An in situ eutectic remelting and oxide replacement reaction for superior thermoelectric performance of InSb

In this work, we demonstrate a synergistic approach to improve the thermoelectric performance of the InSb compound by introducing a replacement reaction of InSb and TiO2 during a hot pressing process. As a consequence of the replacement reaction, TiIn+ point defects, In2O3, stacking faults and InSb–Sb eutectic structures have been introduced into the InSb matrix. Accordingly, the electrical conductivity and the power factor (PF) have been significantly improved due to the electron donating nature of TiIn+ point defects, and the thermal conductivity has also been greatly reduced owing to the extra phonon scattering by dispersed In2O3 nanoparticles and stacking faults. More importantly, the melt of the introduced InSb–Sb eutectic structures plays an important role in filtering the transverse acoustic phonons, causing an abrupt reduction of lattice thermal conductivity at high temperature (753–773 K). Therefore, a relatively high ZT value ∼1.1 at 773 K has been obtained for the 0.1 wt% TiO2 added InSb sample. Moreover, the Vickers hardness of InSb also increases largely (∼210 Hv) deriving from the strengthening effects by introduced point defects and nanoinclusions, which is tougher than many well established mid-temperature TE materials.

[1]  Yue Chen,et al.  3D charge and 2D phonon transports leading to high out-of-plane ZT in n-type SnSe crystals , 2018, Science.

[2]  M. Kanatzidis,et al.  n‐Type SnSe2 Oriented‐Nanoplate‐Based Pellets for High Thermoelectric Performance , 2018 .

[3]  Li-dong Zhao,et al.  Promising Thermoelectric Bulk Materials with 2D Structures , 2017, Advanced materials.

[4]  Junyou Yang,et al.  Synergistic effect by Na doping and S substitution for high thermoelectric performance of p-type MnTe , 2017 .

[5]  Dongsheng He,et al.  New insight into InSb-based thermoelectric materials: from a divorced eutectic design to a remarkably high thermoelectric performance , 2017 .

[6]  Zhiwei Chen,et al.  Electronic origin of the high thermoelectric performance of GeTe among the p-type group IV monotellurides , 2017 .

[7]  Gangjian Tan,et al.  Rationally Designing High-Performance Bulk Thermoelectric Materials. , 2016, Chemical reviews.

[8]  Zhiwei Chen,et al.  Thermoelectric Properties of Cu2SnSe4 with Intrinsic Vacancy , 2016 .

[9]  S. Dou,et al.  Thermoelectric Enhancement of Different Kinds of Metal Chalcogenides , 2016 .

[10]  M. Kanatzidis,et al.  Optimization of the Electronic Band Structure and the Lattice Thermal Conductivity of Solid Solutions According to Simple Calculations: A Canonical Example of the Mg2Si1–x–yGexSny Ternary Solid Solution , 2016 .

[11]  Wenqing Zhang,et al.  Low Sound Velocity Contributing to the High Thermoelectric Performance of Ag8SnSe6 , 2016, Advanced science.

[12]  B. Vishal,et al.  The origin of low thermal conductivity in Sn1−xSbxTe: phonon scattering via layered intergrowth nanostructures , 2016 .

[13]  Zhiwei Zhou,et al.  Progressive Regulation of Electrical and Thermal Transport Properties to High‐Performance CuInTe2 Thermoelectric Materials , 2016 .

[14]  Di Wu,et al.  Low-cost, abundant binary sulfides as promising thermoelectric materials , 2016 .

[15]  J. Zou,et al.  Planar Vacancies in Sn1-xBixTe Nanoribbons. , 2016, ACS nano.

[16]  Lei Yang,et al.  n-Type Bi2Te3-xSex Nanoplates with Enhanced Thermoelectric Efficiency Driven by Wide-Frequency Phonon Scatterings and Synergistic Carrier Scatterings. , 2016, ACS nano.

[17]  Junyou Yang,et al.  Ternary CuSbSe2 chalcostibite: facile synthesis, electronic-structure and thermoelectric performance enhancement , 2016 .

[18]  J. Zou,et al.  BixSb2−xTe3 nanoplates with enhanced thermoelectric performance due to sufficiently decoupled electronic transport properties and strong wide-frequency phonon scatterings , 2016 .

[19]  Heng Wang,et al.  Ultrahigh power factor and thermoelectric performance in hole-doped single-crystal SnSe , 2016, Science.

[20]  Marco Buongiorno Nardelli,et al.  Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites. , 2015, Nature materials.

[21]  D. Negi,et al.  High Thermoelectric Performance and Enhanced Mechanical Stability of p-type Ge1–xSbxTe , 2015 .

[22]  Xiaoguang Li,et al.  Enhancement of thermoelectric performance of β-Zn4Sb3 through resonant distortion of electronic density of states doped with Gd , 2015 .

[23]  G. J. Snyder,et al.  High thermoelectric and mechanical performance in highly dense Cu2−xS bulks prepared by a melt-solidification technique , 2015 .

[24]  G. J. Snyder,et al.  Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics , 2015, Science.

[25]  Gang Chen,et al.  Enhancement of thermoelectric performance in n-type PbTe 1−y Se y by doping Cr and tuning Te:Se ratio , 2015 .

[26]  Vladan Stevanović,et al.  Material descriptors for predicting thermoelectric performance , 2015 .

[27]  Xianli Su,et al.  Mechanically Robust BiSbTe Alloys with Superior Thermoelectric Performance: A Case Study of Stable Hierarchical Nanostructured Thermoelectric Materials , 2015 .

[28]  W. Fei,et al.  Enhancement of thermoelectric properties by Na doping in Te-free p-type AgSbSe2. , 2015, Dalton transactions.

[29]  G. J. Snyder,et al.  Optimum Carrier Concentration in n‐Type PbTe Thermoelectrics , 2014 .

[30]  G. J. Snyder,et al.  Thermoelectric transport in Cu7PSe6 with high copper ionic mobility. , 2014, Journal of the American Chemical Society.

[31]  M. Kanatzidis,et al.  Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals , 2014, Nature.

[32]  M. Caplan,et al.  Analytical model for the effects of wetting on thermal boundary conductance across solid/classical liquid interfaces , 2014 .

[33]  G. J. Snyder,et al.  T-Shaped Bi2Te3–Te Heteronanojunctions: Epitaxial Growth, Structural Modeling, and Thermoelectric Properties , 2013 .

[34]  G. J. Snyder,et al.  Copper ion liquid-like thermoelectrics. , 2012, Nature materials.

[35]  P. Cui,et al.  Enhanced thermoelectric performance in In(1-x)Ga(x)Sb originating from the scattering of point defects and nanoinclusion , 2011 .

[36]  D. Hurle A thermodynamic analysis of native point defect and dopant solubilities in zinc-blende III–V semiconductors , 2010 .

[37]  X. Su,et al.  Synthesis and thermoelectric properties of p-type Zn-doped ZnxIn1−xSb compounds , 2010 .

[38]  Eric S. Toberer,et al.  Characterization and analysis of thermoelectric transport in n-type Ba_(8)Ga_(16−x)Ge_(30+x) , 2009 .

[39]  Min Zhou,et al.  Thermoelectric and mechanical properties of nano-SiC-dispersed Bi2Te3 fabricated by mechanical alloying and spark plasma sintering , 2008 .

[40]  Z. Dashevsky,et al.  Mechanical properties of PbTe-based thermoelectric semiconductors , 2008 .

[41]  A. Yamamoto,et al.  Thermoelectric properties and figure of merit of a Te-doped InSb bulk single crystal , 2005 .

[42]  Donald T. Morelli,et al.  Estimation of the isotope effect on the lattice thermal conductivity of group IV and group III-V semiconductors , 2002 .

[43]  Eugene E. Haller,et al.  Thermal conductivity of germanium crystals with different isotopic compositions , 1997 .

[44]  R. Roy,et al.  Micro-indentation hardness variation as a function of composition for polycrystalline solutions in the systems PbS/PbTe, PbSe/PbTe, and PbS/PbSe , 1969 .

[45]  R. Bowers,et al.  InAs and InSb as Thermoelectric Materials , 1959 .

[46]  J. Callaway Model for Lattice Thermal Conductivity at Low Temperatures , 1959 .

[47]  Zhiwei Zhou,et al.  Enhancement of thermoelectric properties of Yb-filled skutterudites by an Ni-Induced “core–shell” structure , 2015 .

[48]  Liangwei Fu,et al.  Enhancement of the Thermoelectric Performance of Polycrystalline In4Se2.5 by Copper Intercalation and Bromine Substitution , 2014 .