The effect of Mg3As2alloying on the thermoelectric properties of n-type Mg3(Sb, Bi)2

Kazuki Imasato; Shashwat Anand; Ramya Gurunathan; G. Jeffrey Snyder

doi:10.1039/d1dt01600h

The effect of Mg₃As₂alloying on the thermoelectric properties of n-type Mg₃(Sb, Bi)₂

Kazuki Imasato^*, Shashwat Anand, Ramya Gurunathan, G. Jeffrey Snyder

^*Corresponding author for this work

Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

Mg₃Sb₂-Mg₃Bi₂alloys have been heavily studied as a competitive alternative to the state-of-the-art n-type Bi₂(Te,Se)₃thermoelectric alloys. Using Mg₃As₂alloying, we examine another dimension of exploration in Mg₃Sb₂-Mg₃Bi₂alloys and the possibility of further improvement of thermoelectric performance was investigated. While the crystal structure of pure Mg₃As₂is different from Mg₃Sb₂and Mg₃Bi₂, at least 15% arsenic solubility on the anion site (Mg₃((Sb_0.5Bi_0.5)_1−xAs_x)₂:x= 0.15) was confirmed. Density functional theory calculations showed the possibility of band convergence by alloying Mg₃Sb₂-Mg₃Bi₂with Mg₃As₂. Because of only a small detrimental effect on the charge carrier mobility compared to cation site substitution, the As 5% alloyed sample showedzT= 0.6-1.0 from 350 K to 600 K. This study shows that there is an even larger composition space to examine for the optimization of material properties by considering arsenic introduction into the Mg₃Sb₂-Mg₃Bi₂system.

Original language	English (US)
Pages (from-to)	9376-9382
Number of pages	7
Journal	Dalton Transactions
Volume	50
Issue number	27
DOIs	https://doi.org/10.1039/d1dt01600h
State	Published - Jul 21 2021

Funding

GJS, KI acknowledge the support of award 70NANB19H005 from U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD). The IMSERC X-ray Facility at Northwestern University is supported by the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the State of Illinois and International Institute for Nanotechnology (IIN). KI was partially supported by a Cluster Fellowship from the Institute for Sustainability and Energy at Northwestern (ISEN). SA acknowledges support from the ?Designing Materials to Revolutionize and Engineer our Future? program of the National Science Foundation under Award No. 1729487. GJS, KI acknowledge the support of award 70NANB19H005 from U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD). The IMSERC X-ray Facility at Northwestern University is supported by the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the State of Illinois and International Institute for Nanotechnology (IIN). KI was partially supported by a Cluster Fellowship from the Institute for Sustainability and Energy at Northwestern (ISEN). SA acknowledges support from the \u201CDesigning Materials to Revolutionize and Engineer our Future\u201D program of the National Science Foundation under Award No. 1729487.

ASJC Scopus subject areas

Inorganic Chemistry

Access to Document

10.1039/d1dt01600h

Cite this

@article{c8628ef82cfb486c804dfa3175cdbef9,

title = "The effect of Mg3As2alloying on the thermoelectric properties of n-type Mg3(Sb, Bi)2",

abstract = "Mg3Sb2-Mg3Bi2alloys have been heavily studied as a competitive alternative to the state-of-the-art n-type Bi2(Te,Se)3thermoelectric alloys. Using Mg3As2alloying, we examine another dimension of exploration in Mg3Sb2-Mg3Bi2alloys and the possibility of further improvement of thermoelectric performance was investigated. While the crystal structure of pure Mg3As2is different from Mg3Sb2and Mg3Bi2, at least 15% arsenic solubility on the anion site (Mg3((Sb0.5Bi0.5)1−xAsx)2:x= 0.15) was confirmed. Density functional theory calculations showed the possibility of band convergence by alloying Mg3Sb2-Mg3Bi2with Mg3As2. Because of only a small detrimental effect on the charge carrier mobility compared to cation site substitution, the As 5% alloyed sample showedzT= 0.6-1.0 from 350 K to 600 K. This study shows that there is an even larger composition space to examine for the optimization of material properties by considering arsenic introduction into the Mg3Sb2-Mg3Bi2system.",

author = "Kazuki Imasato and Shashwat Anand and Ramya Gurunathan and Snyder, {G. Jeffrey}",

note = "Publisher Copyright: {\textcopyright} The Royal Society of Chemistry 2021.",

year = "2021",

month = jul,

day = "21",

doi = "10.1039/d1dt01600h",

language = "English (US)",

volume = "50",

pages = "9376--9382",

journal = "Dalton Transactions",

issn = "1477-9226",

publisher = "Royal Society of Chemistry",

number = "27",

}

TY - JOUR

T1 - The effect of Mg3As2alloying on the thermoelectric properties of n-type Mg3(Sb, Bi)2

AU - Imasato, Kazuki

AU - Anand, Shashwat

AU - Gurunathan, Ramya

AU - Snyder, G. Jeffrey

PY - 2021/7/21

Y1 - 2021/7/21

N2 - Mg3Sb2-Mg3Bi2alloys have been heavily studied as a competitive alternative to the state-of-the-art n-type Bi2(Te,Se)3thermoelectric alloys. Using Mg3As2alloying, we examine another dimension of exploration in Mg3Sb2-Mg3Bi2alloys and the possibility of further improvement of thermoelectric performance was investigated. While the crystal structure of pure Mg3As2is different from Mg3Sb2and Mg3Bi2, at least 15% arsenic solubility on the anion site (Mg3((Sb0.5Bi0.5)1−xAsx)2:x= 0.15) was confirmed. Density functional theory calculations showed the possibility of band convergence by alloying Mg3Sb2-Mg3Bi2with Mg3As2. Because of only a small detrimental effect on the charge carrier mobility compared to cation site substitution, the As 5% alloyed sample showedzT= 0.6-1.0 from 350 K to 600 K. This study shows that there is an even larger composition space to examine for the optimization of material properties by considering arsenic introduction into the Mg3Sb2-Mg3Bi2system.

AB - Mg3Sb2-Mg3Bi2alloys have been heavily studied as a competitive alternative to the state-of-the-art n-type Bi2(Te,Se)3thermoelectric alloys. Using Mg3As2alloying, we examine another dimension of exploration in Mg3Sb2-Mg3Bi2alloys and the possibility of further improvement of thermoelectric performance was investigated. While the crystal structure of pure Mg3As2is different from Mg3Sb2and Mg3Bi2, at least 15% arsenic solubility on the anion site (Mg3((Sb0.5Bi0.5)1−xAsx)2:x= 0.15) was confirmed. Density functional theory calculations showed the possibility of band convergence by alloying Mg3Sb2-Mg3Bi2with Mg3As2. Because of only a small detrimental effect on the charge carrier mobility compared to cation site substitution, the As 5% alloyed sample showedzT= 0.6-1.0 from 350 K to 600 K. This study shows that there is an even larger composition space to examine for the optimization of material properties by considering arsenic introduction into the Mg3Sb2-Mg3Bi2system.

UR - http://www.scopus.com/inward/record.url?scp=85110004689&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85110004689&partnerID=8YFLogxK

U2 - 10.1039/d1dt01600h

DO - 10.1039/d1dt01600h

M3 - Article

C2 - 34190299

AN - SCOPUS:85110004689

SN - 1477-9226

VL - 50

SP - 9376

EP - 9382

JO - Dalton Transactions

JF - Dalton Transactions

IS - 27

ER -