New class of high-entropy pseudobrookite titanate with excellent thermal stability, low thermal expansion coefficient, and low thermal conductivity

Abstract

As a type of titanate, the pseudobrookite (MTi2O5/M2TiO5) exhibits a low thermal expansion coefficient and thermal conductivity, as well as excellent dielectric and solar spectrum absorption properties. However, the pseudobrookite is unstable and prone to decomposing below 1200 °C, which limits the practical application of the pseudobrookite. In this paper, the high-entropy pseudobrookite ceramic is synthesized for the first time. The pure high-entropy (Mg,Co,Ni,Zn)Ti2O5 with the pseudobrookite structure and the biphasic high-entropy ceramic composed of the high-entropy pseudobrookite (Cr,Mn,Fe,Al,Ga)2TiO5 and the high-entropy spinel (Cr,Mn,Fe,Al,Ga,Ti)3O4 are successfully prepared by the in-situ solid-phase reaction method. The comparison between the theoretical crystal structure of the pseudobrookite and the aberration-corrected scanning transmission electron microscopy (AC-STEM) images of high-entropy (Mg,Co,Ni,Zn)Ti2O5 shows that the metal ions (M and Ti ions) are disorderly distributed at the A site and the B site in high-entropy (Mg,Co,Ni,Zn)Ti2O5, leading to an unprecedentedly high configurational entropy of high-entropy (Mg,Co,Ni,Zn)Ti2O5. The bulk high-entropy (Mg,Co,Ni,Zn)Ti2O5 ceramics exhibit a low thermal expansion coefficient of 6.35×10−6 K−1 in the temperature range of 25–1400 °C and thermal conductivity of 1.840 W·m−1·K−1 at room temperature, as well as the excellent thermal stability at 200, 600, and 1400 °C. Owing to these outstanding properties, high-entropy (Mg,Co,Ni,Zn)Ti2O5 is expected to be the promising candidate for high-temperature thermal insulation. This work has further extended the family of different crystal structures of high-entropy ceramics reported to date.