• Acta Physica Sinica
  • Vol. 68, Issue 11, 117201-1 (2019)
Guo-Cai Yuan1, Xi Chen2, Yu-Yang Huang2, Jun-Xi Mao1, Jin-Qiu Yu1, Xiao-Bo Lei1, and Qin-Yong Zhang1、2、*
Author Affiliations
  • 1School of Materials Science and Engineering, Xihua University, Chengdu 610039, China
  • 2Xihua Honor College, Xihua University, Chengdu 610039, China
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    DOI: 10.7498/aps.68.20190247 Cite this Article
    Guo-Cai Yuan, Xi Chen, Yu-Yang Huang, Jun-Xi Mao, Jin-Qiu Yu, Xiao-Bo Lei, Qin-Yong Zhang. Comparative study of thermoelectric properties of Mg2Si0.3Sn0.7 doped by Ag or Li [J]. Acta Physica Sinica, 2019, 68(11): 117201-1 Copy Citation Text show less

    Abstract

    In recent decades, Mg2(Si, Sn) solid solutions have long been considered as one of the most important classes of eco-friendly thermoelectric materials. The thermoelectric performance of Mg2(Si, Sn) solid solutions with outstanding characteristics of low-price, non-toxicity, earth-abundant and low-density has been widely studied. The n-type Mg2(Si, Sn) solid solutions have achieved the dimensionless thermoelectric figure of merit ZT ~1.4 through Bi/Sb doping and convergence of conduction bands. However, the thermoelectric performances for p-type Mg2(Si, Sn) solid solutions are mainly improved by optimizing the carrier concentration. In this work, the thermoelectric properties for p-type Mg2Si0.3Sn0.7 are investigated and compared with those for different p-type dopant Ag or Li. The homogeneous Mg2Si0.3Sn0.7 with Ag or Li doping is synthesized by two-step solid-state reaction method at temperatures of 873 K and 973 K for 24 h, respectively. The transport parameters and the thermoelectric properties are measured at temperatures ranging from room temperature to 773 K for Mg2(1–x)Ag2xSi0.3Sn0.7 (x = 0, 0.01, 0.02, 0.03, 0.04, 0.05) and Mg2(1–y)Li2ySi0.3Sn0.7 (y = 0, 0.02, 0.04, 0.06, 0.08) samples. The influences of different dopants on solid solubility, microstructure, carrier concentration, electrical properties and thermal transport are also investigated. The X-ray diffraction (XRD) patterns and scanning electron microscopy (SEM) images show that the solid solubility for Ag and for Li are x = 0.03 and y = 0.06, respectively. Based on the assumption of single parabolic band model, the value of effective mass ~1.2m0 of p-type Mg2(1–x)Ag2xSi0.3Sn0.7 and Mg2(1–y)Li2ySi0.3Sn0.7 are similar to that reported in the literature. The comparative results demonstrate that the maximum carrier concentration for Ag doping and for Li doping are 4.64×1019 cm–3 for x = 0.01 and 15.1×1019 cm–3 for y = 0.08 at room temperature, respectively; the Li element has higher solid solubility in Mg2(Si, Sn), which leads to higher carrier concentration and power factor PF ~1.62×10–3${\rm W}\cdot{\rm m^{–1}}\cdot{\rm K^{–2}}$ in Li doped samples; the higher carrier concentration of Li doped samples effectively suppresses the bipolar effect; the maximum of ZT ~0.54 for Mg1.92Li0.08Si0.3Sn0.7 is 58% higher than that of Mg1.9Ag0.1Si0.3Sn0.7 samples. The lattice thermal conductivity of Li or Ag doped sample decreases obviously due to the stronger mass and strain field fluctuations in phonon transport.
    $ S = \pm \frac{{{k_{\rm{B}}}}}{e}\left[ {\frac{{\left[ {\left( {r + 5/2} \right){F_{r + 3/2}}\left( \eta \right)} \right]}}{{\left[ {\left( {r + 3/2} \right){F_{r + 1/2}}\left( \eta \right)} \right]}} - \eta } \right], $ (1)

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    $ {F_i}\left( \eta \right) = \int_0^\infty {\frac{{{x^i}}}{{1 + {{\rm{e}}^{x - \eta }}}}{\rm{d}}x} , $ (2)

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    $ \eta = {E_{\rm{F}}}/\left( {{k_{\rm{B}}}T} \right), $ (3)

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    $ p = 4{\text{π}}{\left( {\frac{{2{m^*}{k_{\rm{B}}}T}}{{{h^2}}}} \right)^{3/2}}{F_{1/2}}\left( \eta \right), $ (4)

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    $ {\kappa _{\rm{L}}} + {\kappa _{{\rm{Bi}}}} = \kappa - L\sigma T, $ (5)

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    $\begin{split} L =& {\left( {\frac{{{k_{\rm{B}}}}}{e}} \right)^2} \bigg[\frac{{\left( {r + 7/2} \right){F_{r + 5/2}}\left( \eta \right)}}{{\left( {r + 3/2} \right){F_{r + 1/2}}\left( \eta \right)}} \\ & - {{\left[ {\frac{{\left( {r + 5/2} \right){F_{r + 3/2}}\left( \eta \right)}}{{\left( {r + 3/2} \right){F_{r + 1/2}}\left( \eta \right)}}} \right]}^2} \bigg], \end{split}$ (6)

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    $ \frac{{{\kappa _{\rm{L}}}}}{{\kappa _{\rm{L}}^P}} = \frac{{{\rm{ta}}{{\rm{n}}^{ - 1}}\left( u \right)}}{u}, $ (7)

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    $ {u^2} = \frac{{{{\text{π}} ^2}{\theta _{\rm{D}}}{{\varOmega }}}}{{h{v^2}}}\kappa _{\rm{L}}^P\varGamma , $ (8)

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    $ \varGamma = {\varGamma _{\rm{M}}} + {\varGamma _{\rm{S}}}, $ (9)

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    $ {\varGamma _{\rm{M}}} = \frac{{\displaystyle\mathop \sum \nolimits_{i = 1}^n {c_i}{{\left( {\frac{{{{\overline M}_i}}}{{\overline{\overline M} }}} \right)}^2}f_i^1f_i^2{{\left( {\frac{{M_i^1 - M_i^2}}{{{{\overline M}_i}}}} \right)}^2}}}{{\displaystyle\mathop \sum \nolimits_{i = 1}^n {c_i}}}, $ (10)

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    $ {\varGamma _S} = \frac{{\displaystyle\sum\nolimits_{i = 1}^n {{c_i}{{\left( {\frac{{\overline {{M_l}} }}{{\overline{\overline M} }}} \right)}^2}f_i^1f_i^2{\varepsilon _i}{{\left( {\frac{{r_i^1 - r_i^2}}{{{{\bar r}_i}}}} \right)}^2}} }}{{\left( {\displaystyle\sum\nolimits_{i = 1}^n {{c_i}} } \right)}}, $ (11)

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    $ {\overline M_i} = f_i^1M_i^1 + f_i^2M_i^2, $ (12)

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    $ {\overline r_i} = f_i^1r_i^1 + f_i^2r_i^2, $ (13)

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    $ \overline{\overline M} = \frac{{\displaystyle\mathop \sum \nolimits_{i = 1}^n {c_i}{{\overline M}_i}}}{{\left( {\displaystyle\mathop \sum \nolimits_{i = 1}^n {c_i}} \right)}}, $ (14)

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    Guo-Cai Yuan, Xi Chen, Yu-Yang Huang, Jun-Xi Mao, Jin-Qiu Yu, Xiao-Bo Lei, Qin-Yong Zhang. Comparative study of thermoelectric properties of Mg2Si0.3Sn0.7 doped by Ag or Li [J]. Acta Physica Sinica, 2019, 68(11): 117201-1
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