Strong Polar Optical Phonon Screening and Softening Enhance the Thermoelectric Performance of Zintl Compounds

IF 24.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Muchun Guo, Ming Liu, Donglin Yuan, Hong Chen, Chenyue Sun, Qinyong Zhang, Yuke Zhu, Fengkai Guo, Yuan Yu, Jiehe Sui
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Abstract

Ternary CaAl2Si2-structure-type Zintl compounds are promising p-type counterparts to n-type Mg3(Sb, Bi)2 for thermoelectric energy conversion. However, many of these p-type Zintl compounds suffer from low carrier concentration and mobility, resulting in poor thermoelectric performance. Here, it is revealed that their ultralow mobility stems from strong polar optical phonon scattering, and demonstrate that their electrical transport properties can be dramatically boosted by employing a screening effect. By employing isovalent alloying with Cd and Yb, along with Li aliovalent acceptor doping in CaMg2Sb2 to increase carrier concentration and induce a strong screening effect, a significant improvement in carrier mobility and, consequently, the power factor is achieved. Moreover, isovalent alloying weakens chemical bonding, causing the softening and deceleration of both acoustic and optical phonons and, thus, a reduction in lattice thermal conductivity. As a result, a ZT of 1.1 is achieved in the Ca0.69Yb0.3Li0.01Mg1.5Cd0.5Sb2 sample at 773 K, representing a 30-fold increase compared to the pristine CaMg2Sb2. It is also proposed that the polar coupling constant can serve as a criterion for identifying materials with low intrinsic carrier concentration and mobility but with potential for thermoelectric applications facilitating the development of other thermoelectric materials beyond CaAl2Si2-structure-type Zintl compounds.

Abstract Image

强极性光声子筛选和软化提高了Zintl化合物的热电性能
三元caal2si2结构型Zintl化合物是有前途的p型Mg3(Sb, Bi)2的n型热电能量转换对应物。然而,许多p型Zintl化合物的载流子浓度低,迁移率低,导致热电性能差。在这里,揭示了它们的超低迁移率源于强极性光学声子散射,并证明了它们的电输运性质可以通过采用筛选效应显着提高。通过在CaMg2Sb2中掺入Cd、Yb等价合金,并掺杂Li等价受体,增加载流子浓度,诱导出较强的筛选效应,显著提高了载流子迁移率,从而实现了功率因数的提高。此外,等价合金削弱了化学键,导致声子和声子的软化和减速,从而降低了晶格的导热性。结果,在773 K下,Ca0.69Yb0.3Li0.01Mg1.5Cd0.5Sb2样品的ZT达到1.1,与原始CaMg2Sb2相比增加了30倍。本文还提出,极性耦合常数可以作为识别具有低本征载流子浓度和迁移率但具有热电应用潜力的材料的标准,促进了caal2si2结构型Zintl化合物以外的其他热电材料的开发。
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来源期刊
Advanced Energy Materials
Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
41.90
自引率
4.00%
发文量
889
审稿时长
1.4 months
期刊介绍: Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.
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