Creating a new low-temperature catalyst in decreasing the emission of volatile organic compounds(VOCs)has great significance under different industrial production situations.In particular,the Zr-UiO-66 is optimized by...Creating a new low-temperature catalyst in decreasing the emission of volatile organic compounds(VOCs)has great significance under different industrial production situations.In particular,the Zr-UiO-66 is optimized by different amounts of cerium,which not only enhances the physicochemical stability but also increases the number of active sites of Ce_(x)Zr_(y)UiO-66.Furthermore,the catalysts with Co_(3)O_(4)nanoparticles supported on Ce_(x)Zr_(y)UiO-66 were successfully prepared via impregnation method.In the process of toluene degradation,the Co/Ce_(1)Zr_(2)-Ui0-66 attains a 90%conversion rate at 210℃with a space velocity of 60000 mL/(g·h)and toluene concentration at 1000×10^(-6).Meanwhile,the carbon dioxide selectivity reaches 100%at 218℃.The Co/Ce_(1)Zr_(2)-UiO-66 shows great water resistance(3 vol%H_(2)O).Multiple characterization methods were used to figure out the physicochemical properties of the catalysts.It is found that the addition of an appropriate amount of cerium can enhance stability of UiO-66 and surface lattice oxygen proportion.Additionally,the stronger electron transfer between Ce^(4+)and Co^(2+)enables the Co/Ce_(1)Zr_(2)-UiO-66 to possess more active surface oxygen species and Co_(3)+cationic species in all samples.展开更多
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
UiO-66,a prototypical and stable zirconium-based metal-organic framework(MOF),consists of zirconium-oxide clusters(Zr_(6)O_(4)(OH)_(4))and benzene-1,4-dicarboxylate(BDC)organic linkers.It exhibits abundant active site...UiO-66,a prototypical and stable zirconium-based metal-organic framework(MOF),consists of zirconium-oxide clusters(Zr_(6)O_(4)(OH)_(4))and benzene-1,4-dicarboxylate(BDC)organic linkers.It exhibits abundant active sites,a high specific surface area,a tunable pore structure,and exceptional chemical and thermal stability,making it highly advantageous for various practical applications.The integration of functional components within UiO-66 has been shown to optimize its electronic properties and coordination environment,thereby enhancing its multifunctionality and catalytic performance.This review highlights the analysis of structural characteristics of UiO-66,explores various modification strategies such as the introduction of functional organic linkers,selection of metal nodes,defect engineering,and doping with external functional components,and discusses its applications in environmental remediation and energy-related fields.展开更多
UiO-66 is a potential material for adsorption heat transformation(AHT)with high specific surface area,and excellent thermal and chemical stability.However,the low water adsorption capacity of UiO-66 in the low relativ...UiO-66 is a potential material for adsorption heat transformation(AHT)with high specific surface area,and excellent thermal and chemical stability.However,the low water adsorption capacity of UiO-66 in the low relative pressure range(0<P/P_(0)<0.3)limits its application in AHT.We prepare the UiO-66 modified by MgCl_(2)through using the solvothermal method and impregnation method,and study their water vapor adsorption performances and heat storage capacities.Attributed to the extremely high saturated water uptake and excellent hydrophilicity of MgCl_(2),the water adsorption performance of UiO-66 is improved,although the introduction of MgCl_(2)reduces its specific surface area and pore volume.The water adsorption capacity at P/P_(0)=0.3 and the saturated water adsorption capacity of the UiO-66(with MgCl_(2)content of 0.57 wt%)modified by the solvothermal method are 0.27 g/g and 0.57 g/g at 298 K,respectively,which are 68.8%and 32.6%higher than the counterparts of pure UiO-66,respectively.Comparing with pure UiO-66,the water adsorption capacity of the UiO-66(with MgCl_(2)content of 1.02 wt%)modified by the impregnation method is increased by 56.3%and 14.0%at the same pressure,respectively.During 20 water adsorption/desorption cycles,the above two materials show high heat storage densities(~1293 J/g and 1378 J/g).Therein,the UiO-66 modified by the solvothermal method exhibits the excellent cyclic stability.These results suggest that the introduction of an appropriate amount of MgCl_(2)makes UiO-66more suitable for AHT applications.展开更多
基金Project supported by National Natural Science Foundation of China(22076180)Youth Innovation Promotion Association of CAS(2019376)Chongqing Bayu Scholar Program(Young Scholar,YS2020048)。
文摘Creating a new low-temperature catalyst in decreasing the emission of volatile organic compounds(VOCs)has great significance under different industrial production situations.In particular,the Zr-UiO-66 is optimized by different amounts of cerium,which not only enhances the physicochemical stability but also increases the number of active sites of Ce_(x)Zr_(y)UiO-66.Furthermore,the catalysts with Co_(3)O_(4)nanoparticles supported on Ce_(x)Zr_(y)UiO-66 were successfully prepared via impregnation method.In the process of toluene degradation,the Co/Ce_(1)Zr_(2)-Ui0-66 attains a 90%conversion rate at 210℃with a space velocity of 60000 mL/(g·h)and toluene concentration at 1000×10^(-6).Meanwhile,the carbon dioxide selectivity reaches 100%at 218℃.The Co/Ce_(1)Zr_(2)-UiO-66 shows great water resistance(3 vol%H_(2)O).Multiple characterization methods were used to figure out the physicochemical properties of the catalysts.It is found that the addition of an appropriate amount of cerium can enhance stability of UiO-66 and surface lattice oxygen proportion.Additionally,the stronger electron transfer between Ce^(4+)and Co^(2+)enables the Co/Ce_(1)Zr_(2)-UiO-66 to possess more active surface oxygen species and Co_(3)+cationic species in all samples.
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supported by the National Natural Science Foundation of China(52371240)the Jiangsu Province Excellent Postdoctoral Program(2022ZB613).
文摘UiO-66,a prototypical and stable zirconium-based metal-organic framework(MOF),consists of zirconium-oxide clusters(Zr_(6)O_(4)(OH)_(4))and benzene-1,4-dicarboxylate(BDC)organic linkers.It exhibits abundant active sites,a high specific surface area,a tunable pore structure,and exceptional chemical and thermal stability,making it highly advantageous for various practical applications.The integration of functional components within UiO-66 has been shown to optimize its electronic properties and coordination environment,thereby enhancing its multifunctionality and catalytic performance.This review highlights the analysis of structural characteristics of UiO-66,explores various modification strategies such as the introduction of functional organic linkers,selection of metal nodes,defect engineering,and doping with external functional components,and discusses its applications in environmental remediation and energy-related fields.
基金Project supported by the National Natural Science Foundation of China(Grant No.51836009)。
文摘UiO-66 is a potential material for adsorption heat transformation(AHT)with high specific surface area,and excellent thermal and chemical stability.However,the low water adsorption capacity of UiO-66 in the low relative pressure range(0<P/P_(0)<0.3)limits its application in AHT.We prepare the UiO-66 modified by MgCl_(2)through using the solvothermal method and impregnation method,and study their water vapor adsorption performances and heat storage capacities.Attributed to the extremely high saturated water uptake and excellent hydrophilicity of MgCl_(2),the water adsorption performance of UiO-66 is improved,although the introduction of MgCl_(2)reduces its specific surface area and pore volume.The water adsorption capacity at P/P_(0)=0.3 and the saturated water adsorption capacity of the UiO-66(with MgCl_(2)content of 0.57 wt%)modified by the solvothermal method are 0.27 g/g and 0.57 g/g at 298 K,respectively,which are 68.8%and 32.6%higher than the counterparts of pure UiO-66,respectively.Comparing with pure UiO-66,the water adsorption capacity of the UiO-66(with MgCl_(2)content of 1.02 wt%)modified by the impregnation method is increased by 56.3%and 14.0%at the same pressure,respectively.During 20 water adsorption/desorption cycles,the above two materials show high heat storage densities(~1293 J/g and 1378 J/g).Therein,the UiO-66 modified by the solvothermal method exhibits the excellent cyclic stability.These results suggest that the introduction of an appropriate amount of MgCl_(2)makes UiO-66more suitable for AHT applications.
