Due to the oxygen storage and release properties,cerium zirconium mixed oxides are recognized as the key material in automotive three-way catalysts.To reveal the effects of co-precipitation temperature on structure,ph...Due to the oxygen storage and release properties,cerium zirconium mixed oxides are recognized as the key material in automotive three-way catalysts.To reveal the effects of co-precipitation temperature on structure,physical and chemical properties of multi-doped cerium zirconium mixed oxides,a series of La and Y doped cerium zirconium mixed oxides(CZLYs)were synthesized via a co-precipitation method,and the physical and chemical properties of CZLYs were systemically characterized by XRD,N_(2) adsorption−desorption,TEM,XPS,oxygen storage capacity(OSC)and hydrogen temperature programmed reduction(H_(2)-TPR).The results show that co-precipitation temperature is an important parameter to influence the crystal size,oxygen storage capacity and thermal stability of CZLYs.When the co-precipitation temperature was 60℃,the best redox properties and thermal stability of CZLYs were obtained.After thermal treatment at 1100℃for 10 h,the specific surface area and oxygen storage capacity of the corresponding aged sample were 15.42 m^(2)/g and 497.7μmol/g,respectively.In addition,a mechanism was proposed to reveal the effects of co-precipitation temperature on the structure and properties of CZLYs.展开更多
The ceria-zirconia compound oxide-supported noble metal Pd(Pd@CZ)is widely used in three-way catalyst.Moreover,the surface structure of CZ plays an important role in catalytic activity of Pd.However,how to regulate th...The ceria-zirconia compound oxide-supported noble metal Pd(Pd@CZ)is widely used in three-way catalyst.Moreover,the surface structure of CZ plays an important role in catalytic activity of Pd.However,how to regulate the surface structure of CZ and clarify the structure–activity relationship is still a challenge.In this paper,a strategy is proposed to develop high activity Pd@CZ nanocatalysts by tuning Y doping sites in CZ.The precipitate-deposition method is developed to prepare the novel Ce_(0.485)Zr_(0.485)Y_(0.03)O_(2) composite with surface doping of Y(CZ-Y-S).In addition,the Pd@CZ-Y-S(Pd supported on CZ-Y-S)exhibits superior catalytic activity for HC,CO,and NO oxide,wherein,for CO and C_(3)H_(6) oxidation,the low-temperature activity of Pd@CZ-Y-S is still 20%higher than that of Pd@CZ-Y-B(Y bulk doping)and commercial Pd@CZ after 1000℃/4 h aging.The effect mechanism is further studied by density functional theory(DFT)calculation.Compared with Pd@CZ-Y-B,Pd@CZ-Y-S shows the lower CO oxide reaction energy barriers due to the weaker adsorption strength of O2.The Y surface doping strategy could provide valuable insights for the development of highly efficient Pd@CZ catalyst with extensive applications.展开更多
基金the Hebei Key Research and Development Program,China(No.20374202D)the Hebei High Level Talent Team Building,China(No.205A1104H).
文摘Due to the oxygen storage and release properties,cerium zirconium mixed oxides are recognized as the key material in automotive three-way catalysts.To reveal the effects of co-precipitation temperature on structure,physical and chemical properties of multi-doped cerium zirconium mixed oxides,a series of La and Y doped cerium zirconium mixed oxides(CZLYs)were synthesized via a co-precipitation method,and the physical and chemical properties of CZLYs were systemically characterized by XRD,N_(2) adsorption−desorption,TEM,XPS,oxygen storage capacity(OSC)and hydrogen temperature programmed reduction(H_(2)-TPR).The results show that co-precipitation temperature is an important parameter to influence the crystal size,oxygen storage capacity and thermal stability of CZLYs.When the co-precipitation temperature was 60℃,the best redox properties and thermal stability of CZLYs were obtained.After thermal treatment at 1100℃for 10 h,the specific surface area and oxygen storage capacity of the corresponding aged sample were 15.42 m^(2)/g and 497.7μmol/g,respectively.In addition,a mechanism was proposed to reveal the effects of co-precipitation temperature on the structure and properties of CZLYs.
基金This study was financially supported by the National Natural Science Foundation of China(No.52204376)Youth Foundation of Hebei Province(No.E2022103007)+2 种基金Young Elite Scientists Sponsorship Program by CAST 2021QNRC001High Tech Zone Science and Technology Project of Yanjiao(No.YJXM211211)Youth Fund Project of GRINM(No.G12620223129035).
文摘The ceria-zirconia compound oxide-supported noble metal Pd(Pd@CZ)is widely used in three-way catalyst.Moreover,the surface structure of CZ plays an important role in catalytic activity of Pd.However,how to regulate the surface structure of CZ and clarify the structure–activity relationship is still a challenge.In this paper,a strategy is proposed to develop high activity Pd@CZ nanocatalysts by tuning Y doping sites in CZ.The precipitate-deposition method is developed to prepare the novel Ce_(0.485)Zr_(0.485)Y_(0.03)O_(2) composite with surface doping of Y(CZ-Y-S).In addition,the Pd@CZ-Y-S(Pd supported on CZ-Y-S)exhibits superior catalytic activity for HC,CO,and NO oxide,wherein,for CO and C_(3)H_(6) oxidation,the low-temperature activity of Pd@CZ-Y-S is still 20%higher than that of Pd@CZ-Y-B(Y bulk doping)and commercial Pd@CZ after 1000℃/4 h aging.The effect mechanism is further studied by density functional theory(DFT)calculation.Compared with Pd@CZ-Y-B,Pd@CZ-Y-S shows the lower CO oxide reaction energy barriers due to the weaker adsorption strength of O2.The Y surface doping strategy could provide valuable insights for the development of highly efficient Pd@CZ catalyst with extensive applications.