Conducting grain boundaries enhancing thermoelectric performance in doped Mg2Si

The thermoelectric properties of Pb doped Mg2Si, synthesized using reactive sintering employing spark plasma sintering, are investigated and are compared with other dopants reported in literature. While a moderate decrease in Seebeck coefficient and thermal conductivity is observed for 2 at. % of Pb doping in Mg2Si, a substantial enhancement in the material's thermoelectric figure-of-merit is observed, which is due to an enormous increase in its electrical conductivity. A brick-layer model is proposed to explain these results, wherein the inter-granular electronic conductivity is facilitated by Pb (or Mg2Pb) phases at grain boundaries, which is supported by microstructural evidences.

[1]  F. Herman,et al.  Relativistic Energy-Band Structure ofMg2Pb , 1970 .

[2]  T. Iida,et al.  Thermoelectric Characteristics of a Commercialized Mg2Si Source Doped with Al, Bi, Ag, and Cu , 2010 .

[3]  Xiang Yang,et al.  Giant scattering parameter and enhanced thermoelectric properties originating from synergetic scattering of electrons in semiconductors with metal nanoinclusions , 2010 .

[4]  L. Heyne,et al.  Correlation between impedance, microstructure and composition of calcia-stabilized zirconia , 1976 .

[5]  Shaohua Xu,et al.  Thermal stability and elastic properties of Mg2X (X = Si, Ge, Sn, Pb) phases from first-principle calculations , 2012 .

[6]  A. Burggraaf,et al.  Grain boundary effects on ionic conductivity in ceramic GdxZr1–xO2–(x/2) solid solutions , 1981 .

[7]  N. Hamada,et al.  The thermoelectric properties of bulk crystalline n- and p-type Mg2Si prepared by the vertical Bridgman method , 2008 .

[8]  M. Bachmann,et al.  Ineffectiveness of energy filtering at grain boundaries for thermoelectric materials , 2012 .

[9]  Jun-ichi Tani,et al.  Thermoelectric properties of Bi-doped Mg2Si semiconductors , 2005 .

[10]  Wei Liu,et al.  Convergence of conduction bands as a means of enhancing thermoelectric performance of n-type Mg2Si(1-x)Sn(x) solid solutions. , 2012, Physical review letters.

[11]  Lei Wang,et al.  Preparation of Mg2Si1−xSnx by Induction Melting and Spark Plasma Sintering, and Thermoelectric Properties , 2010 .

[12]  N. Mott,et al.  Observation of Anderson Localization in an Electron Gas , 1969 .

[13]  B. Bouhafs,et al.  First‐principles calculations of the structural, electronic and optical properties of IIA–IV antifluorite compounds , 2005 .

[14]  X. Qin,et al.  Enhanced thermoelectric performance through energy-filtering effects in nanocomposites dispersed with metallic particles , 2012 .

[15]  J. Tani,et al.  Fabrication and thermoelectric properties of Mg2Si-based composites using reduction reaction with additives , 2013 .

[16]  J. Tani,et al.  Thermoelectric properties of Sb-doped Mg 2Si semiconductors , 2007 .

[17]  Gang Chen,et al.  Bulk nanostructured thermoelectric materials: current research and future prospects , 2009 .

[18]  E. A. Gurieva,et al.  Highly effective Mg 2 Si 1 − x Sn x thermoelectrics , 2006 .

[19]  H. Scherrer,et al.  Thermoelectric properties and electronic structure of p-type Mg2Si and Mg2Si0.6Ge0.4 compounds doped with Ga , 2011 .

[20]  Xinbing Zhao,et al.  High figures of merit and natural nanostructures in Mg2Si0.4Sn0.6 based thermoelectric materials , 2008 .

[21]  Il-ho Kim,et al.  Solid-State Synthesis of Te-Doped Mg2Si , 2011 .

[22]  M. Nygren,et al.  Enhanced thermoelectric properties of Mg2Si by addition of TiO2 nanoparticles , 2012 .

[23]  J. Tani,et al.  Thermoelectric properties of Al-doped Mg2Si1−xSnx (x ≦ 0.1) , 2008 .

[24]  M. Y. Au-Yang,et al.  Electronic Structure and Optical Properties of Mg 2 Si, Mg 2 Ge, and Mg 2 Sn , 1969 .

[25]  M. Umemoto,et al.  Thermoelectric Properties of Ca-Mg-Si Alloys , 2009 .

[26]  J. Mercure,et al.  Gross violation of the Wiedemann–Franz law in a quasi-one-dimensional conductor , 2011, Nature communications.

[27]  Z. A. Munir,et al.  Thermoelectric properties of Sc- and Y-doped Mg2Si prepared by field-activated and pressure-assisted reactive sintering , 2011 .

[28]  D. Lynch,et al.  Pressure Coefficient of the Band Gap in Mg2Si, Mg2Ge, and Mg2Sn , 1967, October 1.

[29]  J. E. Bauerle Study of solid electrolyte polarization by a complex admittance method , 1969 .