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Title: In situ neutron scattering study of nanoscale phase evolution in PbTe-PbS thermoelectric material

Abstract

Introducing nanostructural second phases has been proved to be an effective approach to reduce the lattice thermal conductivity and thus enhance the figure of merit for many thermoelectric materials. Furthermore studies of the formation and evolution of these second phases are central to understanding temperature dependent material behavior, improving thermal stabilities, as well as designing new materials. We examined powder samples of PbTe-PbS thermoelectric material using in situ neutron diffraction and small angle neutron scattering (SANS) techniques from room temperature to elevated temperature up to 663 K, to explore quantitative information on the structure, weight fraction, and size of the second phase. Neutron diffraction data showed the as-milled powder was primarily solid solution before heat treatment. During heating, PbS second phase precipitated out of the PbTe matrix around 480 K, while re-dissolution started around 570 K. The second phase remained separated from the matrix upon cooling. Furthermore, SANS data indicated there are two populations of nanostructures. The size of the smaller nanostructure increased from initially 5 nm to approximately 25 nm after annealing at 650 K, while the size of the larger nanostructure remained unchanged. Our study demonstrated that in situ neutron techniques are effective means to obtain quantitative informationmore » to study temperature dependent nanostructural behavior of thermoelectrics and likely other high-temperature materials.« less

Authors:
 [1]; ORCiD logo [2];  [3];  [1];  [2];  [3]; ORCiD logo [3]
  1. Temple Univ., Philadelphia, PA (United States). Dept. of Mechanical Engineering
  2. Michigan State Univ., East Lansing, MI (United States). Dept. of Chemical Engineering and Materials Science
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1327606
Alternate Identifier(s):
OSTI ID: 1306681
Grant/Contract Number:  
AC05-00OR22725; SC0001054
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 109; Journal Issue: 8; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Ren, Fei, Schmidt, Robert, Keum, Jong K., Qian, Bosen, Case, Eldon D., Littrell, Ken C., and An, Ke. In situ neutron scattering study of nanoscale phase evolution in PbTe-PbS thermoelectric material. United States: N. p., 2016. Web. doi:10.1063/1.4961677.
Ren, Fei, Schmidt, Robert, Keum, Jong K., Qian, Bosen, Case, Eldon D., Littrell, Ken C., & An, Ke. In situ neutron scattering study of nanoscale phase evolution in PbTe-PbS thermoelectric material. United States. https://doi.org/10.1063/1.4961677
Ren, Fei, Schmidt, Robert, Keum, Jong K., Qian, Bosen, Case, Eldon D., Littrell, Ken C., and An, Ke. 2016. "In situ neutron scattering study of nanoscale phase evolution in PbTe-PbS thermoelectric material". United States. https://doi.org/10.1063/1.4961677. https://www.osti.gov/servlets/purl/1327606.
@article{osti_1327606,
title = {In situ neutron scattering study of nanoscale phase evolution in PbTe-PbS thermoelectric material},
author = {Ren, Fei and Schmidt, Robert and Keum, Jong K. and Qian, Bosen and Case, Eldon D. and Littrell, Ken C. and An, Ke},
abstractNote = {Introducing nanostructural second phases has been proved to be an effective approach to reduce the lattice thermal conductivity and thus enhance the figure of merit for many thermoelectric materials. Furthermore studies of the formation and evolution of these second phases are central to understanding temperature dependent material behavior, improving thermal stabilities, as well as designing new materials. We examined powder samples of PbTe-PbS thermoelectric material using in situ neutron diffraction and small angle neutron scattering (SANS) techniques from room temperature to elevated temperature up to 663 K, to explore quantitative information on the structure, weight fraction, and size of the second phase. Neutron diffraction data showed the as-milled powder was primarily solid solution before heat treatment. During heating, PbS second phase precipitated out of the PbTe matrix around 480 K, while re-dissolution started around 570 K. The second phase remained separated from the matrix upon cooling. Furthermore, SANS data indicated there are two populations of nanostructures. The size of the smaller nanostructure increased from initially 5 nm to approximately 25 nm after annealing at 650 K, while the size of the larger nanostructure remained unchanged. Our study demonstrated that in situ neutron techniques are effective means to obtain quantitative information to study temperature dependent nanostructural behavior of thermoelectrics and likely other high-temperature materials.},
doi = {10.1063/1.4961677},
url = {https://www.osti.gov/biblio/1327606}, journal = {Applied Physics Letters},
issn = {0003-6951},
number = 8,
volume = 109,
place = {United States},
year = {Wed Aug 24 00:00:00 EDT 2016},
month = {Wed Aug 24 00:00:00 EDT 2016}
}

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Cited by: 8 works
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Works referenced in this record:

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Works referencing / citing this record:

Thermoelectric stability of Eu- and Na-substituted PbTe
journal, January 2018


RHEGAL: Resistive heating gas enclosure loadframe for in situ neutron scattering
journal, September 2018


A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory
journal, September 2018