Improvement of Low‐Temperature zT in a Mg3Sb2–Mg3Bi2 Solid Solution via Mg‐Vapor Annealing

Materials with high zT over a wide temperature range are essential for thermoelectric applications. n‐Type Mg3Sb2‐based compounds have been shown to achieve high zT at 700 K, but their performance at low temperatures (30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric mate...

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Veröffentlicht in:	Advanced materials (Weinheim) 2019-08, Vol.31 (35), p.n/a
Hauptverfasser:	Wood, Maxwell, Kuo, Jimmy Jiahong, Imasato, Kazuki, Snyder, Gerald Jeffrey
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Sprache:	eng
Schlagworte:	Annealing Bismuth tellurides Carrier density Electrical resistivity Electron mobility Grain boundaries Grain size Hall effect ionized impurities Low temperature Materials science Mg3Sb2 Optimization Solid solutions Temperature Thermoelectric materials thermoelectrics vapor annealing
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creator	Wood, Maxwell Kuo, Jimmy Jiahong Imasato, Kazuki Snyder, Gerald Jeffrey
description	Materials with high zT over a wide temperature range are essential for thermoelectric applications. n‐Type Mg3Sb2‐based compounds have been shown to achieve high zT at 700 K, but their performance at low temperatures (30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric materials used at room temperature (n‐type Bi2Te3) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale. By developing a novel annealing technique in Mg vapor, the high‐resistance grain boundaries of Mg3Sb1.49Bi0.5Te0.01 can be effectively eliminated. This increases the room‐temperature thermoelectric figure of merit, zT, from 0.3 to 0.8, making it the first real competitor to state‐of‐the‐art Bi2Te3‐based n‐type thermoelectric materials.
doi_str_mv	10.1002/adma.201902337
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Syntheses and optimization processes to mitigate this grain‐boundary effect has been limited due to loss of Mg, which hinders a sample's n‐type dopability. A Mg‐vapor anneal processing step that grows a sample's grain size and preserves its n‐type carrier concentration during annealing is demonstrated. The electrical conductivity and mobility of the samples with large grain size follows a phonon‐scattering‐dominated T−3/2 trend over a large temperature range, further supporting the conclusion that the temperature‐activated mobility in Mg3Sb2‐based materials is caused by resistive grain boundaries. The measured Hall mobility of electrons reaches 170 cm2 V−1 s−1 in annealed 800 °C sintered Mg3 + δSb1.49Bi0.5Te0.01, the highest ever reported for Mg3Sb2‐based thermoelectric materials. In particular, a sample with grain size >30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric materials used at room temperature (n‐type Bi2Te3) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale. By developing a novel annealing technique in Mg vapor, the high‐resistance grain boundaries of Mg3Sb1.49Bi0.5Te0.01 can be effectively eliminated. This increases the room‐temperature thermoelectric figure of merit, zT, from 0.3 to 0.8, making it the first real competitor to state‐of‐the‐art Bi2Te3‐based n‐type thermoelectric materials.</description><identifier>ISSN: 0935-9648</identifier><identifier>EISSN: 1521-4095</identifier><identifier>DOI: 10.1002/adma.201902337</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Annealing ; Bismuth tellurides ; Carrier density ; Electrical resistivity ; Electron mobility ; Grain boundaries ; Grain size ; Hall effect ; ionized impurities ; Low temperature ; Materials science ; Mg3Sb2 ; Optimization ; Solid solutions ; Temperature ; Thermoelectric materials ; thermoelectrics ; vapor annealing</subject><ispartof>Advanced materials (Weinheim), 2019-08, Vol.31 (35), p.n/a</ispartof><rights>2019 WILEY‐VCH Verlag GmbH & Co. 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Syntheses and optimization processes to mitigate this grain‐boundary effect has been limited due to loss of Mg, which hinders a sample's n‐type dopability. A Mg‐vapor anneal processing step that grows a sample's grain size and preserves its n‐type carrier concentration during annealing is demonstrated. The electrical conductivity and mobility of the samples with large grain size follows a phonon‐scattering‐dominated T−3/2 trend over a large temperature range, further supporting the conclusion that the temperature‐activated mobility in Mg3Sb2‐based materials is caused by resistive grain boundaries. The measured Hall mobility of electrons reaches 170 cm2 V−1 s−1 in annealed 800 °C sintered Mg3 + δSb1.49Bi0.5Te0.01, the highest ever reported for Mg3Sb2‐based thermoelectric materials. In particular, a sample with grain size >30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric materials used at room temperature (n‐type Bi2Te3) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale. By developing a novel annealing technique in Mg vapor, the high‐resistance grain boundaries of Mg3Sb1.49Bi0.5Te0.01 can be effectively eliminated. 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Syntheses and optimization processes to mitigate this grain‐boundary effect has been limited due to loss of Mg, which hinders a sample's n‐type dopability. A Mg‐vapor anneal processing step that grows a sample's grain size and preserves its n‐type carrier concentration during annealing is demonstrated. The electrical conductivity and mobility of the samples with large grain size follows a phonon‐scattering‐dominated T−3/2 trend over a large temperature range, further supporting the conclusion that the temperature‐activated mobility in Mg3Sb2‐based materials is caused by resistive grain boundaries. The measured Hall mobility of electrons reaches 170 cm2 V−1 s−1 in annealed 800 °C sintered Mg3 + δSb1.49Bi0.5Te0.01, the highest ever reported for Mg3Sb2‐based thermoelectric materials. In particular, a sample with grain size >30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric materials used at room temperature (n‐type Bi2Te3) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale. By developing a novel annealing technique in Mg vapor, the high‐resistance grain boundaries of Mg3Sb1.49Bi0.5Te0.01 can be effectively eliminated. This increases the room‐temperature thermoelectric figure of merit, zT, from 0.3 to 0.8, making it the first real competitor to state‐of‐the‐art Bi2Te3‐based n‐type thermoelectric materials.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/adma.201902337</doi><tpages>5</tpages><orcidid>https://orcid.org/0000-0003-2758-6155</orcidid><orcidid>https://orcid.org/0000-0002-3434-1984</orcidid><orcidid>https://orcid.org/0000-0001-7294-1780</orcidid><orcidid>https://orcid.org/0000-0003-1414-8682</orcidid></addata></record>
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subjects	Annealing Bismuth tellurides Carrier density Electrical resistivity Electron mobility Grain boundaries Grain size Hall effect ionized impurities Low temperature Materials science Mg3Sb2 Optimization Solid solutions Temperature Thermoelectric materials thermoelectrics vapor annealing
title	Improvement of Low‐Temperature zT in a Mg3Sb2–Mg3Bi2 Solid Solution via Mg‐Vapor Annealing
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