设计自旋交叉系统以增强顺磁材料的热功率和热电功勋值

IF 13 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Md Mobarak Hossain Polash, Matthew Stone, Songxue Chi, Daryoosh Vashaee
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引用次数: 0

摘要

热电材料能够将温度梯度转化为电能,但传统上一直受限于热功率和导电率之间的权衡。本研究介绍了一种新颖、广泛适用的方法,即利用温度驱动的自旋交叉,在不影响导电性的情况下增强自旋驱动热功率和热电效应(zT)。我们的方法得到了理论和实验证据的支持,并通过对掺铬碲化锰的案例研究得到了证明,但并不局限于这种材料,还可以扩展到其他磁性材料。通过引入掺杂剂以产生高晶场,并利用与温度驱动的自旋交叉相关的熵变化,我们实现了热功率的显著提高,提高了约 136 μV K-1,这意味着在顺磁畴内的高温下,热功率提高了 200% 以上。我们对这些材料双极半导体性质的探索表明,抑制双极磁子/顺磁子曳光热功率是理解和利用自旋交叉驱动热功率的关键。这些发现经过非弹性中子散射、X 射线光发射光谱、热传输和能量转换测量的验证,揭示了关键的材料设计参数。我们提供了一个全面的框架,分析了自旋熵、跳跃传输和磁子/副磁子寿命之间的相互作用,为开发高性能的自旋驱动热电材料铺平了道路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Designing Spin-Crossover Systems to Enhance Thermopower and Thermoelectric Figure-of-Merit in Paramagnetic Materials

Designing Spin-Crossover Systems to Enhance Thermopower and Thermoelectric Figure-of-Merit in Paramagnetic Materials
Thermoelectric materials, capable of converting temperature gradients into electrical power, have been traditionally limited by a trade-off between thermopower and electrical conductivity. This study introduces a novel, broadly applicable approach that enhances both the spin-driven thermopower and the thermoelectric figure-of-merit (zT) without compromising electrical conductivity, using temperature-driven spin crossover. Our approach, supported by both theoretical and experimental evidence, is demonstrated through a case study of chromium doped-manganese telluride, but is not confined to this material and can be extended to other magnetic materials. By introducing dopants to create a high crystal field and exploiting the entropy changes associated with temperature-driven spin crossover, we achieved a significant increase in thermopower, by approximately 136 μV K−1, representing more than a 200% enhancement at elevated temperatures within the paramagnetic domain. Our exploration of the bipolar semiconducting nature of these materials reveals that suppressing bipolar magnon/paramagnon-drag thermopower is key to understanding and utilizing spin crossover-driven thermopower. These findings, validated by inelastic neutron scattering, X-ray photoemission spectroscopy, thermal transport, and energy conversion measurements, shed light on crucial material design parameters. We provide a comprehensive framework that analyzes the interplay between spin entropy, hopping transport, and magnon/paramagnon lifetimes, paving the way for the development of high-performance spin-driven thermoelectric materials.
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来源期刊
Energy & Environmental Materials
Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
17.60
自引率
6.00%
发文量
66
期刊介绍: Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.
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