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(钡锶钙镧钠)钴酸盐基钙钛矿型高熵钴酸盐的热电行为

Thermoelectric behavior of (BaSrCaLaNa)CoO high entropy cobaltate-based perovskite.

作者信息

Bhattacharya Tathagata, Banerjee Ritwik, Maiti Tanmoy

机构信息

Plasmonics and Perovskite Laboratory, Department of Materials Science and Engineering, IIT Kanpur, UP 208016, India.

出版信息

Phys Chem Chem Phys. 2024 Nov 27;26(46):28874-28883. doi: 10.1039/d4cp03550j.

DOI:10.1039/d4cp03550j
PMID:39533859
Abstract

Oxides are considered as promising thermoelectric materials due to their excellent thermal and chemical stability at elevated temperatures. However, their thermoelectric performances are hindered by high thermal conductivity due to the relatively simple structure compared to the layered or cage-like structure of intermetallics and chalcogenides. In this study, we have successfully crafted a novel cobaltate-based high-entropy oxide perovskite, (BaSrCaLaNa)CoO (BSCLN), based on detailed thermodynamic calculation. XRD analysis of the as-synthesized ceramics confirms the formation of a cubic perovskite phase, while SEM-EDXS data reveals a dense microstructure with a uniform distribution of all the constituent elements. By employing high-entropy engineering in this cobaltate-based ceramic, we have managed to reduce thermal conductivity significantly while optimizing electrical conductivity. Five different elements populating the A-site induce extensive structural defects and disorder causing enhanced phonon scattering. This results in a glass-like low thermal conductivity of 1.43 W m K at 1023 K for the high-entropy cobaltate. Moreover, we have achieved a comparatively high electrical conductivity on the order of 10 S m. This study illustrates the effectiveness of introducing structural disorder through high-entropy engineering to enhance the overall thermoelectric performance of the material.

摘要

由于氧化物在高温下具有优异的热稳定性和化学稳定性,它们被认为是很有前景的热电材料。然而,与金属间化合物和硫族化物的层状或笼状结构相比,其结构相对简单,导致其热导率较高,从而阻碍了它们的热电性能。在本研究中,我们基于详细的热力学计算,成功制备了一种新型的钴酸盐基高熵氧化物钙钛矿(BaSrCaLaNa)CoO(BSCLN)。对合成后的陶瓷进行XRD分析证实形成了立方钙钛矿相,而SEM-EDXS数据显示微观结构致密,所有组成元素分布均匀。通过在这种钴酸盐基陶瓷中采用高熵工程,我们在优化电导率的同时成功显著降低了热导率。占据A位的五种不同元素会引发大量结构缺陷和无序,导致声子散射增强。这使得高熵钴酸盐在1023 K时具有类似玻璃的低热导率,为1.43 W m⁻¹ K⁻¹。此外,我们还实现了约10 S m⁻¹的较高电导率。本研究说明了通过高熵工程引入结构无序以提高材料整体热电性能的有效性。

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