silica containing soluble fluoride,which was a ...The nanowires-reticulated calcium silicate with a specific surface area more than 100 m^2/g was prepared by a hydrothermalprocess using hydrated lime(Ca(OH)_2,HL)and silica containing soluble fluoride,which was a by-product of fluorine industry,and the soluble fluoride in raw silica was fixed as CaSiF_6 at the same time.The kinetic characteristics and mechanism of adsorbing phosphate by fluorine-containing calcium silicate were investigated in the experiments of phosphorus(P)removalfrom aqueous solution.The results show that the prepared fluorine-containing calcium silicate has excellent performance for adsorbing phosphate,the adsorption process appears to follow pseudo-second-order reaction kinetics and the process is mainly controlled by chemisorption.The product resulted from P adsorption is mainly composed of hydroxyapatite(HAP)and fluorapatite(FAP),which are further used as adsorbents of heavy metalion Cd^(2+) in aqueous solution and display excellent performance.展开更多
Competition of hydrocarbon compounds with sulfides in gasoline has caused a not very high selectivity of sulfides in adsorption desulfurization so far,resulting in a reduction of catalyst lifetime as well as more sulf...Competition of hydrocarbon compounds with sulfides in gasoline has caused a not very high selectivity of sulfides in adsorption desulfurization so far,resulting in a reduction of catalyst lifetime as well as more sulfur oxide emissions.Tostudy the whole competitive process changing with the increase of the loading,the dynamic competition adsorption mechanism of cyclohexene and thiophene in siliceous faujasite(FAU)zeolite was analyzed by the Monte Carlo simulation.The results showed that with the increase of the loading,thiophene and cyclohexene had different performances before and after the inflection point of 40 molecule/UC.The adsorbates were distributed ideally at optimal sites during the stage that occurred before the inflection point,which is called the“optimal-displacement adsorption”stage.When approaching the inflection point,the competition became apparent and the displacement appeared accordingly,some thiophene molecules at S sites(refers to the sites inside the supercages)were displaced by cyclohexene.After the inflection point,the concentration of adsorbates at W sites(refers to the 12-membered ring connecting the supercages)was significantly reduced,whereas the adsorbates at S sites got more concentrated.The stage some cyclohexene molecules displaced by thiophene and inserted into the center of the supercage can be named as the“insertion-displacement adsorption”stage,and both the adsorption behavior and the competitive relationship became localized when the adsorption amount became saturated.This shift in the competitive adsorption mechanism was due to the sharp increase of interaction energy between the adsorbates.Besides,the increase in temperature and ratio of Si/Al will allow the adsorbates,especially thiophene molecules to occupy more adsorption sites,and it is beneficial to improve the desulfurization selectivity.展开更多
Rare earth element is an important strategic metal,but the supply of high purity rare earth ores is growing slowly,which is in sharp contradiction with the rapidly growing demand.Froth flotation has been confirmed to ...Rare earth element is an important strategic metal,but the supply of high purity rare earth ores is growing slowly,which is in sharp contradiction with the rapidly growing demand.Froth flotation has been confirmed to be an effective method to separate bastnaesite from its gangue minerls.However,the traditional collectors are facing serious problems in flotation separation of minerals,requiring the addition of excess depressant and regulator in the flotation process.Herein,we proposed and synthesized novel Gemini hydroxamic acids Octyl-bishydroxamic acid(OTBHA),Decyl-bishydroxamic acid(DCBHA)and Dodecyl-bishydroxamic acid(DDBHA)as the collectors in bastnaesite-barite flotation system.The effect of different carbon chain lengths on the molecular properties were explored by density functional theory(DFT)calculations.DCBHA possessed a stronger reactivity compared with OCBHA and DDBHA.The flotation results verified the consistency of the computational calculation about the performance prediction of Gemini hydroxamic acids.Compared with OCBHA and DDBHA,DCBHA displayed superior collecting affinity toward bastnaesite,and did not float barite.Zeta potential results showed that the presence of DCBHA increased the potential of bastnaesite,while it had almost no effect on barite,indicating DCBHA had a stronger affinity for bastnaesite.Then,Fourier transform infrared(FTIR)and X-ray photoelectron spectroscopy(XPS)analyses indicated that the adsorption mechanism was due to two hydroxamate groups of DCBHA co-anchored on bastnaesite surface by forming five-membered hydroxamic―(O―O)―Ce complexes.In addition,atomic force microscopy(AFM)clearly observed that DCBHA uniformly aggregated on bastnaesite surface,which increased surface contact angle and improved the hydrophobicity of bastnaesite.展开更多
The adsorption behaviors and mechanism of a novel chelate resin, macroporous phosphonic acid resin(PAR)for Gd(Ⅲ)were investigated. The statically and dynamically saturated adsorption capacity is respectively 308 mg...The adsorption behaviors and mechanism of a novel chelate resin, macroporous phosphonic acid resin(PAR)for Gd(Ⅲ)were investigated. The statically and dynamically saturated adsorption capacity is respectively 308 mg·g^(-1)resin and 296 mg·g^(-1)resin at 298 K in HAc-NaAc medium at pH 5.6. Gd(Ⅲ)adsorbed on PAR can be reductively eluted by 0.5~5.0 mol·L^(-1) HCl used as eluant and the elution percentage is up to 94.7% in 1.0 mol·L^(-1) HCl. The resin can be regenerated and reused without apparent decrease in adsorption capacity. The apparent adsorption rate constant is k_(298)=3.96×10^(-5) s^(-1). The adsorption behavior of PAR for Gd(Ⅲ) conforms to the Freundlich isotherm. The thermodynamic adsorption parameter, enthalpy change △H of PAR for Gd(Ⅲ)is 22.6kJ·mol^(-1). The apparent adsorption activation energy(Ea)of PAR for Gd(Ⅲ)is 5.0 kJ·mol^(-1). The molar coordination ratio of the functional group of PAR to Gd(Ⅲ)is about 3∶1. The adsorption mechanism of PAR for Gd(Ⅲ)was examined by using chemical method and IR spectrometry.展开更多
Lignocellulose has the potential to become a bio-based adsorbent due to its biodegradability and renewability.In this study,a novel polydopamine functionalized-lignin(lignin@PDA),prepared via self-polymerization of do...Lignocellulose has the potential to become a bio-based adsorbent due to its biodegradability and renewability.In this study,a novel polydopamine functionalized-lignin(lignin@PDA),prepared via self-polymerization of dopamine(PDA)on lignin,was used as a bio-based adsorbent for rapid scavenging of hexavalent chromium(Cr(VI)).The morphology,functional groups,crystalline structure,and chemical composition of lignin@PDA were characterized with a scanning electron microscope-energy dispersive spectrometer,Fourier transform infrared spectroscopy,X-ray diffraction,and X-ray photoelectron spectroscopy.The Cr(VI)adsorption process of lignin@PDA was studied using batch experiments as a function of pH,ionic strength,adsorbent dose,and contact time at room temperature.The adsorption rate of lignin@PDA was five times greater than that of the unmodified lignin,with a maximum adsorption capacity of 102.6 mg/g in an acidic medium.The adsorption of Cr(VI)on lignin@PDA fit the pseudo-secondorder equation and the Freundlich model,indicating that the adsorption process was mainly dominated by chemisorption and surface complexation.The thermodynamic parameters showed that adsorption of Cr(VI)on lignin@PDA was an endothermic and spontaneous process.The X-ray absorption fine structure results showed that sorption and reduction of Cr(VI)into Cr(II)occurred simultaneously on lignin.Moreover,PDA coating not only improved the reactivity of lignin but also promoted the complete reduction of Cr(VI)by lignin.According to these results,polydopamine functionalized-lignin is a promising bio-based adsorbent for immobilization of Cr(VI)from wastewater.展开更多
This study investigates the removal of Congo Red dye from aqueous solution using functionalized generation 3.0 and 5.0 polyamidoamine dendrimer-silica gel composite (G-3PS, G-5PS). Fourier Transform-Infra Red spectros...This study investigates the removal of Congo Red dye from aqueous solution using functionalized generation 3.0 and 5.0 polyamidoamine dendrimer-silica gel composite (G-3PS, G-5PS). Fourier Transform-Infra Red spectroscopy, Brunauer Emmett and Teller, Thermo Gravimetric Analysis, pH at point of zero charge, and scanning electron microscopy measurements have been applied to characterize the synthetic nanohybrid composite, these techniques revealed the successful functionalization of both dendrimer molecules and subsequent immobilization onto silica gel. The implications of varying adsorption parameters such as contact time, initial concentration of adsorbate, temperature and pH on both composites were studied. Experimental data obtained from batch adsorption processes were fitted into two equilibrium isotherms (Langmuir and Freundlich) and 3 kinetic models (Pseudo-First-Order, Pseudo-Second-Order, Intra Particle Diffusion). Adsorption mechanism was mainly governed by film diffusion due to electrostatic interactions between the functionalized dendrimer surface and Congo Red molecules. Thermodynamic parameters illustrate that the adsorption is endothermic and spontaneous. Findings suggest the Nanocomposites (G-3PS and G-5PS) are good adsorbents for the removal of Congo Red dye from aqueous solutions.展开更多
This study aimed to present a novel clay/biochar composite adsorption particle, which made from abandoned reed straw and clay to remove ammonia nitrogen(NH4^+-N) from micro-contaminated water. The removal performance ...This study aimed to present a novel clay/biochar composite adsorption particle, which made from abandoned reed straw and clay to remove ammonia nitrogen(NH4^+-N) from micro-contaminated water. The removal performance of NH4^+-N by composite adsorption particle was monitored under different raw material proportions and initial NH4^+-N concentration. Besides, adsorption kinetics and adsorption isotherms were investigated to reveal the adsorption mechanisms. The results showed that NH4^+-N was effectively removed under optimal proportion of biochar, foaming agent and crosslinker with 20%, 3%, and 3%, respectively. The optimal contact time was 150 min and the best removal efficiency was 88.6% at initial NH4^+-N concentration of 20 mg L^-1. The adsorption performance was well described by the second order kinetic model and Freundlich model. The novel clay/biochar composite adsorption particle in this study demonstrated a high potential for NH4^+-N removal from surface water.展开更多
A series of amine-based adsorbents were synthesized using siliceous MCM-41 individually impregnated with four different amines(ethylenediamine(EDA),diethylenetriamine(DETA),tetraethylenepentamine(TEPA) and pent...A series of amine-based adsorbents were synthesized using siliceous MCM-41 individually impregnated with four different amines(ethylenediamine(EDA),diethylenetriamine(DETA),tetraethylenepentamine(TEPA) and pentaethylenehexamine(PEHA)) to study the effect of amine chain length and loading weight on their CO2 adsorption performances in detail.The adsorbents were characterized by FT-IR,elemental analysis,and thermo-gravimetric analysis to confirm their structure properties.Thermo-gravimetric analysis was also used to evaluate the CO2 adsorption performance of adsorbents.Longer chain amine-based materials can achieve higher amine loadings and show better thermal stability.The CO2 adsorption capacities at different temperatures indicate that the CO2 adsorption is thermodynamically controlled over EDAMCM41 and DETA-MCM41,while the adsorption over TEPA-MCM41 and PEHA-MCM41 is under kinetic control at low temperature.The chain length of amines affects the CO2 adsorption performance and the adsorption mechanism significantly.The results also indicate that CO2 adsorption capacity can be enhanced despite of high operation temperatures,if appropriate amines(TEPA and PEHA) are applied.However,adsorbents with short chain amine exhibit higher adsorption and desorption rates due to the collaborative effect of rapid reaction mechanisms of primary amines and less diffusion resistance of shorter chain length amines.展开更多
Pt(Ⅳ) was quantitatively adsorbed by D301R resin in the medium of pH = 3.47. The statically saturated adsorption capacity is 410 mg/g. Pt(Ⅳ) adsorbed on D301R resin can be eluted by 1.0-2.0 mol/L NaOH. The rate ...Pt(Ⅳ) was quantitatively adsorbed by D301R resin in the medium of pH = 3.47. The statically saturated adsorption capacity is 410 mg/g. Pt(Ⅳ) adsorbed on D301R resin can be eluted by 1.0-2.0 mol/L NaOH. The rate constant is k298 = 5.43 × 10^-5 s^-1. The adsorption of Pt(Ⅳ) on D301R resin obeys the Freundlich isotherm. The adsorption parameters of thermodynamics are as follows: enthalpy change AH = 4.37 kJ/mol, Gibbs free energy change AG = -5.39 kJ/mol, and entropy change AS = 32.76 J/(mol.K). The apparent activation energy is Ea = 22.5 kJ/mol. The coordination molar ratio of the functional group of D301R resin to Pt(Ⅳ) is 2:1.展开更多
The separation of ethylene glycol(EG)and 1,2-butanediol(1,2-BDO)azeotrope in the synthesis process of EG via coal and biomass is becoming of increasing commercial and environmental importance.Selective adsorption is d...The separation of ethylene glycol(EG)and 1,2-butanediol(1,2-BDO)azeotrope in the synthesis process of EG via coal and biomass is becoming of increasing commercial and environmental importance.Selective adsorption is deemed as the most promising methods because of energy saving and environment favorable.In this paper,NaY zeolite was used to separate 1,2-BDO from EG,and its adsorption properties was then investigated.The isotherms of EG and 1,2-BDO in vapor and liquid phases from 298 to 328 K indicated that they fitted Langmuir model quite well,and the NaY zeolite absorbent favored EG more than 1,2-BDO.The Grand Canonical Monte Carlo(GCMC)and molecular dynamics(MD)simulation techniques were conducted to investigate the competition adsorption and diffusion characteristics in different adsorption regions.It was observed that EG and 1,2-BDO molecules all have the most probable locations of the center of the 12-membered ring near the Na cations.The diffusivities of EG are lower than those of 1,2-BDO at the same adsorption concentration.At last,the breakthrough curves of the binary mixture regressed from the empirical Dose–Response model in fixed-bed column showed that the adsorption selectivity of EG could reach to as high as 2.43,verified that the NaY zeolite could effectively separate EG from 1,2-BDO.This work is also helpful for further separation of other dihydric alcohol mixtures from coal and biomass fermentation.展开更多
In shale reservoirs,the organic pores with various structures formed during the thermal evolution of organic matter are the main storage site for adsorbed methane.However,in the process of thermal evolution,the adsorp...In shale reservoirs,the organic pores with various structures formed during the thermal evolution of organic matter are the main storage site for adsorbed methane.However,in the process of thermal evolution,the adsorption characteristics of methane in multi type and multi-scale organic matter pores have not been sufficiently studied.In this study,the molecular simulation method was used to study the adsorption characteristics of methane based on the geological conditions of Longmaxi Formation shale reservoir in Sichuan Basin,China.The results show that the characteristics of pore structure will affect the methane adsorption characteristics.The adsorption capacity of slit-pores for methane is much higher than that of cylindrical pores.The groove space inside the pore will change the density distribution of methane molecules in the pore,greatly improve the adsorption capacity of the pore,and increase the pressure sensitivity of the adsorption process.Although the variation of methane adsorption characteristics of different shapes is not consistent with pore size,all pores have the strongest methane adsorption capacity when the pore size is about 2 nm.In addition,the changes of temperature and pressure during the thermal evolution are also important factors to control the methane adsorption characteristics.The pore adsorption capacity first increases and then decreases with the increase of pressure,and increases with the increase of temperature.In the early stage of thermal evolution,pore adsorption capacity is strong and pressure sensitivity is weak;while in the late stage,it is on the contrary.展开更多
基金Supported by Research Foundation of Overseas Chinese Affairs Office,the State Council,P.R.China,and FujianProvincial Science and Technology Creation Foundation for Young Researchers(No.2 0 0 1J0 2 3)
文摘Sieve effect, complexation, ionic exchange, electrostatic interaction, hydrogen bonding, hydrophobic interaction, and molecular recognition based on molecular imprinting are comprehensively discussed.
基金the National Key R&D Program of China(No.2018YFC0311202)the Key-Area Research and Development Program of Guang-dong Province(No.2020B1111030004)+4 种基金the Science and Technology Program of Guangzhou,China(Nos.201804010364 and 201804010321)the Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(No.GML2019ZD0406)the National Key R&D Program of China(No.2018YFC0311202)the Natural Science Foun-dation of Guangdong Province,China(Nos.2018A030313088,2018A030313626)the Academician Work-station Foundation for Young Scientists of Chinese Aca-demy of Sciences Guangzhou Branch(No.20180313).
文摘In this study,seven coal-based activated carbons(ACs)were adopted to remove trimethylamine(TMA)in an aqueous solution as environmentally friendly and harmless adsorbents.The results showed that columnar AC(CAC)had a clear scale and honeycomb structures with few fragments and micropores,contributing to superior TMA removal capacity compared to granular AC(GAC)(71.67%for 6.0 mm CAC and 69.92%for 40–60 mesh GAC).In addition,the process of adsorption was accompanied by desorption,and the recommended absorbed time was 120–180 min.The short time to achieve equilibrium indicated that adsorption was kinetically controlled,and pseudo-second-order kinetics was more appropriate than pseudo-first-order kinetics in explaining the adsorption mechanism in both water and oyster enzymatic hydrolysate.The intraparticle diffusion model presented that the adsorption processes could be divided into three steps for GAC and two steps for CAC.The adsorption processes were consistent with the Freundlich model,indicating the existence of physisorption and chemisorption as multilayer adsorption.The results indicated that AC,especially CAC,has great potential for TMA elimination in aquatic product processing.
基金Supported by the Innovative Talent Funds for Project 985 under Grant No WLYJSBJRCTD201102the Fundamental Research Funds for the Central Universities under Grant No CQDXWL-2013-014+1 种基金the Natural Science Foundation of Chongqing under Grant No CSTC2006BB5240the Program for New Century Excellent Talents in Universities of China under Grant No NCET-07-0903
文摘Support vector regression (SVR) combined with particle swarm optimization for its parameter optimization is employed to establish a model for predicting the Henry constants of multi-walled carbon nanotubes (MWNTs) for adsorption of volatile organic compounds (VOCs). The prediction performance of SVR is compared with those of the model of theoretical linear salvation energy relationship (TLSER). By using leave-one-out cross validation of SVR test Henry constants for adsorption of 35 VOCs on MWNTs, the root mean square error is 0.080, the mean absolute percentage error is only 1.19~, and the correlation coefficient (R2) is as high as 0.997. Compared with the results of the TLSER model, it is shown that the estimated errors by SVR are ali smaller than those achieved by TLSER. It reveals that the generalization ability of SVR is superior to that of the TLSER model Meanwhile, multifactor analysis is adopted for investigation of the influences of each molecular structure descriptor on the Henry constants. According to the TLSER model, the adsorption mechanism of adsorption of carbon nanotubes of VOCs is mainly a result of van der Waals and interactions of hydrogen bonds. These can provide the theoretical support for the application of carbon nanotube adsorption of VOCs and can make up for the lack of experimental data.
基金supported by the Natural Science Foundation of China under Grant(No.52172099)the Provincial Joint Fund of Shaanxi(2021JLM-28).
文摘The large accumulation of coal gangue,a common industrial solid waste,causes severe environmental problems,and green development strategies are required to transform this waste into high-value-added products.In this study,low-cost ceramsites adsorbents were prepared from waste gangue,silt coal,and peanut shells and applied to remove the organic dye methylene blue from wastewater.We investigated the microstructure of ceramsites and the effects of the sintering atmosphere,sintering temperature,and solution pH on their adsorption performance.The ceramsites sintered at 800℃under a nitrogen atmosphere exhibited the largest three-dimensional-interconnected hierarchical porous structure among the prepared ceramsites;further,it exhibited the highest methylene blue adsorption performance,with an adsorption capacity of 0.954 mg·g^(−1),adsorption efficiency of over 95%,and adsorption equilibrium time of 1 h at a solution pH of 9.The removal efficiency remained greater than 75%after five adsorption cycles.The adsorption kinetics data were analyzed using various models,including the pseudosecond-order kinetic model and Langmuir equation,and the adsorption was attributed to electrostatic interactions between the dyes and ceramsites,n-interactions,and hydrogen bonds.The prepared coal gangue ceramsites exhibited excellent adsorption capacities,removal rates,and cyclic stabilities,demonstrating their promising application prospects for the comprehensive utilization of solid waste and for wastewater treatment.
基金This work was supported by the Natural Science Foundation of the Jiangxi Province,China(No.20202BABL203004)Opening Project of the State Key Laboratory of Nuclear Resources and Environment(East China University of Technology)(No.2022NRE23)Opening Project of the Jiangxi Province Key Laboratory of Polymer Micro/Nano Manufacturing and Devices(No.PMND202101).
文摘To explore the kinetic adsorption under continuous and nonequilibrium states, an integration of continuous measurement and adsorption platform kinetics method was proposed, which was initially called the ICM-AP kinetics method, and a corresponding kinetic adsorption experimental method was developed. Adsorption experiments of europium(Eu) on Ca-bentonite,Na-bentonite, and the D231 cation exchange resin were performed using the ICM-AP kinetics method and continuous measurements. Because the kinetic experimental results observed in this study were different from those of traditional batch adsorption data, pseudo-first-order or pseudo-second-order kinetic models were unsuitable for fitting the experimental data.Hence, a liquid membrane diffusion(LMD) model was developed based on the assumption of simultaneous adsorption/desorption to discuss the mechanism of kinetic adsorption. The kinetic adsorption mechanism was also studied by using XPS.The results indicated that the proposed adsorption model can fit the experimental data more suitably, and the adsorption/desorption behaviors of Eu on bentonite and the D231 resin were simultaneously observed, suggesting that the adsorption kinetics of Eu(Ⅲ) was mainly dominated by hydrated Eu(Ⅲ) ions on the liquid membrane.
基金the support by National Natural Science Foundation of China under grants (11202006)University’s Science and technology exploiture of Shangxi Province (20121010)the National Basic Research Program of China (G2010CB832701)
文摘Polyvinylpyrrolidone-reduced graphene oxide was prepared by modified hummers method and was used as adsorbent for removing Cu ions from wastewater. The effects of contact time and ions concentration on adsorption capacity were examined. The maximum adsorption capacity of 1689 mg/g was observed at an initial p H value of 3.5 after agitating for 10 min. It was demonstrated that polyvinylpyrrolidone-reduced graphene oxide had a huge adsorption capacity for Cu ions, which was 10 times higher than maximal value reported in previous works. The adsorption mechanism was also discussed by density functional theory. It demonstrates that Cu ions are attracted to surface of reduced graphene oxide by C atoms in reduced graphene oxide modified by polyvinylpyrrolidone through physisorption processes, which may be responsible for the higher adsorption capacity. Our results suggest that polyvinylpyrrolidone-reduced graphene oxide is an effective adsorbent for removing Cu ions in wastewater. It also provides a new way to improve the adsorption capacity of reduced graphene oxide for dealing with the heavy metal ion in wastewater.
文摘Carbonate shells have an astonishing ability in the removal of Cd^2+ in a short time period with emphasis on being a low cost adsorbent. In the present study, the sorption capacity of carbonate shells was studied for Cd^2+ in batch experiments. The influence of different carbonate shell sizes and physico-chemical factors were evaluated and the results were analyzed for its correlation matrices by using Predictive Analytics Software (PASW). The miner- alogy state of aqueous solution regarding the saturation index was simulated using PHREEQC to identify the Cd^2+ uptake mechanism. The Cd uptake rates were calculated as well as Ca^2+, HCO3- concentration, pH, ambient humidity and temperature were measured. Cd2+ removal of 91.52% was achieved after 5 h adsorption. The adsorption efficiencies were significantly influenced by pH as they increased with the increase of pH from acidic solution (5.50±0.02) to slightly alkaline (7.60±0.05). In addition, the mineralogy state of aqueous solution calculated from PHREEQC confirmed that the increment of Ca^2+ and HCO3- concentrations in solution was attributed to the dissolution of carbonate shells. Moreover, the ion exchange adsorption mechanism of Cd^2+ toward Ca^2+ was identified as the process involved in Cd^2+ uptake.
基金the Hubei Provincial Department of Education Science and Technology Research Program Young Talent Project(Q20201102)the National Natural Science Foundation of China(51864042 and 51804220).
文摘Mercury(Hg)ions can lead to a serious impact on the environment;therefore,it was necessary to find an effective method for absorbing these toxic Hg ions.Here,the adsorbent(Zn-AHMT)was synthesized from zinc nitrate and 4-amino 3-hydrazine-5 mercapto-1,2,4-triazole(AHMT)by one-step method and,characterized the microstruc-ture and absorption performance by fourier transform infrared spectroscopy(FTIR),field emission scanning electron microscopy(FESEM),X-ray diffraction(XRD),Brunauer-Emmett Teller(BET),Thermal Gravimetric Analyzer(TGA)and X-ray photoelectron spectroscopy(XPS).Through a plethora of measurements,we found that the maximum adsorption capacity was 802.8 mg/g when the optimal pH of Zn-AHMT was 3.0.The isothermal and kinetic experiments confirm that the reaction process of Zn-AHMT was chemisorption,while the adsorption process conforms to the Hill model and pseudo second order kinetic model.Thermodynamic experiments showed that the adsorption process was spontaneous and exothermic.Selective experiments were performed in the simulated wastewater containing Mn,Mg,Cr,Al,Co,Ni,Hg ions.Our results showed that the Zn-AHMT has a stronger affinity for Hg ions.The removal rate of Zn-AHMT remained above 98%,indicating that the Zn-AHMT had a good stability validated by three adsorption-desorption repeatable tests.According to the XPS results,the adsorption reaction of Zn-AHMT was mainly attributed to the chelation and ion exchange.This was further explained by both density functional theory(DFT)calculation and frontier molecular orbital theory.We therefore propose the adsorption mechanism of Zn-AHMT.The adsorption reaction facilitates via the synergistic action of S and N atoms.Moreover,the bonding between the adsorbent and the N atom has been proved to be more stable.Our study demonstrated that Zn-AHMT had a promising application prospect in mercury removal.
基金funding from Evoqua Companythe National Natural Science Foundation of China (Nos. 51878090 and 51808066)the Chinese Scholarship Council for financial support。
文摘When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PFOA) from groundwater. With favorable tailoring, QAE-AC removed PFOA from groundwater for 118,000 bed volumes before halfbreakthrough in rapid small scale column tests, while the influent PFOA concentration was 200 ng/L. The tailoring involved pre-dosing QAE at an array of proportions onto this carbon, and then monitoring bed life for PFOA removal. When pre-dosing with 1 mL QAE, this PFOA bed life reached an interim peak, whereas bed life was less following 3 mL QAE pre-dosing, then PFOA bed life exhibited a steady rise for yet subsequently higher QAE pre-dosing levels. Large-scale atomistic modelling was used herein to provide new insight into the mechanism of PFOA removal by QAE-AC. Based on experimental results and modelling, the authors perceived that the QAE's epoxide functionalities cross-linked with phenolics that were present along the activated carbon's graphene edge sites, in a manner that created mesopores within macroporous regions or created micropores within mesopores regions. Also, the QAE could react with hydroxyls outside of these pore, including the hydroxyls of both graphene edge sites and other QAE molecules. This latter reaction formed new pore-like structures that were external to the activated carbon grains. Adsorption of PFOA could occur via either charge balance between negatively charged PFOA with positively charged QAE, or by van der Waals forces between PFOA's fluoro-carbon tail and the graphene or QAE carbon surfaces.
基金Funded by the Science and Technology-oriented Mid and Small-scale Enterprises Innovational Foundation of Ministry of Science and Technology of China(11C26216406395)
文摘The nanowires-reticulated calcium silicate with a specific surface area more than 100 m^2/g was prepared by a hydrothermalprocess using hydrated lime(Ca(OH)_2,HL)and silica containing soluble fluoride,which was a by-product of fluorine industry,and the soluble fluoride in raw silica was fixed as CaSiF_6 at the same time.The kinetic characteristics and mechanism of adsorbing phosphate by fluorine-containing calcium silicate were investigated in the experiments of phosphorus(P)removalfrom aqueous solution.The results show that the prepared fluorine-containing calcium silicate has excellent performance for adsorbing phosphate,the adsorption process appears to follow pseudo-second-order reaction kinetics and the process is mainly controlled by chemisorption.The product resulted from P adsorption is mainly composed of hydroxyapatite(HAP)and fluorapatite(FAP),which are further used as adsorbents of heavy metalion Cd^(2+) in aqueous solution and display excellent performance.
基金the National Natural Science Foundation of China(21822810,21838011)the National Key Research and Development Program(2018YFC1902603).
文摘Competition of hydrocarbon compounds with sulfides in gasoline has caused a not very high selectivity of sulfides in adsorption desulfurization so far,resulting in a reduction of catalyst lifetime as well as more sulfur oxide emissions.Tostudy the whole competitive process changing with the increase of the loading,the dynamic competition adsorption mechanism of cyclohexene and thiophene in siliceous faujasite(FAU)zeolite was analyzed by the Monte Carlo simulation.The results showed that with the increase of the loading,thiophene and cyclohexene had different performances before and after the inflection point of 40 molecule/UC.The adsorbates were distributed ideally at optimal sites during the stage that occurred before the inflection point,which is called the“optimal-displacement adsorption”stage.When approaching the inflection point,the competition became apparent and the displacement appeared accordingly,some thiophene molecules at S sites(refers to the sites inside the supercages)were displaced by cyclohexene.After the inflection point,the concentration of adsorbates at W sites(refers to the 12-membered ring connecting the supercages)was significantly reduced,whereas the adsorbates at S sites got more concentrated.The stage some cyclohexene molecules displaced by thiophene and inserted into the center of the supercage can be named as the“insertion-displacement adsorption”stage,and both the adsorption behavior and the competitive relationship became localized when the adsorption amount became saturated.This shift in the competitive adsorption mechanism was due to the sharp increase of interaction energy between the adsorbates.Besides,the increase in temperature and ratio of Si/Al will allow the adsorbates,especially thiophene molecules to occupy more adsorption sites,and it is beneficial to improve the desulfurization selectivity.
基金the National Key R&D Program of China(No.2021YFC2900800)National Natural Science Foundation of China(Nos.51922091,51874247 and 52204285)+1 种基金Sichuan Science and Technology Program(Nos.2023NSFSC1978 and 2022YFS0455)Open Foundation of State Key Laboratory of Mineral Processing(No.BGRIMM-KJSKL-2023-05).
文摘Rare earth element is an important strategic metal,but the supply of high purity rare earth ores is growing slowly,which is in sharp contradiction with the rapidly growing demand.Froth flotation has been confirmed to be an effective method to separate bastnaesite from its gangue minerls.However,the traditional collectors are facing serious problems in flotation separation of minerals,requiring the addition of excess depressant and regulator in the flotation process.Herein,we proposed and synthesized novel Gemini hydroxamic acids Octyl-bishydroxamic acid(OTBHA),Decyl-bishydroxamic acid(DCBHA)and Dodecyl-bishydroxamic acid(DDBHA)as the collectors in bastnaesite-barite flotation system.The effect of different carbon chain lengths on the molecular properties were explored by density functional theory(DFT)calculations.DCBHA possessed a stronger reactivity compared with OCBHA and DDBHA.The flotation results verified the consistency of the computational calculation about the performance prediction of Gemini hydroxamic acids.Compared with OCBHA and DDBHA,DCBHA displayed superior collecting affinity toward bastnaesite,and did not float barite.Zeta potential results showed that the presence of DCBHA increased the potential of bastnaesite,while it had almost no effect on barite,indicating DCBHA had a stronger affinity for bastnaesite.Then,Fourier transform infrared(FTIR)and X-ray photoelectron spectroscopy(XPS)analyses indicated that the adsorption mechanism was due to two hydroxamate groups of DCBHA co-anchored on bastnaesite surface by forming five-membered hydroxamic―(O―O)―Ce complexes.In addition,atomic force microscopy(AFM)clearly observed that DCBHA uniformly aggregated on bastnaesite surface,which increased surface contact angle and improved the hydrophobicity of bastnaesite.
文摘The adsorption behaviors and mechanism of a novel chelate resin, macroporous phosphonic acid resin(PAR)for Gd(Ⅲ)were investigated. The statically and dynamically saturated adsorption capacity is respectively 308 mg·g^(-1)resin and 296 mg·g^(-1)resin at 298 K in HAc-NaAc medium at pH 5.6. Gd(Ⅲ)adsorbed on PAR can be reductively eluted by 0.5~5.0 mol·L^(-1) HCl used as eluant and the elution percentage is up to 94.7% in 1.0 mol·L^(-1) HCl. The resin can be regenerated and reused without apparent decrease in adsorption capacity. The apparent adsorption rate constant is k_(298)=3.96×10^(-5) s^(-1). The adsorption behavior of PAR for Gd(Ⅲ) conforms to the Freundlich isotherm. The thermodynamic adsorption parameter, enthalpy change △H of PAR for Gd(Ⅲ)is 22.6kJ·mol^(-1). The apparent adsorption activation energy(Ea)of PAR for Gd(Ⅲ)is 5.0 kJ·mol^(-1). The molar coordination ratio of the functional group of PAR to Gd(Ⅲ)is about 3∶1. The adsorption mechanism of PAR for Gd(Ⅲ)was examined by using chemical method and IR spectrometry.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(Grant No.LQ19E030017)the Research Start-up Fund(Grant No.KYS205619042)the Technological Research Project for Public Welfare of Zhejiang Province(Grant No.LGG19E030005).
文摘Lignocellulose has the potential to become a bio-based adsorbent due to its biodegradability and renewability.In this study,a novel polydopamine functionalized-lignin(lignin@PDA),prepared via self-polymerization of dopamine(PDA)on lignin,was used as a bio-based adsorbent for rapid scavenging of hexavalent chromium(Cr(VI)).The morphology,functional groups,crystalline structure,and chemical composition of lignin@PDA were characterized with a scanning electron microscope-energy dispersive spectrometer,Fourier transform infrared spectroscopy,X-ray diffraction,and X-ray photoelectron spectroscopy.The Cr(VI)adsorption process of lignin@PDA was studied using batch experiments as a function of pH,ionic strength,adsorbent dose,and contact time at room temperature.The adsorption rate of lignin@PDA was five times greater than that of the unmodified lignin,with a maximum adsorption capacity of 102.6 mg/g in an acidic medium.The adsorption of Cr(VI)on lignin@PDA fit the pseudo-secondorder equation and the Freundlich model,indicating that the adsorption process was mainly dominated by chemisorption and surface complexation.The thermodynamic parameters showed that adsorption of Cr(VI)on lignin@PDA was an endothermic and spontaneous process.The X-ray absorption fine structure results showed that sorption and reduction of Cr(VI)into Cr(II)occurred simultaneously on lignin.Moreover,PDA coating not only improved the reactivity of lignin but also promoted the complete reduction of Cr(VI)by lignin.According to these results,polydopamine functionalized-lignin is a promising bio-based adsorbent for immobilization of Cr(VI)from wastewater.
文摘This study investigates the removal of Congo Red dye from aqueous solution using functionalized generation 3.0 and 5.0 polyamidoamine dendrimer-silica gel composite (G-3PS, G-5PS). Fourier Transform-Infra Red spectroscopy, Brunauer Emmett and Teller, Thermo Gravimetric Analysis, pH at point of zero charge, and scanning electron microscopy measurements have been applied to characterize the synthetic nanohybrid composite, these techniques revealed the successful functionalization of both dendrimer molecules and subsequent immobilization onto silica gel. The implications of varying adsorption parameters such as contact time, initial concentration of adsorbate, temperature and pH on both composites were studied. Experimental data obtained from batch adsorption processes were fitted into two equilibrium isotherms (Langmuir and Freundlich) and 3 kinetic models (Pseudo-First-Order, Pseudo-Second-Order, Intra Particle Diffusion). Adsorption mechanism was mainly governed by film diffusion due to electrostatic interactions between the functionalized dendrimer surface and Congo Red molecules. Thermodynamic parameters illustrate that the adsorption is endothermic and spontaneous. Findings suggest the Nanocomposites (G-3PS and G-5PS) are good adsorbents for the removal of Congo Red dye from aqueous solutions.
基金supported by the National Major Project of Water Pollution Control and Management Technology in China (No.2013ZX07202-007)the Shenzhen Science and Technology Project (No.GRCK2017042116092660)the National Natural Science Foundation of China (No.51308066)。
文摘This study aimed to present a novel clay/biochar composite adsorption particle, which made from abandoned reed straw and clay to remove ammonia nitrogen(NH4^+-N) from micro-contaminated water. The removal performance of NH4^+-N by composite adsorption particle was monitored under different raw material proportions and initial NH4^+-N concentration. Besides, adsorption kinetics and adsorption isotherms were investigated to reveal the adsorption mechanisms. The results showed that NH4^+-N was effectively removed under optimal proportion of biochar, foaming agent and crosslinker with 20%, 3%, and 3%, respectively. The optimal contact time was 150 min and the best removal efficiency was 88.6% at initial NH4^+-N concentration of 20 mg L^-1. The adsorption performance was well described by the second order kinetic model and Freundlich model. The novel clay/biochar composite adsorption particle in this study demonstrated a high potential for NH4^+-N removal from surface water.
基金supported by the National Natural Science Foundation of China(91434120)the Fundamental Research Funds for the Central Universities(2014ZD06),and the 111 Project(No.B12034)
文摘A series of amine-based adsorbents were synthesized using siliceous MCM-41 individually impregnated with four different amines(ethylenediamine(EDA),diethylenetriamine(DETA),tetraethylenepentamine(TEPA) and pentaethylenehexamine(PEHA)) to study the effect of amine chain length and loading weight on their CO2 adsorption performances in detail.The adsorbents were characterized by FT-IR,elemental analysis,and thermo-gravimetric analysis to confirm their structure properties.Thermo-gravimetric analysis was also used to evaluate the CO2 adsorption performance of adsorbents.Longer chain amine-based materials can achieve higher amine loadings and show better thermal stability.The CO2 adsorption capacities at different temperatures indicate that the CO2 adsorption is thermodynamically controlled over EDAMCM41 and DETA-MCM41,while the adsorption over TEPA-MCM41 and PEHA-MCM41 is under kinetic control at low temperature.The chain length of amines affects the CO2 adsorption performance and the adsorption mechanism significantly.The results also indicate that CO2 adsorption capacity can be enhanced despite of high operation temperatures,if appropriate amines(TEPA and PEHA) are applied.However,adsorbents with short chain amine exhibit higher adsorption and desorption rates due to the collaborative effect of rapid reaction mechanisms of primary amines and less diffusion resistance of shorter chain length amines.
基金This project was financially supported by the Natural Science Foundation of Zhejiang Province, China (No. 200072).
文摘Pt(Ⅳ) was quantitatively adsorbed by D301R resin in the medium of pH = 3.47. The statically saturated adsorption capacity is 410 mg/g. Pt(Ⅳ) adsorbed on D301R resin can be eluted by 1.0-2.0 mol/L NaOH. The rate constant is k298 = 5.43 × 10^-5 s^-1. The adsorption of Pt(Ⅳ) on D301R resin obeys the Freundlich isotherm. The adsorption parameters of thermodynamics are as follows: enthalpy change AH = 4.37 kJ/mol, Gibbs free energy change AG = -5.39 kJ/mol, and entropy change AS = 32.76 J/(mol.K). The apparent activation energy is Ea = 22.5 kJ/mol. The coordination molar ratio of the functional group of D301R resin to Pt(Ⅳ) is 2:1.
基金the National Natural Science Foundation of China(21576272)“Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of Chinese Academy of Sciences,Grant No.XDA 21030600,Science and Technology Service Network Initiative,Chinese Academy of Sciences(KFJ-STS-QYZD-138).
文摘The separation of ethylene glycol(EG)and 1,2-butanediol(1,2-BDO)azeotrope in the synthesis process of EG via coal and biomass is becoming of increasing commercial and environmental importance.Selective adsorption is deemed as the most promising methods because of energy saving and environment favorable.In this paper,NaY zeolite was used to separate 1,2-BDO from EG,and its adsorption properties was then investigated.The isotherms of EG and 1,2-BDO in vapor and liquid phases from 298 to 328 K indicated that they fitted Langmuir model quite well,and the NaY zeolite absorbent favored EG more than 1,2-BDO.The Grand Canonical Monte Carlo(GCMC)and molecular dynamics(MD)simulation techniques were conducted to investigate the competition adsorption and diffusion characteristics in different adsorption regions.It was observed that EG and 1,2-BDO molecules all have the most probable locations of the center of the 12-membered ring near the Na cations.The diffusivities of EG are lower than those of 1,2-BDO at the same adsorption concentration.At last,the breakthrough curves of the binary mixture regressed from the empirical Dose–Response model in fixed-bed column showed that the adsorption selectivity of EG could reach to as high as 2.43,verified that the NaY zeolite could effectively separate EG from 1,2-BDO.This work is also helpful for further separation of other dihydric alcohol mixtures from coal and biomass fermentation.
基金This work was supported by the National Natural Science Foundation of China(Nos.41772141,41972171)the Natural Science Foundation of Jiangsu Province(BK20181362),the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘In shale reservoirs,the organic pores with various structures formed during the thermal evolution of organic matter are the main storage site for adsorbed methane.However,in the process of thermal evolution,the adsorption characteristics of methane in multi type and multi-scale organic matter pores have not been sufficiently studied.In this study,the molecular simulation method was used to study the adsorption characteristics of methane based on the geological conditions of Longmaxi Formation shale reservoir in Sichuan Basin,China.The results show that the characteristics of pore structure will affect the methane adsorption characteristics.The adsorption capacity of slit-pores for methane is much higher than that of cylindrical pores.The groove space inside the pore will change the density distribution of methane molecules in the pore,greatly improve the adsorption capacity of the pore,and increase the pressure sensitivity of the adsorption process.Although the variation of methane adsorption characteristics of different shapes is not consistent with pore size,all pores have the strongest methane adsorption capacity when the pore size is about 2 nm.In addition,the changes of temperature and pressure during the thermal evolution are also important factors to control the methane adsorption characteristics.The pore adsorption capacity first increases and then decreases with the increase of pressure,and increases with the increase of temperature.In the early stage of thermal evolution,pore adsorption capacity is strong and pressure sensitivity is weak;while in the late stage,it is on the contrary.