As a new frontier in catalysis field,single-atom catalysts(SACs)hold unique electronic structure and high atom utilization,which have displayed unprecedented activity and selectivity toward a wide range of catalytic r...As a new frontier in catalysis field,single-atom catalysts(SACs)hold unique electronic structure and high atom utilization,which have displayed unprecedented activity and selectivity toward a wide range of catalytic reactions.However,many reported SACs are susceptible to Ostwald ripening process in high temperature environment or long-term catalytic application,which will cause sintering and deactivation.This is due to the weak interaction between the metal atom and supports.The regeneration and recycling of deactivated catalysts will greatly increase the time and economic cost of industrial production.Therefore,it is necessary to develop SACs with excellent thermal stability to meet the industrial demands.Here,we discuss the fundamental comprehension of the stability of thermally stable SACs obtained from different synthesis methods.The influences of the speciation of metal centers and coordination environments on thermal stability are summarized.The importance of using novel in situ and operando characterizations to reveal dynamic structural evolution under synthesis and reaction conditions and to identify active sites of thermally stable SACs is highlighted.The mechanistic understanding of the unique role of thermally stable SACs in thermocatalytic application is also discussed.At last,a brief perspective on the remaining challenges and future directions of thermally stable SACs is presented.展开更多
Ti4+-mixed FePO4·xH2O precursor was prepared by co-precipitation method,with which Ti4+ cations were added in the process of preparing FePO4·xH2O to pursue an effective and homogenous doping way.Ti4+-doped L...Ti4+-mixed FePO4·xH2O precursor was prepared by co-precipitation method,with which Ti4+ cations were added in the process of preparing FePO4·xH2O to pursue an effective and homogenous doping way.Ti4+-doped LiFePO4 was prepared by an ambient-reduction and post-sintering method using the as-prepared precursor,Li2CO3 and oxalic acid as raw materials.The samples were characterized by scanning electron microscopy (SEM),X-ray diffractometry (XRD),electrochemical impedance spectroscopy (EIS),and electrochemical charge/discharge test.Effects of Ti4+-doping and sintering temperature on the physical and electrochemical performance of LiFePO4 powders were investigated.It is noted that Ti4+-doping can improve the electrochemical performance of LiFePO4 remarkably.The Ti4+-doped sample sintered at 600 ℃ delivers an initial discharge capacity of 150,130 and 125 mA·h/g with 0.1C,1C and 2C rates,respectively,without fading after 40 cycles.展开更多
The desulfurater(BaAl2O4) was successfully synthesized with BaCO3 and Al(OH)3 powders as raw materials by microwave sintering method.The mass loss of raw materials and the characterization of the outcome were investig...The desulfurater(BaAl2O4) was successfully synthesized with BaCO3 and Al(OH)3 powders as raw materials by microwave sintering method.The mass loss of raw materials and the characterization of the outcome were investigated by means of TG-DSC,XRD and optical microscopy.The reaction mechanism was discussed.The experimental results show that synthesized BaAl2O4 by microwave sintering method is feasible.Compared with conventional sintering method,microwave sintering is a better way to synthesize BaAl2O4 with advantages of low temperature sintering,short time sintering and high synthesis rate.展开更多
Pure Ca-SiAlON:Eu2+ was synthesized by microwave sintering method at a relatively low temperature of 1550℃.Photoluminescence intensity of the resultant phosphor was higher than those of the samples synthesized by con...Pure Ca-SiAlON:Eu2+ was synthesized by microwave sintering method at a relatively low temperature of 1550℃.Photoluminescence intensity of the resultant phosphor was higher than those of the samples synthesized by conventional gas-pressure sintering technique at 1750℃.When it was excited at 450 nm,the as-prepared yellow Ca-SiAlON:Eu2+ sample had an external quantum efficiency of 42%,comparable to the sample synthesized at 1750℃ under 0.5 MPaN2 gas pressure by the GPS method reported in reference.The experimental results demonstrated that the microwave sintering method was also an interesting approach for synthesizing nitride phosphors,which promises lower firing temperature than those by carbothermal reduction and nitridation (CRN) methods,higher heating rate and shorter duration time compared with those by gas-pressure sintering.展开更多
Porous tetragonal BaTiO 3 ceramic was successfully prepared by a combination of hydrothermal and low-temperature-sintering method.The hollow TiO2@BaCO 3 as the sintering precursor was synthesized via a simple hydrothe...Porous tetragonal BaTiO 3 ceramic was successfully prepared by a combination of hydrothermal and low-temperature-sintering method.The hollow TiO2@BaCO 3 as the sintering precursor was synthesized via a simple hydrothermal method,and then porous BaTiO 3 was generated by calcining the hollow TiO2@BaCO 3 precursor at 900 ℃ without additive.The hollow TiO2@BaCO 3 structure plays two important roles in the preparing of the porous BaTiO 3 ceramic.First,the TiO2@BaCO 3 hollow structure provides high surface areas and increases the contact points between BaCO 3 and TiO2,which can reduce the sintering temperature of the BaTiO 3 ceramic.Second,the cavity of the ordered arranged TiO2@BaCO 3 hollow sphere shows important influence on the porous structure,and the pore size of the as-prepared porous BaTiO 3 ceramic can be tuned from several nanometers to hundreds nanomters by changing the sintering temperature.The formation mechanism of the porous BaTiO 3 ceramic was proposed.展开更多
文摘As a new frontier in catalysis field,single-atom catalysts(SACs)hold unique electronic structure and high atom utilization,which have displayed unprecedented activity and selectivity toward a wide range of catalytic reactions.However,many reported SACs are susceptible to Ostwald ripening process in high temperature environment or long-term catalytic application,which will cause sintering and deactivation.This is due to the weak interaction between the metal atom and supports.The regeneration and recycling of deactivated catalysts will greatly increase the time and economic cost of industrial production.Therefore,it is necessary to develop SACs with excellent thermal stability to meet the industrial demands.Here,we discuss the fundamental comprehension of the stability of thermally stable SACs obtained from different synthesis methods.The influences of the speciation of metal centers and coordination environments on thermal stability are summarized.The importance of using novel in situ and operando characterizations to reveal dynamic structural evolution under synthesis and reaction conditions and to identify active sites of thermally stable SACs is highlighted.The mechanistic understanding of the unique role of thermally stable SACs in thermocatalytic application is also discussed.At last,a brief perspective on the remaining challenges and future directions of thermally stable SACs is presented.
基金Project(2007CB613607) supported by the National Basic Research Program of China
文摘Ti4+-mixed FePO4·xH2O precursor was prepared by co-precipitation method,with which Ti4+ cations were added in the process of preparing FePO4·xH2O to pursue an effective and homogenous doping way.Ti4+-doped LiFePO4 was prepared by an ambient-reduction and post-sintering method using the as-prepared precursor,Li2CO3 and oxalic acid as raw materials.The samples were characterized by scanning electron microscopy (SEM),X-ray diffractometry (XRD),electrochemical impedance spectroscopy (EIS),and electrochemical charge/discharge test.Effects of Ti4+-doping and sintering temperature on the physical and electrochemical performance of LiFePO4 powders were investigated.It is noted that Ti4+-doping can improve the electrochemical performance of LiFePO4 remarkably.The Ti4+-doped sample sintered at 600 ℃ delivers an initial discharge capacity of 150,130 and 125 mA·h/g with 0.1C,1C and 2C rates,respectively,without fading after 40 cycles.
基金Project(50264001) supported by the National Natural Science Foundation of ChinaProject(QKH-J-2008-2009) supported by Guizhou Science and Technology Department, China
文摘The desulfurater(BaAl2O4) was successfully synthesized with BaCO3 and Al(OH)3 powders as raw materials by microwave sintering method.The mass loss of raw materials and the characterization of the outcome were investigated by means of TG-DSC,XRD and optical microscopy.The reaction mechanism was discussed.The experimental results show that synthesized BaAl2O4 by microwave sintering method is feasible.Compared with conventional sintering method,microwave sintering is a better way to synthesize BaAl2O4 with advantages of low temperature sintering,short time sintering and high synthesis rate.
基金supported by the National Natural Science Foundation of China(51102252 and 51272259)the Special Foundation for Young Scientists of Zhejiang Province(R12E020005)
文摘Pure Ca-SiAlON:Eu2+ was synthesized by microwave sintering method at a relatively low temperature of 1550℃.Photoluminescence intensity of the resultant phosphor was higher than those of the samples synthesized by conventional gas-pressure sintering technique at 1750℃.When it was excited at 450 nm,the as-prepared yellow Ca-SiAlON:Eu2+ sample had an external quantum efficiency of 42%,comparable to the sample synthesized at 1750℃ under 0.5 MPaN2 gas pressure by the GPS method reported in reference.The experimental results demonstrated that the microwave sintering method was also an interesting approach for synthesizing nitride phosphors,which promises lower firing temperature than those by carbothermal reduction and nitridation (CRN) methods,higher heating rate and shorter duration time compared with those by gas-pressure sintering.
基金supported by the National Natural Science Foundation of China (50972130,20701033,51172209,91122022)Zhejiang Environmental Protection Bureau Foundation (2011B19)China Postdoctoral Science Foundation (201003048)
文摘Porous tetragonal BaTiO 3 ceramic was successfully prepared by a combination of hydrothermal and low-temperature-sintering method.The hollow TiO2@BaCO 3 as the sintering precursor was synthesized via a simple hydrothermal method,and then porous BaTiO 3 was generated by calcining the hollow TiO2@BaCO 3 precursor at 900 ℃ without additive.The hollow TiO2@BaCO 3 structure plays two important roles in the preparing of the porous BaTiO 3 ceramic.First,the TiO2@BaCO 3 hollow structure provides high surface areas and increases the contact points between BaCO 3 and TiO2,which can reduce the sintering temperature of the BaTiO 3 ceramic.Second,the cavity of the ordered arranged TiO2@BaCO 3 hollow sphere shows important influence on the porous structure,and the pore size of the as-prepared porous BaTiO 3 ceramic can be tuned from several nanometers to hundreds nanomters by changing the sintering temperature.The formation mechanism of the porous BaTiO 3 ceramic was proposed.