{"title":"Chalcogenide perovskite BaZrS3 bulks for thermoelectric conversion with ultra-high carrier mobility and low thermal conductivity","authors":"Zhe Yang , Yanbing Han , Yurun Liang, Weixia Shen, Zhuangfei Zhang, Chao Fang, Qianqian Wang, Biao Wan, Liangchao Chen, Yuewen Zhang, Xiaopeng Jia","doi":"10.1016/j.actamat.2024.120156","DOIUrl":null,"url":null,"abstract":"<div><p>Chalcogenide perovskites are expected to be promising thermoelectric materials, since they not only possess efficient carrier transport and defect tolerance, but also demonstrate unique advantages of high thermodynamic stability, eco-friendly and earth-abundant constituents. Especially, theoretical reports have predicted their “glass-like” thermal conductivities. However, experimental investigation on thermoelectric performances of chalcogenide perovskite BaZrS<sub>3</sub> is extremely scarce due to the difficulty in preparing high-quality bulk samples, which originates from the brittle nature, high melting point, and the large difference in melting points between Ba/S and Zr. In this work, pure phase BaZrS<sub>3</sub> bulks with high relative density reaching 100 % are realized by optimized sulfurization from low-cost BaZrO<sub>3</sub> powders combined with fast spark plasma sintering. A maximum zT value of 0.37 at 623 K in BaZrS<sub>3</sub> bulks is achieved, which is the record-high value among the reported sulfide, halide, and hybrid perovskite materials. A room-temperature electron mobility up to 385 cm<sup>2</sup>V<sup>−1</sup>s<sup>−1</sup> is among the highest values for perovskites due to the high phase purity, dense morphology and corner-sharing ZrS<sub>6</sub> octahedral three-dimensional network as effective carrier channels. Meanwhile, a measured low lattice thermal conductivity of 1.11 Wm<sup>−1</sup>K<sup>−1</sup> at 623 K is attributed to the intense phonon scattering from the intrinsic distorted-perovskite structure and the lattice defects by sulfur deficiency. Moreover, the BaZrS<sub>3</sub> bulks in this work are stable against moisture/air and high temperature test. This work provides new insights into the fundamental electrical and thermal properties of chalcogenide perovskites, and highlights their great potential in the practical thermoelectric applications.</p></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":null,"pages":null},"PeriodicalIF":8.3000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Acta Materialia","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S135964542400507X","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Chalcogenide perovskites are expected to be promising thermoelectric materials, since they not only possess efficient carrier transport and defect tolerance, but also demonstrate unique advantages of high thermodynamic stability, eco-friendly and earth-abundant constituents. Especially, theoretical reports have predicted their “glass-like” thermal conductivities. However, experimental investigation on thermoelectric performances of chalcogenide perovskite BaZrS3 is extremely scarce due to the difficulty in preparing high-quality bulk samples, which originates from the brittle nature, high melting point, and the large difference in melting points between Ba/S and Zr. In this work, pure phase BaZrS3 bulks with high relative density reaching 100 % are realized by optimized sulfurization from low-cost BaZrO3 powders combined with fast spark plasma sintering. A maximum zT value of 0.37 at 623 K in BaZrS3 bulks is achieved, which is the record-high value among the reported sulfide, halide, and hybrid perovskite materials. A room-temperature electron mobility up to 385 cm2V−1s−1 is among the highest values for perovskites due to the high phase purity, dense morphology and corner-sharing ZrS6 octahedral three-dimensional network as effective carrier channels. Meanwhile, a measured low lattice thermal conductivity of 1.11 Wm−1K−1 at 623 K is attributed to the intense phonon scattering from the intrinsic distorted-perovskite structure and the lattice defects by sulfur deficiency. Moreover, the BaZrS3 bulks in this work are stable against moisture/air and high temperature test. This work provides new insights into the fundamental electrical and thermal properties of chalcogenide perovskites, and highlights their great potential in the practical thermoelectric applications.
期刊介绍:
Acta Materialia serves as a platform for publishing full-length, original papers and commissioned overviews that contribute to a profound understanding of the correlation between the processing, structure, and properties of inorganic materials. The journal seeks papers with high impact potential or those that significantly propel the field forward. The scope includes the atomic and molecular arrangements, chemical and electronic structures, and microstructure of materials, focusing on their mechanical or functional behavior across all length scales, including nanostructures.