Improving and optimizing the target properties of ceramics via the high entropy strategy has attracted significant attention.Rare earth niobate is a potential thermal barrier coating(TBCs)material,but its poor high-te...Improving and optimizing the target properties of ceramics via the high entropy strategy has attracted significant attention.Rare earth niobate is a potential thermal barrier coating(TBCs)material,but its poor high-temperature phase stability limits its further application.In this work,four sets of TBCs high-entropy ceramics,(Sm_(1/5)Dy_(1/5)Ho_(1/5)Er_(1/5)Yb_(1/5))(Nb_(1/2)Ta_(1/2))O_(4)(5NbTa),(Sm_(1/6)Dy_(1/6)Ho_(1/6)Er_(1/6)Yb_(1/6)Lu_(1/6))(Nb_(1/2)Ta_(1/2))O_(4)(6NbTa),(Sm_(1/7)Gd_(1/7)Dy_(1/7)Ho_(1/7)Er_(1/7)Yb_(1/7)Lu_(1/7))(Nb_(1/2)Ta_(1/2))O_(4)(7NbTa),(Sm_(1/8)Gd_(1/8)Dy_(1/8)Ho_(1/8)Er_(1/8)Tm_(1/8)Yb_(1/8)Lu_(1/8))(Nb_(1/2)Ta_(1/2))O_(4)(8NbTa)are synthesized using a solid-state reaction method at 1650℃for 6 h.Firstly,the X-ray diffractometer(XRD)patterns display that the samples are all single-phase solid solution structures(space group C 2/c).Differential scanning calorimetry(DSC)and the high-temperature XRD of 8NbTa cross-check that the addition of Ta element in 8HERN increases the phase transition temperature above 1400℃,which can be attributed to that the Ta/Nb co-doping at B site introduces the fluctuation of the bond strength of Ta-O and Nb-O.Secondly,compared to high-entropy rare-earth niobates,the introduction of Ta atoms at B site substantially reduce thermal conductivity(re-duced by 44%,800℃)with the seven components high entropy ceramic as an example.The low thermal conductivity means strong phonon scattering,which may originate from the softening acoustic mode and flattened phonon dispersion in 5–8 principal element high entropy rare earth niobium tantalates(5–8NbTa)revealed by the first-principles calculations.Thirdly,the Ta/Nb co-doping in 5–8NbTa systems can further optimize the insulation performance of oxygen ions.The oxygen-ion conductivity of 8NbTa(3.31×10^(−6)S cm^(−1),900℃)is about 5 times lower than that of 8HERN(15.8×10^(−6)S cm^(−1),900℃)because of the sluggish diffusion effect,providing better oxygen barrier capacity in 5–8NbTa systems to inhibit the overgrowth of the thermal growth oxide(TGO)of TBCs.In addition,influenced by lattice dis-tortion and solid solution strengthening,the samples possess higher hardness(7.51–8.15 GPa)and TECs(9.78×10^(−6)K−1^(-1)0.78×10^(−6)K^(−1),1500℃)than the single rare-earth niobates and tantalates.Based on their excellent overall properties,it is considered that 5–8NbTa can be used as auspicious TBCs.展开更多
To improve the conductivity of Y2O3-stabilized ZrO2 （YSZ） based oxygen-ion conductor, Zr0.85Y0.15O1.925-La9.33Si6O26 （YSZ-LSO） composite ceramics with the mass fraction of La9.33Si6O26 （LSO） of 15% were prepared...To improve the conductivity of Y2O3-stabilized ZrO2 （YSZ） based oxygen-ion conductor, Zr0.85Y0.15O1.925-La9.33Si6O26 （YSZ-LSO） composite ceramics with the mass fraction of La9.33Si6O26 （LSO） of 15% were prepared by using a modified coprecipitation method. The phases, microstructures and conductivities of the YSZ, LSO and YSZ-LSO were investigated by X-ray diffraction, electron microscopy and complex impedance, respectively. The results show that the as-calcined powder of YSZ-LSO composite has the grain size less than 10 nm, and the as-sintered composite ceramics are composed of YSZ and LSO phases. The conductivity can be enhanced obviously by composite method. At 700 ℃, the conductivity of the composite ceramic is 0.125 S/cm, which is one order in magnitude higher than that of the YSZ ceramic and two orders in magnitude higher than that of LSO ceramic. By analyzing the impedance spectra and modulus spectra, the interfacial effect on the conductivity improvement was proposed.展开更多
基金support from Yunnan Major Scientific and Technological Projects(No.202302AG050010)Yunnan Fundamental Research Projects(Nos.202101AW070011 and202101BE070001–015)+1 种基金National Natural Science Foundation of China(No.52303295)Project Funds of“Xingdian Talent Support Program”.
文摘Improving and optimizing the target properties of ceramics via the high entropy strategy has attracted significant attention.Rare earth niobate is a potential thermal barrier coating(TBCs)material,but its poor high-temperature phase stability limits its further application.In this work,four sets of TBCs high-entropy ceramics,(Sm_(1/5)Dy_(1/5)Ho_(1/5)Er_(1/5)Yb_(1/5))(Nb_(1/2)Ta_(1/2))O_(4)(5NbTa),(Sm_(1/6)Dy_(1/6)Ho_(1/6)Er_(1/6)Yb_(1/6)Lu_(1/6))(Nb_(1/2)Ta_(1/2))O_(4)(6NbTa),(Sm_(1/7)Gd_(1/7)Dy_(1/7)Ho_(1/7)Er_(1/7)Yb_(1/7)Lu_(1/7))(Nb_(1/2)Ta_(1/2))O_(4)(7NbTa),(Sm_(1/8)Gd_(1/8)Dy_(1/8)Ho_(1/8)Er_(1/8)Tm_(1/8)Yb_(1/8)Lu_(1/8))(Nb_(1/2)Ta_(1/2))O_(4)(8NbTa)are synthesized using a solid-state reaction method at 1650℃for 6 h.Firstly,the X-ray diffractometer(XRD)patterns display that the samples are all single-phase solid solution structures(space group C 2/c).Differential scanning calorimetry(DSC)and the high-temperature XRD of 8NbTa cross-check that the addition of Ta element in 8HERN increases the phase transition temperature above 1400℃,which can be attributed to that the Ta/Nb co-doping at B site introduces the fluctuation of the bond strength of Ta-O and Nb-O.Secondly,compared to high-entropy rare-earth niobates,the introduction of Ta atoms at B site substantially reduce thermal conductivity(re-duced by 44%,800℃)with the seven components high entropy ceramic as an example.The low thermal conductivity means strong phonon scattering,which may originate from the softening acoustic mode and flattened phonon dispersion in 5–8 principal element high entropy rare earth niobium tantalates(5–8NbTa)revealed by the first-principles calculations.Thirdly,the Ta/Nb co-doping in 5–8NbTa systems can further optimize the insulation performance of oxygen ions.The oxygen-ion conductivity of 8NbTa(3.31×10^(−6)S cm^(−1),900℃)is about 5 times lower than that of 8HERN(15.8×10^(−6)S cm^(−1),900℃)because of the sluggish diffusion effect,providing better oxygen barrier capacity in 5–8NbTa systems to inhibit the overgrowth of the thermal growth oxide(TGO)of TBCs.In addition,influenced by lattice dis-tortion and solid solution strengthening,the samples possess higher hardness(7.51–8.15 GPa)and TECs(9.78×10^(−6)K−1^(-1)0.78×10^(−6)K^(−1),1500℃)than the single rare-earth niobates and tantalates.Based on their excellent overall properties,it is considered that 5–8NbTa can be used as auspicious TBCs.
基金Project(50872155) supported by the National Natural Science Foundation of China
文摘To improve the conductivity of Y2O3-stabilized ZrO2 （YSZ） based oxygen-ion conductor, Zr0.85Y0.15O1.925-La9.33Si6O26 （YSZ-LSO） composite ceramics with the mass fraction of La9.33Si6O26 （LSO） of 15% were prepared by using a modified coprecipitation method. The phases, microstructures and conductivities of the YSZ, LSO and YSZ-LSO were investigated by X-ray diffraction, electron microscopy and complex impedance, respectively. The results show that the as-calcined powder of YSZ-LSO composite has the grain size less than 10 nm, and the as-sintered composite ceramics are composed of YSZ and LSO phases. The conductivity can be enhanced obviously by composite method. At 700 ℃, the conductivity of the composite ceramic is 0.125 S/cm, which is one order in magnitude higher than that of the YSZ ceramic and two orders in magnitude higher than that of LSO ceramic. By analyzing the impedance spectra and modulus spectra, the interfacial effect on the conductivity improvement was proposed.
