Efficient and selective extraction of uranium(U(VI))from seawater is essential for sustainable nuclear power production.This study reports a novel adsorbent zeolitic imidazolate framework(ZIF)-67@SiO_(2)-A/polyacrylam...Efficient and selective extraction of uranium(U(VI))from seawater is essential for sustainable nuclear power production.This study reports a novel adsorbent zeolitic imidazolate framework(ZIF)-67@SiO_(2)-A/polyacrylamide(PAM)which was synthesized by grafting the core–shell metal–organic frameworks(MOFs)-based nanostructures coated with the 3-aminopropyl triethoxysilane(APTES)functionalized SiO_(2)(SiO_(2)-A)onto PAM hydrogel.The SiO_(2) shell was grown on the surface of MOF,which improved the acid-base resistance of MOF.The introduction of ZIF-67@SiO_(2)-A enhances the specific surface area and adsorption efficiency of the PAM.The ZIF-67@SiO_(2)-A/PAM shows remarkable adsorption capacity,fast adsorption kinetics,and good reusability for uranium.It has excellent adsorption property(6.33 mg·g^(-1),30 d)in natural seawater.The X-ray photoelectron spectroscopy(XPS),Fourier transform infrared(FTIR),energy dispersive spectroscopy(EDS)mappings,and density functional theory reveal that the coordination by N and O in ZIF-67@SiO_(2)-A/PAM with uranium is the main mechanism of uranium adsorption.Thus,ZIF-67@SiO_(2)-A/PAM has great potential to capture uranium from natural seawater.展开更多
Efficient capture of uranium(VI)(U(VI))from seawater is of great significance to the sustainable development of nuclear energy and environmental protection,which is also a serious challenge at present.In this study,ho...Efficient capture of uranium(VI)(U(VI))from seawater is of great significance to the sustainable development of nuclear energy and environmental protection,which is also a serious challenge at present.In this study,hollow Zn/Co zeolitic imidazolate framework(H-ZIF)was decorated on polyacrylamide/sodium alginate(PAM/SA)hydrogel by chelating and covalently crosslinking,and a new type of PAM/SA/H-ZIF hydrogel was synthesized.The combination of PAM/SA and H-ZIF gives PAM/SA/H-ZIF hydrogel excellent mechanical properties,good stability,and abundant surface functional groups,which is beneficial to improving the adsorption properties.The extraction amount of U(VI)by PAM/SA/H-ZIF is 171.14 mg·g^(-1)at C_(0)=99.52 mg·L^(-1)and pH=5.0.The adsorption equilibrium is reached in 120 min and the adsorption process fits well with Langmuir isotherm model and pseudo-second-order rate equation.The PAM/SA/H-ZIF also showed good recyclability and stability after 10 cycles of adsorption-desorption.More importantly,the rate of uranium adsorption is 0.196 mg·g^(-1)·day^(-1)after 30 days,which implies that the PAM/SA/H-ZIF could serve as a potential adsorbent for the development of uranium capture from seawater.展开更多
基金supported by the National Key R&D Program of China(No.2019YFA0706802)the National Natural Science Foundation of China(No.52002356 and U20A20141)+1 种基金China Postdoctoral Science Foundation(No.2023M731020)Project for Young Scientists in Basic Research(No.YSBR-039).
文摘Efficient and selective extraction of uranium(U(VI))from seawater is essential for sustainable nuclear power production.This study reports a novel adsorbent zeolitic imidazolate framework(ZIF)-67@SiO_(2)-A/polyacrylamide(PAM)which was synthesized by grafting the core–shell metal–organic frameworks(MOFs)-based nanostructures coated with the 3-aminopropyl triethoxysilane(APTES)functionalized SiO_(2)(SiO_(2)-A)onto PAM hydrogel.The SiO_(2) shell was grown on the surface of MOF,which improved the acid-base resistance of MOF.The introduction of ZIF-67@SiO_(2)-A enhances the specific surface area and adsorption efficiency of the PAM.The ZIF-67@SiO_(2)-A/PAM shows remarkable adsorption capacity,fast adsorption kinetics,and good reusability for uranium.It has excellent adsorption property(6.33 mg·g^(-1),30 d)in natural seawater.The X-ray photoelectron spectroscopy(XPS),Fourier transform infrared(FTIR),energy dispersive spectroscopy(EDS)mappings,and density functional theory reveal that the coordination by N and O in ZIF-67@SiO_(2)-A/PAM with uranium is the main mechanism of uranium adsorption.Thus,ZIF-67@SiO_(2)-A/PAM has great potential to capture uranium from natural seawater.
基金This work was supported by the National Natural Science Foundation of China(Nos.52002356 and U20A20141)the National Key Research and Development Program of China(No.2019YFA0706802)+1 种基金the China Postdoctoral Science Foundation(No.2020M672269)the Project for Young Scientists in Basic Research(No.YSBR-039).
文摘Efficient capture of uranium(VI)(U(VI))from seawater is of great significance to the sustainable development of nuclear energy and environmental protection,which is also a serious challenge at present.In this study,hollow Zn/Co zeolitic imidazolate framework(H-ZIF)was decorated on polyacrylamide/sodium alginate(PAM/SA)hydrogel by chelating and covalently crosslinking,and a new type of PAM/SA/H-ZIF hydrogel was synthesized.The combination of PAM/SA and H-ZIF gives PAM/SA/H-ZIF hydrogel excellent mechanical properties,good stability,and abundant surface functional groups,which is beneficial to improving the adsorption properties.The extraction amount of U(VI)by PAM/SA/H-ZIF is 171.14 mg·g^(-1)at C_(0)=99.52 mg·L^(-1)and pH=5.0.The adsorption equilibrium is reached in 120 min and the adsorption process fits well with Langmuir isotherm model and pseudo-second-order rate equation.The PAM/SA/H-ZIF also showed good recyclability and stability after 10 cycles of adsorption-desorption.More importantly,the rate of uranium adsorption is 0.196 mg·g^(-1)·day^(-1)after 30 days,which implies that the PAM/SA/H-ZIF could serve as a potential adsorbent for the development of uranium capture from seawater.