In this study,the surface properties and adsorption properties of the Le An River sedi- ment were modelled via surface complexation approach.The model parameters were determined based on the data of our potentiometric...In this study,the surface properties and adsorption properties of the Le An River sedi- ment were modelled via surface complexation approach.The model parameters were determined based on the data of our potentiometric titration experiments and the metal adsorption experiments with the Le An River sediment samples.Consequently,the surface complexation models for the natural sediment,in our case the Le An River sediments,which can interpret the experimental data very well were successfully established.Three typical surface complexation models that is the con- stant capacitance model,the diffuse layer model and the triple layer model,were considered in this research.This work indicated that the consistency and the interdependency among model parame- ters together with the selection of the surface adsorbed species should be emphasized.展开更多
Radionuclide migration in aquatic environment is influenced by its sorption onto colloids/mineral oxides and the presence of organic complexing anions.With a view to understand the sorption of trivalent actinides by m...Radionuclide migration in aquatic environment is influenced by its sorption onto colloids/mineral oxides and the presence of organic complexing anions.With a view to understand the sorption of trivalent actinides by mineral oxides in presence of organic acid,in the present study,Eu(Ⅲ),malonic acid(MA)andγ-alumina are considered as representatives of trivalent actinides,low molecular weight natural occurring organic acid and aluminol sites,respectively.The influence of MA on sorption of Eu(Ⅲ)byγ-alumina was elucidated by batch sorption,spectroscopic techniques and surface complexation modeling,for the first time.Attenuated Total Reflection-Fourier Transform Infrared spectroscopic studies of MA sorbed onγ-alumina revealed the presence of two inner-sphere surface complexes.Batch sorption for binary(alumina-Eu(Ⅲ))and ternary(alumina-Eu(Ⅲ)-MA)systems were investigated as a function of p H,Eu(Ⅲ)concentration and sequential addition of Eu(Ⅲ)/MA.The p H edge for Eu(Ⅲ)sorption shifts to higher p H with increasing Eu(Ⅲ)concentration.In ternary systems,Eu(Ⅲ)sorption is significantly enhanced at p H<4.5.Eu(Ⅲ)speciation onγ-alumina is independent of addition sequence of Eu(Ⅲ)/MA.Time resolved fluorescence spectroscopy of Eu(Ⅲ)sorbed onγ-alumina exhibited two surface species,≡XOEu^2+and(≡YO)2 Eu^(+).The enhancement in I 616/I 592 and lifetime for ternary systems,as compared to binary system,at low p H,indicates the participation of Eu-MA complexes in the formation of surface species in ternary systems.The diffuse layer model has been employed to successfully model the experimental sorption profiles of binary and ternary systems,using code FITEQL 4.0,by considering the surface species identified by spectroscopic techniques.展开更多
In this work,an adsorbent,which we call MnPT,was prepared by combining MnO_(2),polyethylenimine and tannic acid,and exhibited efficient performance for Cu(Ⅱ) and Cr(VI) removal from aqueous solution.The oxygen/nitrog...In this work,an adsorbent,which we call MnPT,was prepared by combining MnO_(2),polyethylenimine and tannic acid,and exhibited efficient performance for Cu(Ⅱ) and Cr(VI) removal from aqueous solution.The oxygen/nitrogen-containing functional groups on the surface of MnPT might increase the enrichment of metal ions by complexation.The maximum adsorption capacities of MnPT for Cu(Ⅱ) and Cr(Ⅵ) were 121.5 and 790.2 mg·g^(-1),respectively.The surface complexation formation model was used to elucidate the physicochemical interplay in the process of Cu(Ⅱ) and Cr(Ⅵ) co-adsorption on MnPT.Electrostatic force,solvation action,adsorbate-adsorbate lateral interaction,and complexation were involved in the spontaneous adsorption process.Physical electrostatic action was dominant in the initial stage,whereas chemical action was the driving force leading to adsorption equilibrium.It should be noted that after adsorption on the surface of MnPT,Cr(Ⅵ) reacted with some reducing functional groups(hydroxylamine-NH_(2))and was converted into Cr(Ⅲ).The adsorption capacity declined by 12% after recycling five times.Understanding the adsorption mechanism might provide a technical basis for the procedural design of heavy metal adsorbents.This MnPT nanocomposite has been proven to be a low-cost,efficient,and promising adsorbent for removing heavy metal ions from wastewater.展开更多
基金This work was supported by the National Natural Science Foundation of China.
文摘In this study,the surface properties and adsorption properties of the Le An River sedi- ment were modelled via surface complexation approach.The model parameters were determined based on the data of our potentiometric titration experiments and the metal adsorption experiments with the Le An River sediment samples.Consequently,the surface complexation models for the natural sediment,in our case the Le An River sediments,which can interpret the experimental data very well were successfully established.Three typical surface complexation models that is the con- stant capacitance model,the diffuse layer model and the triple layer model,were considered in this research.This work indicated that the consistency and the interdependency among model parame- ters together with the selection of the surface adsorbed species should be emphasized.
文摘Radionuclide migration in aquatic environment is influenced by its sorption onto colloids/mineral oxides and the presence of organic complexing anions.With a view to understand the sorption of trivalent actinides by mineral oxides in presence of organic acid,in the present study,Eu(Ⅲ),malonic acid(MA)andγ-alumina are considered as representatives of trivalent actinides,low molecular weight natural occurring organic acid and aluminol sites,respectively.The influence of MA on sorption of Eu(Ⅲ)byγ-alumina was elucidated by batch sorption,spectroscopic techniques and surface complexation modeling,for the first time.Attenuated Total Reflection-Fourier Transform Infrared spectroscopic studies of MA sorbed onγ-alumina revealed the presence of two inner-sphere surface complexes.Batch sorption for binary(alumina-Eu(Ⅲ))and ternary(alumina-Eu(Ⅲ)-MA)systems were investigated as a function of p H,Eu(Ⅲ)concentration and sequential addition of Eu(Ⅲ)/MA.The p H edge for Eu(Ⅲ)sorption shifts to higher p H with increasing Eu(Ⅲ)concentration.In ternary systems,Eu(Ⅲ)sorption is significantly enhanced at p H<4.5.Eu(Ⅲ)speciation onγ-alumina is independent of addition sequence of Eu(Ⅲ)/MA.Time resolved fluorescence spectroscopy of Eu(Ⅲ)sorbed onγ-alumina exhibited two surface species,≡XOEu^2+and(≡YO)2 Eu^(+).The enhancement in I 616/I 592 and lifetime for ternary systems,as compared to binary system,at low p H,indicates the participation of Eu-MA complexes in the formation of surface species in ternary systems.The diffuse layer model has been employed to successfully model the experimental sorption profiles of binary and ternary systems,using code FITEQL 4.0,by considering the surface species identified by spectroscopic techniques.
基金supported by the National Natural Science Foundation of China(Grant Nos.41573103,41340037)the Shandong Provincial Key Research and Development Program(Grant Nos.2017GSF16105,2018GGX102004,2018GSF117007)the Taishan Scholar Program(Grant No.ts201712045)of Shandong Province of China.
文摘In this work,an adsorbent,which we call MnPT,was prepared by combining MnO_(2),polyethylenimine and tannic acid,and exhibited efficient performance for Cu(Ⅱ) and Cr(VI) removal from aqueous solution.The oxygen/nitrogen-containing functional groups on the surface of MnPT might increase the enrichment of metal ions by complexation.The maximum adsorption capacities of MnPT for Cu(Ⅱ) and Cr(Ⅵ) were 121.5 and 790.2 mg·g^(-1),respectively.The surface complexation formation model was used to elucidate the physicochemical interplay in the process of Cu(Ⅱ) and Cr(Ⅵ) co-adsorption on MnPT.Electrostatic force,solvation action,adsorbate-adsorbate lateral interaction,and complexation were involved in the spontaneous adsorption process.Physical electrostatic action was dominant in the initial stage,whereas chemical action was the driving force leading to adsorption equilibrium.It should be noted that after adsorption on the surface of MnPT,Cr(Ⅵ) reacted with some reducing functional groups(hydroxylamine-NH_(2))and was converted into Cr(Ⅲ).The adsorption capacity declined by 12% after recycling five times.Understanding the adsorption mechanism might provide a technical basis for the procedural design of heavy metal adsorbents.This MnPT nanocomposite has been proven to be a low-cost,efficient,and promising adsorbent for removing heavy metal ions from wastewater.
