Zirconium-based metal-organic framework UiO-66 was successfully prepared by solvothermal method,and UiO-66 was modified by adding regulators such as formic acid,acetic acid,and hydrochloric acid.The NH_(3)-SCR reactiv...Zirconium-based metal-organic framework UiO-66 was successfully prepared by solvothermal method,and UiO-66 was modified by adding regulators such as formic acid,acetic acid,and hydrochloric acid.The NH_(3)-SCR reactivity of the samples was evaluated by the denitration activity evaluation system,and the UiO-66 and the regulator-modified UiO-66 were characterized by XRD,SEM,BET,FTIR,TG,NH_(3)-TPD,etc.,the effects of regulator types on the structure and properties of UiO-66 were investigated.The experimental results show that,after adding the modifier,the morphology of UiO-66 changes from irregular quadrilateral with serious agglomeration to particles with regular crystal shape and good dispersibility,and the crystal morphology of the catalyst is improved.In addition,after adding the modifier,UiO-66 has a larger specific surface area and stronger surface acidity,which optimizes the catalytic performance of UiO-66.The catalytic performance test results of NH_(3)-SCR show that the low-temperature activity of UiO-66 is poor,and it only shows a certain catalytic activity at higher temperatures.The catalytic activity of UiO-66 was significantly improved after adding the regulator.Among them,the UiO-66-HCl modified with hydrochloric acid had the best catalytic activity,and the denitration rate reached 70%when the denitration temperature was 380℃.展开更多
Metal–organic frameworks(MOFs)with angstrom-sized pores are promising functional nanomaterials for the fabrication of cation permselective membranes(MOF-CPMs).However,only a few research reports show successful prepa...Metal–organic frameworks(MOFs)with angstrom-sized pores are promising functional nanomaterials for the fabrication of cation permselective membranes(MOF-CPMs).However,only a few research reports show successful preparation of the MOF-CPMs with good cation separation performance due to several inherent problems in MOFs,such as arduous selfassembly,poor water resistance,and tedious fabrication strategies.Besides,low cation permeation flux due to the absence of the cation permeation assisting functionalities in MOFs is another big issue,which limits their widespread use in membrane technology.Therefore,it is necessary to fabricate functional MOF-CPMs using simplistic strategies to improve cation permeation.In this context,we report a facile in situ smart growth strategy to successfully produce ultrathin(<600 nm)and leaflike UiO-66-SO3H membranes at the surface of anodic alumina oxide.The physicochemical characterizations confirm that sulfonated angstrom-sized ion transport channels exist in the as-prepared UiO-66-SO3H membranes,which accelerate the cation permeation(~3×faster than non-functionalized UiO-66 membrane)and achieve a high ion selectivity(Na^+/Mg^2+>140).The outstanding cation separation performance validates the importance of introducing sulfonic acid groups in MOF-CPMs.展开更多
Metal-organic frameworks(MOFs)have emerged as a class of promising membrane materials.UiO-66 is a prototypical and stable MOF material with a number of analogues.In this article,we review five approaches for fabricati...Metal-organic frameworks(MOFs)have emerged as a class of promising membrane materials.UiO-66 is a prototypical and stable MOF material with a number of analogues.In this article,we review five approaches for fabricating UiO-66 polycrystalline membranes including synthesis,secondary synthesis,biphase synthesis,gas-phase deposition and electrochemical deposition,as well as their applications in gas separation,pervaporation,nanofiltration and ion separation.On this basis,we propose possible methods for scalable synthesis of UiO-66 membranes and their potential separation applications in the future.展开更多
基金Funded by the National Key Research and Development Program of China(No.2016YFC0209302)。
文摘Zirconium-based metal-organic framework UiO-66 was successfully prepared by solvothermal method,and UiO-66 was modified by adding regulators such as formic acid,acetic acid,and hydrochloric acid.The NH_(3)-SCR reactivity of the samples was evaluated by the denitration activity evaluation system,and the UiO-66 and the regulator-modified UiO-66 were characterized by XRD,SEM,BET,FTIR,TG,NH_(3)-TPD,etc.,the effects of regulator types on the structure and properties of UiO-66 were investigated.The experimental results show that,after adding the modifier,the morphology of UiO-66 changes from irregular quadrilateral with serious agglomeration to particles with regular crystal shape and good dispersibility,and the crystal morphology of the catalyst is improved.In addition,after adding the modifier,UiO-66 has a larger specific surface area and stronger surface acidity,which optimizes the catalytic performance of UiO-66.The catalytic performance test results of NH_(3)-SCR show that the low-temperature activity of UiO-66 is poor,and it only shows a certain catalytic activity at higher temperatures.The catalytic activity of UiO-66 was significantly improved after adding the regulator.Among them,the UiO-66-HCl modified with hydrochloric acid had the best catalytic activity,and the denitration rate reached 70%when the denitration temperature was 380℃.
基金funding supported by the National Natural Science Foundation of China(Nos.21490581,91534203,21878282,and 21606215)
文摘Metal–organic frameworks(MOFs)with angstrom-sized pores are promising functional nanomaterials for the fabrication of cation permselective membranes(MOF-CPMs).However,only a few research reports show successful preparation of the MOF-CPMs with good cation separation performance due to several inherent problems in MOFs,such as arduous selfassembly,poor water resistance,and tedious fabrication strategies.Besides,low cation permeation flux due to the absence of the cation permeation assisting functionalities in MOFs is another big issue,which limits their widespread use in membrane technology.Therefore,it is necessary to fabricate functional MOF-CPMs using simplistic strategies to improve cation permeation.In this context,we report a facile in situ smart growth strategy to successfully produce ultrathin(<600 nm)and leaflike UiO-66-SO3H membranes at the surface of anodic alumina oxide.The physicochemical characterizations confirm that sulfonated angstrom-sized ion transport channels exist in the as-prepared UiO-66-SO3H membranes,which accelerate the cation permeation(~3×faster than non-functionalized UiO-66 membrane)and achieve a high ion selectivity(Na^+/Mg^2+>140).The outstanding cation separation performance validates the importance of introducing sulfonic acid groups in MOF-CPMs.
文摘Metal-organic frameworks(MOFs)have emerged as a class of promising membrane materials.UiO-66 is a prototypical and stable MOF material with a number of analogues.In this article,we review five approaches for fabricating UiO-66 polycrystalline membranes including synthesis,secondary synthesis,biphase synthesis,gas-phase deposition and electrochemical deposition,as well as their applications in gas separation,pervaporation,nanofiltration and ion separation.On this basis,we propose possible methods for scalable synthesis of UiO-66 membranes and their potential separation applications in the future.
