Sm_2(Zr_(1-x)Ti_x)_2O_7陶瓷材料的结构及热物理性能
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摘要
目的研究氧化物TiO_2 B位掺杂对Sm_2Zr2O_7陶瓷材料的结构及热物理性能的影响。方法以Sm_2O_3、ZrO_2、TiO_2为原料,通过高温固相合成法制备用过渡金属氧化物TiO_2掺杂Sm_2Zr2O_7的Sm_2(Zr_(1-x)Ti_x)_2O_7(x=0,0.2,0.4,x为摩尔分数)陶瓷材料。利用X射线衍射仪(XRD)、扫描电子显微镜(SEM)研究陶瓷材料的物相结构以及显微形貌,利用阿基米德原理测定陶瓷材料的体积密度。根据Neumann-Kopp定律计算材料热容,采用高温热膨胀仪及激光导热仪对材料的热膨胀性能和热导率进行表征。结果 Sm_2(Zr_(1-x)Ti_x)_2O_7体系陶瓷材料为立方烧绿石结构,显微结构致密,晶界清晰。Sm_2Zr2O_7掺杂小离子半径Ti~(4+)使其热膨胀系数有所提高,热扩散系数降低,并在高温下表现出类似于玻璃的超低热导率。800℃时,Sm_2Zr_(1.6)Ti_(0.4)O_7的热导率为1.29 W/(m·K),平均热膨胀系数达到10.6×10~(-6) K~(-1)。结论由于基质原子与取代原子之间的原子量差随Ti掺杂量的增加而逐渐降低,其热导率随Ti掺杂量增加而升高。
Objective To explore the effects of dopping of TiO_2 oxide to Sm_2 Zr2 O_7 on B site on structure and thermal physical property of Sm_2 Zr2 O_7. Methods Sm_2(Zr_(1-x)Ti_x)2 O_7(x=0, 0.2, 0.4, x is mole fraction) ceramic materials doped with Sm_2 Zr2 O_7 with transition metal oxide TiO_2 were prepared by high temperature solid phase synthesis with Sm_2 O_3, ZrO_2 and TiO_2 as raw materials. X-ray diffractometry(XRD) and scanning electron microscopy(SEM) were used to study the phase structure and microscopic morphology of ceramic materials. The Archimedes principle was used to determine the bulk density of ceramic materials. The heat capacity of materials was calculated according to Neumann–Kopp's law. The thermal expansion properties and thermal conductivity of materials were characterized by high temperature thermal dilatometer and laser thermal conductivity meter. Results The Sm_2(Zr_(1-x)Ti_x)2 O_7 system ceramic material was a cubic pyrochlore structure with dense microstructure and clear grain boundaries. Sm_2 Zr2 O_7 was doped with a small ionic radius Ti~(4+), which resulted in the improvement of thermal expansion coefficient and the decrease of the thermal diffusivity, exhibited an extremely low thermal conductivity similar to glass at high temperature. At 800 ℃, the thermal conductivity of Sm_2 Zr_(1.6) Ti_(0.4) O_7 was 1.29 W/(m·K), and the average thermal expansion coefficient was 10.6×10~(-6) K~(-1). Conclusion Since the atomic weight difference between the matrix atom and the substituted atom gradually decreases as the Ti doping amount increases, the thermal conductivity increases as the Ti doping amount increases.
Objective To explore the effects of dopping of TiO_2 oxide to Sm_2 Zr2 O_7 on B site on structure and thermal physical property of Sm_2 Zr2 O_7. Methods Sm_2(Zr_(1-x)Ti_x)2 O_7(x=0, 0.2, 0.4, x is mole fraction) ceramic materials doped with Sm_2 Zr2 O_7 with transition metal oxide TiO_2 were prepared by high temperature solid phase synthesis with Sm_2 O_3, ZrO_2 and TiO_2 as raw materials. X-ray diffractometry(XRD) and scanning electron microscopy(SEM) were used to study the phase structure and microscopic morphology of ceramic materials. The Archimedes principle was used to determine the bulk density of ceramic materials. The heat capacity of materials was calculated according to Neumann–Kopp's law. The thermal expansion properties and thermal conductivity of materials were characterized by high temperature thermal dilatometer and laser thermal conductivity meter. Results The Sm_2(Zr_(1-x)Ti_x)2 O_7 system ceramic material was a cubic pyrochlore structure with dense microstructure and clear grain boundaries. Sm_2 Zr2 O_7 was doped with a small ionic radius Ti~(4+), which resulted in the improvement of thermal expansion coefficient and the decrease of the thermal diffusivity, exhibited an extremely low thermal conductivity similar to glass at high temperature. At 800 ℃, the thermal conductivity of Sm_2 Zr_(1.6) Ti_(0.4) O_7 was 1.29 W/(m·K), and the average thermal expansion coefficient was 10.6×10~(-6) K~(-1). Conclusion Since the atomic weight difference between the matrix atom and the substituted atom gradually decreases as the Ti doping amount increases, the thermal conductivity increases as the Ti doping amount increases.
引文
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[22]ZHANG Hong-song,YAN Shu-qing,CHEN Xiao-ge.Preparation and Thermophysical Properties of Fluorite-type Samarium-dysprosium-cerium Oxides[J].Journal of the European Ceramic Society,2014,34(1):55-61.
[23]ZHANG H,LV J,GANG L,et al.Investigation about Thermophysical Properties of Ln2Ce2O7,(Ln=Sm,Er and Yb)Oxides for Thermal Barrier Coatings[J].Materials Research Bulletin,2012,47(12):4181-4186.
[24]LIU Z G,OU-YANG J H,ZHOU Y,et al.Influence of Ytterbium-and Samarium-oxides Codoping on Structure and Thermal Conductivity of Zirconate Ceramics[J].J Eur Ceram Soc,2009,29:647-652.
[25]BANSAL N P,ZHU D M.Effects of Doping on Thermal Conductivity of Pyrochlore Oxides for Advanced Thermal Barrier Coatings[J].Mater Sci Eng A,2007,459:192-195.
[26]GUO L,GUO H,GONG S.The Ordering Degree and Thermal Conductivity in the Pyrochlore-type Composition Systems with a Constant Cation Radius Ratio[J].Mater Lett,2013,106:119-121.
[2]LIN F,JIANG X L.Research Progress on Plasma Spraying[J].Journal of Functional Materials,2003,34(3):254-257.
[3]吴琼,张鑫,彭浩然,等.烧绿石结构A2B2O7热障涂层材料热物理性能综述[J].热喷涂技术,2014,6(1):1-9.
[4]MILLER R A.Current Status of the Thermal Barrier Coatings-an Overview[J].Journal of Thermal Spray Technology,1987,30(1):1-11.
[5]PADTURE N P,GELL M,JORDAN E H.Materials Science Thermal Barrier Coatings for Gas Turbine Engine Apptications[J].Science,2002,296(5566):280-284.
[6]XIE X Y,GUO H B,GONG S K,et al.Lanthanum-titanium-aluminum Oxide:A Novel Thermal Barrier Coating Material for Applications at 1300 Degrees C[J].Journal of the European Ceramic Society,2011,31(9):1677-1683.
[7]GUO H B,WANG Y,WANG L,et al.Thermo-physical Properties and Thermal Shock Resistance of Segmented La2Ce2O7/YSZ Thermal Barrier Coatings[J].Journal of Thermal Spray Technology,2009,18(4):665-671
[8]郭洪波,宫声凯,徐惠彬.先进航空发动机热障涂层技术研究进展[J].中国材料进展,2009,28(9):18-26.
[9]陈晓鸽,廖肃然,张红松,等.Sm2(Zr0.9Ce0.1)2O7陶瓷的溶胶凝胶法制备及热导率[J].材料工程,2010,30(1):32-40
[10]孙现凯,陈玉峰,王广海,等.大气等离子喷涂Sm2Zr2O7热障涂层的隔热性能研究[J].稀有金属材料与工程,2015(s1):735-739.
[11]WU J,WEI X,PADTURE N P,et al.Low-thermal-conductivity Rare-Earth Zirconates for Potential Thermalbarrier-coating Applications[J].Journal of the American Ceramic Society,2003,34(10):3031-3035.
[12]KOSTORZ G,HERMAN H,ALPER A M.Phase Diagrams in Advanced Ceramics[M].Amsterdam:Elsevier,1995.
[13]ZHANG Hong-song,SUN Kun,XU Qiang,et al.Thermal Conductivity of(Sm1-x Lax)2Zr2O7(x=0,0.25,0.5,0.75 and1)Oxides for Advanced Thermal Barrier Coatings[J].稀土学报(英文版),2009,27(2):222-226.
[14]谢敏,宋希文,周芬,等.稀土(Ln=Y/Yb)掺杂对Sm2Zr2O7陶瓷材料结构及热导率的影响[J].材料导报:纳米与新材料专辑,2016(2):244-247.
[15]SOHN Y H,LEE E Y,NAGARAJ B A,et al.Microstructural Characterization of Thermal Barrier Coatings on High Pressure Turbine Blades[J].Surface and Coatings Technology,2001,146-147(10):132-139.
[16]WU J,WEI X,PADTURE N P,et al.Low-Thermal Conductivity Rar Earth Zirconates for Potential Thermal Barrier Coating Applications[J].Cheminform,2003,34(10):517-521.
[17]WAN C L,ZHANG W,WANG Y F,et al.Glass-like Thermal Conductivity in Ytterbium-doped Lanthanum Zirconate Pyrochlore[J].Acta Mater,2010,58(18):6166-6172.
[18]SUBRAMANIAN M A,ARAVAMUDAN G,SUBBARAO G V.Oxide Pyrochlores-A Review[J].Progr in Solid State Chem,1983,15(2):55-143.
[19]NISHINO H,YAMAMURA H,ARAI T,et al.Effect of Cation Radius Ratio and Unit Cell Free Volume on Oxide-Ion Conductivity in Oxide Systems with Pyrochlore-type Composition[J].Journal of the Ceramic Society of Japan,2004,112(3):417-421.
[20]KINGERY W D,BOWEN H K,UHLMANN D R.Introduction to Ceramics[M].New York:John Wiley Sons,1976:589-594.
[21]关振铎,张中太,焦金生.无机材料物理性能[M].北京:清华大学出版社,1992:116-117.
[22]ZHANG Hong-song,YAN Shu-qing,CHEN Xiao-ge.Preparation and Thermophysical Properties of Fluorite-type Samarium-dysprosium-cerium Oxides[J].Journal of the European Ceramic Society,2014,34(1):55-61.
[23]ZHANG H,LV J,GANG L,et al.Investigation about Thermophysical Properties of Ln2Ce2O7,(Ln=Sm,Er and Yb)Oxides for Thermal Barrier Coatings[J].Materials Research Bulletin,2012,47(12):4181-4186.
[24]LIU Z G,OU-YANG J H,ZHOU Y,et al.Influence of Ytterbium-and Samarium-oxides Codoping on Structure and Thermal Conductivity of Zirconate Ceramics[J].J Eur Ceram Soc,2009,29:647-652.
[25]BANSAL N P,ZHU D M.Effects of Doping on Thermal Conductivity of Pyrochlore Oxides for Advanced Thermal Barrier Coatings[J].Mater Sci Eng A,2007,459:192-195.
[26]GUO L,GUO H,GONG S.The Ordering Degree and Thermal Conductivity in the Pyrochlore-type Composition Systems with a Constant Cation Radius Ratio[J].Mater Lett,2013,106:119-121.