Amine modification is an effective strategy to improve the H_(2)S removal performance of Cu-BTC.In order to avoid the problem of pore blockage after amine modification in post synthesis impregnation,herein a series of...Amine modification is an effective strategy to improve the H_(2)S removal performance of Cu-BTC.In order to avoid the problem of pore blockage after amine modification in post synthesis impregnation,herein a series of Cu-BTC modified with organic amine adsorbents were prepared via an in-situ one-pot method and the H_(2)S removal performance under ambient conditions was tested.It is found that the introduced organic amines,depending on the types of amine selected,have a significant influence on the growth of Cu-BTC and its textural properties.The H_(2)S removal performance on the as-prepared materials suggested that the amine modified samples remarkably improved the H_(2)S removal capacities with an order of BA-Cu-BTC>TEA-Cu-BTC>TEOA-Cu-BTC>Cu-BTC.Besides the enlarged surface area and the increased mesopores volumes,BA has the advantages of smaller steric hindrance and-NH_(2)groups,among which the former increased the accessibility of Cu active sites while the latter acted as additional active sites for H_(2)S capturing,thus affording BA-Cu-BTC highest breakthrough capacity of 77.3 mg S/g.Overall,this study elaborates the effect of organic amines in-situ modification on the Cu-BTC structure and desulfurization.展开更多
Developing an efficient photocatalytic system for hydrogen peroxide(H_(2)O_(2))activation in Fenton-like processes holds significant promise for advancing water purification technologies.However,challenges such as hig...Developing an efficient photocatalytic system for hydrogen peroxide(H_(2)O_(2))activation in Fenton-like processes holds significant promise for advancing water purification technologies.However,challenges such as high carrier recombination rates,limited active sites,and suboptimal H_(2)O_(2)activation efficiency impede optimal performance.Here we show that single-iron-atom dispersed Bi_(2)WO_(6)monolayers(SIAD-BWOM),designed through a facile hydrothermal approach,can offer abundant active sites for H_(2)O_(2)activation.The SIAD-BWOM catalyst demonstrates superior photo-Fenton degradation capabilities,particularly for the persistent pesticide dinotefuran(DNF),showcasing its potential in addressing recalcitrant organic pollutants.We reveal that the incorporation of iron atoms in place of tungsten within the electron-rich[WO_(4)]^(2-)layers significantly facilitates electron transfer processes and boosts the Fe(II)/Fe(III)cycle efficiency.Complementary experimental investigations and theoretical analyses further elucidate how the atomically dispersed iron induces lattice strain in the Bi_(2)WO_(6)monolayer,thereby modulating the d-band center of iron to improve H_(2)O_(2)adsorption and activation.Our research provides a practical framework for developing advanced photo-Fenton catalysts,which can be used to treat emerging and refractory organic pollutants more effectively.展开更多
基金Supported by National Natural Science Foundation of China[Grant No.21878209,Grant No.22078223 and Grant No.22208233]Basic Research Project of Shanxi Province[Grant No.20210302123065].
文摘Amine modification is an effective strategy to improve the H_(2)S removal performance of Cu-BTC.In order to avoid the problem of pore blockage after amine modification in post synthesis impregnation,herein a series of Cu-BTC modified with organic amine adsorbents were prepared via an in-situ one-pot method and the H_(2)S removal performance under ambient conditions was tested.It is found that the introduced organic amines,depending on the types of amine selected,have a significant influence on the growth of Cu-BTC and its textural properties.The H_(2)S removal performance on the as-prepared materials suggested that the amine modified samples remarkably improved the H_(2)S removal capacities with an order of BA-Cu-BTC>TEA-Cu-BTC>TEOA-Cu-BTC>Cu-BTC.Besides the enlarged surface area and the increased mesopores volumes,BA has the advantages of smaller steric hindrance and-NH_(2)groups,among which the former increased the accessibility of Cu active sites while the latter acted as additional active sites for H_(2)S capturing,thus affording BA-Cu-BTC highest breakthrough capacity of 77.3 mg S/g.Overall,this study elaborates the effect of organic amines in-situ modification on the Cu-BTC structure and desulfurization.
基金financial support from the Natural Science Foundation of China(51979081,52100179)Fundamental Research Funds for the Central Universities(B200202103)+1 种基金National Science Funds for Creative Research Groups of China(No.51421006)PAPD and Photon Science Research center for Carbon Dioxide.
文摘Developing an efficient photocatalytic system for hydrogen peroxide(H_(2)O_(2))activation in Fenton-like processes holds significant promise for advancing water purification technologies.However,challenges such as high carrier recombination rates,limited active sites,and suboptimal H_(2)O_(2)activation efficiency impede optimal performance.Here we show that single-iron-atom dispersed Bi_(2)WO_(6)monolayers(SIAD-BWOM),designed through a facile hydrothermal approach,can offer abundant active sites for H_(2)O_(2)activation.The SIAD-BWOM catalyst demonstrates superior photo-Fenton degradation capabilities,particularly for the persistent pesticide dinotefuran(DNF),showcasing its potential in addressing recalcitrant organic pollutants.We reveal that the incorporation of iron atoms in place of tungsten within the electron-rich[WO_(4)]^(2-)layers significantly facilitates electron transfer processes and boosts the Fe(II)/Fe(III)cycle efficiency.Complementary experimental investigations and theoretical analyses further elucidate how the atomically dispersed iron induces lattice strain in the Bi_(2)WO_(6)monolayer,thereby modulating the d-band center of iron to improve H_(2)O_(2)adsorption and activation.Our research provides a practical framework for developing advanced photo-Fenton catalysts,which can be used to treat emerging and refractory organic pollutants more effectively.
