期刊
CHEMISTRY OF MATERIALS
卷 23, 期 23, 页码 5256-5263出版社
AMER CHEMICAL SOC
DOI: 10.1021/cm202445d
关键词
Mg2(1+z)Si0.5-ySn0.5Sby; adjustment of the Mg content; point defects; thermoelectric properties
资金
- National Basic Research Program of China [2007CB607S01, 2007CB607503]
- Natural Science Foundation of China [50672118, 50731006, 51002112]
- 111 Project [B07040]
- Fundamental Research Funds for the Central Universities [2010-IV-046]
- International Science & Technology Cooperation Program of China [2011DFB60150]
- U.S. Department of Energy
- Marlow Industries, Inc.
Mg2Si1-xSnx compounds are low-cost and environmentally friendly thermoelectric materials expected to be applied as power generators in the intermediate temperature range. Optimization of the thermoelectric properties of Mg2Si1-xSnx compounds can be accomplished by the precise control and adjustment of the Mg content. A series of Mg2(1+z)Si0.5-ySn0.5Sby (0 <= y <= 0.015 and 0 <= z <= 0.15) compounds with controlled Mg content were synthesized by a two-step solid-state reaction method, followed by a spark plasma sintering technique. On the basis of optimized thermoelectric properties via doping with Sb, the effect of a variable content of Mg spanning from understoichiometry to overstoichiometry has been systematically explored. The results indicate that when the actual Mg content exceeds the stoichiometric amount, the dominant point defects in Mg2(1+z)Si0.49Sn0.5Sb0.01 compounds are interstitial Mg and Si/Sn vacancies. At the same time, the electron concentration is enhanced with increasing content of Mg. However, when the actual Mg content is substoichiometric, the point defects consist mainly of Mg vacancies that tend to counteract the doping effect of Sb. Thus, the electron concentration of the nominal Mg2Si0.49Sn0.5Sb0.01 compound (in reality a 2 mol % deficiency of Mg) is markedly lower compared with the Mg2.10Si0.49Sn0.5Sb0.01 compound, which actually had a 2 mol % excess of Mg. Furthermore, a modest overstoichiometry of Mg enhances the power factor and improves the dimensionless figure of merit. The highest value of ZT = 1.25 at 800 K among the compounds was obtained on Mg2.20Si0.49Sn0.5Sb0.01, which had an actual Mg excess of 5.5 mol %. The study suggests that point defects, such as interstitial Mg and Si/Sn vacancies, which are created by an overstoichiometric content of Mg, have a positive effect on the electron concentration and thermoelectric properties of n-type Mg2Si1-xSnx-based compounds. This research has also established an essential foundation for further optimization of the thermoelectric properties of Mg2Si1-xSnx compounds.
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