Post-synthetic functionalization of covalent organic frameworks(COFs)is an alternative way to enhance and broaden their properties and potential applications.However,the chemical functionalization of COFs is a great c...Post-synthetic functionalization of covalent organic frameworks(COFs)is an alternative way to enhance and broaden their properties and potential applications.However,the chemical functionalization of COFs is a great challenge because traditional procedures are often time-and energy-consuming,while the crystallinity of COFs can be damaged under harsh conditions.Here we report the in-situ introduction of functional graft chains onto the skeleton of COFs during the synthesis process through the combination of radiation-induced synthesis and graft polymerization techniques under ^(60)Co gamma-ray radiation.The synthesis and functionalization of COFs are simultaneously accomplished in a chemical system under ambient conditions yielding a large number of different functionalized COFs.The obtained carboxyl-functionalized COFs exhibit excellent radioactive uranium removal capabilities from aqueous solution with fast uptake dynamics,high adsorption capacity,and excellent selectivity over other competing metal ions.展开更多
To further improve the removal ability of layered double hydroxide(LDH) for iodide(I^-) anions from wastewater, we prepared hierarchically porous Cu5Mg10Al5-LDH and used as a matrix for in suit growth of Cu/Cu2O on it...To further improve the removal ability of layered double hydroxide(LDH) for iodide(I^-) anions from wastewater, we prepared hierarchically porous Cu5Mg10Al5-LDH and used as a matrix for in suit growth of Cu/Cu2O on its surface, forming Cu/Cu2O-LDH, which was characterized and applied as an adsorbent.Results displayed high I^-saturation uptake capability(137.8 mg/g) of Cu/Cu2O-LDH compared with Cu5Mg10Al5-LDH(26.4 mg/g) even thermal activated LDH(76.1 mg/g).Thermodynamic analysis showed that the reaction between I^-anions and Cu/Cu2O-LDH is a spontaneous and exothermic.Uptake kinetics analysis exhibited that adsorption equilibrium can be reached after 265 min.Additionally, the adsorbent showed satisfactory selectivity in the presence of competitive anions(e.g., SO4^2-), and could achieve good adsorption performance in a wide pH range of 3–8.A cooperative adsorption mechanism was proposed on the basis of the following two aspects:(1) ion exchange between iodide and interlayer anions;(2) the adsorption performance of Cu, Cu(Ⅱ) and Cu2O for I^-.Meanwhile, the difference between the adsorption mechanism of Cu/Cu2O-LDH, Cu5Mg10Al5-LDH and Cu5Mg10Al5-CLDH adsorbents was also elaborated and verified.展开更多
基金supported by the National Key R&D Program of China(2021YFB3200400)the National Natural Science Foundation of China(21825601,21790374)+2 种基金the fellowship of China National Postdoctoral Program for Innovative Talents(BX20220223)the fellowship of China Postdoctoral Science Foundation(2022M710103)Jiangsu Postdoctoral Program for Excellence(2022ZB588)。
文摘Post-synthetic functionalization of covalent organic frameworks(COFs)is an alternative way to enhance and broaden their properties and potential applications.However,the chemical functionalization of COFs is a great challenge because traditional procedures are often time-and energy-consuming,while the crystallinity of COFs can be damaged under harsh conditions.Here we report the in-situ introduction of functional graft chains onto the skeleton of COFs during the synthesis process through the combination of radiation-induced synthesis and graft polymerization techniques under ^(60)Co gamma-ray radiation.The synthesis and functionalization of COFs are simultaneously accomplished in a chemical system under ambient conditions yielding a large number of different functionalized COFs.The obtained carboxyl-functionalized COFs exhibit excellent radioactive uranium removal capabilities from aqueous solution with fast uptake dynamics,high adsorption capacity,and excellent selectivity over other competing metal ions.
基金supported by the National Natural Science Foundation of China(Nos.11805101 and 11205089)the Jiangsu Engineering Technology Research Center of Environmental Cleaning Materials(No.KFK1504)the Environmental Protection Research Project of Jiangsu Province(No.JSZC-D2018-044).
文摘To further improve the removal ability of layered double hydroxide(LDH) for iodide(I^-) anions from wastewater, we prepared hierarchically porous Cu5Mg10Al5-LDH and used as a matrix for in suit growth of Cu/Cu2O on its surface, forming Cu/Cu2O-LDH, which was characterized and applied as an adsorbent.Results displayed high I^-saturation uptake capability(137.8 mg/g) of Cu/Cu2O-LDH compared with Cu5Mg10Al5-LDH(26.4 mg/g) even thermal activated LDH(76.1 mg/g).Thermodynamic analysis showed that the reaction between I^-anions and Cu/Cu2O-LDH is a spontaneous and exothermic.Uptake kinetics analysis exhibited that adsorption equilibrium can be reached after 265 min.Additionally, the adsorbent showed satisfactory selectivity in the presence of competitive anions(e.g., SO4^2-), and could achieve good adsorption performance in a wide pH range of 3–8.A cooperative adsorption mechanism was proposed on the basis of the following two aspects:(1) ion exchange between iodide and interlayer anions;(2) the adsorption performance of Cu, Cu(Ⅱ) and Cu2O for I^-.Meanwhile, the difference between the adsorption mechanism of Cu/Cu2O-LDH, Cu5Mg10Al5-LDH and Cu5Mg10Al5-CLDH adsorbents was also elaborated and verified.
