Machine learning combined with density functional theory(DFT)enables rapid exploration of catalyst descriptors space such as adsorption energy,facilitating rapid and effective catalyst screening.However,there is still...Machine learning combined with density functional theory(DFT)enables rapid exploration of catalyst descriptors space such as adsorption energy,facilitating rapid and effective catalyst screening.However,there is still a lack of models for predicting adsorption energies on oxides,due to the complexity of elemental species and the ambiguous coordination environment.This work proposes an active learning workflow(LeNN)founded on local electronic transfer features(e)and the principle of coordinate rotation invariance.By accurately characterizing the electron transfer to adsorption site atoms and their surrounding geometric structures,LeNN mitigates abrupt feature changes due to different element types and clarifies coordination environments.As a result,it enables the prediction of^(*)H adsorption energy on binary oxide surfaces with a mean absolute error(MAE)below 0.18 eV.Moreover,we incorporate local coverage(θ_(l))and leverage neutral network ensemble to establish an active learning workflow,attaining a prediction MAE below 0.2 eV for 5419 multi-^(*)H adsorption structures.These findings validate the universality and capability of the proposed features in predicting^(*)H adsorption energy on binary oxide surfaces.展开更多
It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity...It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity gases such as H_(2)S that might impact CO_(2) sequestration due to competitive adsorption.This study makes a commendable effort to explore the adsorption behavior of CO_(2)/H_(2)S mixtures in calcite slit nanopores.Grand Canonical Monte Carlo(GCMC)simulation is employed to reveal the adsorption of CO_(2),H_(2)S as well as their binary mixtures in calcite nanopores.Results show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO_(2) and H_(2)S in calcite nanopores,respectively.CO_(2)exhibits stronger adsorption on calcite surface than H_(2)S.Electrostatic energy plays the dominating role in the adsorption behavior.Electrostatic energy accounts for 97.11%of the CO_(2)-calcite interaction energy and 56.33%of the H_(2)S-calcite interaction energy at 10 MPa and 323.15 K.The presence of H_(2)S inhibits the CO_(2) adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H_(2)S leads to less CO_(2) adsorption.The quantity of CO_(2) adsorbed is lessened by approximately 33%when the mole fraction of H_(2)S reaches 0.25.CO_(2) molecules preferentially occupy the regions near the po re wall and H_(2)S molecules tend to reside at the center of nanopore even when the molar ratio of CO_(2) is low,indicating that CO_(2) has an adsorption priority on the calcite surface over H_(2)S.In addition,moisture can weaken the adsorption of both CO_(2) and H_(2)S,while CO_(2) is more affected.More interestingly,we find that pure CO_(2) is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO_(2)with H_(2)S impurity should be settled in the deeper reservoirs.展开更多
This paper investigates the bioseparation of binary protein mixtures using polystyrene based anion exchange resin. Adsorption experiments were conducted in batch mode using draft-tube internally recirculate dair lift ...This paper investigates the bioseparation of binary protein mixtures using polystyrene based anion exchange resin. Adsorption experiments were conducted in batch mode using draft-tube internally recirculate dair lift biocontactor in comparison with the conventional shake flask batch adsorption equilibrium experiments. Binary protein mixtures contained bovine serum albumin (BSA) and bovine haemoglobin (BHb) at different initial fractions. Results from single solute adsorption experiments in biocontactor showed that both proteins were equally adsorbed onto the resin with equilibrium reached in an equal time period. This represents similar affinities towards the negatively charged resin surface, although BSA was expected to adsorb through specific forces. Adsorption results showed that BSA has hindered the BHb adsorption in the biocontactor, although adsorption of both proteins was equally hindered in the shake flasks adsorption experiments. Moreover, adsorption of BHb was inhibited up to 29% in the presence of BSA compared to the adsorption of BHb from a solution containing single solute of BHb at the same initial concentration. Similarly, the presence of BHb has hindered the adsorption of BSA by 59%. Adsorptions of both BSA and BHb from binary solution when each formed 75% initial fraction while the other protein formed the remaining 25% were relatively low with equilibrium reached in shorter time. Moreover, considerable amount of proteins remained in the solution, which demonstrates that multilayer adsorption most likely didn’t occur at the relatively small protein concentrations used in the present study. In general, the higher adsorption of BHb can also be related to the compressibility of its molecules which allowed for higher adsorption capacity. The homogeneous and lower shear environment in the airlift biocontactor compared to the other conventional batch adsorption in shake flask reduced the compressibility of BHb that caused higher BSA adsorption from binary solutions of BSA and BHb, which allowed for better bioseparation of both proteins.展开更多
Adsorption-desorption experiments on CO2-CH4 gas mixtures with varying compositions have been conducted to study the fractionation characteristics of CO2-CH4 on Haishiwan coal samples. These were carried out at consta...Adsorption-desorption experiments on CO2-CH4 gas mixtures with varying compositions have been conducted to study the fractionation characteristics of CO2-CH4 on Haishiwan coal samples. These were carried out at constant temperature but different equilibrium pressure conditions. Based on these experimental results, the temporal evolution of component fractionation in the field was investigated. The results show that the CO2 concentration in the adsorbed phase is always greater than that in the original gas mixture during the desorption process, while CH4 shows the opposite characteristics. This has confirmed that CO2 , with a greater adsorption ability has a predominant position in the competition with CH4 under different pressures. Where gas drainage is employed, the ratio of CO2 to CH4 varies with time and space in floor roadways used for gas drainage, and in the ventilation air in Nos.1 and 2 coal seams, which is consistent with laboratory results.展开更多
Single and binary adsorption behaviors of salicylic acid and 5-sulfosalicylic acid onto hypercrosslinked polymeric adsorbents,i.e.NDA-101 and NDA-99 were investigated.The Freundlich model can successfully describe all...Single and binary adsorption behaviors of salicylic acid and 5-sulfosalicylic acid onto hypercrosslinked polymeric adsorbents,i.e.NDA-101 and NDA-99 were investigated.The Freundlich model can successfully describe all the adsorption isotherms tested,which indicates a favorable and exothermic adsorption process.The adsorption of salicylic acid relies on π-π interaction,while the electrostatic interaction further influences the adsorption of 5-sulfosalicylic acid onto NDA-99.The adsorptive capacity of salicylic acid on NDA-99 decreases but increases on NDA-101 with 5-sulfosalicylic acid as the background component in a binary solute system.The amount of 5-sulfosalicylic acid adsorbed was decreased with the increase in initial concentration of salicylic acid on both adsorbents.The competition for the adsorption sites is considered to be predominant in the solid-to-liquid interaction process.The adsorption selectivity of salicylic acid onto NDA-101 is higher than onto NDA-99 by more than an order of magnitude.Thus,combination technique involving NDA-101 followed by NDA-99 can be effectively applied to separate and recover salicylic acid and 5-sulfosalicylic acid from wastewater.展开更多
The dynamic competitive adsorption behaviors of different binary organic vapor mixtures on ACF-Ps under different operation conditions were investigated by gas chromatography in this paper. The studied mixtures includ...The dynamic competitive adsorption behaviors of different binary organic vapor mixtures on ACF-Ps under different operation conditions were investigated by gas chromatography in this paper. The studied mixtures included benzene/toluene, toluene/xylene, benzene/isopropylbenzene, ethyl acetate/toluene and benzene/ethyl acetate. Experimental results show that various ACF-Ps, as with ACF-W, can remove both vapors in binary vapor mixtures with over 99% of removal efficiency before the breakthrough point of the more weakly adsorbed vapor. In dynamic competitive adsorption, the more weakly adsorbed vapor not only penetrates early, but also will be displaced and desorbed consequently by stronger adsorbate and therefore produces a rolling up in the breakthrough curve. The ACF-Ps prepared at different temperatures have somewhat different adsorption selectivity. The feed concentration ratio of vapors, the length/diameter ratio and the thick of bed have effect on competitive adsorption. The competitive adsorption ability of a vapor is mainly related to its boiling point. Usually, the higher the boiling point, the stronger the vapor adsorbed on ACF-P.展开更多
The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging research.The great similarity in the molecular size of C_(2)H_(4)and C...The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging research.The great similarity in the molecular size of C_(2)H_(4)and C_(2)H_(6)brings challenges to the regulation of adsorbents to realize efficient dynamic separation.Herein,we reported the enhancement of the kinetic separation of C_(2)H_(4)/C_(2)H_(6)by controlling the crystal size of ZnAtzPO_(4)(Atz=3-amino-1,2,4-triazole)to amplify the diffusion difference of C_(2)H_(4)and C_(2)H_(6).Through adjusting the synthesis temperature,reactant concentration,and ligands/metal ions molar ratio,ZnAtzPO4 crystals with different sizes were obtained.Both single-component kinetic adsorption tests and binary-component dynamic breakthrough experiments confirmed the enhancement of the dynamic separation of C_(2)H_(4)/C_(2)H_(6)with the increase in the crystal size of ZnAtzPO_(4).The separation selectivity of C_(2)H_(4)/C_(2)H_(6)increased from 1.3 to 98.5 with the increase in the crystal size of ZnAtzPO_(4).This work demonstrated the role of morphology and size control of adsorbent crystals in the improvement of the C_(2)H_(4)/C_(2)H_(6)kinetic separation performance.展开更多
Considering the different geochemical enrichment behaviors of W and Mo,Fe?Mn binary oxide(FMBO),ferric hydroxide(Fe(OH)3)and manganese dioxide(MnO2)were studied to separate W from molybdate solution,respectively.The e...Considering the different geochemical enrichment behaviors of W and Mo,Fe?Mn binary oxide(FMBO),ferric hydroxide(Fe(OH)3)and manganese dioxide(MnO2)were studied to separate W from molybdate solution,respectively.The experimental results demonstrated that Fe?Mn binary oxide(FMBO)was the most suitable adsorbent for the separation.Under a wide pH(6.9?11.3)region,more than80%W removal efficiency and less than3%Mo loss could be obtained.In addition,the Fe?Mn binary oxide adsorbent can be regenerated by treating with3mol/L NaOH,and the W adsorption efficiency was retained after five adsorption?desorption?regeneration cycles.All these indicate that the Fe?Mn binary oxides have the potential for the separation of W from molybdate solution.展开更多
The adsorption potential of FMBO, FeOOH, MnO2 for the removal of Cd^2＋, Cu^2＋ and Pb^2＋ in aqueous systems was investigated in this study. Comparing to FMBO and FeOOH, MnO2 offered a much higher removal capacity to...The adsorption potential of FMBO, FeOOH, MnO2 for the removal of Cd^2＋, Cu^2＋ and Pb^2＋ in aqueous systems was investigated in this study. Comparing to FMBO and FeOOH, MnO2 offered a much higher removal capacity towards the three metal ions. The maximal adsorption capacity of MnO2 for Cd^2＋, Cu^2＋ and Pb^2＋ were 1.23, 2.25 and 2.60 mmol· g^-1, respectively. And that for FMBO were 0.37, 1.13, and 1.18mmol·g^-1 and for FeOOH were 0.11, 0.86 and 0.48 mmol·g^-1, respectively. The adsorption behaviors of the three metal ions on the three adsorbents were all significantly affected by pH values and heavy metal removal efficiency increased with pH increased. The Langmuir and Freundlieh adsorption models were used to describe the adsorption equilibrium of the three metal ions onto the three adsorbents. Results showed that the adsorption equilibrium data fitted well to Langmuir isotherm and this indicated that adsorption of metal ions occurred on the three metal oxides adsorbents limited to the formation of a monolayer. More negative charged of MnOa surface than that of FMBO and FeOOH could be ascribed by lower pHiep of MnO2 than that of FMBO and FeOOH and this could contribute to more binding sites on MnO2 surface than that of FMBO and FeOOH. The higher metal ions uptake by MnO2 than FMBO and FeOOH could be well explained by the surface charge mechanism.展开更多
The adsorptive removal of arsenic by synthetically-prepared nano Fe-Mn binary oxides（FM） was investigated. A novel method using potassium permanganate and ferric chloride as raw materials was used to synthesise FM. ...The adsorptive removal of arsenic by synthetically-prepared nano Fe-Mn binary oxides（FM） was investigated. A novel method using potassium permanganate and ferric chloride as raw materials was used to synthesise FM. The molar ratio of Fe and Mn in the synthetic Fe-Mn binary oxides was 4 ： 3. The FM-1 and FM-2（prepared at different activation temperatures） having high specific surface areas（358.87 and 128.58 m^2/g, respectively） were amorphous and of nano particle types. The amount of arsenic adsorbed on FM-1 was higher than that adsorbed on FM-2 particles. After adsorption by FM-1, residual arsenic concentration decreased to less than 10 μg/L. The adsorption kinetics data were analyzed using different kinetic models including pseudo first-order model, pseudo second-order model, Elovich model and intraparticle diffusion model. Pseudo second-order kinetic model was the most appropriate model to describe the adsorption kinetics. The adsorption percentage of As（Ⅲ） increased in the p H range of 2–3 while it decreased with the increase of pH（ 3〈pH〈10）. The effects of coexisting anions on As（Ⅲ） removal using FM-1 and FM-2 were also studied and the order of the effects is as follows： NO_3^-, Cl-, F-〈SO_4^（2-）, HCO_3-〈H_2PO_4^-, indicating that H_2PO_4^- is the major competitor with As（Ⅲ） for adsorptive sites on the surface of the adsorbents. The higher adsorption capacity of FM-1 makes it potentially attractive adsorbent for the removal of As（Ⅲ） from groundwater.展开更多
The present work was mainly focused on the single and binary adsorption of methylene blue(MB)and methyl orange(MO)from alcohol aqueous solution over rice husk based activated carbon(RHAC).The study of single dye adsor...The present work was mainly focused on the single and binary adsorption of methylene blue(MB)and methyl orange(MO)from alcohol aqueous solution over rice husk based activated carbon(RHAC).The study of single dye adsorption equilibrium experiments found that the Langmuir adsorption model was consistent with the adsorption behavior of RHAC on MB and MO,indicating that it was a single layer adsorption.The adsorption behavior con-formed to the pscudo-second-order kinetic model.The binary dye adsorption experiments showed that the Lang-muir-Freundlich model could be applied to describe the adsorption behavior of RHAC on MB and MO.Comparation with the single dye system,the adsorption capacity on the binary dye system was larger,and there was"competitive adsorption"and"synergistic adsorption"effects existed.Meanwhile,the pseudo-second-order kinetic model also fit for the binary dye adsorption behavior.展开更多
A study of nonlinear competitive adsorption equilibria of proteins is of fundamental importance in understanding the behavior of preparative chromatographic separation.This work describes the nonlinear binary protein ...A study of nonlinear competitive adsorption equilibria of proteins is of fundamental importance in understanding the behavior of preparative chromatographic separation.This work describes the nonlinear binary protein adsorption equilibria on ion exchangers by the statistical thermodynamic(ST)model.The single-component and binary protein adsorption isotherms of bovine hemoglobin(Hb)and bovine serum albumin(BSA)on SP Sepharose FF were determined by batch adsorption experiments in 0.05 mol/L sodium acetate buffer at three pH values(4.5,5.0 and 5.5)and three NaCl concentrations(0.05,0.10 and 0.15 mol/L)at pH 5.0.The ST model was found to depict the effects of pH and ionic strength on the single-component equilibria well,with model parameters depending on the pH and ionic strength.Moreover,the ST model gave acceptable fitting to the binary adsorption data with the fitted single-component model parameters,leading to the estimation of the binary ST model parameter.The effects of pH and ionic strength on the model parameters are reasonably interpreted by the electrostatic and thermodynamic theories.Results demonstrate the availability of the ST model for describing nonlinear competitive protein adsorption equilibria in the presence of two proteins.展开更多
基金supported by the National Natural Science Foundation of China(No.52488201)the Natural Science Basic Research Program of Shaanxi(No.2024JC-YBMS-284)+1 种基金the Key Research and Development Program of Shaanxi(No.2024GHYBXM-02)the Fundamental Research Funds for the Central Universities.
文摘Machine learning combined with density functional theory(DFT)enables rapid exploration of catalyst descriptors space such as adsorption energy,facilitating rapid and effective catalyst screening.However,there is still a lack of models for predicting adsorption energies on oxides,due to the complexity of elemental species and the ambiguous coordination environment.This work proposes an active learning workflow(LeNN)founded on local electronic transfer features(e)and the principle of coordinate rotation invariance.By accurately characterizing the electron transfer to adsorption site atoms and their surrounding geometric structures,LeNN mitigates abrupt feature changes due to different element types and clarifies coordination environments.As a result,it enables the prediction of^(*)H adsorption energy on binary oxide surfaces with a mean absolute error(MAE)below 0.18 eV.Moreover,we incorporate local coverage(θ_(l))and leverage neutral network ensemble to establish an active learning workflow,attaining a prediction MAE below 0.2 eV for 5419 multi-^(*)H adsorption structures.These findings validate the universality and capability of the proposed features in predicting^(*)H adsorption energy on binary oxide surfaces.
基金financial support from the National Natural Science Foundation of China (Grant No.52004320)the Science Foundation of China University of Petroleum,Beijing (No.2462021QNXZ012,No.2462022BJRC001,and No.2462021YJRC012)the funding from the State Key Laboratory of Petroleum Resources and Engineering (No.PRP/indep-1-2103)。
文摘It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity gases such as H_(2)S that might impact CO_(2) sequestration due to competitive adsorption.This study makes a commendable effort to explore the adsorption behavior of CO_(2)/H_(2)S mixtures in calcite slit nanopores.Grand Canonical Monte Carlo(GCMC)simulation is employed to reveal the adsorption of CO_(2),H_(2)S as well as their binary mixtures in calcite nanopores.Results show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO_(2) and H_(2)S in calcite nanopores,respectively.CO_(2)exhibits stronger adsorption on calcite surface than H_(2)S.Electrostatic energy plays the dominating role in the adsorption behavior.Electrostatic energy accounts for 97.11%of the CO_(2)-calcite interaction energy and 56.33%of the H_(2)S-calcite interaction energy at 10 MPa and 323.15 K.The presence of H_(2)S inhibits the CO_(2) adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H_(2)S leads to less CO_(2) adsorption.The quantity of CO_(2) adsorbed is lessened by approximately 33%when the mole fraction of H_(2)S reaches 0.25.CO_(2) molecules preferentially occupy the regions near the po re wall and H_(2)S molecules tend to reside at the center of nanopore even when the molar ratio of CO_(2) is low,indicating that CO_(2) has an adsorption priority on the calcite surface over H_(2)S.In addition,moisture can weaken the adsorption of both CO_(2) and H_(2)S,while CO_(2) is more affected.More interestingly,we find that pure CO_(2) is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO_(2)with H_(2)S impurity should be settled in the deeper reservoirs.
文摘This paper investigates the bioseparation of binary protein mixtures using polystyrene based anion exchange resin. Adsorption experiments were conducted in batch mode using draft-tube internally recirculate dair lift biocontactor in comparison with the conventional shake flask batch adsorption equilibrium experiments. Binary protein mixtures contained bovine serum albumin (BSA) and bovine haemoglobin (BHb) at different initial fractions. Results from single solute adsorption experiments in biocontactor showed that both proteins were equally adsorbed onto the resin with equilibrium reached in an equal time period. This represents similar affinities towards the negatively charged resin surface, although BSA was expected to adsorb through specific forces. Adsorption results showed that BSA has hindered the BHb adsorption in the biocontactor, although adsorption of both proteins was equally hindered in the shake flasks adsorption experiments. Moreover, adsorption of BHb was inhibited up to 29% in the presence of BSA compared to the adsorption of BHb from a solution containing single solute of BHb at the same initial concentration. Similarly, the presence of BHb has hindered the adsorption of BSA by 59%. Adsorptions of both BSA and BHb from binary solution when each formed 75% initial fraction while the other protein formed the remaining 25% were relatively low with equilibrium reached in shorter time. Moreover, considerable amount of proteins remained in the solution, which demonstrates that multilayer adsorption most likely didn’t occur at the relatively small protein concentrations used in the present study. In general, the higher adsorption of BHb can also be related to the compressibility of its molecules which allowed for higher adsorption capacity. The homogeneous and lower shear environment in the airlift biocontactor compared to the other conventional batch adsorption in shake flask reduced the compressibility of BHb that caused higher BSA adsorption from binary solutions of BSA and BHb, which allowed for better bioseparation of both proteins.
基金financially supported by the Natural Science Foundation for the Youth of China (No. 41202118)the Fundamental Research Funds for the Central Universities (No.2012QNB03)
文摘Adsorption-desorption experiments on CO2-CH4 gas mixtures with varying compositions have been conducted to study the fractionation characteristics of CO2-CH4 on Haishiwan coal samples. These were carried out at constant temperature but different equilibrium pressure conditions. Based on these experimental results, the temporal evolution of component fractionation in the field was investigated. The results show that the CO2 concentration in the adsorbed phase is always greater than that in the original gas mixture during the desorption process, while CH4 shows the opposite characteristics. This has confirmed that CO2 , with a greater adsorption ability has a predominant position in the competition with CH4 under different pressures. Where gas drainage is employed, the ratio of CO2 to CH4 varies with time and space in floor roadways used for gas drainage, and in the ventilation air in Nos.1 and 2 coal seams, which is consistent with laboratory results.
基金This work was supported by the National Natural Science Foundation of China(No.20274017)
文摘Single and binary adsorption behaviors of salicylic acid and 5-sulfosalicylic acid onto hypercrosslinked polymeric adsorbents,i.e.NDA-101 and NDA-99 were investigated.The Freundlich model can successfully describe all the adsorption isotherms tested,which indicates a favorable and exothermic adsorption process.The adsorption of salicylic acid relies on π-π interaction,while the electrostatic interaction further influences the adsorption of 5-sulfosalicylic acid onto NDA-99.The adsorptive capacity of salicylic acid on NDA-99 decreases but increases on NDA-101 with 5-sulfosalicylic acid as the background component in a binary solute system.The amount of 5-sulfosalicylic acid adsorbed was decreased with the increase in initial concentration of salicylic acid on both adsorbents.The competition for the adsorption sites is considered to be predominant in the solid-to-liquid interaction process.The adsorption selectivity of salicylic acid onto NDA-101 is higher than onto NDA-99 by more than an order of magnitude.Thus,combination technique involving NDA-101 followed by NDA-99 can be effectively applied to separate and recover salicylic acid and 5-sulfosalicylic acid from wastewater.
基金supported by Major Natural Science Foundation of Guangdong Provincethe Trans-century Training Programmed Foundation for the Talents of the State Education Ministry of Chinaand the Foundation for the Key Teachers in Chinese University
文摘The dynamic competitive adsorption behaviors of different binary organic vapor mixtures on ACF-Ps under different operation conditions were investigated by gas chromatography in this paper. The studied mixtures included benzene/toluene, toluene/xylene, benzene/isopropylbenzene, ethyl acetate/toluene and benzene/ethyl acetate. Experimental results show that various ACF-Ps, as with ACF-W, can remove both vapors in binary vapor mixtures with over 99% of removal efficiency before the breakthrough point of the more weakly adsorbed vapor. In dynamic competitive adsorption, the more weakly adsorbed vapor not only penetrates early, but also will be displaced and desorbed consequently by stronger adsorbate and therefore produces a rolling up in the breakthrough curve. The ACF-Ps prepared at different temperatures have somewhat different adsorption selectivity. The feed concentration ratio of vapors, the length/diameter ratio and the thick of bed have effect on competitive adsorption. The competitive adsorption ability of a vapor is mainly related to its boiling point. Usually, the higher the boiling point, the stronger the vapor adsorbed on ACF-P.
基金supported by the National Key Research and Development Program of China(2022YFB3806800)the National Natural Science Foundation of China(22122811,22008209)the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(2021SZ-TD008).
文摘The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging research.The great similarity in the molecular size of C_(2)H_(4)and C_(2)H_(6)brings challenges to the regulation of adsorbents to realize efficient dynamic separation.Herein,we reported the enhancement of the kinetic separation of C_(2)H_(4)/C_(2)H_(6)by controlling the crystal size of ZnAtzPO_(4)(Atz=3-amino-1,2,4-triazole)to amplify the diffusion difference of C_(2)H_(4)and C_(2)H_(6).Through adjusting the synthesis temperature,reactant concentration,and ligands/metal ions molar ratio,ZnAtzPO4 crystals with different sizes were obtained.Both single-component kinetic adsorption tests and binary-component dynamic breakthrough experiments confirmed the enhancement of the dynamic separation of C_(2)H_(4)/C_(2)H_(6)with the increase in the crystal size of ZnAtzPO_(4).The separation selectivity of C_(2)H_(4)/C_(2)H_(6)increased from 1.3 to 98.5 with the increase in the crystal size of ZnAtzPO_(4).This work demonstrated the role of morphology and size control of adsorbent crystals in the improvement of the C_(2)H_(4)/C_(2)H_(6)kinetic separation performance.
基金Projects(51334008,51304243,51604160)supported by the National Natural Science Foundation of ChinaProject(2016zzts037)supported by the Fundamental Research Funds for the Central Universities,China
文摘Considering the different geochemical enrichment behaviors of W and Mo,Fe?Mn binary oxide(FMBO),ferric hydroxide(Fe(OH)3)and manganese dioxide(MnO2)were studied to separate W from molybdate solution,respectively.The experimental results demonstrated that Fe?Mn binary oxide(FMBO)was the most suitable adsorbent for the separation.Under a wide pH(6.9?11.3)region,more than80%W removal efficiency and less than3%Mo loss could be obtained.In addition,the Fe?Mn binary oxide adsorbent can be regenerated by treating with3mol/L NaOH,and the W adsorption efficiency was retained after five adsorption?desorption?regeneration cycles.All these indicate that the Fe?Mn binary oxides have the potential for the separation of W from molybdate solution.
文摘The adsorption potential of FMBO, FeOOH, MnO2 for the removal of Cd^2＋, Cu^2＋ and Pb^2＋ in aqueous systems was investigated in this study. Comparing to FMBO and FeOOH, MnO2 offered a much higher removal capacity towards the three metal ions. The maximal adsorption capacity of MnO2 for Cd^2＋, Cu^2＋ and Pb^2＋ were 1.23, 2.25 and 2.60 mmol· g^-1, respectively. And that for FMBO were 0.37, 1.13, and 1.18mmol·g^-1 and for FeOOH were 0.11, 0.86 and 0.48 mmol·g^-1, respectively. The adsorption behaviors of the three metal ions on the three adsorbents were all significantly affected by pH values and heavy metal removal efficiency increased with pH increased. The Langmuir and Freundlieh adsorption models were used to describe the adsorption equilibrium of the three metal ions onto the three adsorbents. Results showed that the adsorption equilibrium data fitted well to Langmuir isotherm and this indicated that adsorption of metal ions occurred on the three metal oxides adsorbents limited to the formation of a monolayer. More negative charged of MnOa surface than that of FMBO and FeOOH could be ascribed by lower pHiep of MnO2 than that of FMBO and FeOOH and this could contribute to more binding sites on MnO2 surface than that of FMBO and FeOOH. The higher metal ions uptake by MnO2 than FMBO and FeOOH could be well explained by the surface charge mechanism.
基金supported by the National Natural Science Foundation of China(No.41120124003)the Ministry of Science and Technology of China(No.2012AA062602)the 111 project and Priority Development Projects of SRFDP of the Ministry of Education of China
文摘The adsorptive removal of arsenic by synthetically-prepared nano Fe-Mn binary oxides（FM） was investigated. A novel method using potassium permanganate and ferric chloride as raw materials was used to synthesise FM. The molar ratio of Fe and Mn in the synthetic Fe-Mn binary oxides was 4 ： 3. The FM-1 and FM-2（prepared at different activation temperatures） having high specific surface areas（358.87 and 128.58 m^2/g, respectively） were amorphous and of nano particle types. The amount of arsenic adsorbed on FM-1 was higher than that adsorbed on FM-2 particles. After adsorption by FM-1, residual arsenic concentration decreased to less than 10 μg/L. The adsorption kinetics data were analyzed using different kinetic models including pseudo first-order model, pseudo second-order model, Elovich model and intraparticle diffusion model. Pseudo second-order kinetic model was the most appropriate model to describe the adsorption kinetics. The adsorption percentage of As（Ⅲ） increased in the p H range of 2–3 while it decreased with the increase of pH（ 3〈pH〈10）. The effects of coexisting anions on As（Ⅲ） removal using FM-1 and FM-2 were also studied and the order of the effects is as follows： NO_3^-, Cl-, F-〈SO_4^（2-）, HCO_3-〈H_2PO_4^-, indicating that H_2PO_4^- is the major competitor with As（Ⅲ） for adsorptive sites on the surface of the adsorbents. The higher adsorption capacity of FM-1 makes it potentially attractive adsorbent for the removal of As（Ⅲ） from groundwater.
基金Supported by the National Natural Science Foundation of China(No.21501069)the National Key R&D Program During the 13th Five-year Plan of China(No.2016YFD0401405)+1 种基金the Fundamental Research Funds for the Central Universities of China(No.JUSRP51626B)MOE&SAFEA for the"111 Project"of China(No.B13025).
文摘The present work was mainly focused on the single and binary adsorption of methylene blue(MB)and methyl orange(MO)from alcohol aqueous solution over rice husk based activated carbon(RHAC).The study of single dye adsorption equilibrium experiments found that the Langmuir adsorption model was consistent with the adsorption behavior of RHAC on MB and MO,indicating that it was a single layer adsorption.The adsorption behavior con-formed to the pscudo-second-order kinetic model.The binary dye adsorption experiments showed that the Lang-muir-Freundlich model could be applied to describe the adsorption behavior of RHAC on MB and MO.Comparation with the single dye system,the adsorption capacity on the binary dye system was larger,and there was"competitive adsorption"and"synergistic adsorption"effects existed.Meanwhile,the pseudo-second-order kinetic model also fit for the binary dye adsorption behavior.
基金supported by the National Natural Science Foundation of China(Grant No.20636040)the Specialized Research Fund for the Doctoral Program of Higher Education(Grant No.20050056001).
文摘A study of nonlinear competitive adsorption equilibria of proteins is of fundamental importance in understanding the behavior of preparative chromatographic separation.This work describes the nonlinear binary protein adsorption equilibria on ion exchangers by the statistical thermodynamic(ST)model.The single-component and binary protein adsorption isotherms of bovine hemoglobin(Hb)and bovine serum albumin(BSA)on SP Sepharose FF were determined by batch adsorption experiments in 0.05 mol/L sodium acetate buffer at three pH values(4.5,5.0 and 5.5)and three NaCl concentrations(0.05,0.10 and 0.15 mol/L)at pH 5.0.The ST model was found to depict the effects of pH and ionic strength on the single-component equilibria well,with model parameters depending on the pH and ionic strength.Moreover,the ST model gave acceptable fitting to the binary adsorption data with the fitted single-component model parameters,leading to the estimation of the binary ST model parameter.The effects of pH and ionic strength on the model parameters are reasonably interpreted by the electrostatic and thermodynamic theories.Results demonstrate the availability of the ST model for describing nonlinear competitive protein adsorption equilibria in the presence of two proteins.
