J. Mater. Sci. Technol. ›› 2022, Vol. 104: 131-144.DOI: 10.1016/j.jmst.2021.06.068

• Research Article • Previous Articles     Next Articles

Improved thermal stability and infrared emissivity of high-entropy REMgAl11O19 and LaMAl11O19 (RE=La, Nd, Gd, Sm, Pr, Dy; M=Mg, Fe, Co, Ni, Zn)

Haolin Zhua,b,c, Ling Liua,c,d,*(), Huimin Xiangb, Fu-Zhi Daib, Xiaohui Wange, Zhuang Maa,c,d, Yanbo Liua,c,d, Yanchun Zhoub,**()   

  1. aSchool of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
    bScience and Technology on Advanced Functional Composite Laboratory, Aerospace Research Institute of Materials & Processing Technology, Beijing 100076, China
    cNational Key Laboratory of Science and Technology on Materials under Shock and Impact, Beijing 100081, China
    dBeijing Institute of Technology Chongqing Innovation Center, Chongqing 401120, China
    eShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
  • Received:2021-05-25 Revised:2021-06-30 Accepted:2021-06-30 Published:2022-03-30 Online:2021-09-09
  • Contact: Ling Liu,Yanchun Zhou
  • About author:** E-mail addresses: yczhou@alum.imr.ac.cn (Y. Zhou).
    * Science and Technology on Advanced Functional Com-posite Laboratory, Aerospace Research Institute of Materials & Processing Technol-ogy, Beijing, 100076, China. E-mail addresses: richard@bit.edu.cn (L. Liu),

Abstract:

LaMgAl11O19 (LMA), characterized by high melting point, low density and thermal conductivity as well as good infrared emissivity, is regarded as a potential candidate for the thermal protection of hypersonic vehicles. Nevertheless, the unsatisfied phase stability at high temperature results in declining of the emissivity below 6 μm, which limits the extensive applications of LaMgAl11O19. In order to overcome this obstacle, three dense bulk high-entropy ceramics, (La0.2Nd0.2Gd0.2Sm0.2Pr0.2)MgAl11O19 (HE LMA-1), (La0.2Nd0.2Gd0.2Sm0.2Dy0.2)Mg Al11O19 (HE LMA-2) and La(Mg0.2Fe0.2Co0.2Ni0.2Zn0.2)Al11O19 (HE LMA-3), were designed and successfully prepared through solid state reaction at 1700 ℃ for 4 h in one step. XRD analyses show that the phase compositions of HE LMA-1, HE LMA-2 and HE LMA-3 are single-phase solid solutions with the relative density of 95.61%, 95.49% and 94.31%, respectively. Heat treatment experiments demonstrate that the phase composition of HE LMA-1 remains a single phase after high-temperature heating, while second phase appears in other two samples. The stability of HE LMA-1 is attributed to small average size difference δ (~4%) of constitute elements. Intriguingly, the average emissivity of HE LMA-1 in the range of 3-6 μm reaches 0.9, which is significantly higher than that of LMA and other two HE LMA samples. The emissivity of all samples remains above 0.95 from 6 to 10 μm. In the far infrared region (10-14 μm), although the emissivity of these specimens decreases slightly, it still exceeds 0.85. The UV-Vis absorption spectra indicate that the formation of many discrete impurity energy levels with small intervals in HE LMA-1 promotes the f electrons to transit between adjacent impurity energy levels and conduction band, which enhances the infrared emission of HE LMA-1 below 6 μm. In a word, with improved phase stability and thermal emissivity in infrared range, high-entropy REMgAl11O19, especially (La0.2Nd0.2Gd0.2Sm0.2Pr0.2)MgAl11O19 (HE LMA-1), is a promising candidate in thermal protection coatings of hypersonic vehicles.

Key words: High-entropy ceramics, LaMgAl11O19, Thermal stability, Infrared emissivity, UV-Vis absorption