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Title: Constructing Highly Porous Thermoelectric Monoliths with High-Performance and Improved Portability from Solution-Synthesized Shape-Controlled Nanocrystals

Journal Article · · Nano Letters
 [1]; ORCiD logo [2];  [3];  [2]; ORCiD logo [3]
  1. Nanjing University of Science and Technology (China); Iowa State Univ., Ames, IA (United States)
  2. Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Iowa State Univ., Ames, IA (United States)

Thermoelectricity offers a viable and reliable solution to convert waste heat into electricity. To enhance the performance and portability of thermoelectric materials, the crystal grain and pore structure should be simultaneously manipulated to achieve high electrical conductivity (σ), low thermal conductivity (κ), high figure of merit (zT), and low relative density. However, they cannot be synchronously realized using nanocrystals with uncontrolled domain size and shape as building blocks. Here, we employ solution-synthesized PbS nanocrystals with large grain size, controllable shape and tunable spatial packing to realize the aforementioned structural tuning. In this work, the as-sintered highly porous and well crystalline monolith exhibits high σ, low κ, high zT (1.06 at 838 K) and low relative density (82%). The phonon transport is studied by density functional theory highlighting the crucial role of phonon–pore scattering in reducing κ to enhance zT. Our strategy may benefit thermoelectrics and shed light on other technical fields such as catalysis, gas sensing, photovoltaics, and so forth.

Research Organization:
Vanderbilt Univ., Nashville, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC)
DOE Contract Number:
FG02-09ER46554; AC02-05CH11231
OSTI ID:
1597890
Journal Information:
Nano Letters, Vol. 18, Issue 6; ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

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