A Simple Chemical Guide for Finding Novel n-type Dopable Zintl Pnictide Thermoelectric Materials

First Principles ◽

Formation Energy ◽

Large Scale ◽

Zintl Phases ◽

Experimental Realization ◽

Average Oxidation State ◽

Simple Chemical

Computations have predicted good thermoelectric performance for a number of Zintl phases when doped n-type. Combined with the successful experimental realization of n-type KGaSb4, KAlSb4, and Mg3Sb2 with zT>1, this has fueled efforts to discover novel n-type dopable Zintl phases. However, a majority of Zintl phases exhibit strong proclivity toward p-type doping and prior successes in finding n-type dopable Zintls were largely serendipitous. Herein we use modern first-principles defect calculations to study trends in the dopability of Zintl pnictides and find that the average oxidation state of the anion is a useful chemical guide to identify novel n-type dopable phases. Specifically, we observe that Zintl pnictides with average oxidation of the anion near -1 are n-type dopable. The trend is mainly a consequence of the high formation energy of native acceptor defects (e.g. cation vacancies) and the resulting absence of charge (electron) compensation. Using the oxidation state guide in conjunction with a descriptor of thermoelectric performance, we conduct a large-scale materials search and identify promising candidates that are n-type dopable.

A simple chemical guide for finding novel n-type dopable Zintl pnictide thermoelectric materials

Journal of Materials Chemistry A ◽

10.1039/c9ta03786a ◽

2019 ◽

Vol 7 (33) ◽

pp. 19385-19395 ◽

Cited By ~ 8

Author(s):

Prashun Gorai ◽

Anuj Goyal ◽

Eric S. Toberer ◽

Vladan Stevanović

Keyword(s):

Large Scale ◽

Zintl Phases ◽

Simple Chemical

Computations have predicted good thermoelectric performance of n-type doped Zintl phases. We present a simple, yet effective, chemical guide for finding n-type dopable Zintl pnictides and perform a large-scale search to identify candidate materials.

Theoretical Considerations for Finding New Thermoelectric Materials

MRS Proceedings ◽

10.1557/proc-691-g1.2 ◽

2001 ◽

Vol 691 ◽

Cited By ~ 2

Author(s):

David J. Singh

Keyword(s):

Transport Properties ◽

First Principles ◽

First Principles Calculations ◽

Theoretical Considerations

ABSTRACTThis paper reviews the connections between the transport properties underlying the thermoelectric performance of a material and microscopic quantities, particularly as they may be obtained from first principles calculations. These are illustrated using examples from work on skutterudites. The results are used to suggest yet to be explored avenues for achieving higher thermoelectric performance within this class of materials.

High Thermoelectric Performance of Cu-Doped PbSe-PbS System Enabled by High-Throughput Experimental Screening

Research ◽

10.34133/2020/1736798 ◽

2020 ◽

Vol 2020 ◽

pp. 1-8

Author(s):

Li You ◽

Zhili Li ◽

Quanying Ma ◽

Shiyang He ◽

Qidong Zhang ◽

...

Keyword(s):

Experimental Technique ◽

High Throughput ◽

High Performance ◽

Large Scale ◽

Transport Model ◽

Trial And Error ◽

Lead Chalcogenides ◽

Experimental Discovery

Recent advances in high-throughput (HTP) computational power and machine learning have led to great achievements in exploration of new thermoelectric materials. However, experimental discovery and optimization of thermoelectric materials have long relied on the traditional Edisonian trial and error approach. Herein, we demonstrate that ultrahigh thermoelectric performance in a Cu-doped PbSe-PbS system can be realized by HTP experimental screening and precise property modulation. Combining the HTP experimental technique with transport model analysis, an optimal Se/S ratio showing high thermoelectric performance has been efficiently screened out. Subsequently, based on the screened Se/S ratio, the doping content of Cu has been subtly adjusted to reach the optimum carrier concentration. As a result, an outstanding peak zT~1.6 is achieved at 873 K for a 1.8 at% Cu-doped PbSe0.6S0.4 sample, which is the superior value among the n-type Te-free lead chalcogenides. We anticipate that current work will stimulate large-scale unitization of the HTP experimental technique in the thermoelectric field, which can greatly accelerate the research and development of new high-performance thermoelectric materials.

Accelerated Discovery of High-Refractive-Index Polyimides via First-Principles Molecular Modeling, Virtual High-Throughput Screening, and Data Mining

10.26434/chemrxiv.7670903.v1 ◽

2019 ◽

Author(s):

Mohammad Atif Faiz Afzal ◽

Mojtaba Haghighatlari ◽

Sai Prasad Ganesh ◽

Chong Cheng ◽

Johannes Hachmann

Keyword(s):

Data Mining ◽

Refractive Index ◽

High Throughput ◽

First Principles ◽

High Throughput Screening ◽

Large Scale ◽

Computational Study ◽

High Refractive Index ◽

Structural Features ◽

Learning Program

<div>We present a high-throughput computational study to identify novel polyimides (PIs) with exceptional refractive index (RI) values for use as optic or optoelectronic materials. Our study utilizes an RI prediction protocol based on a combination of first-principles and data modeling developed in previous work, which we employ on a large-scale PI candidate library generated with the ChemLG code. We deploy the virtual screening software ChemHTPS to automate the assessment of this extensive pool of PI structures in order to determine the performance potential of each candidate. This rapid and efficient approach yields a number of highly promising leads compounds. Using the data mining and machine learning program package ChemML, we analyze the top candidates with respect to prevalent structural features and feature combinations that distinguish them from less promising ones. In particular, we explore the utility of various strategies that introduce highly polarizable moieties into the PI backbone to increase its RI yield. The derived insights provide a foundation for rational and targeted design that goes beyond traditional trial-and-error searches.</div>

High Thermoelectric Performance in the Cubic Inorganic Cesium Iodide Perovskites CsBI3 (B = Pb, Sn, and Ge) from First-Principles

The Journal of Physical Chemistry C ◽

10.1021/acs.jpcc.0c09929 ◽

2021 ◽

Author(s):

Un-Gi Jong ◽

Yun-Sim Kim ◽

Chol-Hyok Ri ◽

Yun-Hyok Kye ◽

Chol-Jun Yu

Keyword(s):

First Principles ◽

Cesium Iodide ◽

Thermoelectric Performance

Thermoelectric Performance of Mechanically Mixed BixSb2-xTe3—ABS Composites

Materials ◽

10.3390/ma14071706 ◽

2021 ◽

Vol 14 (7) ◽

pp. 1706

Author(s):

Zacharias Viskadourakis ◽

Argiri Drymiskianaki ◽

Vassilis M. Papadakis ◽

Ioanna Ioannou ◽

Theodora Kyratsi ◽

...

Keyword(s):

Polymer Composites ◽

Large Scale ◽

Low Cost ◽

Acrylonitrile Butadiene Styrene ◽

Scale Production ◽

Bismuth Antimony Telluride ◽

Mechanical Mixing ◽

Large Scale Production ◽

Bi Doping

In the current study, polymer-based composites, consisting of Acrylonitrile Butadiene Styrene (ABS) and Bismuth Antimony Telluride (BixSb2−xTe3), were produced using mechanical mixing and hot pressing. These composites were investigated regarding their electrical resistivity and Seebeck coefficient, with respect to Bi doping and BixSb2-xTe3 loading into the composite. Experimental results showed that their thermoelectric performance is comparable—or even superior, in some cases—to reported thermoelectric polymer composites that have been produced using other complex techniques. Consequently, mechanically mixed polymer-based thermoelectric materials could be an efficient method for low-cost and large-scale production of polymer composites for potential thermoelectric applications.

First-principles predictions of low lattice thermal conductivity and high thermoelectric performance of AZnSb (A = Rb, Cs)

RSC Advances ◽

10.1039/d1ra01938d ◽

2021 ◽

Vol 11 (25) ◽

pp. 15486-15496

Author(s):

Enamul Haque

Keyword(s):

Thermal Conductivity ◽

Debye Temperature ◽

Layered Structure ◽

First Principles ◽

Lattice Thermal Conductivity ◽

Phonon Scattering ◽

Thermoelectric Performance

The layered structure, and presence of heavier elements Rb/Cs and Sb induce high anharmonicity, low Debye temperature, intense phonon scattering, and hence, low lattice thermal conductivity.

Thermoelectric performance of silicene under uniform biaxial strain: A first principles study

Superlattices and Microstructures ◽

10.1016/j.spmi.2021.106944 ◽

2021 ◽

pp. 106944

Author(s):

Neelsh Gupta ◽

Rekha Verma

Keyword(s):

First Principles ◽

Biaxial Strain ◽

First Principles Study

Hydrogenation and oxidation enhances the thermoelectric performance of Si2BN monolayer

New Journal of Chemistry ◽

10.1039/d0nj06000c ◽

2021 ◽

Author(s):

H. R. Mahida ◽

Deobrat Singh ◽

Yogesh Sonvane ◽

Sanjeev K. Gupta ◽

P. B. Thakor ◽

...

Keyword(s):

Density Functional Theory ◽

Charge Transport ◽

Transport Properties ◽

First Principles ◽

Density Functional ◽

First Principles Calculations ◽

Functional Theory

In the present study, we have investigated the structural, electronic, and charge transport properties of pristine, hydrogenated, and oxidized Si2BN monolayers via first-principles calculations based on density functional theory (DFT).