Various materials have been developed for environmental remediation of mercury ion pollution.Among these materials,covalent organic frameworks(COFs)can efficiently adsorb Hg(II)fromwater.Herein,two thiol-modified COFs...Various materials have been developed for environmental remediation of mercury ion pollution.Among these materials,covalent organic frameworks(COFs)can efficiently adsorb Hg(II)fromwater.Herein,two thiol-modified COFs(COF-S-SH and COF-OH-SH)were prepared,through the reaction between 2,5-divinylterephthalaldehyde and 1,3,5-tris-(4-aminophenyl)benzene,followed by post-synthetic modification using bis(2-mercaptoethyl)sulfide and dithiothreitol,respectively.The modified COFs showed excellent Hg(II)adsorption abilities with maximum adsorption capacities of 586.3 and 535.5 mg g^(-1)for COF-S-SH and COF-OH-SH,respectively.The prepared materials showed excellent selective absorbability for Hg(II)against multiple cationic metals in water.Unexpectedly,the experimental data showed that both co-existing toxic anionic diclofenac sodium(DCF)and Hg(II)performed positive effect for capturing another pollutant by these two modified COFs.Thus,a synergistic adsorption mechanism between Hg(II)and DCF on COFs was proposed.Moreover,density functional theory calculations revealed that synergistic adsorption occurred between Hg(II)and DCF,which resulted in a significant reduction in the adsorption system's energy.This work highlights a new direction for application of COFs to simultaneous removal of heavy metals and co-existing organic pollutants from water.展开更多
基金supported by the International Cooperation Project of Qinghai Province(Grant No.2021-HZ-809)the Key Youth Foundation of Qinghai University(Grant No.2021-QGY-1).
文摘Various materials have been developed for environmental remediation of mercury ion pollution.Among these materials,covalent organic frameworks(COFs)can efficiently adsorb Hg(II)fromwater.Herein,two thiol-modified COFs(COF-S-SH and COF-OH-SH)were prepared,through the reaction between 2,5-divinylterephthalaldehyde and 1,3,5-tris-(4-aminophenyl)benzene,followed by post-synthetic modification using bis(2-mercaptoethyl)sulfide and dithiothreitol,respectively.The modified COFs showed excellent Hg(II)adsorption abilities with maximum adsorption capacities of 586.3 and 535.5 mg g^(-1)for COF-S-SH and COF-OH-SH,respectively.The prepared materials showed excellent selective absorbability for Hg(II)against multiple cationic metals in water.Unexpectedly,the experimental data showed that both co-existing toxic anionic diclofenac sodium(DCF)and Hg(II)performed positive effect for capturing another pollutant by these two modified COFs.Thus,a synergistic adsorption mechanism between Hg(II)and DCF on COFs was proposed.Moreover,density functional theory calculations revealed that synergistic adsorption occurred between Hg(II)and DCF,which resulted in a significant reduction in the adsorption system's energy.This work highlights a new direction for application of COFs to simultaneous removal of heavy metals and co-existing organic pollutants from water.
