The efficient extraction of sodium(Na^(+))and lithium(Li^(+))from seawater and salt lakes is increasingly demanding due to their great application value in chemical industries.However,coexisting cations such as divale...The efficient extraction of sodium(Na^(+))and lithium(Li^(+))from seawater and salt lakes is increasingly demanding due to their great application value in chemical industries.However,coexisting cations such as divalent calcium(Ca^(2+))and magnesium(Mg^(2+))ions are at the subnanometer scale in diameter,similar to target monovalent ions,making ion separation a great challenge.Here,we propose a simple and fast secondary growth method for the preparation of MIL-53(Al)-NH_(2)membranes on the surface of anodic aluminum oxide.Such membranes contain angstrom-scale(~7Å)channels for the entrance of small monovalent ions and water molecules,endowing the selectivities for monovalent cations over divalent cations and water over salt molecules.The resulting high-connectivity MIL-53(Al)-NH_(2)membranes exhibit excellent ion separation performance(a selectivity of 121.42 for Na^(+)/Ca^(2+)and 93.81 for Li^(+)/Mg^(2+))and desalination performance(a water/salt selectivity of up to 5196).This work highlights metal–organic framework membranes as potential candidates for realizing ion separation and desalination in liquid treatment.展开更多
High yield production of phenol from hydroxylation of benzene with low energy consumption is of paramount importance,but still challenging.Herein,a new strategy,consisting of using diatomic synergistic modulation(DSM)...High yield production of phenol from hydroxylation of benzene with low energy consumption is of paramount importance,but still challenging.Herein,a new strategy,consisting of using diatomic synergistic modulation(DSM)to effectively control the separation of photo-generated carriers for an enhanced production of phenol is reported.The atomic level dispersion of Fe and Cr respectively decorated on Al based MIL-53-NH_(2)photocatalyst(Fe1/Cr:MIL-53-NH_(2))is designed,in which Cr single atoms are substituted for Al3+while Fe single atoms are coordinated by N.Notably,the Fe1/Cr:MIL-53-NH_(2)significantly boosts the photooxidation of benzene to phenol under visible light irradiation,which is much higher than those of MIL-53-NH_(2),Cr:MIL-53-NH_(2),Fe1/MIL-53-NH_(2),and Fe nanoparticles/Cr:MIL-53-NH_(2)catalysts.Theoretical and experimental results reveal that the Cr single atoms and Fe single atoms can act as electron acceptor and electron donor,respectively,during photocatalytic reaction,exhibiting a synergistic effect on the separation of the photo-generated carriers and thereby causing great enhancement on the benzene oxidation.This strategy provides new insights for rational design of advanced photocatalysts at the atomic level.展开更多
The binary Ag3 P04/MIL-125-NH2(AMN-X)composites were synthesized through ion exchange-solution method,and the ternary Ag/Ag3 PO_(4)/MIL-125-NH2(AAMN-X)Z-scheme heterojunctions were prepared via the photo chemical redu...The binary Ag3 P04/MIL-125-NH2(AMN-X)composites were synthesized through ion exchange-solution method,and the ternary Ag/Ag3 PO_(4)/MIL-125-NH2(AAMN-X)Z-scheme heterojunctions were prepared via the photo chemical reduction deposition strategy.The photocatalytic hexavalent chromium(Cr(VI))sequestration over AMN-X and AAMN-X were investigated under visible light.AAMN-120 accomplished superior reduction performance due to that Ag nanoparticles(NPs)act as electrons transfer bridge to enhance the separation efficiency of photogenerated e-h+pairs,in which the reaction rates(k.value)were 2.77 and 124.2 fold higher than those of individual MIL-125-NH2 and Ag3 PO_(4),respectively.The influences of different pH values,small organic acids and coexisting ions on the photocatalytic perfo rmance of AAMN-120 were also investigated.In addition,the AAMN-120 heterojunction expressed great reusability and stability in cycling experiments.The mechanism of photocatalytic Cr(VI)was investigated and verified through photoluminescence(PL),electrochemistry,electron spin resonance(ESR),active species capture,and Pt element deposition experiments.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(WK2060000030)USTC Research Funds of the Double First Class Initiative(YD2060002022)Major Science and Technology Innovation Projects in Shandong Province(2022CXGC020415).
文摘The efficient extraction of sodium(Na^(+))and lithium(Li^(+))from seawater and salt lakes is increasingly demanding due to their great application value in chemical industries.However,coexisting cations such as divalent calcium(Ca^(2+))and magnesium(Mg^(2+))ions are at the subnanometer scale in diameter,similar to target monovalent ions,making ion separation a great challenge.Here,we propose a simple and fast secondary growth method for the preparation of MIL-53(Al)-NH_(2)membranes on the surface of anodic aluminum oxide.Such membranes contain angstrom-scale(~7Å)channels for the entrance of small monovalent ions and water molecules,endowing the selectivities for monovalent cations over divalent cations and water over salt molecules.The resulting high-connectivity MIL-53(Al)-NH_(2)membranes exhibit excellent ion separation performance(a selectivity of 121.42 for Na^(+)/Ca^(2+)and 93.81 for Li^(+)/Mg^(2+))and desalination performance(a water/salt selectivity of up to 5196).This work highlights metal–organic framework membranes as potential candidates for realizing ion separation and desalination in liquid treatment.
基金the National Natural Science Foundation of China(No.21971002)the Natural Science Foundation of Anhui Province(Nos.1908085QB45 and 2008085QB81)。
文摘High yield production of phenol from hydroxylation of benzene with low energy consumption is of paramount importance,but still challenging.Herein,a new strategy,consisting of using diatomic synergistic modulation(DSM)to effectively control the separation of photo-generated carriers for an enhanced production of phenol is reported.The atomic level dispersion of Fe and Cr respectively decorated on Al based MIL-53-NH_(2)photocatalyst(Fe1/Cr:MIL-53-NH_(2))is designed,in which Cr single atoms are substituted for Al3+while Fe single atoms are coordinated by N.Notably,the Fe1/Cr:MIL-53-NH_(2)significantly boosts the photooxidation of benzene to phenol under visible light irradiation,which is much higher than those of MIL-53-NH_(2),Cr:MIL-53-NH_(2),Fe1/MIL-53-NH_(2),and Fe nanoparticles/Cr:MIL-53-NH_(2)catalysts.Theoretical and experimental results reveal that the Cr single atoms and Fe single atoms can act as electron acceptor and electron donor,respectively,during photocatalytic reaction,exhibiting a synergistic effect on the separation of the photo-generated carriers and thereby causing great enhancement on the benzene oxidation.This strategy provides new insights for rational design of advanced photocatalysts at the atomic level.
文摘The binary Ag3 P04/MIL-125-NH2(AMN-X)composites were synthesized through ion exchange-solution method,and the ternary Ag/Ag3 PO_(4)/MIL-125-NH2(AAMN-X)Z-scheme heterojunctions were prepared via the photo chemical reduction deposition strategy.The photocatalytic hexavalent chromium(Cr(VI))sequestration over AMN-X and AAMN-X were investigated under visible light.AAMN-120 accomplished superior reduction performance due to that Ag nanoparticles(NPs)act as electrons transfer bridge to enhance the separation efficiency of photogenerated e-h+pairs,in which the reaction rates(k.value)were 2.77 and 124.2 fold higher than those of individual MIL-125-NH2 and Ag3 PO_(4),respectively.The influences of different pH values,small organic acids and coexisting ions on the photocatalytic perfo rmance of AAMN-120 were also investigated.In addition,the AAMN-120 heterojunction expressed great reusability and stability in cycling experiments.The mechanism of photocatalytic Cr(VI)was investigated and verified through photoluminescence(PL),electrochemistry,electron spin resonance(ESR),active species capture,and Pt element deposition experiments.
