We modified Zr/Ce-UiO-66-NH_(2) using dual bimetallization and amination strategies to efficiently extract uranium from water resources.XRD,FTIR,and XPS indicated the successful alteration of material amination.Moreov...We modified Zr/Ce-UiO-66-NH_(2) using dual bimetallization and amination strategies to efficiently extract uranium from water resources.XRD,FTIR,and XPS indicated the successful alteration of material amination.Moreover,the metal Zr was partially replaced by Ce in Zr-oxygen atom clusters in Zr/Ce-UiO-66-NH_(2).It possessed commendable structural stability in acidic and alkaline solutions.Irrespective of whether it was submerged in a 6 M strong acid or in a 0.5M strong base solution,the structural integrity of Zr/Ce-UiO-66-NH_(2) remained unaffected.Batch experiments at pH=6.0 revealed that uranium adsorption by Zr/Ce-UiO-66-NH_(2) reached 376.8 mg g^(−1) and 611.33 mg g^(−1) at 298 K and 328 K,respectively.These values are much better than those obtained using bimetallic-modified Zr/Ce-UiO-66 or amine-functionalized UiO-66-NH_(2).After five consecutive sorption and desorption cycles,the material retained a uranium removal rate of more than 80%,proving its excellent regenerative properties.Kinetic modeling of U(VI)adsorption on Zr/Ce-UiO-66-NH_(2) implied that chemisorption dominated the rapid uranium sorption rate.We propose potential adsorption mechanisms involving three interactions:inner-sphere surface complexation,chemisorption,and electrostatic interactions.This study shows that the dual strategies of bimetallization and amination can effectively enhance U(VI)extraction from water.This approach has potential applications for the structural design of uranium adsorbents.展开更多
Inorganic anions such as phosphates and carbonates are essential in the natural system and it is important for the detec-tion of such species.In this work,the fluorescence sensing capacity of Zr(IV)framework with an a...Inorganic anions such as phosphates and carbonates are essential in the natural system and it is important for the detec-tion of such species.In this work,the fluorescence sensing capacity of Zr(IV)framework with an amino-functional group,namely UiO-66-NH_(2),towards specific inorganic anions was investigated in aqueous media.The results revealed that the fluorescence emission intensity of UiO-66-NH2 could be strongly enhanced by phosphate and carbonate anions including HPO_(4)^(2-),H_(2)PO_(4)^(-),PO_(4)^(3-),P_(2)O_(7)^(4-),HCO_(3)^(-)and CO_(3)^(2-),implying its sensing capacity towards phosphate and carbonate anions.Furthermore,fluorescence titration experiments exhibit that the emission intensity enhancement ratio depends linearly on the concentration of anions,suggesting the possibility of quantitative detection of these anions.Further studies suggest that the sensing of UiO-66-NH,towards HPO_(4)^(2-)/PO_(4)^(3-)/P_(2)O_(4)^(-)/HCO_(3)^(-)/CO_(2)-could be ascribed to the collapse of the framework,while that for H_(2)PO_(4)-could be attributed to the adsorption of H,PO4-by UiO-66-NH2 with hydrogen bonding interactions between H,PO4-and the amino group of UiO-66-NH_(2) supported by the different fluorescence response of UiO-66 and UiO-66-NH,towards the anions.展开更多
基金supported by the National Natural Science Foundation of China(No.22376058).
文摘We modified Zr/Ce-UiO-66-NH_(2) using dual bimetallization and amination strategies to efficiently extract uranium from water resources.XRD,FTIR,and XPS indicated the successful alteration of material amination.Moreover,the metal Zr was partially replaced by Ce in Zr-oxygen atom clusters in Zr/Ce-UiO-66-NH_(2).It possessed commendable structural stability in acidic and alkaline solutions.Irrespective of whether it was submerged in a 6 M strong acid or in a 0.5M strong base solution,the structural integrity of Zr/Ce-UiO-66-NH_(2) remained unaffected.Batch experiments at pH=6.0 revealed that uranium adsorption by Zr/Ce-UiO-66-NH_(2) reached 376.8 mg g^(−1) and 611.33 mg g^(−1) at 298 K and 328 K,respectively.These values are much better than those obtained using bimetallic-modified Zr/Ce-UiO-66 or amine-functionalized UiO-66-NH_(2).After five consecutive sorption and desorption cycles,the material retained a uranium removal rate of more than 80%,proving its excellent regenerative properties.Kinetic modeling of U(VI)adsorption on Zr/Ce-UiO-66-NH_(2) implied that chemisorption dominated the rapid uranium sorption rate.We propose potential adsorption mechanisms involving three interactions:inner-sphere surface complexation,chemisorption,and electrostatic interactions.This study shows that the dual strategies of bimetallization and amination can effectively enhance U(VI)extraction from water.This approach has potential applications for the structural design of uranium adsorbents.
基金the National Natural Science Foundation of China (grant No.22171131) for financial support of this worksupported by a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Inorganic anions such as phosphates and carbonates are essential in the natural system and it is important for the detec-tion of such species.In this work,the fluorescence sensing capacity of Zr(IV)framework with an amino-functional group,namely UiO-66-NH_(2),towards specific inorganic anions was investigated in aqueous media.The results revealed that the fluorescence emission intensity of UiO-66-NH2 could be strongly enhanced by phosphate and carbonate anions including HPO_(4)^(2-),H_(2)PO_(4)^(-),PO_(4)^(3-),P_(2)O_(7)^(4-),HCO_(3)^(-)and CO_(3)^(2-),implying its sensing capacity towards phosphate and carbonate anions.Furthermore,fluorescence titration experiments exhibit that the emission intensity enhancement ratio depends linearly on the concentration of anions,suggesting the possibility of quantitative detection of these anions.Further studies suggest that the sensing of UiO-66-NH,towards HPO_(4)^(2-)/PO_(4)^(3-)/P_(2)O_(4)^(-)/HCO_(3)^(-)/CO_(2)-could be ascribed to the collapse of the framework,while that for H_(2)PO_(4)-could be attributed to the adsorption of H,PO4-by UiO-66-NH2 with hydrogen bonding interactions between H,PO4-and the amino group of UiO-66-NH_(2) supported by the different fluorescence response of UiO-66 and UiO-66-NH,towards the anions.
