Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides

Thermoelectric materials enable the mutual energy conversion of waste heat and electricity, critical to relieve global energy crisis. Hightemperature thermoelectric materials are special species due to their high-temperature stability and noticeable energy conversion efficiency. Here, we report a sy...

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Main Authors: Qin, Feiyu, Nikolaev, Sergey A., Suwardi, Ady, Wood, Maxwell, Zhu, Yingcai, Tan, Xianyi, Aydemir, Umut, Ren, Yang, Yan, Qingyu, Hu, Lei, Snyder, G. Jeffrey
Other Authors: School of Materials Science and Engineering
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Language:English
Published: 2021
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Online Access:https://hdl.handle.net/10356/148336
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spelling sg-ntu-dr.10356-1483362023-07-14T15:51:46Z Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides Qin, Feiyu Nikolaev, Sergey A. Suwardi, Ady Wood, Maxwell Zhu, Yingcai Tan, Xianyi Aydemir, Umut Ren, Yang Yan, Qingyu Hu, Lei Snyder, G. Jeffrey School of Materials Science and Engineering Engineering Engineering::Materials Phonons Crystal Structure Thermoelectric materials enable the mutual energy conversion of waste heat and electricity, critical to relieve global energy crisis. Hightemperature thermoelectric materials are special species due to their high-temperature stability and noticeable energy conversion efficiency. Here, we report a systematic investigation on high-temperature thermoelectric gadolinium selenides, cubic Gd3-xSe4 (x = 0.16, 0.21 and 0.25) and orthorhombic Gd2Se3-y (y = 0.02, 0.06 and 0.08). High energy synchrotron x-ray diffraction and total scattering are used to investigate the crystallographic and local structures. The atomic-scale cluster of Gd vacancy in cubic Gd2.84Se4 is observed by employing the reverse Monte Carlo simulation. For cubic Gd3-xSe4, its carrier concentration is tuned and multiple conduction bands are incorporated by adjusting Gd vacancy. Experimentally, the gradual increase in effective masses is evidently observed in cubic Gd3-xSe4, which is consistent with the density functional theory (DFT) calculation. A reasonable peak zT value of 0.27 is achieved at 850 K for Gd2.84Se4. On the other hand, adjusting Se vacancy enables the optimization of electron concentration for orthorhombic Gd2Se3-y phase. Its low deformation potential (Ξ = 12eV) with single conduction band gives rise to enhanced electron mobility and higher peak zT value of 0.54 at 850 K for Gd2Se2.98. In addition, a higher zT of 1.2 at1200 K is reasonably predicted for Gd2Se2.98 by using quality factor analysis. This work not just presents a systematic crystallographic investigation of gadolinium selenides, but also provides a deep insight into the charge transport and phonon scattering mechanisms. This study facilitates the exploration of more high-temperature thermoelectric materials. Ministry of Education (MOE) Accepted version The authors would like to acknowledge EFRC Solid-State-Thermal Energy Conversion Center (S3TEC), Grant DE-SC000XXXX. This work is also supported by Japan Society for the Promotion of Science (JSPS) KAKENHI, Grant JP 19F19057. L. H. acknowledge the International Research Fellow of JSPS. Q. F. Y. acknowledge the Chinese Scholarship Council (CSC) for the scholarship in Tokyo Institute of Technology. A. Q. Yan acknowledges Singapore MOE Tier 2 under Grant MOE2018-T2-1- 010. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, under Contract No. DE-AC02-06CH11357. 2021-05-06T08:35:10Z 2021-05-06T08:35:10Z 2020 Journal Article Qin, F., Nikolaev, S. A., Suwardi, A., Wood, M., Zhu, Y., Tan, X., Aydemir, U., Ren, Y., Yan, Q., Hu, L. & Snyder, G. J. (2020). Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides. Chemistry of Materials, 32(23), 10130-10139. https://dx.doi.org/10.1021/acs.chemmater.0c03581 1520-5002 https://hdl.handle.net/10356/148336 10.1021/acs.chemmater.0c03581 23 32 10130 10139 en Chemistry of Materials This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.chemmater.0c03581 application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering
Engineering::Materials
Phonons
Crystal Structure
spellingShingle Engineering
Engineering::Materials
Phonons
Crystal Structure
Qin, Feiyu
Nikolaev, Sergey A.
Suwardi, Ady
Wood, Maxwell
Zhu, Yingcai
Tan, Xianyi
Aydemir, Umut
Ren, Yang
Yan, Qingyu
Hu, Lei
Snyder, G. Jeffrey
Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides
description Thermoelectric materials enable the mutual energy conversion of waste heat and electricity, critical to relieve global energy crisis. Hightemperature thermoelectric materials are special species due to their high-temperature stability and noticeable energy conversion efficiency. Here, we report a systematic investigation on high-temperature thermoelectric gadolinium selenides, cubic Gd3-xSe4 (x = 0.16, 0.21 and 0.25) and orthorhombic Gd2Se3-y (y = 0.02, 0.06 and 0.08). High energy synchrotron x-ray diffraction and total scattering are used to investigate the crystallographic and local structures. The atomic-scale cluster of Gd vacancy in cubic Gd2.84Se4 is observed by employing the reverse Monte Carlo simulation. For cubic Gd3-xSe4, its carrier concentration is tuned and multiple conduction bands are incorporated by adjusting Gd vacancy. Experimentally, the gradual increase in effective masses is evidently observed in cubic Gd3-xSe4, which is consistent with the density functional theory (DFT) calculation. A reasonable peak zT value of 0.27 is achieved at 850 K for Gd2.84Se4. On the other hand, adjusting Se vacancy enables the optimization of electron concentration for orthorhombic Gd2Se3-y phase. Its low deformation potential (Ξ = 12eV) with single conduction band gives rise to enhanced electron mobility and higher peak zT value of 0.54 at 850 K for Gd2Se2.98. In addition, a higher zT of 1.2 at1200 K is reasonably predicted for Gd2Se2.98 by using quality factor analysis. This work not just presents a systematic crystallographic investigation of gadolinium selenides, but also provides a deep insight into the charge transport and phonon scattering mechanisms. This study facilitates the exploration of more high-temperature thermoelectric materials.
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Qin, Feiyu
Nikolaev, Sergey A.
Suwardi, Ady
Wood, Maxwell
Zhu, Yingcai
Tan, Xianyi
Aydemir, Umut
Ren, Yang
Yan, Qingyu
Hu, Lei
Snyder, G. Jeffrey
format Article
author Qin, Feiyu
Nikolaev, Sergey A.
Suwardi, Ady
Wood, Maxwell
Zhu, Yingcai
Tan, Xianyi
Aydemir, Umut
Ren, Yang
Yan, Qingyu
Hu, Lei
Snyder, G. Jeffrey
author_sort Qin, Feiyu
title Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides
title_short Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides
title_full Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides
title_fullStr Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides
title_full_unstemmed Crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides
title_sort crystal structure and atomic vacancy optimized thermoelectric properties in gadolinium selenides
publishDate 2021
url https://hdl.handle.net/10356/148336
_version_ 1772825490911920128