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复杂硼化物的新合成路线;通过液相辅助反应性放电等离子体烧结快速合成热电钇铝硼化物

New Synthesis Route for Complex Borides; Rapid Synthesis of Thermoelectric Yttrium Aluminoboride via Liquid-Phase Assisted Reactive Spark Plasma Sintering.

作者信息

Son Hyoung-Won, Berthebaud David, Yubuta Kunio, Yoshikawa Akira, Shishido Toetsu, Suzuta Keiko, Mori Takao

机构信息

WPI International Center for Materials Nanoarchitechtonics (WPI-MANA), National Institute for Materials Science (NIMS), Namiki 1-1, Tsukuba, 305-0044, Ibaraki, Japan.

Graduate School of Pure and Applied Sciences, University of Tsukuba, Tennoudai 1-1-1, Tsukuba, 305-8671, Ibaraki, Japan.

出版信息

Sci Rep. 2020 Jun 2;10(1):8914. doi: 10.1038/s41598-020-65818-z.

Abstract

YAlB ceramics are of high interest as high temperature thermoelectric materials with excellent p, n control. In this study, direct synthesis of dense polycrystalline YAlB (x ~0.64, 0.52 ≤ y ≤ 0.67) ceramics was successfully carried out by spark plasma sintering using commercially available precursors. YB, AlB and B powders were reactively sintered with an additive AlF at 1773 K for 5-60 min in reduced Ar atmosphere. The sinterability was remarkably enhanced by liquid phase sintering comparing to conventional synthesis techniques. Phase composition analysis by X-ray diffraction showed that main peaks belong to YAlB with the MgAlB structure type and no peaks of AlF were detected. The thermoelectric behavior was changed from p-type to n-type with increasing Al occupancy. Power factor and ZT values measured in this study were found to be in the same range as the best values previously reported. This original synthesis process is found to be less precursor-consuming as compared to previous synthesis processes, and strikingly, less time-consuming, as the synthesis time, is shortened from 8 h to 5 min for p-type and to 1 h for n-type. The total process time is shortened from ≥3 days to ~4-5 h. This discovery opens the door for more accessible synthesis of complex borides.

摘要

YAlB陶瓷作为具有优异p型、n型控制的高温热电材料备受关注。在本研究中,使用市售前体通过放电等离子烧结成功地直接合成了致密的多晶YAlB(x≈0.64,0.52≤y≤0.67)陶瓷。在1773K下,在还原的氩气氛中,将YB、AlB和B粉末与添加剂AlF进行反应烧结5 - 60分钟。与传统合成技术相比,通过液相烧结显著提高了烧结性。X射线衍射的相组成分析表明,主峰属于具有MgAlB结构类型的YAlB,未检测到AlF的峰。随着Al占有率的增加,热电行为从p型转变为n型。本研究中测得的功率因子和ZT值与先前报道的最佳值处于同一范围。发现这种原始合成过程与先前的合成过程相比,消耗的前体更少,而且引人注目的是,耗时更少,因为合成时间从p型的8小时缩短到5分钟,n型缩短到1小时。总工艺时间从≥3天缩短到约4 - 5小时。这一发现为更易于合成复杂硼化物打开了大门。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7488/7265475/9501f74ddae0/41598_2020_65818_Fig1_HTML.jpg

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